In Press

Articles in press have been peer-reviewed and accepted, which are not yet assigned to volumes/issues, but are citable by Digital Object Identifier (DOI).
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Interfacial regulation for zinc metal anode of aqueous zinc-ion battery
Jing Zhu, Xumeng Ge, Zhi Peng, Liang Pan, Ziyu Peng, Yingqiao Jiang, Wei Meng, Zekun Zhang, Ningning Zhao, Bin Li, Lei Dai, Ling Wang, Zhangxing He
, Available online  , doi: 10.1016/j.gee.2024.11.001
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Aqueous zinc-ion batteries (AZIBs) have attracted significant attention due to their high energy density, low cost, high efficiency, and environmental friendliness. Nevertheless, the development of AZIBs has been significantly hindered by the unavoidable issues with zinc dendrites and the side reactions of the anode. The strategies for stable and controllable interfacial regulation have recently made rapid progress, due to their dual function of improving zinc ion transport dynamics and preventing direct contact of zinc with electrolytes. Therefore, it’s imperative to conduct a comprehensive summary of the interfacial regulation of zinc anodes and to engage in in-depth research into the underlying mechanisms. Subsequently, the interfacial regulation was classified based on battery structure, including anode coating strategy, electrolyte engineering, and separator optimization. Eventually, the current limitations of interfacial regulation and a deep outlook on AZIBs interface engineering are summarized.
Valorization of spent lithium-ion battery cathode materials for energy conversion reactions
Jin Zhang, Ding Chen, Jixiang Jiao, Weihao Zeng, Shichun Mu
, Available online  , doi: 10.1016/j.gee.2024.10.006
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With large-scale commercial applications of lithium-ion batteries (LIBs), lots of spent LIBs will be produced and cause huge waste of resources and greatly increased environmental problems. Thus, recycling spent LIB materials is inevitable. Due to high added-value features, converting spent LIB cathode materials into catalysts exhibits broad application prospects. Inspired by this, we review the high-added-value reutilization of spent LIB materials toward catalysts of energy conversion. First, the failure mechanism of spent LIB cathode materials are discussed, and then the transformation and modification strategies are summarized and analyzed to improve the transformation efficiency of failed cathode materials and the catalytic performance of catalysts, respectively. Moreover, the electrochemical applications of failed cathode material derived catalysts are introduced, and the key problems and countermeasures are analyzed and proposed. Finally, the future development trend and prospect of high-added-value reutilization for spent LIB cathode materials toward catalysts are also given. This review will predictably advance the awareness of valorizing spent lithium-ion battery cathode materials for catalysis.
Dual-bonded Polyethyleneimine Network with Electron-withdrawing Groups at α, β-sites for Ultra-stable and Low-energy CO2 Capture in Harsh Environments
Tong Zhou, Yunxia Wen, Zhinan Wu, Shuailong Song, Bohong Wu, Hongwei Guo, Huanhao Chen, Xin Feng, Liwen Mu, Xiaohua Lu, Tuo Ji, Jiahua Zhu
, Available online  , doi: 10.1016/j.gee.2024.10.005.
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As an innovative approach to addressing climate change, significant efforts have been dedicated to the development of amine sorbents for CO2 capture. However, the high energy requirements and limited lifespan of these sorbents, such as oxidative and water stability, pose significant challenges to their widespread commercial adoption. Moreover, the understanding of the relationship between adsorption energy and adsorption sites is not known. In this work, a dual-bond strategy was used to create novel secondary amine structures by a polyethyleneimine (PEI) network with electron-extracted (EE) amine sites at adjacent sites, thereby weakening the CO2 binding energy while maintaining the binding ability. In-situ FT-IR and DFT demonstrated the oxygen-containing functional groups adjacent to the amino group withdraw electrons from the N atom, thereby reducing the CO2 adsorption capacity of the secondary amine, resulting in lower regeneration energy consumption of 1.39 GJ·t-1-CO2. In addition, the EE sorbents demonstrated remarkable performance with retention of over 90% of their working capacity after 100 cycles, even under harsh conditions containing 10% O2 and 20% H2O. DFT calculations were employed to clarify for the first time the mechanism that the oxygen functional group at the α-site hinders the formation of the urea structure, thereby being an antioxidant. These findings highlight the promising potential of such sorbents for deployment in various CO2 emission scenarios, irrespective of environmental conditions.
Heterointerface of Nickel-ferric Hydroxide/Cobalt-phosphide-boride Boosting Hydrazine-assisted Water Electrolysis
Jiayi Wang, Shaojun Qing, Xili Tong, Ting Xiang, Guangnan Luo, Kun Zhang, Liangji Xu
, Available online  , doi: 10.1016/j.gee.2024.10.003
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Sustainable H2 production based on hydrogen evolution reaction (HER) and hydrazine oxidation reaction (HzOR) has attracted wide attention due to minimal energy consumption compared to overall water electrolysis. The present study focuses on the design and construction of heterostructured CoPB@NiFe-OH applied as efficient bifunctional catalysts to sustainable produce hydrogen and remove hydrazine in alkaline media. Impressively, CoPB@NiFe-OH heterointerface exhibits an HzOR potential of -135 mV at the current density of 10 mA cm-2 when the P to B atom ratio was 0.2, simultaneously an HER potential of -32 mV toward HER when the atom ratio of P and B was 0.5. Thus, hydrogen production without an outer voltage accompanied by a small current density output of 25 mA cm-2 is achieved, surpassing most reported catalysts. In addition, DFT calculations demonstrate the Co sites in CoPB upgrades H* adsorption, while the Ni sites in NiFe-OH optimizes the adsorption energy of N2H4* due to electron transfer from CoPB to NiFeOH at the heterointerface, ultimately leading to exceptional wonderful performance in hydrazine-assistant water electrolysis via HER coupled with HzOR.
Eco-friendly and facile nanomanufacturing of amorphous Co-Ce-Fe trimetallic molybdates composites for accelerated anodic oxygen evolution in alkaline water electrolysis: Evaluation of active sites performance
Jiejie Feng, Liling Wei, Huayi Li, Jianquan Shen
, Available online  , doi: 10.1016/j.gee.2024.09.012
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Currently, endeavors to scale up the production of amorphous catalysts are still impeded by intricate synthesis conditions. Here, we have prepared a series of metal-based molybdate via one-step coprecipitation method. After ingredient optimization, amorphous Co2CeFe2-MoO4 was identified as exhibiting the highest intrinsic activity among its counterparts. Modulation of electron structure enables Co2CeFe2-MoO4 to balance the adsorption behavior towards reactive intermediates. Ultimately, the obtained Co2CeFe2-MoO4 molybdate demonstrated a captivating OER performance, showcasing a low overpotential of 230 mV at 10 mA cm-2. Moreover, the alkaline electrolyzer employing the Co2CeFe2-MoO4 anode exhibited a low cell voltage of 1.50 V for water splitting and underwent an acceptable attenuation of 4.99% after 165 hours of continuous operation, demonstrating its favorable catalytic activity and durability. This work provides a facile and eco-friendly synthesis pathway for crafting cost-effective and durable earth-abundant OER electrocatalysts tailored for water splitting to produce clean hydrogen.
Coupling adsorption and in-situ Fenton-like oxidation by iron-containing low-grade attapulgite clay towards organic pollutant removal: From batch experiment to continuous operation
Chao Jiang, Xiaoli Liu, Xingpeng Wang, Qihui Wang, Huiyu Li, Weiliang Tian, Saeed Ahmed, Yongjun Feng
, Available online  , doi: 10.1016/j.gee.2024.10.004
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Coupling adsorption and in-situ Fenton-like oxidation process was developed for Methylene blue (MB) using refined iron-containing low-grade attapulgite (ATP) clay, and the removal mechanism was investigated. The MB was initially adsorbed on the porous ATPs, and then the enriched MB was removed by the H2O2-assisted Fenton-like oxidation with the iron-containing ATP catalyst. Under optimal conditions, the ATP powder exhibits the maximum removal efficiency of 100% with negligible iron leaching (1.5 mg L-1) and no sludge formation. Furthermore, polysulfone/ATP (PSF/ATP) pellets were fabricated through a water-induced phase separation process to construct a fixed-bed reactor (FBR) for continuous contaminant removal. For the first cycle, the maximum adsorption capacity was 15.5 L with an outlet MB concentration of 1.973 mg L-1 (< 2 mg L-1, GB4287-2012) using the PSF/ATP pellets containing 50.0 g of ATP powders, and the maximum Fenton-like oxidation capacity was 35.5 L with the outlet concentration of 0.831 mg L-1. After five cycles, the total treated volume of the MB solution was ca. 255 L, and the efficiency remained above 99%. After 10 hours of continuous treatment towards practical resin industrial wastewater, the chemical oxygen demand (COD) removal efficiency was still measured at 83.05%, costing 0.398 $ m-3. These results demonstrate the practical applicability of iron-containing low-grade ATP clay for textile water treatment.
CCUS: A Panacea or a Placebo in the Fight Against Climate Change?
Yuxin Zhao
, Available online  , doi: 10.1016/j.gee.2024.10.001
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Carbon Capture, Utilization, and Storage (CCUS) is a crucial technology for achieving carbon neutrality, but it faces significant challenges. Despite substantial investments and policy support, CCUS projects have underperformed due to technical difficulties, high costs, and controversies surrounding the fossil fuel industry's involvement. The effectiveness and feasibility of CCUS in reducing carbon emissions remain uncertain. This viewpoint provides a comprehensive analysis of the current state of CCUS technology, examining its potential to reduce carbon emissions, the challenges hindering its deployment, and the strategies needed to overcome these barriers. We discuss the need for a combinatorial approach to unlock CCUS's full potential, and also emphasize the importance of selecting optimal CO2 utilization pathways to maximize economic benefits and CO2 absorption. Although CCUS faces technical, economic, and social barriers, it can still play a valuable role in mitigating emissions from hard-to-abate sectors when supported by comprehensive strategies and collaborative efforts among governments, industries, and research institutions. By addressing these challenges and investing in innovation, CCUS can contribute to achieving carbon neutrality and building a sustainable, low-carbon future.
Solvent-free Synthesis of Highly Dispersed Zinc-doped Porous Carbons as Efficient Dibenzothiophene Adsorbents
Ping Lu, Zhenhua Sun, Xinrong Ke, Changshen Ye, Zhixian Huang, Ting Qiu
, Available online  , doi: 10.1016/j.gee.2024.09.010
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Designing efficient adsorbents for the deep removal of refractory dibenzothiophene (DBT) from fuel oil is vital for addressing environmental issues such as acid rain. Herein, zinc gluconate and urea-derived porous carbons SF-ZnNC-T (T represents the carbonization temperature) were synthesized without solvents. Through a temperature-controlled process of “melting the zinc gluconate and urea mixture, forming H-bonded polymers, and carbonizing the polymers,” the optimal carbon, SF-ZnNC-900, was obtained with a large surface area (2280 m2/g), highly dispersed Zn sites, and hierarchical pore structures. Consequently, SF-ZnNC-900 demonstrated significantly higher DBT adsorption capacity of 43.2 mg S/g, compared to just 4.3 mg S/g for the precursor. It also demonstrated good reusability, a fast adsorption rate, and the ability for ultra-deep desulfurization. The superior DBT adsorption performance resulted from the evaporation of residual zinc species, which generated abundant mesopores that facilitated DBT transformation, as well as the formation of Zn-N sites that strengthened the host-guest interaction (ΔE = -1.466 eV). The solvent-free synthesized highly dispersed Zn-doped carbon shows great potential for producing sulfur-free fuel oil and for designing metal-loaded carbon adsorbents.
Poly (lactic acid)/Poly (butylene adipate-co-terephthalate) Films with Simultaneous High Oxygen Barrier and Fast Degradation Properties
Mengjing Yang, Yuxi Mao, Penghui Zhang, Jie Li, Zeming Tong, Zhenguo Liu, Yanhui Chen
, Available online  , doi: 10.1016/j.gee.2024.09.011
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Although poly (lactic acid) (PLA) is a good environmentally-friendly bio-degradable polymer which is used to substitute traditional petrochemical-based polymer packaging films, the barrier properties of PLA films are still insufficient for high-barrier packaging applications. In this study, oxygen scavenger hydroxyl-terminated polybutadiene (HTPB) and cobalt salt catalyst were incorporated into the PLA/poly (butylene adipate-co-terephthalate) (PLA/PBAT), followed by melting extrusion and three-layer co-extrusion blown film process to prepare the composite films. The oxygen permeability coefficient of the composite film combined with 6 wt% oxygen scavenger and 0.4 wt% catalyst was decreased significantly from 377.00 cc·mil·m-2·day-1·0.1MPa-1 to 0.98 cc·mil·m-2·day-1·0.1MPa-1, showing a remarkable enhancement of 384.69 times compared with the PLA/PBAT composite film. Meanwhile, the degradation behavior of the composite film was also accelerated, exhibiting a mass loss of nearly 60% of the original mass after seven days of degradation in an alkaline environment, whereas PLA/PBAT composite film only showed a mass loss of 32%. This work has successfully prepared PLA/PBAT composite films with simultaneously improved oxygen barrier property and degradation behavior, which has great potential for high-demanding green chemistry packaging industries, including food, agricultural, and military packaging.
Fe-O-Bi efficient electron transfer channels and photo-Fenton synergy in S-scheme heterojunctions: insights into interfacial interactions and ofloxacin degradation
Jiawei Liu, Jun Shi, Huiping Deng
, Available online  , doi: 10.1016/j.gee.2024.09.008
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Fenton method combined with light to accelerate the production of free radicals from H2O2 can achieve more efficient pollutant degradation. In this paper, a novel BiOI/FeWO4 S-scheme heterojunction photocatalyst was obtained by in situ synthesis, which can activate H2O2 and degrade the organic pollutant OFC (ofloxacin) under visible light. The S-scheme charge transfer mechanism was confirmed by XPS spectroscopy, in situ KPFM and theoretical calculation. The photogenerated electrons were transferred from FeWO4 to BiOI driven by the built-in electric field and band bending, which inhibited carrier recombination and facilitated the activation of H2O2.The BiFe-5/Vis/H2O2 system degraded OFC up to 96.4% in 60 min. This study provides new systematic insights into the activation of H2O2 by S-scheme heterojunctions, which is of great significance for the treatment of antibiotic wastewater.
Lamellar COF Solid-state Electrolytes for Robust Ambient-temperature Lithium-ion transfer enhanced by PEI-driven Channel Alignment
Yafang Zhang, Xinji Zhang, Jiajia Huang, Zhirong Yang, Shiyue Zhou, Chenye Wang, Wenjia Wu, Jingtao Wang
, Available online  , doi: 10.1016/j.gee.2024.09.009
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Ionic covalent organic framework (COF) lamellar membranes are the alternative materials as promising Li+ conductors for all-solid-state lithium batteries. However, COF lamellar membrane suffers from poor structural stability and inevitable cross-layer transfer resistance due to the weak interaction at interface of adjacent nanosheets. Herein, a lamellar polymer-threaded ionic COF (PEI@TpPa-SO3Li) composite electrolyte with single Li+ conduction was prepared by assembling lithium sulfonated COF (TpPa-SO3Li) nanosheets and then threading them with polyethyleneimine (PEI) chains. It reveals that the threaded PEI chains induce the oriented permutation of pore channel of PEI@TpPa-SO3Li electrolyte through electrostatic interaction between -NH2/-NH- and -SO3Li groups. This enables the construction of continuous and aligned -SO3-...Li+...-NH2/-NH- pairs along pore channels, which act as efficient Li+ conducting sites and afford high Li+ hopping conduction (1.4×10-4 S cm-1 at 30 ℃) with a high Young's modulus of 408.7 MP and wide electrochemical stability window of 0~4.7 V. The assembled LiFePO4Li and LiNi0.8Mn0.1Co0.1O2Li half-cells achieve high discharge capacities of 155.0 mAh g-1 and 167.2 mAh g-1 at 30 ℃ under 0.2 C, respectively, with high capacity retention of 98% after 300 cycles. This study provides an alternative route to highly ion-conductive lamellar porous electrolytes for high-performance energy devices.
Study on the effect of controlled disproportionation pore-forming and relative vacuum mechanism on the reduction rate of continuous magnesium smelting process
Jing-zhong Xu, Ting-an Zhang, Yan Liu, Zhihe Dou, Yishan Liu, Baiao Feng, Hongxuan Liu
, Available online  , doi: 10.1016/j.gee.2024.09.006
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Compared with the vacuum continuous magnesium smelting process (RVCMS), its excellent energy saving and emission reduction performance provides a feasible method for green magnesium smelting. In the process of industrialization, the reduction rate of prefabricated pellets affects the yield of metal magnesium and the utilization of reducing slag. In this paper, the reduction mechanism under different carbonate structures is analyzed by controlled disproportionation of prefabricated pellets and micro-nano simulation. The results show that the low temperature decomposition of NH4·HCO3 pore-forming, improve the reduction rate (99.72 %) effect is remarkable. Combined with thermodynamics and relative vacuum mechanism, a theoretical model of the relationship between disproportionation pore-forming and reduction rate was established. It was concluded that the energy consumption required to produce per ton of magnesium by adding NH4·HCO3 to the prefabricated pellets was reduced by 0.29 ~ 0.34 tce, and the carbon emission was reduced by 1.069 ~ 1.263 t. The reduction slag had good compressive strength (Side 101.19 N/cm2, Bottom 466.4 N/cm2). Compared with the 20 MPa reduction slag sample without pore-forming agent, the side compressive strength increased by 51.66 %, and the bottom compressive strength increased by 119.10 %. The amount of single furnace filler is increased by more than 50 %.
Recent progress in carbon-based composite materials for advanced sodium ion batteries: from storage mechanism to structural design to applications as flexible electrodes
Ao Song, Yunchao Li, Dingkun Yuan, Jie Wu, Hailin Gu, Guangxue Zhang, Angjian Wu, Jiangrong Xu
, Available online  , doi: 10.1016/j.gee.2024.09.007
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Sodium ion batteries (SIBs) are one of the most prospective energy storage devices recently. Carbon materials have been commonly used as anode materials for SIBs because of their wide sources and low price. However, pure carbon materials still have the disadvantage of low theoretical capacity. New design and preparation strategies for carbon-based composites can overcome the problems. Based on the analysis of Na+ storage mechanism of carbon-based composite materials, the factors influencing the performance of SIBs are discussed. Adjustment methods for improving the electrochemical performance of electrodes are evaluated in detail, including carbon skeleton design and composite material selection. Some advanced composite materials, i.e., carbon-conversion composite and carbon-MXene composite, are also being explored. New advances in flexible electrodes based on carbon-based composite on flexible SIBs is investigated. The existing issues and future issues of carbon-based composite materials are discussed.
Cyclic Ethers-Based Solid Electrolyte Derived from In Situ Ring-Opening Polymerization Strategy
Wubin Du, Yong Wu, Hao Cheng, Ran Bu, Kang Shen, Yuanzhong Tan, Zhijun Wu, Hongge Pan, Yifan Wang, Yingying Lu
, Available online  , doi: 10.1016/j.gee.2024.09.005
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Although solid-state polymer electrolytes (SPEs) are expected to solve the safety hazards and limited energy density in the energy storage systems, they still encounter an inferior electrode/electrolyte interface when prepared via an ex situ manner. Recently, in situ polymerization of SPEs favors high interfacial infiltrability, improved interface contact, and reduced interface resistance, owing to the formation of a "super-conformal" interface between electrode and electrolyte. Especially, in situ strategies employing ring-opening polymerization (ROP) are emerging as a dazzling star, further enabling moderate polymerization conditions, controllable molecular structure, and reduced interfacial side reaction. As the main monomers which can be in situ polymerized via ROP strategy, cyclic ethers have been used to construct the CE-SPEs with many merits including good battery electrochemical performances and simple assembly process. Here, as a systematic summarization to the existing reports, this review focuses the polymerization mechanism of ROP, the design principles of CE-SPEs electrolytes, and recent application of in situ CE-SPEs. In particular, this review thoroughly discusses the selection of different cyclic monomers, initiators and various modification approaches in in situ fabricating CE-SPEs. Ending with offering the future challenges and perspectives, this review envisions shedding light on the profound understanding and scientific guidance for further development of high-performance in situ CE-SPEs.
Recent progress on photothermal nanomaterials: Design, mechanism, and applications
Xiao Yu, Shilin Fan, Bin Zhu, Soliman I. El-Hout, Jian Zhang, Chunlin Chen
, Available online  , doi: 10.1016/j.gee.2024.09.002
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Photothermal energy conversion represents a cornerstone process in the renewable energy technologies domain, enabling the capture of solar irradiance and its subsequent transformation into thermal energy. This mechanism is paramount across many applications, facilitating the exploitation of solar energy for different purposes. The photothermal conversion efficiency and applications are fundamentally contingent upon the characteristics and performance of the materials employed. Consequently, deploying high-caliber materials is essential for optimizing energy capture and utilization. Within this context, photothermal nanomaterials have emerged as pivotal components in various applications, ranging from catalysis and sterilization to medical therapy, desalination, and electric power generation via the photothermal conversion effect.
This review endeavors to encapsulate the current research landscape, delineating both the developmental trajectories and application horizons of photothermal conversion materials. It aims to furnish a detailed exposition of the mechanisms underlying photothermal conversion across various materials, shedding light on the principles guiding the design of photothermal nanomaterials. Furthermore, addressing the prevailing challenges and outlooks within the field elucidates potential avenues for future research and identifying priority areas. This review aspires to enrich the understanding of photothermal materials within the framework of energy conversion, offering novel insights and fostering a more profound comprehension of their role and potential in harnessing solar energy.
Sustainable Aviation Fuels from Biomass and Biowaste via Bio- and Chemo-Catalytic Conversion: Catalysis, Process Challenges, and Opportunities
Junyan Zhang, Matthew S. Webber, Yunqiao Pu, Zhenglong Li, Xianzhi Meng, Michael L. Stone, Bingqing Wei, Xueqi Wang, Sainan Yuan, Bruno Klein, Bhogeswararao Seemala, Charles E. Wyman, Karthikeyan K. Ramasamy, Mike Thorson, Matthew H. Langholtz, Joshua S. Heyne, Aibolat Koishybay, Shiba Adhikari, Sufeng Cao, Andrew Sutton, Gerald A. Tuskan, Yuriy Román-Leshkov, Arthur J. Ragauskas, Tao Ling, Brian H. Davison
, Available online  , doi: 10.1016/j.gee.2024.09.003
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Sustainable aviation fuel (SAF) production from biomass and biowaste streams is an attractive option for decarbonizing the aviation sector, one of the most-difficult-to-electrify transportation sectors. Despite ongoing commercialization efforts using ASTM-certified pathways (e.g., lipid conversion, Fischer-Tropsch synthesis), production capacities are still inadequate due to limited feedstock supply and high production costs. New conversion technologies that utilize lignocellulosic feedstocks are needed to meet these challenges and satisfy the rapidly growing market. Combining bio- and chemo-catalytic approaches can leverage advantages from both methods, i.e., high product selectivity via biological conversion, and the capability to build C-C chains more efficiently via chemical catalysis. Herein, conversion routes, catalysis, and processes for such pathways are discussed, while key challenges and meaningful R&D opportunities are identified to guide future research activities in the space. Bio- and chemo-catalytic conversion primarily utilize the carbohydrate fraction of lignocellulose, leaving lignin as a waste product. This makes lignin conversion to SAF critical in order to utilize whole biomass, thereby lowering overall production costs while maximizing carbon efficiencies. Thus, lignin valorization strategies are also reviewed herein with vital research areas identified, such as facile lignin depolymerization approaches, highly integrated conversion systems, novel process configurations, and catalysts for the selective cleavage of aryl C–O bonds. The potential efficiency improvements available via integrated conversion steps, such as combined biological and chemo-catalytic routes, along with the use of different parallel pathways, are identified as key to producing all components of a cost-effective, 100% SAF.
Recent advances on the electrocatalytic oxidation of biomass-derived aldehydes
Zhikeng Zheng, Ke Li, Lu Lin, Zhiwei Jiang, Yuchen Wang, Kai Yan
, Available online  , doi: 10.1016/j.gee.2024.09.004
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The escalating demand for sustainable and environmentally benign chemical processes has driven the exploration of biomass as an alternative to non-renewable resources. Electrocatalytic upgrading of biomass-derived aldehydes plays a crucial role in biomass refining, and has become a frontier of mainstream research. This paper reviews the recent advances on the electrocatalytic oxidation of typical biomass-derived aldehydes (5-hydroxymethylfurfural, furfural, glucose, xylose, vanillin and benzaldehyde, etc.). The research presented in this review covers a wide range of oxidation mechanisms for each aldehyde. It is evident from the current literature that challenges related to the comprehensiveness of mechanistic studies, catalyst stability, and reaction scalability remain, but the rapid progress offers hope for future advancements. Finally, we elucidate the challenges in this domain and provide the perspectives on future developments. This review corroborates the significance of investigating the electrocatalytic oxidation of biomass-derived aldehydes and emphasizes the need for continued research to refine these processes for industrial applications.
Construction of two-dimensional heterojunctions based on metal-free semiconductor materials and Covalent Organic Frameworks for exceptional solar energy catalysis
Haijun Hu, Daming Feng, Kailai Zhang, Hui Li, Hongge Pan, Hongwei Huang, Xiaodong Sun, Tianyi Ma
, Available online  , doi: 10.1016/j.gee.2024.09.001
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Covalent organic frameworks (COFs) are newly developed crystalline substances that are garnering growing interest because of their ultra-high porosity, crystalline nature, and easy modified architecture, showing promise in the field of photocatalysis. However, it is difficult for pure COFs materials to achieve excellent photocatalytic hydrogen production due to their severe carrier recombination problems. To mitigate this crucial issue, establishing heterojunction is deemed an effective approach. Nonetheless, many of the metal-containing materials that have been used to construct heterojunctions with COFs own a number of drawbacks, including small specific surface area and rare active sites (for inorganic semiconductor materials), wider bandgaps and higher preparation costs (for MOFs). Therefore, it is necessary to choose metal-free materials that are easy to prepare. Red phosphorus (RP), as a semiconductor material without metal components, with suitable bandgap, moderate redox potential, relatively minimal toxicity, is affordable and readily available. Herein, a range of RP/TpPa-1-COF (RP/TP1C) composites have been successfully prepared through solvothermal method. The two-dimensional structure of the two materials causes strong interactions between the materials, and the construction of heterojunctions effectively inhibits the recombination of photogenic charge carrier. As a consequence, the 9% RP/TP1C composite, with the optimal photocatalytic ability, achieves a photocatalytic H2 evolution rate of 6.93 mmol·g-1·h-1, demonstrating a 10.19-fold increase compared to that of bare RP and a 4.08-fold improvement over that of pure TP1C. This article offers a novel and innovative method for the advancement of efficient COFs-based photocatalysts.
Recent advancements in two-dimensional transition metal dichalcogenide materials towards hydrogen-evolution electrocatalysis
Jianmin Yua, Gongao Peng, Lishan Peng, Qingjun Chen, Chenliang Su, Lu Shang, Tierui Zhang
, Available online  , doi: 10.1016/j.gee.2024.08.009
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Hydrogen evolution reaction (HER) plays a crucial role in developing clean and renewable hydrogen energy technologies. However, conventional HER catalysts rely on expensive and scarce noble metals, which is a significant challenge for practical application. Recently, twodimensional transition metal dichalcogenides (2D-TMDs) have emerged as attractive and costeffective alternatives for efficient electrocatalysis in the HER. Substantial efforts have been dedicated to advancing the synthesis and application of 2D-TMDs. This review highlights the design and synthesis of high-performance 2D-TMDs-based HER electrocatalysts by combining theoretical calculations with experimental methods. Subsequently, recent advances in synthesizing different types of 2D TMDs with enhanced HER activity are summarized. Finally, the conclusion and perspectives of the 2D TMDs-based HER electrocatalysts are discussed. We expect that this review will provide new insights into the design and development of highly efficient 2D TMDs-based HER electrocatalysts for industrial applications.
Research on the application of defect engineering in the field of environmental catalysis
Sirui Gao, Shunzheng Zhao, Xiaolong Tang, Long Sun, Qiyu Li, Honghong Yi
, Available online  , doi: 10.1016/j.gee.2024.08.008
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Researchers have recently developed various surface engineering approaches to modify environmental catalysts and improve their catalytic activity. Defect engineering has proved to be one of the most promising modification methods. Constructing defects on the surface of catalytic materials can effectively modulate the coordination environment of the active sites, affecting and changing the electrons, geometry, and other important properties at the catalytic active sites, thus altering the catalytic activity of the catalysts. However, the conformational relationship between defects and catalytic activity remains to be clarified. This dissertation focuses on an overview of recent advances in defect engineering in environmental catalysis. Based on defining the classification of defects in catalytic materials, defect construction methods, and characterization techniques are summarized and discussed. Focusing on an overview of the characteristics of the role of defects in electrocatalytic, photocatalytic, and thermal catalytic reactions and the mechanism of catalytic reactions. An elaborate link is given between the reaction activity and the structure of catalyst defects. Finally, the existing challenges and possible future directions for the application of defect engineering in environmental catalysis are discussed, which are expected to guide the design and development of efficient environmental catalysts and mechanism studies.
Recyclable bio-based epoxy resin thermoset polymer from wood for circular economy
Bowen Zhang, Saravanakumar Elangovan, Zhuohua Sun
, Available online  , doi: 10.1016/j.gee.2024.08.007
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Due to their extraordinary durability and thermal stability, Epoxy Resin Thermosets (ERTs) are essential in various industries. However, their poor recyclability leads to unacceptable environmental pollution. In this study, Wu et al. successfully synthesized a completely bio-based ERT using lignocellulose-derived building blocks which exhibit outstanding thermal and mechanical properties. Remarkably, these bio-materials degrade via methanolysis without the need of any catalyst, presenting a smart and costeffective recycling strategy. Furthermore, this approach could be employed for fabricating reusable composites comprising glass fiber and plant fiber, thereby expanding its applications in sustainable transportation, coatings, paints or biomedical devices.
Challenges and strategies for production of diesel-like hydrocarbons by deoxygenation of biomass-derived fatty acids
Hongju Lin, Xiyan Chen, Yanchang Chu, Jie Fu, Le Yang
, Available online  , doi: 10.1016/j.gee.2024.08.005
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The valorization of biomass to produce biofuels has become a heavily investigated field due to the depletion of fossil fuels and environmental concerns. Among them, the research on deoxygenation of fatty acids or esters derived from biomass as well as municipal sludge organics to produce diesel-like hydrocarbons has become a hot topic. Fatty acid is a key intermediate derived from ester hydrolysis, therefore has attracted more attention as a model compound. In this review, we first introduce and compare the three reaction pathways of hydrodeoxygenation, decarboxylation and decarbonylation, for the deoxygenation of fatty acids and esters. The preference of reaction pathway is closely related to the type of raw materials and catalysts as well as reaction conditions. The special purpose of this review is to summarize the dilemma and possible strategies for deoxygenation of fatty acids, which is expected to provide guidance for future exploration and concentrates. The atom utilization along with stability during reaction in a long time is the most important index for commercial economy. Herein, we propose that the rational design and delicate synthesis of stable single-atom non-noble catalysts may be the best solution. The ultimately goal is aiming to develop sustainable production of green diesel hydrocarbons.
Ti3C2 MXene nanosheets integrated cobalt-doped nickel hydroxide heterostructured composite: An efficient electrocatalyst for overall water-splitting
Amaranadha Reddy Manchuri, Kamakshaiah Charyulu Devarayapalli, Bolam Kim, Youngsu Lim, Dae Sung Lee
, Available online  , doi: 10.1016/j.gee.2024.08.006
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Developing an efficient electrocatalyst for superior electrochemical water splitting (EWS) is crucial for achieving comprehensive hydrogen production. A heterostructured electrocatalyst, free of noble metals, Ti3C2 MXene nanosheet-integrated cobalt-doped nickel hydroxide (NHCoMX) composite was synthesized via a hydrothermal method. The abundant pores in the Ti3C2 MXene nanosheet (MX)-integrated microarchitecture increased the number of active sites and facilitated charge transfer, thus enhancing electrocatalysis. Specifically, the MX- enhanced charge transfer considerably transformed the microelectronic structure of cobalt-doped Ni(OH)2 (NHCo), which promoted its hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Hence, as an EWS catalyst, NHCoMX exhibited an exceptional electrocatalytic activity, demonstrating OER and HER overpotentials of 310 mV and 73 mV, respectively, with low Tafel slopes of 65 mV dec-1 and 85 mV dec-1, respectively; it exhibited a current density of 10 mV cm-2 in 1.0 mol L-1 KOH, representing the closest efficiency to the noble state-of-the-art RuO2 and Pt/C catalyst. Furthermore, the developed electrocatalyst improved the activities of both HER and OER, leading to an overall EWS current density of 10 mA cm-2 at 1.72 V in an alkaline electrolyte with two electrodes. This study describes an efficient heterostructured NHCoMX composite electrocatalyst. It is significantly comparable to the noble state-of-the-art electrocatalysts and can be extended to fabricate resourceful catalysts for large-scale EWS applications.
2,6-Diaminoanthraquinone modified MXene (Ti3C2Tx)/graphene as the negative electrode materials for ionic liquid-based asymmetric supercapacitors
Li Sun, Lujia Chai, Liangqi Jing, Yujuan Chen, Kelei Zhuo, Jianji Wang
, Available online  , doi: 10.1016/j.gee.2024.08.004
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Due to insufficient energy density, supercapacitors (SCs) with preeminent-power and long cycle stability cannot be implemented in some practical applications. Exploring hybrid materials with redox activity to emerge high specific capacitance in ionic liquid (IL) electrolytes can solve this problem. Herein, we report a redox-organic molecule 2,6-diaminoanthraquinone (DAAQ) modified MXene (2,6-Diaminoanthraquinone modified MXene (Ti3C2Tx)/graphene as the negative electrode materials for ionic liquid-based asymmetric supercapacitors)/Graphene (DAAQ-M/G) composite material. With the assist of graphene oxide (GO), MXene and graphene fabricate a three-dimensional (3D) interconnected structure as a conductive framework, which inhibits self-stacking of MXene monolayers and ensures high electronic conductivity. Meanwhile, DAAQ is loaded onto the M/G framework through covalent/non-covalent functionalization. The DAAQ as a spacer effectively enlarges the interlayer spacing of MXene nanosheets, and meanwhile produces reversible redox reactions during charge/discharge processes to provide additional Faradaic contribution to capacity. Therefore, the specific capacitance (capacity) of the DAAQ-M/G as the negative electrode material reaches to 226 F g-1 (306 C g-1) at 1 A g-1 in 1-ethyl-3-methylimidazolium tetrafluoroborate (EmimBF4) electrolyte. Furthermore, an asymmetric supercapacitor (ASC) is assembled using DAAQ-M/G as the negative electrode and self-prepared organic molecule hydroquinone modified reduced graphene oxide (HQ- RGO) material as the positive electrode, with a high energy density of 43 Wh kg-1 at high power density of 1669 W kg-1. The ASC can maintain 80% of initial specific capacitance after 9000 cycles. This research can provide better support to develop advanced organic molecules-modified MXene composite materials for ionic liquid-based SCs.
Mechano-driven chemical reactions
Shaoxin Li, Jiajin Liu, Zhong Lin Wang, Di Wei
, Available online  , doi: 10.1016/j.gee.2024.08.001
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Traditional chemical processes often generate substantial waste, leading to significant pollution of water, air, and soil. Developing eco-friendly chemical methods is crucial for economic and environmental sustainability. Mechano-driven chemistry, with its potential for material recyclability and minimal byproducts, is well-aligned with green chemistry principles. Despite its origins over 2000 years ago and nearly 200 years of scientific investigation, mechano-driven chemistry has not been widely implemented in practice. This is likely due to a lack of comprehensive understanding and the complex physical effects of mechanical forces, which challenge reaction efficiency and scalability. This review summarizes the historical development of mechano-driven chemistry and discusses its progress across various physical mechanisms, including mechanochemistry, tribochemistry, piezochemistry, and contact electrification (CE) chemistry. CE-induced chemical reactions, involving ion transfer, electron transfer, and radical generation, are detailed, emphasizing the dominant role of radicals initiated by electron transfer and the influence of ion transfer through electrical double layer (EDL) formation. Advancing efficient, eco-friendly, and controllable green chemical technologies can reduce reliance on traditional energy sources (such as electricity and heat) and toxic chemical reagents, fostering innovation in material synthesis, catalytic technologies, and establishing a new paradigm for broader chemical applications.
Superhydrophobic Ceramic Membrane Coupled with a Biphasic Solvent for Efficient CO2 Capture
Kaili Xue, Zhen Chen, Xiaona Wu, Heng Zhang, Haiping Chen, Junhua Li
, Available online  , doi: 10.1016/j.gee.2024.07.010
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An innovative strategy was proposed by integration of membrane contactor (MC) with biphasic solvent for efficient CO2 capture from flue gas. The accessible fly ashbased ceramic membrane (CM) underwent hydrophobic modification through silane grafting, followed by fluoroalkylsilane decoration, to prepare the superhydrophobic membrane (CSCM). The CSCM significantly improved resistance to wetting by the biphasic solvent, consisting of amine (DETA) and sulfolane (TMS). Morphological characterizations and chemical analysis revealed the notable enhancements in pore structure and hydrophobic chemical groups for the modified membrane. Predictions of wetting/bubbling behavior based on static wetting theory referred the liquid entry pressure (LEP) of CSCM increased by 20 kPa compared to pristine CM. Compared with traditional amine solvents, the biphasic solvent presented the expected phase separation. Performance experiments demonstrated that the CO2 capture efficiency of the biphasic solvent increased by 7%, and the electrical energy required for desorption decreased by 32%. The 60-h continuous testing and supplemental characterization of used membrane confirmed the excellent adaptability and durability of the CSCMs. This study provides a potential approach for accessing hydrophobic ceramic membranes and biphasic solvents for industrial CO2 capture.
Electronic structure modulation of high entropy materials for advanced electrocatalysis
Luoluo Qi, Jingqi Guan
, Available online  , doi: 10.1016/j.gee.2024.07.009
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High-entropy materials (HEMs) have managed to make their mark in the field of electrocatalysis. The flexibly adjustable component, unique configuration and proprietary core effect endow HEMs with excellent functional feature, superior stability and fast reaction kinetics. Recently, the relationship between the compositions and structures of high-entropy catalysts and their electrocatalytic performances has been extensively investigated. Based on this motivation, we comprehensively and systematically summarize HEMs, outline their intrinsic properties and electrochemical advantages, generalize current state-of-the-art synthetic methods, analyze electrochemical active centers in conjunction with characterization techniques, utilize theoretical research to conduct a high-throughput screening of the targeted high-entropy catalyst and the exploration of the reaction mechanisms, and importantly, focus specially on the electrochemical applications of high-entropy catalysts and propose strategies for regulating electronic structure to accelerate electrochemical reaction kinetics, including morphological control, defect engineering, element regulation, strain engineering and so forth. Finally, we provide our personal views on the challenges and further technical improvements of high-entropy catalysts. This work can provide valuable guidance for future research on high-entropy electrocatalysts.
Enhanced interlayer interaction in sulfonated CONs membrane by amino-rich CONs enabling ultrafast proton transport
Ping Li, Bo He, Xuan Li, Yunfei Lin, Shaokun Tang
, Available online  , doi: 10.1016/j.gee.2024.07.008
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Covalent organic framework nanosheets (CONs) with porous crystalline features and ultrathin thickness are ideal candidates as membrane building blocks to form well-defined transfer nanochannels. The formidable challenge behind self-supporting CONs membrane lies in weak non-covalent interlayer interactions and thus loose stacking, insufficient strength and structure stabilities. Herein, we propose the fabrication of interlayer force-strengthened freestanding CONs membrane through the electrostatic attraction bridge effect of positively-charged amino-rich CONs (CON-NH2) to negatively-charged sulfonated CONs (CON-SO3H). Ultrathin and large lateral sized CON-SO3H and CON-NH2 are synthesized, followed by restacking to prepare freestanding CONs membrane with CON-SO3H as the membrane bulk. Benefiting from effective interlayer interconnection due to strong electrostatic interaction, the obtained CON-SO3H/CON-NH2 membrane displays features of ultrahigh integrity, dense stacking, eminent water/acid/base/organic solvents stabilities and mechanical strength (109 MPa). The shortened −SO3H distance contributes to construct site-continuous transfer pathways, and the deprotonated −SO3H and protonated –NH2 form acid-base pairs to decrease interfacial resistance, which impart membrane superior proton conductivity of 486 mS cm-1 (80 ℃, 100% RH). This interlayer force enhancement strategy offers a promising perspective on achieving densely-stacked CONs membrane with ultrahigh mechanical property and conduction performance for fuel cell application.
Antibiotics-heavy metals combined pollution in agricultural soils: Sources, fate, risks, and countermeasures
Yuanxiang Shu, Donghao Li, Tong Xie, Ke Zhao, Lu Zhou, Fengxiang Li
, Available online  , doi: 10.1016/j.gee.2024.07.007
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Agricultural soil is related to food security and human health, antibiotics and heavy metals (HMs), as two typical pollutants, possess a high coexistence rate in the environmental medium, which is extremely prone to inducing antibiotic-HMs combined pollution. Recently, frequent human activities have led to more prominent antibiotics-HMs combined contamination in agricultural soils, especially the production and spread of antibiotic resistance genes (ARGs), heavy metal resistance genes (MRGs), antibiotic resistant bacteria (ARB), and antibiotics-HMs complexes (AMCs), which seriously threaten soil ecology and human health. This review describes the main sources (Intrinsic and manmade sources), composite mechanisms (co- selective resistance, oxidative stress, and Joint toxicity mechanism), environmental fate and the potential risks (soil ecological and human health risks) of antibiotics and HMs in agricultural soils. Finally, the current effective source blocking, transmission control, and attenuation strategies are classified for discussion, such as the application of additives and barrier materials, as well as plant and animal remediation and bioremediation, etc., pointing out that future research should focus on the whole chain process of “source-process-terminal”, intending to provide a theoretical basis and decision-making reference for future research.
Boosting electrochemical reduction of CO2 to CO using molecule-regulated Ag nanoparticle in ionic liquids
Fangfang Li, Kuilin Peng, Chongyang Jiang, Shaojuan Zeng, Xiangping Zhang, Xiaoyan Ji
, Available online  , doi: 10.1016/j.gee.2024.07.005
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Electrochemical reduction of CO2 is a promising approach to convert CO2 to high-valued chemicals and fuels. However, developing efficient electrocatalysts featuring desirable activity and selectivity is still a big challenge. In this work, a strategy of introducing functionalized molecules with desirable CO2 affinity to regulate Ag catalyst for promoting electrochemical reduction of CO2 was proposed. Specifically, 3-mercapto-1,2,4-triazole was introduced onto the Ag nanoparticle (Ag-m-Triz) for the first time to achieve selectively converting CO2 to carbon monoxide (CO). This Ag-m-Triz exhibits excellent performance for CO2 reduction with a high CO Faradaic efficiency (FECO) of 99.2% and CO partial current density of 85.0 mA/cm2 at -2.3 V vs. Ag/Ag+ in H-cell when combined with the ionic liquid-based electrolyte, 30 wt% 1-butyl-3-methylimidazolium hexafluorophosphate ([Bmim][PF6])-65 wt% acetonitrile (AcN)-5 wt% H2O, which is 2.5-fold higher than the current density in Ag-powder under the same condition. Mechanism studies confirm that the significantly improved performance of Ag-mTriz originates from (i) the stronger adsorption ability of CO2 molecule and (ii) the weaker binding energy to form the COOH* intermediate on the surface of Ag-m-Triz compared with the Ag-powder catalyst, which boosts the conversion of CO2 to CO. This research provides a facile way to regulate electrocatalysts for efficient CO2 reduction by introducing functionalized molecules.
Heterogeneous iron-based catalysts for a sustainable photoinduced nitrogen fixation
Amalia M. Grigoras, Federica Valentini, Loredana Latterini, Luigi Vaccaro
, Available online  , doi: 10.1016/j.gee.2024.07.003
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Ammonia is nowadays one of the most important commodities chemicals intensively produced at about 175 million tons per year, contributing to 1.8 % of the global energy demand. The constantly increasing NH3 demand is also paralleled to the high CO2 emissions associated with its production. Therefore, decarbonizing NH3 synthesis is one of the most urgent contemporary challenges. Taking inspiration from Nature, solar-driven nitrogen fixation under mild conditions is one of the most promising yet challenging alternatives to classic methods. In this review, we focused our attention on the photocatalytic methods for the synthesis of ammonia; in particular, we concentrated on stable and recyclable heterogeneous Fe-based photocatalysts for the production of NH3. Indeed, recoverable and widely abundant and low-cost iron catalysts may represent a very promising tool for future sustainable access to this largely desired chemical target. After an overview of the pioneering works on Fe-driven nitrogen photofixation, the recent strategies on the use of Fe are herein reported. From the comparison with pristine photocatalysts, the addition of Fe as dopant or composite and heterojunction highly enhances the photocatalytic performances, opening the way to sustainable and low-cost nitrogen production.
Copper Silicate Nanoneedle Arrays on Reduced Graphene Oxide Like “Shelter Forest” Guiding Zn Gradient Deposition
Na Gao, Yang Wang, Zhanming Gao, Tianming Lv, Mengyu Rong, Xueying Dong, Dongzhi Chen, Changgong Meng, Yifu Zhang
, Available online  , doi: 10.1016/j.gee.2024.07.004
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With the sustainable and efficient development of aqueous zinc ion batteries (AZIBs), the research on addressing the issues of the adaptability and durability of zinc anodes has been hot-topic and is still of great challenge. In this work, inspired by the sand treatment and afforestation of the Gobi Beach in Northwest China to ameliorate the problem of wind and sand encroachment, we propose a material with a morphology similar to that of a “shelter forest”, CuSiO3 nanoneedles arrays grown on both sides of reduced graphene oxide (rGO@CuSi), as a coating layer on the zinc metal surface to guide Zn gradient deposition. The presence of rGO improves the electrical conductivity of CuSiO3, and the finite element simulation of the electric field and Zn2+ concentration proves that the electric field distribution can be effectively homogenized and the local current density can be reduced for the rGO@CuSi-Zn electrode with the surface presenting the shape of a protective forest. This is due to the abundant pores between the nano-needle array structures on the surface of the electrode, which provides high electron and ion transport paths, and are conducive to achieve uniform Zn deposition, like the principle of wind-sand stabilization by protective forest. Both electrochemical experiments and density functional theory calculations show that the negatively charged surface of rGO@CuSi with good Zn affinity is more capable of guiding Zn2+ transport. Thanks to its inherent material and structural characteristics, the rGO@CuSi-Zn anode has a high specific capacity and good cycling stability. This study provides an insight for interface engineering like protective forest to accelerate the commercialization of high-performance Zn-based batteries.
Rational engineering of triazine-benzene linked covalent-organic frameworks for efficient CO2 photoreduction
Yanghe Fu, Yijing Gao, Huilin Jia, Yuncai Zhao, Yan Feng, Weidong Zhu, Fumin Zhang, Morris D. Argyle, Maohong Fan
, Available online  , doi: 10.1016/j.gee.2024.07.002
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Three large π-conjugated and imine-based COFs, named TFP-TAB, TFP-TTA, and TTA-TTB, were synthesized via the ordered incorporation of benzene and triazine rings in the same host framework to study how the structural units affect the efficiency of CO2 photoreduction. Results from both experiments and density-functional theory (DFT) calculations indicate the separation and transfer of the photoinduced charges is highly related to the triazine-N content and the conjugation degree in the skeletons of COFs. High-efficiency CO2 photoreduction can be achieved by rationally adjusting the number and position of both benzene and triazine rings in the COFs. Specifically, TTA-TTB, with orderly interlaced triazine-benzene heterojunctions, can suppress the recombination probability of electrons and holes, which effectively immobilizes the key species (COOH) and lowers the free energy change of the potential-determining step, and thus exhibits a superior visible-light-induced photocatalytic activity that yields 121.7 μmol HCOOH g-1 h-1. This research, therefore, helps to elucidate the effects of the different structural blocks in COFs on inherent heterogeneous photocatalysis for CO2 reduction at a molecular level.
Synergistic Li6PS5Cl@Li3OCl Composite Electrolyte for High-Performance AllSolid-State Lithium Batteries
Yuzhe Zhang, Haolong Chang, Aiguo Han, Shijie Xu, Xinyu Wang, Shunjin Yang, Xiaohu Hu, Yujiang Sun, Xiao Sun, Xing Chen, Yongan Yang
, Available online  , doi: 10.1016/j.gee.2024.07.001
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Li6PS5Cl is a highly wanted sulfide-solid-electrolyte (SSE) for developing allsolid-state lithium batteries, due to its high ionic conductivity, good processability and abundant compositional elements. However, its cyclability is poor because of harmful side reactions at the Li6PS5Cl/Li interface and growth of lithium dendrites inside Li6PS5Cl phase. Herein, we report a simple interface-engineering remedy to boost the electrochemical performance of Li6PS5Cl, by coating its surface with a Li-compatible electrolyte Li3OCl having low electronic conductivity. The obtained Li6PS5Cl@Li3OCl core@shell structure exhibits a synergistic effect. Consequently, compared with the bare Li6PS5Cl, this composite electrolyte exhibits great performance improvements: 1) In Li|electrolyte|Li symmetric cells, the critical current density at 30℃ gets increased from 0.6 mA/cm2 to 1.6 mA/cm2, and the lifetime gets prolonged from 320 h to 1400 h mA/cm2; 2) In Li|electrolyte|NCM721 full cells running at 30°C, the cycling capacity at 0.2 C (or 0.5 C) gets enhanced by 20% (or from unfeasible to be feasible) for 100 cycles and the rate capability reaches up to 2 C from 0.2 C; and in full cells running at 60°C, the cycling capacity is increased by 7% at 0.2 C and the rate capability is enhanced to 3.0 C from 0.5 C. The experimental studies and theoretical computations show that the performance enhancements are due to the confined electron penetration and suppressed lithium dendrites growth at the Li6PS5Cl@Li3OCl interface.
Research progress on lithium isotopes separation by chemical exchange with crown ethers decorated materials
Yi Fang, Rui Ha, Jun Sun, Xue Liu, XiangDong Ding, WeiQun Shi
, Available online  , doi: 10.1016/j.gee.2024.06.009
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The separation of lithium isotopes (6Li and 7Li) is of great importance for the nuclear industry. The lithium amalgam method is the only lithium isotopes separation process in industry, and the extensive use of mercury has raised concerns about its potential environmental hazards, which have prompted the search for more efficient and environmentally friendly alternatives. Crown ethers can bind lithium ions highly selectively and separate lithium isotopes effectively. A chemical exchange-based lithium isotopes separation method using crown ether decorated materials could be a viable and cost-effective alternative to the lithium amalgam method. In this review, we provide a systematic summary of the recent advances in lithium isotopes separation using crown ether decorated materials.
2D/2D homojunction-mediated charge separation: Synergistic effect of crystalline C3N5 and g-C3N4 via electrostatic self-assembly for photocatalytic hydrogen and benzaldehyde production
Sue-Faye Ng, Joel Jie Foo, Peipei Zhang, Steven Hao Wan Kok, Lling-Lling Tan, Binghui Chen, Wee-Jun Ong
, Available online  , doi: 10.1016/j.gee.2024.06.008
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Homojunction engineering is a promising modification strategy to improve charge carrier separation and photocatalytic performance of carbon nitrides. Leveraging intrinsic heptazine/triazine phase and face-to-face contact, crystalline C3N5 (CC3N5) was combined with protonated g-C3N4 (pgCN) through electrostatic self-assembly to achieve robust 2D/2D homojunction interfaces. The highest photocatalytic performance was obtained through crystallinity and homojunction engineering, by controlling the pgCN:CC3N5 ratio. The 25:100 pgCN:CC3N5 homojunction (25CgCN) had the highest hydrogen production (1409.51 µmol h-1) and apparent quantum efficiency (25.04%, 420 nm), 8-fold and 180-fold higher than CC3N5 and pgCN, respectively. This photocatalytic homojunction improves benzaldehyde and hydrogen production activity, retaining 89% performance after 3 cycles (12 h ) on a 3D-printed substrate. Electron paramagnetic resonance demonstrated higher ·OH-, ·O2- and hole production of irradiated 25CgCN, attributed to crystallinity and homojunction interaction. Thus, electrostatic self-assembly to couple CC3N5 and pgCN in a 2D/2D homojunction interface ameliorates the performance of multifunctional solar-driven applications.
Microfluidic Reactors for Paired Electrosynthesis: Fundamentals, Applications and Future Prospects
Hao Xue, Zhi-Hao Zhao, Menglei Yuan, Guangjin Zhang
, Available online  , doi: 10.1016/j.gee.2024.06.006
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Paired electrosynthesis has received considerable attention as a consequence of simultaneously synthesizing target products at both cathode and anode, whereas the related synthetic efficiency in batch reactors is still undesirable under certain circumstances. Encouragingly, laminar microfluidic reactor offers prospective options that possess controllable flow characteristics such as enhanced mass transport, precise laminar flow control and the ability to expand production scale progressively. In this comprehensive review, the underlying fundamentals of the paired electrosynthesis are initially summarized, followed by categorizing the paired electrosynthesis including parallel paired electrosynthesis, divergent paired electrosynthesis, convergent paired electrosynthesis, sequential paired electrosynthesis and linear paired electrosynthesis. Thereafter, a holistic overview of microfluidic reactor equipment, integral fundamentals and research methodology as well as channel extension and scale-up strategies is proposed. The established fundamentals and evaluated metrics further inspired the applications of microfluidic reactors in paired electrosynthesis. This work stimulated the overwhelming investigation of mechanism discovery, material screening strategies, and device assemblies.
Transformation of discarded biomass into value-added flexible electronic materials
Sijia Bao, Xuenan Yang, Ziqi Yu, Yuanbo Shi, Yuan Lu
, Available online  , doi: 10.1016/j.gee.2024.06.005
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The development of electronic products and increased electronic waste have triggered a series of ecological problems on Earth. Meanwhile, amidst energy crises and the pursuit of carbon neutrality, the recycling of discarded biomass has attracted the attention of many researchers. In recent years, the transformation of discarded biomass into value-added electronic products has emerged as a promising endeavor in the field of green and flexible electronics. In this review, the attempts and advancements in biomass conversion into flexible electronic materials and devices are systematically summarized. We focus on reviewing the research progress in biomass conversion into substrates, electrodes, and materials tailored for optical and thermal management. Furthermore, we explore component combinations suitable for applications in environmental monitoring and health management. Finally, we discuss the challenges in techniques and cost-effectiveness currently faced by biomass conversion into flexible electronic devices and propose improvement strategies. Drawing insights from both fundamental research and industrial applications, we offer prospects for future developments in this burgeoning field.
Conjugated polyaniline as “conveyor” in tungstate boosting cation storage for high-performance aqueous batteries
Yanyan Liu, Zirui Shao, Tianming Lv, Zilong Zhang, Zhenhua Zhou, Tao Hu, Changgong Meng, Yifu Zhang
, Available online  , doi: 10.1016/j.gee.2024.06.004
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Aqueous ion storage systems have motivated great interest by virtue of low reduction, high eco-sustainability and safety. Among various cathode candidates, transition metal compounds are featured with easy dissolution in aqueous solutions and inferior conductivity, which severely hinder their application. Herein, advantages are taken of the “conveyor effect” of conjugated polyaniline to prepare an oxygen defective tungstate-linked polyaniline (Od-WOP) material with chrysanthemum-like microstructure. By virtue of the high electronic conductivity derived from conductive conjugated polyaniline skeleton, unbalanced charge distribution triggered by the defective structure, and reversibly rapid ion (de)intercalation benefited from the open framework with porous chrysanthemum-like microstructure, it delivers outstanding rate capability with a maximum specific capacity of 162.2 mAh g-1 and great cycle stability for storing NH4+. Additionally, it also adopts a high reversible capacity of 140.4 mAh g-1 and outstanding cycling performance to store Ca2+. Consequently, the assembled Od-WOP//PTCDI flexible aqueous ammonium ion batteries and calcium ion batteries exhibit superior capacities, energy densities and flexibilities. Od-WOP achieves the NH4+ and Ca2+ storage capability by interacting with them through hydrogen and ionic bonds, respectively. The deep insight from this work sheds light upon a novel strategy to excavate greater potential of transition metal compounds for aqueous ion batteries.
NiCoMn-LDH with core-shell heterostructures based on CoS nanotube arrays containing multiple ion diffusion channels for boosted supercapacitor applications
Xiaojie Xu, Huachen Lin, Jinrui Ding, Pengjie Zhou, Yulong Ying, Hong Jia, Longhua Li, Yu Liu
, Available online  , doi: 10.1016/j.gee.2024.06.002
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Nanostructure engineering and composition rationalization are crucial for materials to become candidates for high-performance supercapacitor. Herein, a novel core-shell heterostructured electrode, combining CoS hollow nanorods with NiCoMn-layered double hydroxides (LDH) ternary metal nanosheets, were prepared on carbon cloth by reasonably controlled vulcanization and electrodeposition. By optimizing electrodeposition conditions, the material's structure and properties can be fine-tuned. The enhanced capacitance of the optimized carbon cloth (CC)@CoS/NiCoMn-LDH- 300 electrode (4256.0 F g-1) lies in the open space provided by CoS and the establishment of a new charge transfer channel across the interfaces of CC@CoS/NiCoMn-LDH-300 nanosheets. This is further demonstrated by Density functional theory (DFT) simulations based on OH- adsorption energy, which produces faster redox charge kinetics and significantly enhances the electrode’s energy storage capacity. The hybrid supercapacitor, integrating the optimized CC@CoS/NiCoMnLDH-300 electrode with active carbon, demonstrates the highest energy density of 86 Wh kg-1 (under the power density of 850 W kg-1) and the long cycle stability of 89.7%. This study aims to go beyond simple binary LDH by constructing a ternary LDH with a hierarchical core-shell heterostructure to provide an effective and feasible new concept for high-performance supercapacitor electrode materials via rational structure design.
Progress in the construction strategy of noble metal active sites for zeolite-based PNA and VOCs catalysts
Yuan Yao, Haodan Cheng, Guocai Zhong, Xiaolong Tang, Honghong Yi, Shunzheng Zhao, Fengyu Gao, Qingjun Yu
, Available online  , doi: 10.1016/j.gee.2024.06.001
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Zeolite-loaded noble metal catalysts have demonstrated excellent performance in addressing cold-start automotive exhaust NOx emissions and catalytic oxidation of VOCs applications. Pd and Pt are the most commonly used active metals in PNA and VOC catalysts, respectively. However, despite the same metal/zeolite composition, the efficient active sites for PNA and VOC catalysts have been viewed as mainly Pd2+ and Pd0, respectively, both of which are different from each other. As a result, various methods need to be applied to dope Pd and Pt in zeolitic support respectively for different usages. No matter which type of metal species is needed, the common requirement for both PNA and VOC catalysts is that the metal species should be highly dispersed in zeolite support and stay stable. The purpose of this paper is to review the progress of synthetic means of zeolite-coated noble metals (Pd, Pt, etc.) as effective PNA or VOC catalysts. To give a better understanding of the relationship between efficient metal species and the introduced methods, the species that contributed to the NOx adsorption (PNA) and VOCs deep catalytic oxidation were first summarized and compared. Then, based on the above discussion, the detailed construction strategies for different active sites in PNA and VOC catalysts, respectively, were elaborated in terms of synthetic routes, precursor selection, and zeolite carrier requirements. It is hoped that this will contribute to a better understanding of noble metal adsorption/catalysis in zeolites and provide promising strategies for the design of adsorption/catalysts with high activity, selectivity and stability.
Designing Carboxymethyl Cellulose Based Hydrogel Electrolyte Membranes Enhanced by Inorganic Nanoparticle Toward Stable Zinc Anode
Xiangye Li, Yuan Li, Yu Jiang, Dahui Wang, Fen Ran
, Available online  , doi: 10.1016/j.gee.2024.05.012
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Aqueous zinc metal batteries have garnered substantial attention ascribing to affordability, intrinsic safety, and environmental benignity. Nevertheless, zinc metal batteries yet are challenged with potential service life issues resulted from dendrites and side reaction. In this paper, a strategy of nanoparticles doped hydrogel is proposed for constructing carboxymethyl cellulose/graphite oxide hybrid hydrogel electrolyte membranes with exceptional ionic conductivity, anti-swelling property, and simultaneously addressing the dendrites and parasitic reaction. The pivotal functions of the carboxymethyl cellulose/graphite oxide hydrogel electrolyte in mitigating hydrogen evolution and fostering accelerated Zn deposition have been elucidated based on principles of thermodynamic and reaction kinetic. The carboxymethyl cellulose /graphite oxide hydrogel electrolyte endows exceptional cycling longevity (800 h at 1 mA·cm-2/1 mAh·cm-2) for Zn||Zn battery, as well as high Coulombic efficiency for Zn||Cu battery (averagely 99.14 % within 439 cycles at 1 mA·cm-2/1 mAh·cm-2). The assembled Zn||NH4V4O10 battery delivers a high reversible specific capacity of 328.5 mAh·g-1 at 0.1 A·g-1. Moreover, the device of Zn||NH4V4O10 pouch battery remains operational under severe conditions like bending and cutting. This work provides valuable reference in developing inorganic nanoparticle hybrid hydrogel electrolyte for realizing high-performance zinc metal batteries.
Improving electrochemical performance of silicon anode through building “soft-hard” double-layer coating
Xiao Zhua, Weibo Feng, Yiman Huang
, Available online  , doi: 10.1016/j.gee.2024.05.011
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Silicon is believed to be a critical anode material for approaching the roadmap of lithium-ion batteries due to its high specific capacity. But this aim has been hindered by the quick capacity fading of its electrodes during repeated charge-discharge cycles. In this work, a “soft-hard” double-layer coating has been proposed and carried out on ball-milled silicon particles. It is composed of inside conductive pathway and outside elastic coating, which is achieved by decomposing a conductive graphite layer on the silicon surface and further coating it with a polymer layer. The incorporation of the second elastic coating on the inside carbon coating enables silicon particles strongly interacted with binders, thereby making the electrodes displaying an obviously improved cycling stability. As-obtained double-coated silicon anodes deliver a reversible capacity of 2280 mAh g-1 at the voltage of 0.05-2 V, and maintains over 1763 mAh g-1 after 50 cycles. The double-layer coating does not crack after the repeated cycling, critical for the robust performance of the electrodes. In addition, as-obtained silicon particles are mixed with commercial graphite to make actual anodes for lithium-ion batteries. A capacity of 714 mAh g-1 has been achieved based on the total mass of the electrodes containing 10 wt.% double-coated silicon particles.Compared with traditional carbon coating or polymeric coating, the double-coating electrodes display a much better performance. Therefore, the double-coating strategy can give inspiration for better design and synthesis of silicon anodes, as well as other battery materials.
TiO2-Cu7S4 modified with a carbazole-based conjugated porous polymer for adsorption and photocatalytic degradation of bisphenol A
Wanjun Xu, Xunxun Li, Dongyun Chen, Najun Li, Qingfeng Xu, Hua Li, Jinghui He, Jianmei Lu
, Available online  , doi: 10.1016/j.gee.2024.05.010
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Adsorption-photocatalytic degradation of organic pollutants in water is an advantageous method for environmental purification. Herein, a feasible strategy is developed to construct a novel dual S-scheme heterojunctions Cu7S4-TiO2-conjugated polymer with a donor-acceptor structure. There are abundant adsorption active sites for adsorption in the porous structure of the composites, which can rapidly capture pollutants through hydrogen bonding and π-π interactions. In addition, the dual Sscheme heterojunctions effectively improve carrier separation while maintaining a strong redox ability. Thus, the optimized 1.5% CST-130 catalysts can adsorb 71% of 20 ppm BPA in 15 min and completely remove it within 30 min with high adsorption capacity and photodegradation efficiency. Therefore, this study provides a new inspiration for synergistic adsorption and degradation of BPA and the construction of dual S-scheme heterojunction.
Constructing Lithiophilic Sites–Rich Artificial Solid Electrolyte Interphase to Enable Dendrite−Free and Corrosion−Free Lithium-Sulfur Batteries
Wei Lu, Anshun Zhao, Qiuxu Chen, Sihan Liu, Mingxi Yu, Zihao Wang, Ze Gao, Xue Zhao, Guiru Sun, Ming Feng
, Available online  , doi: 10.1016/j.gee.2024.05.008
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An artificial solid electrolyte interphase (SEI) with lithiophilic sites and chemical bonds anchoring lithium polysulfides (LiPSs) has been developed as a potential solution to protect the lithium (Li) metal anode of Lithium−sulfur (Li−S) batteries. This strategy aims to guide consistent Li deposition and relieve lithium corrosion. Herein, the evolution process of lithiophilic sites based on aluminum fluoride (AlF3) in an artificial SEI is disclosed in Li−S batteries with metal−based lithiophilic sites. The polyester polymer (PMMA and PPC) / AlF3 artificial SEI (MPAF−SEI) was homogeneously anchored on Li anode by in−situ polymerization. The conversion of AlF3 into Li−Al and LiF lithiophilic sites effectively reduce the Li nucleation overpotential and prevents the formation of Li dendrites. At the same time, the polymer can anchor LiPSs by chemical bonds and prevents Li corrosion. The optimized MPAF−SEI protected Li demonstrates excellent stability for over 3000 hours at a capacity of 1 mAh cm−2 in Li || Li symmetric cells. The Li−S battery with low N/P (4) exhibits a capacity of 532.6 mAh g −1 over 300 cycles lifespan at 0.5 C.
Mechanism of Brønsted-acid-promoted self-photosensitized [2+2] cycloaddition for synthesis of high-performance biospiral fuel
Ying Chen, Yumei Shu, Minhua Ai, Wenbiao Chen, Chengwen Liu, Songyi Zhang, Shaojie Wang, Haopeng Shi, Ji-Jun Zou, Lun Pan
, Available online  , doi: 10.1016/j.gee.2024.05.006
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Photoinduced [2+2] cycloaddition of biomass-derived cycloolefin is a promising approach to synthesize high-energy bio-fuels, however, the conversion efficiency and selectivity are still low. Herein, we provide an acid-promoted photocycloaddition approach to synthesize a new kind of spiral fuel from biomass-derived cyclohexanone (CHOE) and camphene (CPE). Brønsted acids show higher catalytic activity than Lewis acids, and acetic acid (HOAc) possesses the best catalytic performance, with CHOE conversion up to 99.1%. Meanwhile, the HOAc-catalytic effect has been confirmed for [2+2] photocycloaddition of other biomass-derived ketenes and olefins. The catalytic mechanism and dynamics had been investigated, and showed that HOAc can bond with C=O groups of CHOE to form H-CHOE complex, which leads to higher light adsorption and longer triplet lifetime. Meanwhile, H-CHOE complex reduces the energy gap between CHOE LUMO and CPE HOMO, shortens the distance of ring- forming atoms, and then decreases the energy barrier (from 103.3 kcal/mol to 95.8 kcal/mol) of rate-limiting step. After hydrodeoxygenation, the targeted bio-spiral fuel shows high density of 0.992 g/cm3, high neat heat of combustion of 41.89 MJ/L, low kinetic viscosity of 5.69 mm2/s at 20℃, which is very promising to serve as high- performance aerospace fuel.
Advances in Enhancing Hydrodeoxygenation Selectivity of Lignin-Derived Oxygenates: From Synthetic Strategies to Fundamental Techniques
Xinru Wu, Hongwei Zhang, Cejun Hu, Xiaojun Bao, Pei Yuan
, Available online  , doi: 10.1016/j.gee.2024.05.004
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In recent years, studies focusing on the conversion of renewable lignin-derived oxygenates (LDOs) have emphasized their potential as alternatives to fossil-based products. However, LDOs, existing as complex aromatic mixtures with diverse oxygen-containing functional groups, pose a challenge as they cannot be easily separated via distillation for direct utilization. A promising solution to this challenge lies in the efficient removal of oxygen-containing functional groups from LDOs through hydrodeoxygenation (HDO), aiming to yield biomass products with singular components. However, the high dissociation energy of the carbon-oxygen bond, coupled with its similarity to the hydrogenation energy of the benzene ring, creates a competition between deoxygenation and benzene ring hydrogenation. Considering hydrogen consumption and lignin properties, the preference is directed towards generating aromatic hydrocarbons rather than saturated components. Thus, the goal is to selectively remove oxygen-containing functional groups while preserving the benzene ring structure. Studies on LDOs conversion have indicated that the design of active components and optimization of reaction conditions play pivotal roles in achieving selective deoxygenation, but a summary of the correlation between these factors and the reaction mechanism is lacking. This review addresses this gap in knowledge by firstly summarizing the various reaction pathways for HDO of LDOs. It explores the impact of catalyst design strategies, including morphology modulation, elemental doping, and surface modification, on the adsorption-desorption dynamics between reactants and catalysts. Secondly, we delve into the application of advanced techniques such as spectroscopic techniques and computational modeling, aiding in uncovering the true active sites in HDO reactions and understanding the interaction of reactive reactants with catalyst surface-interfaces. Additionally, fundamental insights into selective deoxygenation obtained through these techniques are highlighted. Finally, we outline the challenges that lie ahead in the design of highly active and selective HDO catalysts. These challenges include the development of detection tools for reactive species with high activity at low concentrations, the study of reaction medium-catalyst interactions, and the development of theoretical models that more closely approximate real reaction situations. Addressing these challenges will pave the way for the development of efficient and selective HDO catalysts, thus advancing the field of renewable LDOs conversion.
Stabilization of Active Ultrathin Amorphous Ruthenium Oxide via Constructing Electronically Interacted Heterostructure for Acidic Water Oxidation
Xiangxiang Pan, Huidong Qian, Jiansheng Xu, Haifeng Wang, Han-Don Um, Chao Lin, Xiaopeng Li, Wei Luo
, Available online  , doi: 10.1016/j.gee.2024.05.003
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Amorphous RuOx (a-RuOx) with disordered atomic arrangement and abundant coordinatively unsaturated Ru sites possesses high intrinsic electrocatalytic activity for oxygen evolution reaction (OER). However, the a-RuOx is prone to fast corrosion during OER in strong acid. Here, we realized the stabilization of an ultrathin a-RuOx layer via constructing heterointerface with crystalline α-MnO2 nanorods array (MnO2@a-RuOx). Benefiting from the strong electronic interfacial interaction, the asformed MnO2@a-RuOx electrocatalyst display an ultralow overpotential of 128 mV to reach 10 mA cm-2 and stable operation for over 100 h in 0.1 M HClO4. The assembled proton exchange membrane (PEM) water electrolyzer reach 1 A cm-2 at applied cell voltage of 1.71 V. Extensive characterizations indicate the MnO2 substrate work as an electron donor pool to prevent the overoxidation of Ru sites and the OER proceeds in adsorbent evolution mechanism process without involving lattice oxygen. Our work provides a promising route to construct robust amorphous phase electrocatalysts.
Engineering crystal plane of NiCo2O4 to regulate oxygen vacancies and acid sites for alkali-free oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid
Hengli Qian, keyuan Zhang, Yongchuo He, Qidong Hou, Chao Xie, Ruite Lai, Guanjie Yu, Tianliang Xia, Xinyu Bai, Haijiao Xie, Meiting Ju
, Available online  , doi: 10.1016/j.gee.2024.05.002
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The catalytic oxidation of HMF involves a cascading reaction with multiple intermediate products, making it crucial to enhance the oriented adsorption capacity of specific functional groups for accelerating the entire process. To achieve the efficient selective oxidation of HMF to FDCA, a series of NiCo2O4 catalysts with different morphologies, such as flaky, echinoids, pompon and corolla, were prepared and characterized by XRD, SEM, TEM, BET, XPS, and FTIR. Among the four catalysts, flaky NiCo2O4 exhibited the most excellent catalytic activity and stability, with a FDCA yield of 60.1% within 12 h at 80 ℃ without alkali participation. The excellent performance of flaky NiCo2O4 catalyst is attributed to the oxygen vacancies and acid sites generated by the exposed (400) facets. The oxygen vacancies and acid sites on the catalyst surface can precisely adsorb -CHO and -CH2-OH of HMF, respectively, and this synergistic effect promotes the efficient production of FDCA. This work is of great significance for fundamentally study the effect of micro-topography or crystal-plane reaction properties on surfaces.
Research Progress of Lignin-Derived Materials in Lithium/Sodium Ion Batteries
Jingke Zhang, Hengxue Xiang, Zhiwei Cao, Shichao Wang, Meifang Zhu
, Available online  , doi: 10.1016/j.gee.2024.05.001
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With the increase of energy consumption, the shortage of fossil resource, and the aggravation of environmental pollution, the development of cost-effective and environmental friendly bio-based energy storage devices has become an urgent need. As the second most abundant natural polymer found in nature, lignin is mainly produced as the by-product of paper pulping and bio-refining industries. It possesses several inherent advantages, such as low-cost, high carbon content, abundant functional groups, and bio-renewable, making it an attractive candidate for the rechargeable battery material. Consequently, there has been a surge of research interest in utilizing lignin or lignin-based carbon materials as the components of lithium-ion (LIBs) or sodium-ion batteries (SIBs), including the electrode, binder, separator, and electrolyte. This review provides a comprehensive overview on the research progress of ligninderived materials used in LIBs/SIBs, especially the application of lignin-based carbons as the anodes of LIBs/SIBs. The preparation methods and properties of lignin-derived materials with different dimensions are systemically discussed, which emphasizes on the relationship between the chemical/physical structures of lignin-derived materials and the performances of LIBs/SIBs. The current challenges and future prospects of lignin-derived materials in energy storage devices are also proposed.
Facilitated transport membranes in post-combustion carbon capture: Recent advancements in polymer materials and challenges towards practical application
Zihan Wang, Zhien Zhang, Mohamad Reza Soltanian, Ruizhi Pang
, Available online  , doi: 10.1016/j.gee.2024.04.010
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Facilitated transport membranes for post-combustion carbon capture are one of the technologies to achieve efficient and large-scale capture. The central principle is to utilize the affinity of CO2 for the carrier to achieve efficient separation and to break the Robson upper bound. This paper reviews the progress of facilitated transport membranes research regarding polymer materials, principles, and problems faced at this stage. Firstly, we briefly introduce the transport mechanism of the facilitated transport membranes. Then the research progress of several major polymers used for facilitated transport membranes for CO2/N2 separation was presented in the past five years. Additionally, we analyze the primary challenges of facilitated transport membranes, including the influence of water, the effect of temperature, the saturation effect of the carrier, and the process configuration. Finally, we also delve into the challenges and competitiveness of facilitated transport membranes.
Interfacial Modulation of Nano Li7La3Zr2O12 Composite Electrolytes Prepared by Solvent-free Method
Qigao Han, Yaqing Guo, Fuhe Wang, Xuechun Lou, Fengqian Wang, Jun Zhong, Jinqiao Du, Jie Tian, Weixin Zhang, Shun Tang, Shijie Cheng, Yuancheng Cao
, Available online  , doi: 10.1016/j.gee.2024.04.009
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Solid-state batteries (SSBs) with high safety are promising for the energy fields, but the development has long been limited by machinability and interfacial problems. Hence, self-supporting , flexible Nano LLZO CSEs are prepared with a solvent-free method at 25 ℃ . The 99.8 wt% contents of Nano LLZO particles enable the Nano LLZO CSEs to maintain good thermal stability while exhibiting a wide electrochemical window of 5.0 V and a high Li+ transfer number of 0.8 . The mean modulus reaches 4376 MPa. Benefiting from the interfacial modulation , the Li|Li symmetric batteries based on the Nano LLZO CSEs show benign stability with lithium at the current densities of 0.1 mA cm-2 , 0.2 mA cm-2 , and 0.5 mA cm-2 . In addition, the Li|LiFePO4 (LFP) SSBs achieve favorable cycling performance: the specific capacity reaches 128.1 mAh g-1 at 0.5 C rate, with a capacity retention of about 80% after 600 cycles . In the further tests of the LiNi0.8Co0.1Mn0.1O2 (NCM811) cathodes with higher energy density, the Nano LLZO CSEs also demonstrate good compatibility: the specific capacities of NCM811-based SSBs reach 177.9 mAh g-1 at 0.5 C rate, while the capacity retention is over 96% after 150 cycles . Furthermore, the Li|LFP soft-pack SSBs verify the safety characteristics and the potential for application, which have a desirable prospect.
Armoring hydrophilic wood-structured ultrathick electrode with bimetallic nitride enables high energy-density supercapacitor
Nannan Ming, Jikun Xu, Jingfang Lei, Cankun Hu, Kaifu Huo
, Available online  , doi: 10.1016/j.gee.2024.04.008
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Thick electrodes can reduce the ratio of inactive constituents in a holistic energy storage system while improving energy and power densities. Unfortunately, traditional slurry-casting electrodes induce high-tortuous ionic diffusion routes that directly depress the capacitance with a thickening design. To overcome this, a novel 3D low-tortuosity, self-supporting, wood-structured ultrathick electrode (NiMoN@WC, a thickness of ~1400 μm) with hierarchical porosity and artificial array-distributed small holes was constructed via anchoring bimetallic nitrides into the monolithic wood carbons. Accompanying the embedded NiMoN nanoclusters with well-designed geometric and electronic structure, the vertically low-tortuous channels, enlarged specific surface area and pore volume, superhydrophilic interface, and excellent charge conductivities, a superior capacitance of NiMoN@WC thick electrodes (~5350 mF cm-2 and 184.5 F g-1) is achieved without the structural deformation. In especial, monolithic wood carbons with gradient porous network not only function as the high-flux matrices to ameliorate the NiMoN loading via cell wall engineering but also allow fully- exposed electroactive substance and efficient current collection, thereby deliver an acceptable rate capability over 75% retention even at a high sweep rate of 20 mA cm-2. Additionally, an asymmetric NiMoN@WC//WC supercapacitor with an available working voltage of 1.0-1.8 V is assembled to demonstrate a maximum energy density of ~2.04 mWh cm-2 (17.4 Wh kg-1) at a power density of 1620 mW cm-2, along with a decent long-term lifespan over 10,000 charging-discharging cycles. As a guideline, the rational design of wood ultrathick electrode with nanostructured transition metal nitrides sketch a promising blueprint for alleviating global energy scarcity while expanding carbon-neutral technologies.
Simultaneous Adsorption-Reduction Boosted by In-situ Magnetic Field
Jianran Ren, Zhiliang Zhu, Yanling Qiu, Fei Yu, Tao Zhou, Jie Ma, Jianfu Zhao
, Available online  , doi: 10.1016/j.gee.2024.04.006
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The mainstream silver recovery has problems such as resource waste, weak silver selectivity, and complicated operation. Here, self-propelled magnetic enhanced capture hydrogel (magnetic NbFeB/MXene/GO, MNMGH) was prepared by self-crosslinking encapsulation method. MNMGH achieved high selectivity (Kd=23.31 mL/g) in the acidic range, and exhibited ultrahigh silver recovery capacity (1604.8 mg/g), which greatly improved by 66 % with the assistance of in-situ magnetic field. The recovered silver crystals could be directly physically exfoliated, without acid/base additions. The selective sieving effect of adsorption, MNMGH preferentially adsorbed Ag(I), and then selectively reduced to Ag(0), realizing dual-selective recovery. The in-situ magnetic field enhanced selective adsorption by enhancing mass transfer, reactivity of oxygen- containing functional groups. Furthermore, density function theory simulations demonstrated that the in-situ magnetic field could lower the silver reduction reaction energy barrier to enhance the selective reduction. Three-drive synergy system (reduction drive, adsorption drive and magnetic drive) achieved ultrahigh silver recovery performance. This study pioneered an in-situ magnetic field assisted enhancement strategy for dual-selective (adsorption/reduction) recovery of precious metal silver, which provided new idea for low-carbon recovery of noble metal from industrial waste liquids.
g-C3N4 nanosheets coupled with CoSe2 as co-catalyst for efficient photooxidation of xylose to xylonic acid
Qi Hao, Yijun Liu, Ren Zou, Ge Shi, Shilian Yang, Linxin Zhong, Wu Yang, Xiao Chi, Yunpeng Liu, Shimelis Admassie, Xinwen Peng
, Available online  , doi: 10.1016/j.gee.2024.04.004
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Photocatalysis has emerged as an effective approach to sustainably convert biomass into value-added products. CoSe2 is a promising non-precious, efficient cocatalyst for photooxidation, which can facilitate the separation of photogenerated electron-holes, increase the reaction rates, and enhance photocatalytic efficiency. In this work, we synthesized a stable and efficient photocatalysis system of CoSe2/g-C3N4 through attaching CoSe2 on g-C3N4 sheets, with a yield of 50.12 % for the selective photooxidation of xylose to xylonic acid. Under light illumination, the photogenerated electrons were prone to migrating from g-C3N4 to CoSe2 due to the higher work function of CoSe2, resulting in the accelerated separation of photogenerated electron-holes and the promoted photooxidation. Herein, this study reveals the unique function of CoSe2, which can significantly promote oxygen adsorption, work as an electron sink and accelerate the generation of · O2-, thereby improving the selectivity toward xylonic acid over other by-products. This work provides useful insights into the design of selective photocatalysts by engineering g-C3N4 for biomass high-value utilization.
Insights into novel indium catalyst to kW scale low cost, high cycle stability of iron-chromium redox flow battery
Yingchun Niu, Yinping Liu, Tianhang Zhoua, Chao Guo, Guangfu Wu, Wenjie Lv, Ali Heydari, Bo Pengb, Chunming Xu, Quan Xua
, Available online  , doi: 10.1016/j.gee.2024.04.005
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Iron-chromium flow batteries (ICRFBs) have emerged as an ideal large-scale energy storage device with broad application prospects in recent years. Enhancement of the Cr3+/Cr2+ redox reaction activity and inhibition of the hydrogen evolution side reaction (HER) are essential for the development of ICRFBs and require a novel catalyst design. However, elucidating the underlying mechanisms for modulating catalyst behaviors remains an unresolved challenge. Here, we show a novel precisely controlled preparation of a novel thermal-treated carbon cloth electrode with a uniform deposit of low-cost indium catalyst particles. The density functional theory analysis reveals the In catalyst has a significant adsorption effect on the reactants and improves the redox reaction activity of Cr3+/Cr2+. Moreover, H+ is more easily absorbed on the surface of the catalyst with a high migration energy barrier, thereby inhibiting the occurrence of HER. The assembled ICRFBs have an average energy efficiency of 83.91% at 140 mA/cm2, and this method minimizes the electrodeposition process and cleans the last obstacle for industry long cycle operation requirements. The ICRFBs exhibit exceptional long-term stability with an energy efficiency decay rate of 0.011% per cycle
Triazine-COF@Silicon nanowire mimicking plant leaf to enhance photoelectrocatalytic CO2 reduction to C2+ chemicals
Wenrui Wan, Fanhua Meng, Si Chen, Jianhua Wang, Chunyan Liu, Yan Wei, Chenpu He, Li Fan, Qiaolan Zhang, Weichun Ye, Huanwang Jing
, Available online  , doi: 10.1016/j.gee.2024.04.007
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Converting CO2 and water into valuable chemicals like plant do is considered a promising approach to address both environmental and energy issues. Taking inspiration from the structures of natural leaves, we designed and synthesized a novel copper-coordinated covalent triazine framework (CuCTF) supported by silicon nanowire arrays on wafer chip. This marks the first-ever application of such a hybrid material in the photoelectrocatalytic reduction of CO2 under mild conditions. The Si@CuCTF6 heterojunction has exhibited exceptional selectivity of 95.6% towards multicarbon products (C2+) and apparent quantum efficiency (AQE) of 0.89% for carbon-based products. The active sites of the catalysts are derived from the nitrogen atoms of unique triazine ring structure in the ordered porous framework and the abundant Cu-N coordination sites with bipyridine units. Furthermore, through DFT calculations and operando FTIR spectra analysis, we proposed a comprehensive mechanism for the photoelectrocatalytic CO2 reduction, confirming the existence of key intermediate species such as *CO2-, *=C=O, *CHO and *CO-CHO etc. This work not only provides a new way to mimic photosynthesis of plant leaves but also gives a new opportunity to enter this research field in the future.
Self-sustaining Alkaline Seawater Electrolysis via Forward Osmosis Membranes
Ke Shi, Hongyi Wan, Keyu Wanga, Fumohan Fang, Shiyi Li, Yixing Wang, Linfeng Lei, Linzhou Zhuang, Zhi Xu
, Available online  , doi: 10.1016/j.gee.2024.04.003
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Seawater electrolysis for hydrogen production faces inherent challenges, including side reactions, corrosion, and scaling, stemming from the intricate composition of seawater. In response, researchers have turned to continuous water splitting using forward osmosis (FO)-driven seawater desalination. However, the necessity of a neutral electrolyte hampers this strategy due to the limited current density and scarcity of precious metals. Herein, this study applies alkali-durable FO membranes to enable self- sustaining seawater splitting, which can selective withdraw water molecules, from seawater, via concentration gradient. The membranes demonstrated outstanding perm-selectivity of water/ions (~5830 mol mol-1) during month-long alkaline resistance tests, preventing electrolyte leaching (>97% OH- retention) while maintaining~95% water balance (VFO=Velectrolysis) via preserved concentration gradient for consistent forward-osmosis influx of water molecules. With the consistent electrolyte environment protected by the polyamide FO membranes, the NiFe-Ar-P catalyst exhibits promising performance:a sustain current density of 360 mA cm-2 maintained at the cell voltage of 2.10 V and 2.15 V for 360 h in the offshore seawater, preventing Cl/Br corrosion (98% rejection) and Mg/Ca passivation (99.6% rejection). This research marks a significant advancement towards efficient and durable seawater-based hydrogen production.
Preparation and performance of highly-conductive dual-doped Li7La3Zr2O12 solid electrolytes for thermal batteries
Wei Li, Shu Zhang, Xinya Bu, Jing Luo, Yi Zhang, Mengyu Yan, Ting Quan, Yanli Zhu
, Available online  , doi: 10.1016/j.gee.2024.04.002
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Garnet Li7La3Zr2O12 (LLZO) electrolytes have been recognized as a promising candidate to replace liquid/molten-state electrolytes in battery applications due to their exceptional performance, particularly Ga-doped LLZO (LLZGO), which exhibits high ionic conductivity. However, the limited size of the Li+ transport bottleneck restricts its high-current discharging performance. The present study focuses on the synthesis of Ga3+ and Ba2+ co-doped LLZO (LLZGBO) and investigates the influence of doping contents on the morphology, crystal structure, Li+ transport bottleneck size, and ionic conductivity. In particular, Ga0.32Ba0.15 exhibits the highest ionic conductivity (6.11E-2 S cm-1 at 550℃) in comparison with other compositions, which can be attributed to its higher-energy morphology, larger bottleneck and unique Li+ transport channel. In addition to Ba2+, Sr2+ and Ca2+ have been co-doped with Ga3+ into LLZO, respectively, to study the effect of doping ion radius on crystal structures and the properties of electrolytes. The characterization results demonstrate that the easier Li+ transport and higher ionic conductivity can be obtained when the electrolyte is doped with larger-radius ions. As a result, the assembled thermal battery with Ga0.32Ba0.15-LLZO electrolyte exhibits a remarkable voltage platform of 1.81 V and a high specific capacity of 455.65 mAh g-1 at an elevated temperature of 525℃. The discharge specific capacity of the thermal cell at 500 mA amounts to 63% of that at 100 mA, showcasing exceptional high-current discharging performance. When assembled as prototypes with fourteen single cells connected in series, the thermal batteries deliver an activation time of 38 ms and a discharge time of 32 s with the current density of 100 mA cm-2. These findings suggest that Ga, Ba co-doped LLZO solid-state electrolytes with high ionic conductivities holds great potential for high-capacity, quick-initiating and high-current discharging thermal batteries.
Energy transfer enhanced photocatalytic hydrogen evolution in organic heterostructure nanoparticles via flash nanoprecipitation processing
Miaojie Yu, Weiwei Zhang, Xueyan Liu, Guohui Zhao, Jun Du, Yongzhen Wu, WeiHong Zhu
, Available online  , doi: 10.1016/j.gee.2024.04.001
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Organic nanophotocatalysts are promising candidates for solar fuels production, but they still face the challenge of unfavorable geminate recombination due to the limited exciton diffusion lengths. Here, we introduce a binary nanophotocatalyst fabricated by blending two polymers, PS-PEG5 (PS) and PBT-PEG5 (PBT), with matched absorption and emission spectra, enabling a Förster resonance energy transfer (FRET) process for enhanced photocatalysis. These heterostructure nanophotocatalysts are processed using a facile and scalable flash nanoprecipitation (FNP) technique with precious kinetic control over binary nanoparticle formation. The resulting nanoparticles exhibits an exceptional photocatalytic hydrogen evolution rate up to 65 mmol g-1 h-1, 2.5 times higher than that single component nanoparticle. Characterizations through fluorescence spectra and transient absorption spectra confirm the hetero-energy transfer within the binary nanoparticles, which prolongs the excited-state lifetime and extends the namely "effective exciton diffusion length". Our finding opens new avenues for designing efficient organic photocatalysts by improving exciton migration.
Construction of an Artificial Zinc Alloy Layer toward Stable Zinc-Metal Anode
Long Jiang, Yizhao Chai, Dongdong Ji, Liwei Li, Le Li, Bingan Lu, Dongmin Li, Jiang Zhou
, Available online  , doi: 10.1016/j.gee.2024.03.006
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Aqueous zinc-ion batteries (AZIBs) present a promising option for next-generation batteries given their high safety, eco-friendliness, and resource sustainability. Nonetheless, the practical application of zinc anodes is hindered by inevitable parasitic reactions and dendrite growth. Here, zinc alloy layers (i.e., ZnCo and ZnFe alloys) were rationally constructed on the zinc surface by chemical displacement reactions. The alloying process exposes more (002) planes of the ZnCo anode to guide the preferential and dendrite-free zinc deposition. Furthermore, the ZnCo alloy layer not only effectively inhibits water-induced side reactions but also accelerates electrode kinetics, enabling highly reversible zinc plating/stripping. As a result, the ZnCo anode achieves a Coulombic efficiency of 99.2% over 1300 cycles, and the ZnCo symmetric cell exhibits a long cycle life of over 2000 h at 4.4 mA cm−2. Importantly, the ZnCo//NH4V4O10 full cell retains a high discharge capacity of 218.4 mAh g−1 after 800 cycles. Meanwhile, the ZnFe-based symmetric cell also displays excellent cycling stability over 2500 h at 1.77 mA cm−2. This strategy provides a facile anode modification approach toward highperformance AZIBs.
Novel Titanium Vanadate with Superior Na+ Transport Kinetics for Rapid Charging and Low-Temperature Sodium Ion Batteries
Dan Lv, Liehao Wei, Cheng Wang, Mingyue Wang, Zhongchao Bai, Yameng Fan, Dongdong Wang, Nana Wang, Jian Yang
, Available online  , doi: 10.1016/j.gee.2024.03.005
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Sodium-ion batteries (SIBs) hold great promise for large-scale energy storage in the post-lithium-ion battery era due to their high rate performance and long lifespan, although their sluggish Na+ transformation kinetics still require improvement. Encouraged by the excellent electrochemical performance of titanium-based anode materials, here, we present a novel titanium vanadate@carbon (TVO@C) material as anode for SIBs. Our TVO@C material is synthesized via a facile coprecipitation method, with the following annealing process in an acetylene atomosphere. The opened ion channel and the oxygen vacancies within TVO@C facilitate the diffusion of Na+ ions, reducing their diffusion barrier. Thus, an ultrahigh rate of 100 Ag-1 and long life of 10000 cycles have been achieved. Furthermore, the TVO@C electrode exhibits stable performance, not only at room temperature, but also at temperatures as low as - 20 °C. The TVO@C||Na3V2(PO4)3@C full cells have also achieved stable discharge/charge for 500 cycles. It is believed that this strategy provides new insight into the development of advanced electrodes and provides a new opportunity for constructing novel high rate electrodes.
CO hydrogenation conversion driven by micro-environments of active sites over iron carbide catalysts
Nan Song, Xingxing Li, Ebtihal Abograin, Wenyao Chen, Junbo Cao, Jing Zhang, De Chen, Xuezhi Duan, Xinggui Zhou
, Available online  , doi: 10.1016/j.gee.2024.03.003
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Essentially clearing the structure–activity relationship between iron carbide catalysts involving multiple active centers to understand the reaction mechanism of CO hydrogenation conversion process is still a great challenge. Here, two main micro-environment factors, namely electronic properties and geometrical effects were found to have an integrated effect on the mechanism of CO hydrogenation conversion, involving active sites on multiple crystal phases. The Bader charge of the surface Fe atoms on the active sites had a guiding effect on the CO activation pathway, while the spatial configuration of the active sites greatly affected the energy barriers of CO activation. Although the defective surfaces were more conducive to CO activation, the defective sites were not the only sites to dissociate CO, as CO always tended to dissociate in a wider area. This synergistic effect of the micro-environment also occurred during the CO conversion process. Surface C atoms on relatively flat configurations were more likely to form methane, while the electronic properties of the active sites could effectively describe the C-C coupling process, as well as distinguish the coupling mechanisms.
Spatially confined synthesis of TiNb2O7 quantum dots onto mesoporous carbon and Ti3C2TX MXene for boosting lithium storage
Daoguang Sun, Cheng Tang, Haitao Li, Xinlin Zhang, Guanjia Zhu, Zhen-Dong Huang, Aijun Du, Haijiao Zhang
, Available online  , doi: 10.1016/j.gee.2024.03.004
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TiNb2O7 has been emerged as one of the most promising electrode materials for highenergy lithium-ion batteries. However, limited by the slow electron/ion transport kinetics, and insufficient active sites in the bulk structure, the TiNb2O7 electrode still suffers from unsatisfactory lithium storage performance. Herein, we demonstrate a spatially confined strategy toward a novel TiNb2O7-NMC/MXene composite through a triblock copolymer-directed one-pot solvothermal route, where TiNb2O7 quantum dots with a particle size of 2-3 nm are evenly embedded into N-doped mesoporous carbon (NMC) and Ti3C2TX MXene. Impressively, the as-prepared TiNb2O7-NMC/MXene anode exhibits a high reversible capacity (486.2 mAh g-1 at 0.1 A g-1 after 100 cycles) and long cycle lifespan (363.4 mAh g-1 at 1 A g-1 after 500 cycles). Both experimental and theorical results further demonstrate that such a superior lithium storage performance is mainly ascribed to the synergistic effect among 0D TiNb2O7 quantum dots, 2D Ti3C2TX MXene nanosheets, and N-doped mesoporous carbon. The strategy presented also opens up new horizon for space-confined preparation of highperformance electrode materials.
Merging Polymers of Intrinsic Microporosity and Porous Carbon-Based Zinc Oxide Composites in Novel Mixed Matrix Membranes for Efficient Gas Separation
Muning Chen, Jiemei Zhou, Jing Ma, Weigang Zheng, Guanying Dong, Xin Li, Zhihong Tian, Yatao Zhang, Jing Wang, Yong Wang
, Available online  , doi: 10.1016/j.gee.2024.03.002
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Mixed matrix membranes (MMMs) have demonstrated significant promise in energy-intensive gas separations by amalgamating the unique properties of fillers with the facile processability of polymers. However, achieving a simultaneous enhancement of permeability and selectivity remains a formidable challenge, due to the difficulty of achieving an optimal match between polymers and fillers. In this study, we incorporate a porous carbon- based zinc oxide composite (C@ZnO) into high-permeability polymers of intrinsic microporosity (PIMs) to fabricate MMMs. The dipole-dipole interaction between C@ZnO and PIMs ensures their exceptional compatibility, mitigating the formation of non-selective voids in the resulting MMMs. Concurrently, C@ZnO with abundant interconnected pores can provide additional low- resistance pathways for gas transport in MMMs. As a result, the CO2 permeability of the optimized C@ZnO/PIM-1 MMMs is elevated to 13215 barrer, while the CO2/N2 and CO2/CH4 selectivity reached 21.5 and 14.4, respectively, substantially surpassing the 2008 Robeson upper bound. Additionally, molecular simulation results further corroborate that the augmented membrane gas selectivity is attributed to the superior CO2 affinity of C@ZnO. In summary, we believe that this work not only expands the application of MMMs for gas separation but also heralds a paradigm shift in the application of porous carbon materials.
Synergistically S/N self-doped biochar as a green bifunctional cathode catalyst in electrochemical degradation of organic pollutant
Xuechun Wang, Huizhong Wu, Jiana Jing, Ge Song, Xuyang Zhang, Minghua Zhou, Raf Dewil
, Available online  , doi: 10.1016/j.gee.2024.03.001
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Biomass-derived heteroatom self-doped cathode catalysts has attracted considerable interest for electrochemical advanced oxidation processes (EAOPs) due to its high performance and sustainable synthesis.Herein,we illustrated the morphological fates of waste leaf-derived graphitic carbon (WLGC) produced from waste ginkgo leaves via pyrolysis temperature regulation and used as bifunctional cathode catalyst for simultaneous H2O2 electrochemical generation and organic pollutant degradation,discovering S/N-self-doping shown to facilitate a synergistic effect on reactive oxygen species (ROS) generation.Under the optimum temperature of 8000°C,the WLGC exhibited a H2O2 selectivity of 94.2% and tetracycline removal of 99.3% within 60 min.Density functional theory calculations and in-situ Fourier transformed infrared spectroscopy verified that graphitic N was the critical site for H2O2 generation.While pyridinic N and thiophene S were the main active sites responsible for •OH generation,Nvacancies were the active sites to produce 1O2 from O2.The performance of the novel cathode for tetracycline degradation remains well under a wide pH range (3–11),maintaining excellent stability in 10 cycles.It is also industrially applicable,achieving satisfactory performance treating in real water matrices.This system facilitates both radical and non-radical degradation,offering valuable advances in the preparation of cost- effective and sustainable electrocatalysts and hold strong potentials in metal-free EAOPs for organic pollutant degradation.
A Functional Cathode Sodium Compensation Agent for Stable Sodium-Ion Batteries
Wei Wu, Zhenglin Hu, Zhengfei Zhao, Aoxuan Wang, Jiayan Luo
, Available online  , doi: 10.1016/j.gee.2024.02.009
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Hard carbon (HC) is widely used in sodium-ion batteries (SIBs), but its performance has always been limited by low initial Coulombic efficiency (ICE) and cycling stability. Cathode compensation agent is a favorable strategy to make up for the loss of active sodium ions consumed by HC anode. Yet it lacks agent that effectively decomposes to increase the active sodium ions as well as regulate carbon defects for decreasing the irreversible sodium ions consumption. Here, we propose 1,2- dihydroxybenzene Na salt (NaDB) as a cathode compensation agent with high specific capacity (347.9 mAh g-1), lower desodiation potential (2.4-2.8 V) and high utilization (99%). Meanwhile, its byproduct could functionalize HC with more C=O groups and promotes its reversible capacity. Consequently, the presodiation hard carbon (pHC) anode exhibits highly reversible capacity of 204.7 mAh g-1 with 98% retention at 5 C rate over 1000 cycles. Moreover, with 5 wt% NaDB initially coated on the Na3V2(PO4)3 (NVP) cathode, the capacity retention of NVP+NaDB|HC cell could increase form 36% to 89% after 1000 cycles at 1 C rate. This work provides a new avenue to improve SIBs reversible capacity and cycling performance through designing functional cathode compensation agent.
Design of Multifunctional Interfaces on Ceramic Solid Electrolytes for High-Performance Lithium-Air Batteries
Yunxin Shi, Ziyang Guo, Changhong Wang, Mingze Gao, Xiaoting Lin, Hui Duan, Yonggang Wang, Xueliang Sun
, Available online  , doi: 10.1016/j.gee.2024.02.010
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High-energy-density lithium (Li)-air cells have been considered a promising energy-storage system, but the liquid electrolyte-related safety and side-reaction problems seriously hinder their development. To address these above issues, solid-state Li-air batteries have been widely developed. However, many commonly-used solid electrolytes generally face huge interface impedance in Li-air cells and also show poor stability towards ambient air/Li electrodes. Herein, we fabricate a differentiating surface-regulated ceramic-based composite electrolyte (DSCCE) by constructing disparately LiI-containing polymethyl methacrylate (PMMA) coating and Poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) layer on both sides of Li1.5Al0.5Ge1.5(PO4)3 (LAGP). The cathode-friendly LiI/PMMA layer displays excellent stability towards O2- and also greatly reduces the decomposition voltage of discharge products in Li-air system. Additionally, the anode-friendly PVDF-HFP coating shows low-resistance properties towards anodes.Moreover, Li dendrite/passivation derived from liquid electrolyte-induced side reactions and air/I-attacking can be obviously suppressed by the uniform and compact composite framework. As a result, the DSCCE-based Li-air batteries possess high capacity/low voltage polarization (11836 mA h g-1/1.45 V under 500 mA g-1), good rate performance (capacity ratio under 1000 mA g-1/250 mA g-1 is 68.2 %) and long-term stable cell operation (300 cycles at 750 mA g-1 with 750 mAh g-1) in ambient air.
Organic Solvent Nanofiltration Membranes for Separation in Non-Polar Solvent System
Shuyun Gu, Siyao Li, Zhi Xu
, Available online  , doi: 10.1016/j.gee.2024.02.007
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Membrane technology holds significant potential for augmenting or partially substituting conventional separation techniques, such as heat-driven distillation, thereby reducing energy consumption. Organic solvent nanofiltration represents an advanced membrane separation technology capable of discerning molecules within a molecular weight range of approximately 100 to 1000 Da in organic solvents, offering low energy requirements and minimal carbon footprints. Molecular separation in non-polar solvent system, such as toluene, n-hexane, and n-heptane, has gained paramount importance due to their extensive use in the pharmaceutical, biochemical, and petrochemical industries. In this review, we presented recent advancements in membrane materials, membrane fabrication techniques and their promising applications for separation in non-polar solvent system, encompassing hydrocarbon separation, bioactive molecule purification and organic solvent recovery. Furthermore, this review highlighted the challenges and opportunities associated with membrane scale-up strategies and the direct translation of this promising technology into industrial applications.
Optimizing Electronic Structure through Point Defect Engineering for Enhanced Electrocatalytic Energy Conversion
Wei Ma, Jiahao Yao, Fang Xie, Xinqi Wang, Hao Wan, Xiangjian Shen, Lili Zhang, Menggai Jiao, Zhen Zhou
, Available online  , doi: 10.1016/j.gee.2024.02.006
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Point defect engineering endows catalysts with novel physical and chemical properties, elevating their electrocatalytic efficiency. The introduction of defects emerges as a promising strategy, effectively modifying the electronic structure of active sites. This optimization influences the adsorption energy of intermediates, thereby mitigating reaction energy barriers, altering paths, enhancing selectivity, and ultimately improving the catalytic efficiency of electrocatalysts. To elucidate the impact of defects on the electrocatalytic process, we comprehensively outline the roles of various point defects, their synthetic methodologies, and characterization techniques. Importantly, we consolidate insights into the relationship between point defects and catalytic activity for hydrogen/oxygen evolution and CO2/O2/N2 reduction reactions by integrating mechanisms from diverse reactions. This underscores the pivotal role of point defects in enhancing catalytic performance. At last, the principal challenges and prospects associated with point defects in current electrocatalysts are proposed, emphasizing their role in advancing the efficiency of electrochemical energy storage and conversion materials.
Atmospheric reductive catalytic fractionation of lignocellulose integrated with one-pot catalytic conversion of carbohydrate yielding valuable lignin monomers and platform chemicals from corn straw
Meng-Ying Liu, Zhe-Hui Zhang, Xue-Qi Wang, Qian Sun, Chen Zhang, Yu Li, Zhuohua Sun, Katalin Barta, Feng Peng, Tong-Qi Yuan
, Available online  , doi: 10.1016/j.gee.2024.02.004
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Developing a cost-effective and environmentally friendly process for the production of valuable chemicals from abundant herbal biomass receives great attentions in recent years. Herein, taking advantage of the “lignin first” strategy, corn straw is converted to valuable chemicals including lignin monomers, furfural and 5-methoxymethylfurfural via a two steps process. The key of this research lies in the development of a green and low-cost catalytic process utilizing magnetic Raney Ni catalyst and high boiling point ethylene glycol. The utilization of neat ethylene glycol as the sole reactant under atmospheric conditions obviates the need for additional additives, thereby facilitating the entire process to be conducted in glass flasks and rendering it highly convenient for scaling up. In the initial step, depolymerization of corn straw lignin resulted in a monomer yield of 18.1 wt%. Subsequently, in a dimethyl carbonate system, the carbohydrate component underwent complete conversion in a one-pot process, yielding furfural and 5- methoxymethylfurfural as the primary products with an impressive yield of 47.7 %.
Recent advances of metal vacancies in energy and environmental catalysis: synthesis, characterization, and roles
Long Sun, Shunzheng Zhao, Sirui Gao, Ronghui Zhu, Yiran Tan, Xiaolong Tang, Honghong Yi
, Available online  , doi: 10.1016/j.gee.2024.02.005
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With the ongoing depletion of fossil fuels, energy and environmental issues have become increasingly critical, necessitating the search for effective solutions. Catalysis, being one of the hallmarks of modern industry, offers a promising avenue for researchers. However, the question of how to significantly enhance the performance of catalysts has gradually drawn the attention of scholars. Defect engineering, a commonly employed and effective approach to improve catalyst activity, has become a significant research focus in the catalysis field in recent years. Non-metal vacancies have received extensive attention due to their simple form. Consequently, exploration of metal vacancies has remained stagnant for a considerable period, resulting in a scarcity of comprehensive reviews on this topic. Therefore, based on the latest research findings, this paper summarizes and consolidates the construction strategies for metal vacancies, characterization techniques, and their roles in typical energy and environmental catalytic reactions. Additionally, it outlines potential challenges in the future, aiming to provide valuable references for researchers interested in investigating metal vacancies.
Boosting high-performance in Zr-rich side protonic solid oxide electrolysis cells by optimizing functional interlayer
Chunmei Tang, Ning Wang, Sho Kitano, Hiroki Habazaki, Yoshitaka Aoki, Siyu Ye
, Available online  , doi: 10.1016/j.gee.2024.02.003
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Protonic solid oxide electrolysis cells (P-SOECs) are a promising technology for water electrolysis to produce green hydrogen. However, there are still challenges related key materials and anode/electrolyte interface. P-SOECs with Zr-rich electrolyte, called Zr-rich side P-SOECs, possess high thermodynamically stability under high steam concentrations but the large reaction resistances and the current leakage, thus the inferior performances. In this study, an efficient functional interlayer Ba0.95La0.05Fe0.8Zn0.2O3-δ (BLFZ) in-between the anode and the electrolyte is developed. The electrochemical performances of P-SOECs are greatly enhanced because the BLFZ can greatly increase the interface contact, boost anode reaction kinetics, and increase proton injection into electrolyte. As a result, the P-SOEC yields high current density of 0.83 A cm-2 at 600 ℃ in 1.3 V among all the reported Zr-rich side cells. This work not only offers an efficient functional interlayer for P-SOECs but also holds the potential to achieve P-SOECs with high performances and long-term stability.
Melting points of ionic liquids: Review and evaluation
Zhengxing Dai, Lei Wang, Xiaohua Lu, Xiaoyan Ji
, Available online  , doi: 10.1016/j.gee.2024.01.009
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The melting points of ionic liquids (ILs) reported since 2020 were surveyed, collected, and reviewed, which were further combined with the previous data to provide a database with 3129 ILs ranging from 177.15 to 645.9 K in melting points. In addition, the factors that affect the melting point of ILs from macro, micro, and thermodynamic perspectives were summarized and analyzed. Then the development of the quantitative structure-property relationship (QSPR), group contribution method (GCM), and conductor-like screening model for realistic solvents (COSMO-RS) for predicting the melting points of ILs were reviewed and further analyzed. Combined with the evaluation together with the preliminary study conducted in this work, it shows that COSMO-RS is more promising and possible to further improve its performance, and a framework was thus proposed.
Ammonia-induced CuO/13X for H2S removal from simulated blast furnace gas at low temperature
Erping Cao, Yuhua Zheng, Hao Zhang, Jianshan Wang, Yuran Li, Tingyu Zhu, Zhan-guo Zhang, Guangwen Xu, Yanbin Cui
, Available online  , doi: 10.1016/j.gee.2024.02.002
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Blast furnace gas (BFG) is an important by-product energy for the iron and steel industry and has been widely used for heating or electricity generation. However, the undesirable contaminants in BFG (especially H2S) generate harmful environmental emissions. The desulfurization of BFG is urgent for integrated steel plants due to the stringent ultra-low emission standards. Compared with other desulfurization materials, zeolite-based adsorbents represent a viable option with low costs and long service life. In this study, an ammonia-induced CuO modified 13X adsorbent (NH3–CuO/13X) was prepared for H2S removal from simulated BFG at low temperature. The XRD, H2-TPR and TEM analysis proved that smaller CuO particles were formed and the dispersion of Cu on the surface of 13X zeolite was improved via the induction of ammonia. Evaluation on H2S adsorption performance of the adsorbent was carried out using simulated BFG, and the results showed that NH3–CuO/13X-3 has better breakthrough sulfur capacity, which was more than twice the sulfur capacity of CuO/13X. It is proposed that the enhanced desulfurization performance of NH3–CuO/13X is attributed to an abundant pore of 13X, and combined action of 13X and CuO. This work provided an effective way to improve the sulfur capacity of zeolite-based adsorbents via impregnation method by ammonia induction.
Direct seawaect seawter splitting for hydrogen production: recent advances in materials synthesis and technological innovation
Yilin Zhao, Zhipeng Yu, Aimin Ge, Lujia Liu, Joaquim Luis Faria, Guiyin Xu, Meifang Zhu
, Available online  , doi: 10.1016/j.gee.2024.02.001
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High-throughput screening of CO2 cycloaddition MOF catalyst with an explainable machine learning model
Xuefeng Bai, Yi Li, Yabo Xie, Qiancheng Chen, Xin Zhang, Jian-Rong Li
, Available online  , doi: 10.1016/j.gee.2024.01.010
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The high porosity and tunable chemical functionality of metal-organic frameworks (MOFs) make it a promising catalyst design platform. High-throughput screening of catalytic performance is feasible since the large MOF structure database is available. In this study, we report a machine learning model for high-throughput screening of MOF catalysts for the CO2 cycloaddition reaction. The descriptors for model training were judiciously chosen according to the reaction mechanism, which leads to high accuracy up to 97% for the 75% quantile of the training set as the classification criterion. The feature contribution was further evaluated with SHAP and PDP analysis to provide a certain physical understanding. 12,415 hypothetical MOF structures and 100 reported MOFs were evaluated under 100 °C and 1 bar within one day using the model, and 239 potentially efficient catalysts were discovered. Among them, MOF-76(Y) achieved the top performance experimentally among reported MOFs, in good agreement with the prediction.
CoTCPP integrates with BiOBr microspheres for improved solar-driven CO2 reduction performance
Lina Li, Yi Zhang, Gaopeng Liu, Tiange Wei, Junze Zhao, Bin Wang, Mengxia Ji, Yuanbin She, Jiexiang Xia, Huaming Li
, Available online  , doi: 10.1016/j.gee.2024.01.008
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CO2 photoreduction into carbon-based chemicals has been considered as an appropriate way to alleviate the energy issue and greenhouse effect. Herein, the 5, 10, 15, 20-tetra (4-carboxyphenyl) porphyrin cobalt(II) (CoTCPP) has been integrated with BiOBr microspheres and formed the CoTCPP/BiOBr composite. The as-prepared CoTCPP/BiOBr-2 shows optimized photocatalytic performance for CO2 conversion into CO and CH4 upon irradiation with 300 W Xe lamp, which is 2.03 and 2.58 times compared to that of BiOBr, respectively. The introduced CoTCPP significantly enhanced light absorption properties, promoted rapid separation of photogenerated carriers and boosted the chemisorption of CO2 molecules. The metal Co2+ at the center of the porphyrin molecules also acts as adsorption center for CO2 molecules, boosting the CO2 convert into CO and CH4. The possible mechanism of CO2 photoreduction was explored by in-situ FT-IR spectra. This work offers a new possibility for the preparation of advance photocatalysts.
Industrial solid wastes to environmental protection materials for removal of gaseous pollutants: A review
Jiacheng Bao, Xin Sun, Ping Ning, Kai Li, Jie Yang, Fei Wang, Lei Shi, Maohong Fan
, Available online  , doi: 10.1016/j.gee.2024.01.006
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The application of industrial solid wastes as environmentally functional materials for air pollutants control has gained much attention in recent years due to its potential to reduce air pollution in a cost-effective manner. In this review, we investigate the development of industrial-waste-based functional materials for various gas pollutant removal and consider the relevant reaction mechanism according to different types of industrial solid waste. We see a recent effort towards achieving high-performance environmental functional materials via chemical or physical modification, in which the active components, pore size, and phase structure can be altered. The review will discuss the potential of using industrial solid wastes, these modified materials, or synthesized materials from raw waste precursors for the removal of air pollutants, including SO2, NOx, Hg0, H2S, VOCs, and CO2. The challenges still need to be addressed to realize this potential and the prospects for future research fully. The suggests for future directions include determining the optimal composition of these materials, calculating the real reaction rate and turnover frequency, developing effective treatment methods, and establishing chemical component databases of raw industrial solid waste for catalysts/adsorbent preparation.
Hybrid Data-Driven and Physics-Based Modeling for Viscosity Prediction of Ionic Liquids
Jing Fan, Zhengxing Dai, Jian Cao, Liwen Mu, Xiaoyan Ji, Xiaohua Lu
, Available online  , doi: 10.1016/j.gee.2024.01.007
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Viscosity is one of the most important fundamental properties of fluids. However, accurate acquisition of viscosity for ionic liquids (ILs) remains a critical challenge. In his study, an approach integrating prior physical knowledge into the machine learning ML) model was proposed to predict the viscosity reliably. The method was based on 16 quantum chemical descriptors determined from the first principles calculations and used as the input of the ML models to represent the size, structure, and interactions of he ILs. Three strategies based on the residuals of the COSMO-RS model were created as the output of ML, where the strategy directly using experimental data was also studied for comparison. The performance of six ML algorithms was compared in all strategies, and the CatBoost model was identified as the optimal one. The strategies employing the relative deviations were superior to that using the absolute deviation, and the relative ratio revealed the systematic prediction error of the COSMO-RS model. The CatBoost model based on the relative ratio achieved the highest prediction accuracy on the test set (R2 = 0.9999, MAE = 0.0325), reducing the average absolute relative deviation (AARD) in modeling from 52.45% to 1.54%. Features importance analysis indicated the average energy correction, solvation-free energy, and polarity moment were the key influencing the systematic deviation.
Reusable Salt-template Strategy for Synthesis of Porous Nitrogen-rich Carbon Boosts H2S Selective Oxidation
Xu Liu, Liang Shan, Xiaoxue Sun, Tianxin Wang, Zhongqing Liu, Yuefeng Liu
, Available online  , doi: 10.1016/j.gee.2024.01.005
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Removing hydrogen sulfide (H2S) via the selective oxidation has been considered an effective way to further purify the indusial sulfur-containing due to it can completely transform residual H2S into elemental sulfur. While N-doped porous carbon was applied to H2S selective oxidation, a sustainable methodology for the synthesis of efficient and stable N-doped carbon catalysts remains a difficulty, limiting its future development in large-scale applications. Herein, we present porous, honeycomb-like N-doped carbon catalysts with large specific surface areas, high pyridinic N content, and numerous structural defects for H2S selective oxidation prepared using reusable NaCl as the template. The as-prepared NC-10-800 catalyst exhibits excellent catalytic performance (sulfur formation rate of 784 gsulfur·kgcat.-1·h-1), outstanding stability (> 100 h), and excellent anti-water vapor, anti-CO2 and anti-oxidation properties, suggesting significant potential for practical industrial application. The characterization results and kinetic study demonstrate that the large surface areas and structural defects created by the molten salt at high temperature enhance the exposure of pyridinic N sites and thus accelerate the catalytic activity. Importantly, the water-soluble NaCl template could be easily washed from the carbon nanomaterials, and thus the downstream salt-containing wastewater could be subsequently reused for the dissolution of carbon precursors. This environment-friendly, low-cost, reusable salt-template strategy has significant implications for the development of N-doped carbon catalysts for practical applications.
Application of ionic liquids in single-molecule junctions: Recent advances and prospects
Li Zhou, Miao Zhang, Yani Huo, Liping Bai, Suhang He, Jinying Wang, Chuancheng Jia, Xuefeng Guo
, Available online  , doi: 10.1016/j.gee.2024.01.003
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Single-molecule junctions, integrating individual molecules as active components between electrodes, serve as fundamental building blocks for advanced electronic and sensing technologies. The application of ionic liquids in single-molecule junctions represents a cutting-edge and rapidly evolving field of research at the intersection of nanoscience, materials chemistry, and electronics. This review explores recent advances where ionic liquids function as electrolytes, dielectric layers, and structural elements within single-molecule junctions, reshaping charge transport, redox reactions, and molecular behaviors in these nanoscale systems. We comprehensively dissect fundamental concepts, techniques, and modulation mechanisms, elucidating the roles of ionic liquids as gates, electrochemical controllers, and interface components in single-molecule junctions. Encompassing applications from functional device construction to unraveling intricate chemical reactions, this review maps the diverse applications of ionic liquids in single-molecule junctions. Moreover, we propose critical future research topics in this field, including catalysis involving ionic liquids at the single-molecule level, functionalizing single-molecule devices using ionic liquids, and probing the structure and interactions of ionic liquids. These endeavors aim to drive technological breakthroughs in nanotechnology, energy, and quantum research.
Constructing interfacial electric field and Zn vacancy modulated ohmic junctions ZnS/NiS for photocatalytic H2 evolution
Yi-lei Li, Xu-jia Liu, Yun-biao Wang, Ying Liu, Rui-hong Liu, Hui-ying Mu, Ying-juan Hao, Xiao-jing Wang, Fa-tang Li
, Available online  , doi: 10.1016/j.gee.2023.12.007
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Adjusting the interfacial transport efficiency of photogenerated electrons and the free energy of hydrogen adsorption through interface engineering is an effective means of improving the photocatalytic activity of semiconductor photocatalysts. Herein, hollow ZnS/NiS nanocages with ohmic contacts containing Zn vacancy (VZn-ZnS/NiS) are synthesized using ZIF-8 as templates. An internal electric field is constructed by Fermi level flattening to form ohmic contacts, which increase donor density and accelerate electron transport at the VZn-ZnS/NiS interface. The experimental and DFT results show that the tight interface and VZn can rearrange electrons, resulting in a higher charge density at the interface, and optimizing the Gibbs free energy of hydrogen adsorption. The optimal hydrogen production activity of VZn-ZnS/NiS is 10636 μmol h-1 g-1, which is 31.9 times that of VZn-ZnS. This study provides an idea for constructing sulfide heterojunctions with ohmic contacts and defects to achieve efficient photocatalytic hydrogen production.
Efficient nitric oxide capture and reduction on Ni-loaded CHA zeolites
Bin Yue, Jianhua Wang, Shanshan Liu, Guangjun Wu, Bin Qin, Landong Li
, Available online  , doi: 10.1016/j.gee.2023.12.005
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As a prominent contributor to air pollution, nitric oxide (NO) has emerged as a critical agent causing detrimental environmental and health ramifications. To mitigate emissions and facilitate downstream utilization, adsorption-based techniques offer a compelling approach for direct NO capture from both stationary and mobile sources. In this study, a comprehensive exploration of NO capture under oxygen-lean and oxygen-rich conditions was conducted, employing Ni ion-exchanged chabazite (CHA-type) zeolites as the adsorbents. Remarkably, Ni/Na-CHA zeolites, with Ni loadings ranging from 3 to 4 wt%, demonstrate remarkable dynamic uptake capacities and exhibit exceptional NO capture efficiencies (NO-to-Ni ratio) for both oxygen-lean (0.17–0.31 mmol/g, 0.32–0.43 of NO/Ni) and oxygen-rich (1.64–1.18 mmol/g) under ambient conditions. An NH3 reduction methodology was designed for the regeneration of absorbents at a relatively low temperature of 673 K. Comprehensive insights into the NO adsorption mechanism were obtained through temperature-programmed desorption experiments, in situ Fourier transform infrared spectroscopy, and density functional theory calculations. It is unveiled that NO and NO2 exhibit propensity to coordinate with Ni2+ via N-terminal or O-terminal, yielding thermally stable complexes and metastable species, respectively, while the low-temperature desorption substances are generated in close proximity to Na+. This study not only offers micro-level perspectives but imparts crucial insights for the advancement of capture and reduction technologies utilizing precious-metal-free materials.
Wood-derived freestanding integrated electrode with robust interface-coupling effect boosted bifunctionality for rechargeable zinc-air batteries
Benji Zhou, Nengneng Xu, Liangcai Wu, Dongqing Cai, Eileen H. Yu, Jinli Qiao
, Available online  , doi: 10.1016/j.gee.2023.12.002
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Fabricating non-noble metal-based carbon air electrodes with highly efficient bifunctionality is big challenge owing to the sluggish kinetics of oxygen reduction/evolution reaction (ORR/OER). The efficient cathode catalyst is urgently needed to further improve the performance of rechargeable zinc-air batteries. Herein, an activation-doping assisted interface modification strategy is demonstrated based on freestanding integrated carbon composite (CoNiLDH@NPC) composed of wood- based N and P doped active carbon (NPC) and CoNi layer double hydroxides (CoNiLDH). In the light of its large specific surface area and unique defective structure, CoNiLDH@NPC with strong interface-coupling effect in 2D-3D micro-nanostructure exhibits outstanding bifunctionality. Such carbon composites show half-wave potential of 0.85 V for ORR, overpotential of 320 mV with current density of 10 mA cm-2 for OER, and ultra-low gap of 0.70 V. Furthermore, highly-ordered open channels of wood provide enormous space to form abundant triple-phase boundary for accelerating the catalytic process. Consequently, Zinc-air batteries using CoNiLDH@NPC show high power density (aqueous: 263 mW cm-2, quasi-solid-state: 65.8 mW cm-2) and long-term stability (aqueous: 500 h, quasi-solid-state: 120 h). This integrated protocol opens a new avenue for the rational design of efficient freestanding air electrode from biomass resources.
Mechanochemical strategy assisted morphology recombination of COFs for promoted kinetics and LiPS transformation in Li-S batteries
Yunchen Ge, Yan Meng, Lin Liu, Jianming Li, Xuechun Huang, Dan Xiao
, Available online  , doi: 10.1016/j.gee.2023.03.005
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A covalent organic frameworks (COFs) material with regular pores and stable structure can be used as the host of lithium-sulfur batteries to improve battery kinetics and polysulfides conversion. Herein, we designed and synthesized two kinds of rod-liked bulk COFs by adjusting different pore sizes (COF-BTD and COF-TFB), unfortunately, the active sites masking and sluggish kinetics have not met our expectations. Generally, the available layered COFs prepared from mechanochemical can expose abundant active sites and favorable kinetics than bulk COFs. Thus, simple mechanical ball milling is applied to activate the above COFs (M-COFs group). It is worth noting that layered R-COF-BTD is directly synthesized from rod-liked precursors by simple morphological reconstruction. A series of characterization methods are used to systematically explore the advantages of the group of M-COFs@S electrodes in the cycling process, including the effects of specific morphology on the kinetics and transformation of polysulfides. Our research provides a feasible plan for the development and selection of the host material of lithium-sulfur batteries.
Potassium-doped hydrated manganese dioxide nanowires-carbon nanotube on graphene for high performance rechargeable zinc-ion battery
Ting-Hao Xu, Sin Liou, Fan-Lin Hou, Yuan-Yao Li
, Available online  , doi: 10.1016/j.gee.2021.10.006
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Aqueous rechargeable Zn-ion battery (ARZIB) is a great candidate for the next generation battery due to its high safety, low cost, and relatively high capacity. Here, we develop hydrated and potassium-doped manganese dioxide (MO) nanowires mixed with carbon nanotubes (CNT) on graphene substrates (hydrated KMO-CNT/graphene) for ARZIB. A simple polyol process (poly(ethyl glycol), KMnO4, CNTs, and graphene) is conducted to form the hydrated KMO-CNT/graphene. MnO2 nanowires with diameters of 15–25 nm have a high specific capacity with a short diffusion path. The intercalated K ions and hydrates in the layered MnO2 nanowires remain the MO structure during the charge and discharge process, while carbon nanomaterials (CNTs and graphene) enhance the conductivity of the materials. As a result, the hydrated KMOCNT/graphene demonstrates a good ARZIB performance. A high capacity of 359.8 mAh g-1 at 0.1 A g-1 can be achieved while, at a high current density of 3.0 A g-1, the capacity of 129 mAh g-1 can be obtained with 77% retention after 1000 cycles.

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