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Low-coordination Nanocrystalline Copper-based Catalysts through Theory-guided Electrochemical Restructuring for Selective CO2Reduction to Ethylene

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Angewandte Chemie 2024年第16期136卷

作者： Wensheng Fang Ruihu Lu Fu-Min Li Chaohui He Dan Wu Kaihang Yue Yu Mao Wei Guo Bo You Fei Song Tao Yao Ziyun Wang Prof. Bao Yu Xia School of Chemistry and Chemical Engineering State Key Laboratory of Materials Processing and Die & Mould Technology Key Laboratory of Material Chemistry for Energy Conversion and Storage (Ministry of Education) Hubei Key Laboratory of Material Chemistry and Service Failure Wuhan National Laboratory for Optoelectronics Huazhong University of Science and Technology (HUST) 1037 Luoyu Rd Wuhan 430074 China School of Chemical Sciences University of Auckland Auckland 1010 New Zealand National Synchrotron Radiation Laboratory University of Science and Technology of China Hefei 230029 P. R. China CAS Key Laboratory of Materials for Energy Conversion Shanghai Institute of Ceramics Chinese Academy of Sciences (SICCAS) Shanghai 200050 China Shanghai Synchrotron Radiation Facility Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201800 China

Revealing the dynamic reconstruction process and tailoring advanced copper (Cu) catalysts is of paramount significance for promoting the conversion of CO 2 into ethylene (C 2 H 4 ), paving the way for carbon neutralization and facilitating renewable energy storage. In this study, we initially employed density functional theory (DFT) and molecular dynamics (MD) simulations to elucidate the restructuring behavior of a catalyst under electrochemical conditions and delineated its restructuring patterns. Leveraging insights into this restructuring behavior, we devised an efficient, low-coordination copper-based catalyst. The resulting synthesized catalyst demonstrated an impressive Faradaic efficiency (FE) exceeding 70 % for ethylene generation at a current density of 800 mA cm −2 . Furthermore, it showed robust stability, maintaining consistent performance for 230 hours at a cell voltage of 3.5 V in a full-cell system. Our research not only deepens the understanding of the active sites involved in designing efficient carbon dioxide reduction reaction (CO 2 RR) catalysts but also advances CO 2 electrolysis technologies for industrial application.

关键词： Carbon dioxide reduction Restructuring behavior Cu catalyst Ethylene Low coordination number

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Fibrous chitosan/cellulose composite as an efficient adsorbent for Co(Ⅱ) removal

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Journal of Cleaner Production 2021年 285卷

作者： Shuting Zhuang Kunkun Zhu Jianlong Wang Collaborative Innovation Center for Advanced Nuclear Energy Technology INET Tsinghua University Beijing 100084 PR China State Key Laboratory of New Textile Materials and Advanced Processing Technologies Wuhan Textile University Wuhan 430200 PR China Beijing Key Laboratory of Radioactive Waste Treatment INET Tsinghua University Beijing 100084 PR China

With the rapid development of industries, the heavy metal-containing wastewater has become one of the most serious environmental problems. Adsorption is a key approach in treating heavy metal-containing wastewater. The performance of adsorbents is determined by the effective exposure of its adsorptive sites, which determines its adsorption capacity . In this study, fibrous chitosan/cellulose composite was prepared using the wet-spinning method to increase its specific surface area, thus enhancing the adsorption capacity. The as-prepared fibrous composite showed a homogeneous fiber structure (diameter: 88 ± 16 μm) and high specific surface area (2.5 m 2 g −1 ). Furthermore, the adsorption capacity towards Co(Ⅱ) was greatly enhanced, more than three times higher than that of the pure chitosan beads (diameter: 2–3 mm). The maximum adsorption capacity was calculated to be 23.6 ± 2.5 mg-Co(Ⅱ) per g-chitosan by the Langmuir isotherm model, an order of magnitude higher than that of pure chitosan beads. In addition, the adsorption kinetic behavior of chitosan/cellulose fibers on Co(Ⅱ) followed the pseudo second-order kinetic model . The optimal pH for Co(Ⅱ) removal was approximately 6.0. Furthermore, FT-IR and XPS analyses indicated the amino groups played a dominant role, with the aid of hydroxyl groups, in the coordination and adsorptive removal of Co(II). Possible interaction configurations were also proposed in this study. In conclusion, the proposed physical modification of chitosan greatly improved its adsorption capacity and mechanical strength, making it a promising biosorbent for Co(II) removal.

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Highly Textured N-Type SnSe Polycrystals with Enhanced Thermoelectric Performance

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研究（英文） 2020年第2期 267-276页

作者： Peng-Peng Shang Jinfeng Dong Jun Pei Fu-Hua Sun Yu Pan Huaichao Tang Bo-Ping Zhang Li-Dong Zhao Jing-Feng Li State Key Laboratory of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua UniversityBeijing 100084 China College of Chemistry and Material Science Shandong Agricultural University Tai'an 271018 China The Beijing Municipal Key Laboratory of New Energy Materials and Technologies School of Materials Science and EngineeringUniversity of Science and Technology Beijing Beijing 100083 China School of Materials Science and Engineering Beihang University Beijing 100191 China

Thermoelectric materials,which directly convert heat into electricity based on the Seebeck effects,have long been investigated for use in semiconductor refrigeration or waste heat *** them,SnSe has attracted significant attention due to its promising performance in both p-type and n-type crystals;in particular,a higher out-of-plane ZT value could be achieved in n-type SnSe due to its 3D charge and 2D phonon *** this work,the thermoelectric transport properties of n-type polycrystalline SnSe were investigated with an emphasis on the out-of-plane transport through producing textural *** textures were fabricated using mechanical alloying and repeated spark plasma sintering (SPS),as a kind of hot pressing,aimed at producing strong anisotropic transports in n-type polycrystalline SnSe as that in crystalline *** show that the lowest thermal conductivity of 0.36Wm-1 K1 was obtained at 783K in perpendicular to texture ***,the electrical transport properties are less anisotropic and even nearly isotropic,and the power factors reach 681.3μWm-1 K-2 at 783 K along both parallel and perpendicular *** combination of large isotropic power factor and low anisotropic thermal conductivity leads to a maximum ZT of 1.5 at 783 *** high performance elucidates the outstanding electrical and thermal transport behaviors in n-type polycrystalline SnSe,and a higher thermoelectric performance can be expected with future optimizing texture in n-type polycrystalline SnSe.

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A Rechargeable Urea-Assisted Zn-Air Battery With High Energy Efficiency and Fast-Charging Enabled by Engineering High-Energy Interfacial Structures

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Angewandte Chemie 2024年第49期136卷

作者： Mingjie Wu Yinghui Xu Jian Luo Siyi Yang Gaixia Zhang Lei Du Huixia Luo Xun Cui Yingkui Yang Shuhui Sun State Key Laboratory of New Textile Materials and Advanced Processing Technologies Wuhan Textile University Wuhan 430200 China Department of Electrical Engineering École de Technologie Supérieure (ÉTS) Montréal Québec H3C 1K3 Canada Huangpu Hydrogen Energy Innovation Centre/School of Chemistry and Chemical Engineering Guangzhou University Wai Huan Xi Road 230 Guangzhou 510006 P. R. China School of Materials Science and Engineering State Key Laboratory of Optoelectronic Materials and Technologies Guangdong Provincial Key Laboratory of Magnetoelectric Physics and Devices Key Lab of Polymer Composite & Functional Materials Sun Yat-Sen University No. 135 Xingang Xi Road Guangzhou 510275 P. R. China Institut National de la Recherche Scientifique (INRS) Center Énergie Matériaux Télécommunications Varennes Québec J3X 1P7 Canada

Electrochemical urea oxidation reaction (UOR) offers a promising alternative to the oxygen evolution reaction (OER) in clean energy conversion and storage systems. Nickel-based catalysts are regarded as highly promising electrocatalysts for the UOR. However, their effectiveness is significantly hindered by the unavoidable self-oxidation reaction of nickel species during UOR. To address this challenge, we proposed an interface chemistry modulation strategy to boost UOR kinetics by creating a high-energy interfacial heterostructure. This heterostructure incorporates Ag at the CoOOH@NiOOH heterojunction interface, where strong interactions significantly promote the electron exchanges at the heterojunction interface between -OH and -O groups. Consequently, the improved electron delocalization leads to the formation of stronger bonds between Co sites and urea CO(NH 2 ) 2 , promoting a preference for urea to occupy Co active sites over OH*. The resulting catalyst, Ag−CoOOH@NiOOH, demonstrates ultrahigh UOR activity with a low potential of 1.33 V at 100 mA cm −2 . The fabricated catalyst exhibits a mass activity over 11.9 times greater than the initial cobalt oxyhydroxide. The rechargeable urea-assisted zinc-air batteries (ZABs) achieve a record-breaking energy efficiency of 74.56 % at 1 mA cm −2 , remarkable durability (1000 hours at a current density of 50 mA cm −2 ), and quick charge performances.

关键词： Zinc-air battery Urea oxidation reaction Oxygen evolution reaction Heterojunction interface Fast-charging

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Adsorption of Co2+ and Sr2+ in aqueous solution by a novel fibrous chitosan biosorbent

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The Science of the total environment 2022年 825卷 153998页

作者： Shuting Zhuang Kunkun Zhu Lejin Xu Jun Hu Jianlong Wang Laboratory of Environmental Technology INET Tsinghua University Beijing 100084 PR China. State Key Laboratory of New Textile Materials and Advanced Processing Technologies Wuhan Textile University Wuhan 430200 PR China. Department of Nuclear Engineering and Technology School of Energy and Power Engineering Huazhong University of Science and Technology Wuhan 430074 PR China. Laboratory of Environmental Technology INET Tsinghua University Beijing 100084 PR China Beijing Key Laboratory of Radioactive Waste Treatment INET Tsinghua University Beijing 100084 PR China. Electronic address: wangjl@***.

In this study, a novel fibrous chitosan biosorbent was prepared using LiOH/KOH/urea/HO (4.5:7:8:80.5 by weight) as spinning solvent. The fibrous chitosan exhibited a higher adsorption capacity and a faster adsorption rate for Co and Sr, compared with spherical chitosan due to its high specific surface area (16.9 m g), uniform fineness (24.1 μm), and good mechanical strength. The adsorption capacity of fibrous chitosan for Co and Sr was 31.3 mg g and 20.0 mg g, respectively, which was higher than that of spherical chitosan (22.5 mg gfor Co and 8.9 mg g for Sr). The coordination between -NH/-OH of chitosan and the nuclide ions was the rate-limiting step. The improvement of adsorption performance was due to the higher specific surface area which increased the exposure degree of functional groups (adsorptive sites). This new wet-spun fibrous chitosan biosorbent showed great potential in the adsorptive removal of nuclides ions from aqueous solution.

关键词： Adsorption Biosorbent Fibrous chitosan Nuclide

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Resonant Inelastic X-ray Scattering for Studying materials for Renewable Energy Conversion and Storage

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iScience 2025年

作者： Rongfu Hong Lixin Xing Mingjie Wu Zhangsen Chen Ning Wang Ling Meng Siyu Ye Liguang Wang Gaixia Zhang Lei Du Huangpu Hydrogen Energy Innovation Centre/School of Chemistry and Chemical Engineering Guangzhou University Guangzhou 510006 P. R. China State Key Laboratory of New Textile Materials and Advanced Processing Technologies Wuhan Textile University Wuhan 430200 P. R. China Institut National de la Recherche Scientifique-Énergie Matériaux et Télécommunications Varennes QC J3X 1S2 Canada College of Chemical and Biological Engineering Zhejiang University Hangzhou 310058 P. R. China Department of Electrical Engineering École de Technologie Supérieure (ÉTS) Montréal QC H3C 1K3 Canada

Renewable energy conversion and storage technologies, including batteries, fuel cells, and electrolyzers, have garnered global attention. Electrode materials are crucial in determining the performance and lifespan of the corresponding devices. Transition metals and light elements are key components in electrode materials, enabling efficient energy conversion by directly providing active sites or indirectly optimizing material electronic structures. To understand the relationship between electronic structures and device performance, advanced technologies like X-ray absorption spectroscopy (XAS) have been developed. Recently, resonant inelastic X-ray scattering (RIXS) features coupled with X-ray emission spectra (XES) have emerged as a complementary tool, providing additional insights into material electronic structures. This review focuses on recent advances in using XES, particularly RIXS, for studying energy conversion and storage materials, highlighting the unique features and potential of RIXS for quantitative analysis. This work aims to stimulate interests in utilizing RIXS features in the field of energy conversion and storage.

关键词： Resonant inelastic X-ray scattering Electronic structure Energy storage and conversion Transition metal element Light element

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Regulating Non-Equilibrium Solvation Structure in Locally Concentrated Ionic Liquid Electrolytes for Wide-Temperature and High-Voltage Lithium Metal Batteries

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Angewandte Chemie 2024年第1期137卷

作者： Haifeng Tu Zhicheng Wang Jiangyan Xue Zhiyong Tang Yang Liu Xiaofang Liu Lingwang Liu Suwan Lu Shixiao Weng Yiwen Gao Guochao Sun Zheng Liu keyang Peng Xin Zhang Dejun Li Guangye Wu Meinan Liu Jianchen Hu Hong Li Jingjing Xu Xiaodong Wu School of Nano-Tech and Nano-Bionics University of Science and Technology of China Hefei Anhui 230026 China i-lab Suzhou Institute of Nano-Tech and Nano-Bionics Chinese Academy of Sciences Suzhou Jiangsu 215123 China These authors contributed equally to this work: Haifeng Tu Zhicheng Wang Institute of Physics Chinese Academy of Sciences Beijing 100190 China Tianmu Lake Institute of Advanced Energy Storage Technologies Liyang 213300 China Jiangxi Key Laboratory of Flexible Electronics Jiangxi Science & Technology Normal University Nanchang 330013 Jiangxi China State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures Guangxi Key Laboratory of Processing for Non-Ferrous Metals and Featured Materials School of Resources Environment and Materials Guangxi University Nanning 530004 China National Engineering Laboratory for Modern Silk College of Textile and Clothing Engineering Research Center of Cooperative Innovation for Functional Organic/Polymer Material Micro/Nanofabrication Soochow University Suzhou 215123 China College of Material Science and Engineering Hohai University Nanjing Jiangsu 210024 China

The development of high-voltage lithium metal batteries (LMBs) encounters significant challenges due to aggressive electrode chemistry. Recently, locally concentrated ionic liquid electrolytes (LCILEs) have garnered attention for their exceptional stability with both Li anodes and high-voltage cathodes. However, there remains a limited understanding of how diluents in LCILEs affect the thermodynamic stability of the solvation structure and transportation dynamics of Li + ions. Herein, we propose a wide-temperature LCILEs with 1,3-dichloropropane (DCP13) diluent to construct a non-equilibrium solvation structure under external electric field, wherein the DCP13 diluent enters the Li + ion solvation sheath to enhance Li + ion transport and suppress oxidative side reactions at high-nickel cathode (LiNi 0.9 Co 0.05 Mn 0.05 O 2 , NCM90). Consequently, a Li/NCM90 cell utilizing this LCILE achieves a high capacity retention of 94 % after 240 cycles at 4.3 V, also operates stably at high cut-off voltages from 4.4 V to 4.6 V and over a wide temperature range from −20 °C to 60 °C. Additionally, an Ah-level pouch cell with this LCILE simultaneously achieves high-energy-density and stable cycling, manifesting the practical feasibility. This work redefines the role of diluents in LCILEs, providing inspiration for electrolyte design in developing high-energy-density batteries.

关键词： Lithium metal batteries locally concentrated ionic liquid electrolyte chloroalkane diluent non-equilibrium solvation structure external electric field

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Strain Sensing Elastic Core-Spun Yarns Based on Long Silver Nanowires

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Journal of Physics: Conference Series 2021年第1期2101卷

作者： Liping Jia Qi Zeng Quanquan Zhu Runxuan Cai Wei Guo Jianhua Ran Shuguang Bi Shiwei Li Hubei Key Laboratory of Biomass Fibers and Eco-Dyeing & Finishing State Key Laboratory of New Textile Materials and Advanced Processing Technologies College of Chemistry and Chemical Engineering Wuhan Textile University Wuhan 430200 China. Department of Biochemistry & Molecular & Cellular Biology Georgetown University Washington DC 20057 United States College of Physical Education Jianghan University Wuhan 430056 China

Strain sensing is one of the important functions of intelligent fabric, which can transform the external stress (or strain) into visible electrical signals and monitor the characteristics of human physiology and motion. At present, the flexible strain sensor has low sensitivity, small strain range and unstable performance after repeated stretching. In this work, core-spun yarns with polyurethane (PU) filament as core and long silver nanowires (AgNWs) loaded cotton fiber as shell was fabricated by spinning technology. The results showed that when the loading of AgNWs was 10 wt%, the strain range of the PU/cotton@AgNWs core-spun yarn was 0-60%, the gauge factor of 12.6 was linear, and the strain sensing and mechanical properties were stable after repeated stretching. This strain sensing elastic core-spun yarns constructed by spinning technology could be used as one of the important materials for intelligent wearable devices.

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Urea/Thiourea Imine Linkages Provide Accessible Holes in Flexible Covalent Organic Frameworks and Dominates Self-Adaptivity and Exciton Dissociation

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Angewandte Chemie 2024年第7期137卷

作者： Chencheng Qin Prof. Xiaodong Wu Wenyan Zhou Miao Li Prof. Shuai Bi Prof. Lin Tang Dr. Hao Huang Prof. Wenguang Tu Prof. Xingzhong Yuan Prof. Edison Huixiang Ang Prof. Weiling Sun Long Chen Zhaoli Liu Prof. Bing He Prof. Lai Lyu Prof. Yan Wu Prof. Wen Liu Prof. Hou Wang College of Environmental Science and Engineering and Key Laboratory of Environmental Biology and Pollution Control (Ministry of Education) Hunan University Changsha 410082 China These authors equally contributed this work College of Materials Science and Engineering Nanjing Tech University Nanjing 211816 China School of Chemistry Chemical Engineering and Biotechnology Nanyang Technological University 21 Nanyang Link Singapore 637371 Singapore School of Science and Engineering The Chinese University of Hong Kong Shenzhen 518172 Guangdong P. R. China Natural Sciences and Science Education National Institute of Education Nanyang Technological University Singapore 637616 Singapore The Key Laboratory of Water and Sediment Sciences Ministry of Education College of Environmental Sciences and Engineering Peking University Beijing 100871 China State Key Laboratory of New Textile Materials and Advanced Processing Technologies Wuhan Textile University 430200 Wuhan China Institute of Rural Revitalization Guangzhou University Guangzhou 510006 China College of Environment and Ecology Hunan Agricultural University Changsha 410128 P. R China National Laboratory for Molecular Sciences Peking University Beijing 100871 China

Unraveling the robust self-adaptivity and minimal energy-dissipation of soft reticular materials for environmental catalysis presents a compelling yet unexplored avenue. Herein, a top-down strategy, tailoring from the unique linkage basis, flexibility degree, skeleton electronics to trace-guest adaptability, is proposed to fill the understanding gap between micro-soft covalent organic frameworks (COFs) and photocatalytic performance. The thio(urea)-basis-dominated linkage within benzotrithiophene-based COFs induce the framework contraction/swelling (intralayer micro-flexibility) in response to tetrahydrofuran or water. Adaptability of micro-flexible thiourea-COF with pore hydrophilicity not only contributes to the favorable mass transfer, but also enhances the accessible redox active sites, culminating in nearly 100 % removal of micropollutant with low-energy dissipation in wastewater. The incorporating urea/thiourea into imine linkage facilitates polarization reduction and exciton dissociation within skeleton wall, inducing strong localization for holes. This transformation facilitates interchain charge transport and unbalanced distribution conducive to oxidative holes-mediated micropollutant decomposition.

关键词： micro-flexible COFs conformation photocatalysis self-adaptivity

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Carbon nanocomposites with high photothermal conversion efficiency

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Science China materials 2018年第7期61卷 905-914页

作者： Qian Zhang Weilin Xu Xianbao Wang Hubei Collaborative Innovation Center for Advanced Organic Chemical Materials Key Laboratory for the Green Preparation and Application of Functional Materials Ministry of Education Hubei Key Laboratory of Polymer Materials School of Materials Science and Engineering Hubei University Wuhan 430062 China State Key Laboratory of New Textile Materials and Advanced Processing Technologies Ministry of Education Wuhan Textile University Wuhan Textile University Wuhan 430200 China

Photothermal conversion for water vapor gen- eration is a novel strategy and an efficient way to utilize solar energy, which has great potential for water purification and desalination. In this review, the development of photothermal conversion and the classification of absorbers for solar vapor generation systems are presented, especially in recent devel- opment of carbon nanocomposites （carbon nanotubes and graphene） as solar vapor generation devices. Combined with recent progresses and achievements in this field, we discuss the challenges and opportunities for photothermal conversion based on carbon nanocomposites as well as their promising applications.

关键词： carbon composites photothermal conversion solarenergy water vapor

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