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).
Display Method:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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.
Perspectives on aqueous organic redox flow batteries
Fulong Zhu, Qiliang Chen, Yongzhu Fu
, Available online  , doi: 10.1016/j.gee.2024.08.003
Abstract HTML PDF
Abstract:
Aqueous organic redox flow batteries (AORFBs) have pioneered new routes for largescale energy storage. The tunable nature of redox-active organic molecules provides a robust foundation for creating innovative AORFBs with exceptional performance. Molecular engineering endows various organic molecules with considerable advantages in solubility, stability, and redox potential. Advanced characterizations have enabled a comprehensive understanding of the redox reaction and degradation mechanisms of these organic molecules. Computational chemistry and machine learning have guided the development of new organic molecules. The practical application of AORFBs will depend on the complementary efforts of multiple parties. This paper consolidates the current design principles of molecular engineering, degradation mechanisms, characterization techniques, and the utilization of computational chemistry. It also offers perspectives and forecasts the necessary attributes and strategic efforts for the next-generation AORFBs, aiming to provide the research community with a deeper understanding.
CO2 mineralization by typical industrial solid wastes for preparing ultrafine CaCO3: A review
Run Xu, Fuxia Zhu, Liang Zou, Shuqing Wang, Yanfang Liu, Jili Hou, Chenghao Li, Kuntong Song, Lingzhao Kong, Longpeng Cui, Zhiqiang Wang
, Available online  , doi: 10.1016/j.gee.2024.08.002
Abstract HTML PDF
Abstract:
Mineral carbonation is a promising CO2 sequestration strategy that can utilize industrial wastes to convert CO2 into high-value CaCO3. This review summarizes the advancements in CO2 mineralization using typical industrial wastes to prepare ultrafine CaCO3. This work surveys the mechanisms of CO2 mineralization using these wastes and its capacities to synthesize CaCO3, evaluates the effects of carbonation pathways and operating parameters on the preparation of CaCO3, analyzes the current industrial application status and economics of this technology. Due to the large amount of impurities in solid wastes, the purity of CaCO3 prepared by indirect methods is greater than that prepared by direct methods. Crystalline CaCO3 includes three polymorphs. The polymorph of CaCO3 synthesized by carbonation process is determined the combined effects of various factors. These parameters essentially impact the nucleation and growth of CaCO3 by altering the CO2 supersaturation in the reaction system and the surface energy of CaCO3 grains. Increasing the initial pH of the solution and the CO2 flow rate favors the formation of vaterite, but calcite is formed under excessively high pH. Vaterite formation is favored at lower temperatures and residence time. With increased temperature and prolonged residence time, it passes through aragonite metastable phase and eventually transforms into calcite. Moreover, polymorph modifiers can decrease the surface energy of CaCO3 grains, facilitating the synthesis of vaterite. However, the large-scale application of this technology still faces many problems, including high costs, high energy consumption, low calcium leaching rate, low carbonation efficiency, and low product yield. Therefore, it is necessary to investigate ways to accelerate carbonation, optimize operating parameters, develop cost-effective agents, and understand the kinetics of CaCO3 nucleation and crystallization to obtain products with specific crystal forms. Furthermore, more studies on life cycle assessment (LCA) should be conducted to fully confirm the feasibility of the developed technologies.
Mechano-driven chemical reactions
Shaoxin Li, Jiajin Liu, Zhong Lin Wang, Di Wei
, Available online  , doi: 10.1016/j.gee.2024.08.001
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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.
Solar-assisted two-stage catalytic membrane reactor for coupling CO2 splitting with methane oxidation reaction
Jinkun Tan, Zhenbin Gu, Zhengkun Liu, Pei Wang, Reinout Meijboom, Guangru Zhang, Wanqin Jin
, Available online  , doi: 10.1016/j.gee.2024.07.006
Abstract HTML PDF
Abstract:
A two-stage catalytic membrane reactor (CMR) that couples CO2 splitting with methane oxidation reactions was constructed based on an oxygen-permeable perovskite asymmetric membrane. The asymmetric membrane comprises a dense SrFe0.9Ta0.1O3-δ (SFT) separation layer and a porous Sr0.9(Fe0.9Ta0.1)0.9Cu0.1O3-δ (SFTC) catalytic layer. In the first stage reactor, a CO2 splitting reaction (CDS: 2CO2→2CO+O2) occurs at the SFTC catalytic layer. Subsequently, the O2 product is selectively extracted through the SFT separation layer to the permeated side for the methane combustion reaction (MCR), which provides an extremely low oxygen partial pressure to enhance the oxygen extraction. In the second stage, a Sr0.9(Fe0.9Ta0.1)0.9Ni0.1O3-δ (SFTN) catalyst is employed to reform the products derived from MCR. The two-stage CMR design results in a remarkable 35.4% CO2 conversion for CDS at 900 °C. The two-stage CMR was extended to a hollow fiber configuration combining with solar irradiation. The solar-assisted two-stage CMR can operate stably for over 50 hours with a high hydrogen yield of 18.1 mL min-1 cm-2. These results provide a novel strategy for reducing CO2 emissions, suggesting potential avenues for the design of the high-performance CMRs and catalysts based on perovskite oxides in the future.
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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.
MOF Synthesis using Waste PET for Applications of Adsorption, Catalysis and Energy Storage
Hongmei Li, Jinming Lei, Liying Zhu, Yanling Yao, Yuanhua Li, Tianhao Li, Chuntian Qiu
, Available online  , doi: 10.1016/j.gee.2024.06.003
Abstract HTML PDF
Abstract:
Polyethylene terephthalate (PET) as one of non-degradable wastes has become a huge threat to the environment and human health. Chemical Recycle of PET is an sustainable way to release 1,4-benzenedicarboxylic acid (BDC) the monomer of PET as common used organic linker for synthesis of functional Metal-organicframeworks (PET-derived MOFs) such as UiO-66, MIL-101, etc. This sustainable and cost-effective “Waste-to-MOFs” model is of great significant to be intensively investigated in the past years. Attributes of substantial porosity, specific surface area, exposed metal centers, uniform structure, and flexible morphology render PET-derived MOFs are well-suited for applications in adsorption, energy storage, catalysis, among others. Herein, in the present work, we have summarized recent advances in synthesis of PET-derived MOFs using ex-situ and in-situ methods for typical applications of adsorption, catalysis and energy storage. Despite those improvements in synthesis methods and potential applications, challenges still remain in development of green and economical routes to fully utilize waste PET for massive manufacture of valuable MOF materials and chemicals. This review provides insights into the conversion of nondegradable PET waste to value-added MOF materials, and further suggests promising perspectives to develop the sustainable “Waste-to-MOFs” model in addressing environmental pollution and energy crises.
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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.
Ultrasonic enhancement of persulfate oxidation system governs emerging pollutants decontamination
Yanpan Li, Yanbo Zhou, Yi Zhou
, Available online  , doi: 10.1016/j.gee.2024.01.004
Abstract HTML PDF
Abstract:
Emerging contaminants (ECs) are widely present in aquatic environments, posing potential risks to both ecosystems and human health. The ultrasound-assisted persulfate oxidation process has attracted considerable attention in the degradation of ECs due to its ability to generate both sulfate radicals and cavitation effects, enhancing degradation effects. In this paper, the principle of ultrasonic synergistic Fenton-like oxidation system for degrading organic pollutants was reviewed, divided into homogeneous system, non-homogeneous system, and single-atom system to explore the synergistic effect of ultrasound-enhanced persulfate technology in three aspects, and the effects of environmental factors such as ultrasonic frequency and power, system pH, temperature, and initial oxidant concentration on the system's decontamination performance were discussed. Finally, future research on ultrasonically activated persulfate technology is summarized and prospected.
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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
Abstract HTML PDF
Abstract:
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.
The transition from 2G to 3G-feedstocks enabled efficient production of fuels and chemicals
Kai Wang, Changsheng Su, Haoran Bi, Changwei Zhang, Di Cai, Yanhiu Liu, Meng Wang, Biqiang Chen, Jens Nielsen, Zihe Liu, Tianwei Tan
, Available online  , doi: 10.1016/j.gee.2023.11.004
Abstract HTML PDF
Abstract:
For decades micoorganisms have been engineered for the utilization of lignocellulose-based second-generation (2G) feedstocks, but with the concerns of increased levels of atmospheric CO2 causing global warming there is an emergent need to transition from the utilization of 2G feedstocks to third-generation (3G) feedstocks such as CO2 and its derivatives. Here, we established a yeast platform that is capable of simultaneously converting 2G and 3G feedstocks into bulk and value- added chemicals. We demonstrated that by adopting 3G substrates such as CO2 and formate, the conversion of 2G feedstocks could be substantially improved. Specifically, formate could provide reducing power and energy for xylose conversion into valuable chemicals. Simultaneously, it can form a concentrated CO2 pool inside the cell, providing thermodynamically and kinetically favoured amounts of precursors for CO2 fixation pathways, e.g. the Calvin–Benson–Bassham (CBB) cycle. Furthermore, we demonstrated that formate could directly be utilized as a carbon source by yeast to synthesize endogenous amino acids. The engineered strain achieved a one-carbon (C1) assimilation efficiency of 9.2%, which was the highest efficiency observed in the co-utilization of 2G and 3G feedstocks. We applied this strategy for productions of both bulk and value-added chemicals, including ethanol, free fatty acids (FFAs), and longifolene, resulting in yield enhancements of 18.4%, 49.0%, and ~100%, respectively. The strategy demonstrated here for co-utilization of 2G and 3G feedstocks sheds lights on both basic and applied research for the up-coming establishment of 3G biorefineries.
A Salt-induced Tackifying Polymer for Enhancing Oil Recovery in High Salinity Reservoirs: Synthesis, Evaluation, and Mechanism
Yining Wu, Peihan Li, Bin Yan, Xiaohan Li, Yongping Huang, Juncong Yuan, Xiang Feng, Caili Dai
, Available online  , doi: 10.1016/j.gee.2023.10.006
Abstract HTML PDF
Abstract:
Polymer flooding is an effective method widely applied for enhancing oil recovery (EOR) by reducing the mobility ratio between the injected water and crude oil. However, traditional polymers encounter challenges in high salinity reservoirs due to their salt sensitivity. To overcome this challenge, we synthesized a zwitterion polymer (PAMNS) with salt-induced tackifying property through copolymerization of acrylamide and a zwitterion monomer, methylacrylamide propyl-N, Ndimethylbutylsulfonate (NS). NS monomer is obtained from the reaction between 1,4-butanesultone and dimethylamino propyl methylacrylamide. In this study, the rheological properties, salt responsiveness, and EOR efficiency of PAMNS were evaluated. Results demonstrate that PAMNS exhibits desirable salt-induced tackifying characteristics, with viscosity increasing up to 2.4 times as the NaCl concentration reaches a salinity of 30 ×104mg L-1. Furthermore, high valence ions possess a much stronger effect on enhancing viscosity, manifested as Mg2+ > Ca2+ > Na+. Molecular dynamics simulations (MD) and fluid dynamics experiment results demonstrate that PAMNS molecules exhibit a more stretched state and enhanced intermolecular associations in high-salinity environments. It is because of the salt-induced tackifying, PAMNS demonstrates superior performance in polymer flooding experiments under salinity ranges from 5 ×104mg L-1 to 20 ×104mg L-1, leading to 10.38-19.83% higher EOR than traditional polymers.
Outstanding proton conductivity over wide temperature and humidity ranges and enhanced mechanical, thermal stabilities for surface-modified MIL-101-Cr-NH2/Nafion composite membranes
Xu Li, Dongwei Zhang, Si Chen, Yingzhao Geng, Yong Liu, Libing Qian, Xi Chen, Jingjing Li, Pengfei Fang, Chunqing He
, Available online  , doi: 10.1016/j.gee.2023.10.007
Abstract HTML PDF
Abstract:
High-performance proton exchange membranes are of great importance for fuel cells. Here, we have synthesized polycarboxylate plasticizer modified MIL-101-Cr-NH2(PCP-MCN), a kind of hybrid metal-organic framework, which exhibits a superior proton conductivity. PCP-MCN nanoparticles are used as additives to fabricate PCP-MCN/Nafion composite membranes. Microstructures and characteristics of PCP-MCN and these membranes have been extensively investigated. Significant enhancement in proton conduction for PCP-MCN around 55 °C is interestingly found due to the thermal motion of the PCP molecular chains. Robust mechanical properties and higher thermal decomposition temperature of the composite membranes are directly ascribed to strong intermolecular interactions between PCP-MCN and Nafion side chains, i.e. the formation of substantial acid-base pairs (-SO3-…+H-NH-), which further improves compatibility between additive and Nafion matrix. At the same humidity and temperature condition, the water uptake of composite membranes significantly increases due to the incorporation of porous additives with abundant functional groups and thus less crystallinity degree in comparison to pristine Nafion. Proton conductivity (σ) over wide ranges of humidities (30 - 100% RH at 25 °C) and temperatures (30 - 98 °C at 100% RH) for prepared membranes is measured. The σ in PCP-MCN/Nafion composite membranes is remarkably enhanced, i.e. 0.245 S/cm for PCP-MCN-3wt.%/Nafion is twice that of Nafion membrane at 98 °C and 100% RH, because of the establishment of well- interconnected proton transport ionic water channels and perhaps faster protonation-deprotonation processes. The composite membranes possess weak humidity-dependence of proton transport and higher water uptake due to excellent water retention ability of PCP-MCN. In particular, when 3 wt.% PCP-MCN was added to Nafion, the power density of a single-cell fabricated with this composite membrane reaches impressively 0.480, 1.098 W/cm2 under 40% RH, 100% RH at 60 °C, respectively, guaranteeing it to be a promising proton exchange membrane.
Interface defect induced upgrade of K-storage properties in KFeSO4F cathode: from lowered Fe-3d orbital energy level to advanced potassium-ion batteries
Yan Liu, Zhen-Yi Gu, Yong-Li Heng, Jin-Zhi Guo, Miao Du, Hao-Jie Liang, Jia-Lin Yang, Kai-Yang Zhang, Kai Li, Xing-Long Wu
, Available online  , doi: 10.1016/j.gee.2023.10.004
Abstract HTML PDF
Abstract:
KFeSO4F (KFSF) is considered a potential cathode due to the large capacity and low cost. However, the inferior electronic conductivity leads to poor electrochemical performance. Defect engineering can facilitate the electron/ion transfer by tuning electronic structure, thus providing favorable electrochemical performance. Herein, through the regulation of surface defect engineering in reduced graphene oxide (rGO), the Fe-C bonds were formed between KFSF and rGO. The Fe-C bonds formed work in regulating the Fe-3d orbital as well as promoting the migration ability of K ions and increasing the electronic conductivity of KFSF. Thus, the KFSF@rGO delivers a high capacity of 119.6 mAh g-1. When matched with a graphite@pitch-derived S-doped carbon anode, the full cell delivers an energy density of 250.5 Wh kg-1 and a capacity retention of 81.5% after 400 cycles. This work offers a simple and valid method to develop high-performance cathodes by tuning defect sites.
Highly defective HKUST-1 with excellent stability and SO2 uptake: The hydrophobic armor effect of functionalized ionic liquids
Ping Liu, Kaixing Cai, Keliang Wang, Tianxiang Zhao, Duan-Jian Tao
, Available online  , doi: 10.1016/j.gee.2023.10.003
Abstract HTML PDF
Abstract:

Water stability is one of the most important factors restricting the practical application of metal organic frameworks (MOFs). In this work, we fabricate a highly defective HKUST-1 framework with a mixed valence of CuI/CuII by mechanical ball milling method. This defective HKUST-1 is embellished by functionalized ionic liquids as hydrophobic armor, making the hybrid HIL1@HKUST-1 exhibits outstanding water stability, remarkable SO2 adsorption (up to 5.71 mmol·g-1), and record-breaking selectivity (1070 for SO2/CO2 and 31515 for SO2/N2) at 25℃ and 0.1 bar, even in wet conditions.
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
Abstract HTML PDF
Abstract:
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.
Biomass-enhanced Janus sponge-like hydrogel with salt resistance and high strength for efficient solar desalination
Aqiang Chu, Meng Yang, Juanli Chen, Jinmin Zhao, Jing Fang, Zhensheng Yang, Hao Li
, Available online  , doi: 10.1016/j.gee.2023.04.003
Abstract HTML PDF
Abstract:
Interfacial solar-driven evaporation technology shows great potential in the field of industrial seawater desalination, and the development of efficient and low-cost evaporation materials is key to achieving large-scale applications. Hydrogels are considered to be promising candidates; however, conventional hydrogel-based interfacial solar evaporators have difficulty in simultaneously meeting multiple requirements, including a high evaporation rate, salt resistance, and good mechanical properties. In this study, a Janus sponge-like hydrogel solar evaporator (CPAS) with excellent comprehensive performance was successfully constructed. The introduction of biomass agar (AG) into the polyvinyl alcohol (PVA) hydrogel backbone reduced the enthalpy of water evaporation, optimized the pore structure, and improved the mechanical properties. Meanwhile, by introducing hydrophobic fumed nano-silica aerogel (SA) and a synergistic foaming-crosslinking process, the hydrogel spontaneously formed a Janus structure with a hydrophobic surface and hydrophilic bottom properties. Based on the reduction of the evaporation enthalpy and the modulation of the pore structure, the CPAS evaporation rate reached 3.56 kg m-2 h-1 under one sun illumination. Most importantly, owing to the hydrophobic top surface and 3D-interconnected porous channels, the evaporator could work stably in high concentrations of salt-water (25 wt% NaCl), showing strong salt resistance. Efficient water evaporation, excellent salt resistance, scalable preparation processes, and low-cost raw materials make CPAS extremely promising for practical applications.
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
Abstract HTML PDF
Abstract:
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.

Publish With GEE

Contact

  • Email：gee@ipe.ac.cn
  • Tel：010-82627075
  • Address：North 2nd street, Zhongguancun, Haidian District, Beijing, China

Links

京ICP备10002620号-1京公网安备 11010802039050号

Supported by: Beijing Renhe Information Technology Co. Ltd