Green Energy&Environment

Recyclable bio-based epoxy resin thermoset polymer from wood for circular economy

Bowen Zhang, Saravanakumar Elangovan, Zhuohua Sun

2024, 9(12): 1781-1783. doi: 10.1016/j.gee.2024.08.007

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Due to their extraordinary durability and thermal stability, Epoxy Resin Thermosets (ERTs) are essential in various industries. However, their poor recyclability leads to unacceptable environmental pollution. In this study, Wu et al. successfully synthesized a completely bio-based ERT using lignocellulose-derived building blocks which exhibit outstanding thermal and mechanical properties. Remarkably, these bio-materials degrade via methanolysis without the need of any catalyst, presenting a smart and cost-effective 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.

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

2024, 9(12): 1784-1801. doi: 10.1016/j.gee.2024.01.003

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Single-molecule junctions, integrating individual molecules as active components between electrodes, serve as fundamental building blocks for advanced electronic and sensing technologies. The application of ionic liquids in single-molecule junctions represents a cutting-edge and rapidly evolving field of research at the intersection of nanoscience, materials chemistry, and electronics. This review explores recent advances where ionic liquids function as electrolytes, dielectric layers, and structural elements within single-molecule junctions, reshaping charge transport, redox reactions, and molecular behaviors in these nanoscale systems. We comprehensively dissect fundamental concepts, techniques, and modulation mechanisms, elucidating the roles of ionic liquids as gates, electrochemical controllers, and interface components in single-molecule junctions. Encompassing applications from functional device construction to unraveling intricate chemical reactions, this review maps the diverse applications of ionic liquids in single-molecule junctions. Moreover, we propose critical future research topics in this field, including catalysis involving ionic liquids at the single-molecule level, functionalizing single-molecule devices using ionic liquids, and probing the structure and interactions of ionic liquids. These endeavors aim to drive technological breakthroughs in nanotechnology, energy, and quantum research.

Melting points of ionic liquids: Review and evaluation

Zhengxing Dai, Lei Wang, Xiaohua Lu, Xiaoyan Ji

2024, 9(12): 1802-1811. doi: 10.1016/j.gee.2024.01.009

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The melting points of ionic liquids (ILs) reported since 2020 were surveyed, collected, and reviewed, which were further combined with the previous data to provide a database with 3129 ILs ranging from 177.15 to 645.9 K in melting points. In addition, the factors that affect the melting point of ILs from macro, micro, and thermodynamic perspectives were summarized and analyzed. Then the development of the quantitative structure-property relationship (QSPR), group contribution method (GCM), and conductor-like screening model for realistic solvents (COSMO-RS) for predicting the melting points of ILs were reviewed and further analyzed. Combined with the evaluation together with the preliminary study conducted in this work, it shows that COSMO-RS is more promising and possible to further improve its performance, and a framework was thus proposed.

Recent advances in water collection based on solar evaporation

Meijie Chen, Shuang Li, Shuai Guo, Hongjie Yan, Swee Ching Tan

2024, 9(12): 1812-1821. doi: 10.1016/j.gee.2024.05.005

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Solar evaporation attracted lots of attention due to its environment-friendly and high efficiency, which is a potential approach to collecting fresh water. Many efforts have been made to improve the evaporation rate in the open space. While the actual water collection rate is far less than the evaporation rate, especially in passive water collection, limiting its practical and scalable applications. In this review, we focus on freshwater collection based on solar evaporation. Firstly, heat and mass transfer behaviors on the evaporation side were summarized to improve evaporation performance, including heat transfer processes in thermal radiation, convection, and conduction; mass transfer processes in water supply, evaporation enthalpy, and salt rejection. Sequentially, subcooling, wettability, and geometry of the condensation side were discussed to improve water collection performance, which should be designed collaboratively with the evaporation side in a confined space. Finally, thermal recovery and electricity generation beyond water collection were also introduced, and some challenges still need to improve in the further for scalable and practical applications, including passive water collection rate, integrated system, and long-term issues.

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

2024, 9(12): 1822-1834. doi: 10.1016/j.gee.2023.03.005

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A covalent organic frameworks (COFs) material with regular pores and stable structure can be used as the host of lithium-sulfur batteries to improve battery kinetics and polysulfides conversion. Herein, we designed and synthesized two kinds of rod-liked bulk COFs by adjusting different pore sizes (COF-BTD and COF-TFB), unfortunately, the active sites masking and sluggish kinetics have not met our expectations. Generally, the available layered COFs prepared from mechanochemical can expose abundant active sites and favorable kinetics than bulk COFs. Thus, simple mechanical ball milling is applied to activate the above COFs (M-COFs group). It is worth noting that layered R–COF–BTD is directly synthesized from rod-liked precursors by simple morphological reconstruction. A series of characterization methods are used to systematically explore the advantages of the group of M-COFs@S electrodes in the cycling process, including the effects of specific morphology on the kinetics and transformation of polysulfides. Our research provides a feasible plan for the development and selection of the host material of lithium-sulfur batteries.

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

2024, 9(12): 1835-1846. doi: 10.1016/j.gee.2023.12.002

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Fabricating non-noble metal-based carbon air electrodes with highly efficient bifunctionality is big challenge owing to the sluggish kinetics of oxygen reduction/evolution reaction (ORR/OER). The efficient cathode catalyst is urgently needed to further improve the performance of rechargeable zinc-air batteries. Herein, an activation-doping assisted interface modification strategy is demonstrated based on freestanding integrated carbon composite (CoNiLDH@NPC) composed of wood-based N and P doped active carbon (NPC) and CoNi layer double hydroxides (CoNiLDH). In the light of its large specific surface area and unique defective structure, CoNiLDH@NPC with strong interface-coupling effect in 2D-3D micro-nanostructure exhibits outstanding bifunctionality. Such carbon composites show half-wave potential of 0.85 V for ORR, overpotential of 320 mV with current density of 10 mA cm^-2 for OER, and ultra-low gap of 0.70 V. Furthermore, highly-ordered open channels of wood provide enormous space to form abundant triple-phase boundary for accelerating the catalytic process. Consequently, zinc-air batteries using CoNiLDH@NPC show high power density (aqueous: 263 mW cm^-2, quasi-solid-state: 65.8 mW cm^-2) and long-term stability (aqueous: 500 h, quasi-solid-state: 120 h). This integrated protocol opens a new avenue for the rational design of efficient freestanding air electrode from biomass resources.

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

2024, 9(12): 1847-1856. doi: 10.1016/j.gee.2023.12.007

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Adjusting the interfacial transport efficiency of photogenerated electrons and the free energy of hydrogen adsorption through interface engineering is an effective means of improving the photocatalytic activity of semiconductor photocatalysts. Herein, hollow ZnS/NiS nanocages with ohmic contacts containing Zn vacancy (V_Zn-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 V_Zn-ZnS/NiS interface. The experimental and DFT results show that the tight interface and V_Zn 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 V_Zn-ZnS/NiS is 10,636 μmol h^-1 g^-1, which is 31.9 times that of V_Zn-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

2024, 9(12): 1857-1865. doi: 10.1016/j.gee.2023.12.005

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As a prominent contributor to air pollution, nitric oxide (NO) has emerged as a critical agent causing detrimental environmental and health ramifications. To mitigate emissions and facilitate downstream utilization, adsorption-based techniques offer a compelling approach for direct NO capture from both stationary and mobile sources. In this study, a comprehensive exploration of NO capture under oxygen-lean and oxygen-rich conditions was conducted, employing Ni ion-exchanged chabazite (CHA-type) zeolites as the adsorbents. Remarkably, Ni/Na-CHA zeolites, with Ni loadings ranging from 3 to 4 wt%, demonstrate remarkable dynamic uptake capacities and exhibit exceptional NO capture efficiencies (NO-to-Ni ratio) for both oxygen-lean (0.17–0.31 mmol/g, 0.32–0.43 of NO/Ni) and oxygen-rich (1.64–1.18 mmol/g) under ambient conditions. An NH₃ reduction methodology was designed for the regeneration of absorbents at a relatively low temperature of 673 K. Comprehensive insights into the NO adsorption mechanism were obtained through temperature-programmed desorption experiments, in situ Fourier transform infrared spectroscopy, and density functional theory calculations. It is unveiled that NO and NO₂ exhibit propensity to coordinate with Ni²⁺ via N-terminal or O-terminal, yielding thermally stable complexes and metastable species, respectively, while the low-temperature desorption substances are generated in close proximity to Na⁺. This study not only offers micro-level perspectives but imparts crucial insights for the advancement of capture and reduction technologies utilizing precious-metal-free materials.

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

2024, 9(12): 1866-1877. doi: 10.1016/j.gee.2024.01.005

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Removing hydrogen sulfide (H₂S) via the selective oxidation has been considered an effective way to further purify the indusial sulfur-containing due to it can completely transform residual H₂S into elemental sulfur. While N-doped porous carbon was applied to H₂S selective oxidation, a sustainable methodology for the synthesis of efficient and stable N-doped carbon catalysts remains a difficulty, limiting its future development in large-scale applications. Herein, we present porous, honeycomb-like N-doped carbon catalysts with large specific surface areas, high pyridinic N content, and numerous structural defects for H₂S selective oxidation prepared using reusable NaCl as the template. The as-prepared NC-10-800 catalyst exhibits excellent catalytic performance (sulfur formation rate of 784 g_sulfur kg_cat.^-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.

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

2024, 9(12): 1878-1890. doi: 10.1016/j.gee.2024.01.007

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Viscosity is one of the most important fundamental properties of fluids. However, accurate acquisition of viscosity for ionic liquids (ILs) remains a critical challenge. In this 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 the 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.

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

2024, 9(12): 1891-1900. doi: 10.1016/j.gee.2024.05.008

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An artificial solid electrolyte interphase (SEI) with lithiophilic sites and chemical bonds anchoring lithium polysulfides (LiPSs) has been developed as a potential solution to protect the lithium (Li) metal anode of Lithium-sulfur (Li–S) batteries. This strategy aims to guide consistent Li deposition and relieve lithium corrosion. Herein, the evolution process of lithiophilic sites based on aluminum fluoride (AlF₃) in an artificial SEI is disclosed in Li–S batteries with metal-based lithiophilic sites. The polyester polymer (PMMA and PPC)/AlF₃ artificial SEI (MPAF-SEI) was homogeneously anchored on Li anode by in-situ polymerization. The conversion of AlF₃ into Li–Al and LiF lithiophilic sites effectively reduce the Li nucleation overpotential and prevents the formation of Li dendrites. At the same time, the polymer can anchor LiPSs by chemical bonds and prevents Li corrosion. The optimized MPAF-SEI protected Li demonstrates excellent stability for over 3000 h 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.

2024 Vol. 9, No. 12

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