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Electrochemical Hydrophobic Tri-layer Interface Rendered Mechanically Graded Solid Electrolyte Interface for Stable Zinc Metal Anode

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Angewandte Chemie 2024年第9期136卷

作者： Dr. Chaozheng Liu Dr. Wangwang Xu Dr. Lei Zhang Daotong Zhang Dr. Weina Xu Dr. Xiaobin Liao Weimin Chen Dr. Yizhong Cao Prof. Mei-Chun Li Prof. Changtong Mei Dr. Kangning Zhao Co-Innovation Center of Efficient Processing and Utilization of Forest Resources College of Materials Science and Engineering Nanjing Forestry University Nanjing 210000 China Mechanical & Industrial Engineering Department Louisiana State University Baton Rouge LA-70803 USA State Key Laboratory of Advanced Technology for Materials Synthesis and Processing International School of Materials Science and Engineering Wuhan University of Technology Wuhan 430070 China School of Materials Science and Engineering Dongguan University of Technology Guangdong 523808 China College of Chemistry and Materials Engineering Zhejiang A&F University Hangzhou 311300 China Laboratory of Advanced Separations (LAS) École Polytechnique Fédérale de Lausanne (EPFL) Sion 1950 Lausanne Switzerland

The aqueous zinc-ion battery is promising as grid scale energy storage device, but hindered by the instable electrode/electrolyte interface. Herein, we report the lean-water ionic liquid electrolyte for aqueous zinc metal batteries. The lean-water ionic liquid electrolyte creates the hydrophobic tri-layer interface assembled by first two layers of hydrophobic OTF − and EMIM + and third layer of loosely attached water, beyond the classical Gouy–Chapman–Stern theory based electrochemical double layer. By taking advantage of the hydrophobic tri-layer interface, the lean-water ionic liquid electrolyte enables a wide electrochemical working window (2.93 V) with relatively high zinc ion conductivity (17.3 mS/cm). Furthermore, the anion crowding interface facilitates the OTF − decomposition chemistry to create the mechanically graded solid electrolyte interface layer to simultaneously suppress the dendrite formation and maintain the mechanical stability. In this way, the lean-water based ionic liquid electrolyte realizes the ultralong cyclability of over 10000 cycles at 20 A/g and at practical condition of N/P ratio of 1.5, the cumulated areal capacity reach 1.8 Ah/cm 2 , which outperforms the state-of-the-art zinc metal battery performance. Our work highlights the importance of the stable electrode/electrolyte interface stability, which would be practical for building high energy grid scale zinc-ion battery.

关键词： Electrochemical Tri-Layer Interface Hydrophobic Ionic Liquid Mechanically Graded Solid Electrolyte Interface Zinc Battery

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Molecularly Tunable Heterostructured Co-Polymers Containing Electron-Deficient and -Rich Moieties for Visible-Light and Sacrificial-Agent-Free H2O2Photosynthesis

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Angewandte Chemie 2024年第29期136卷

作者： Jingzhao Cheng Wang Wang Jianjun Zhang Sijie Wan Prof. Bei Cheng Prof. Jiaguo Yu Prof. Shaowen Cao State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 122 Luoshi Road Wuhan 430070 P. R. China Hubei Technology Innovation Center for Advanced Composites Wuhan University of Technology 122 Luoshi Road Wuhan 430070 P. R. China Laboratory of Solar Fuel Faculty of Materials Science and Chemistry China University of Geosciences 68 Jincheng Street Wuhan 430078 P. R. China

As an alternative to hydrogen peroxide (H 2 O 2 ) production by complex anthraquinone oxidation process, photosynthesis of H 2 O 2 from water and oxygen without sacrificial agents is highly demanded. Herein, a covalently connected molecular heterostructure is synthesized via sequential C−H arylation and Knoevenagel polymerization reactions for visible-light and sacrificial-agent-free H 2 O 2 synthesis. The subsequent copolymerization of the electron-deficient benzodithiophene-4,8-dione (BTD) and the electron-rich biphenyl (B) and p -phenylenediacetonitrile (CN) not only expands the π-conjugated domain but also increases the molecular dipole moment, which largely promotes the separation and transfer of the photoinduced charge carriers. The optimal heterostructured BTDB-CN 0.2 manifested an impressive photocatalytic H 2 O 2 production rate of 1920 μmol g −1 h −1 , which is 2.2 and 11.6 times that of BTDB and BTDCN. As revealed by the femtosecond transient absorption (fs-TA) and theoretical calculations, the linkage serves as a channel for the rapid transfer of photogenerated charge carriers, enhancing the photocatalytic efficiency. Further, in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) uncovers that the oxygen reduction reaction occurs through the step one-electron pathway and the mutual conversion between C=O and C−OH with the anchoring of H + during the catalysis favored the formation of H 2 O 2 . This work provides a novel perspective for the design of efficient organic photocatalysts.

关键词： molecular heterostructure H2O2 dipole moment channel reaction path

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[email protected] core-shell nanowires towards oxygen reduction reaction

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Chemical Engineering Journal 2021年 421卷

作者： Qi Xue Hui-Ying Sun Ya-Nan Li Ming-Jun Zhong Fu-Min Li Xinlong Tian Pei Chen Shi-Bin Yin Yu Chen Key Laboratory of Macromolecular Science of Shaanxi Province Key Laboratory of Applied Surface and Colloid Chemistry (Ministry of Education) Shaanxi Key Laboratory for Advanced Energy Devices Shaanxi Engineering Lab for Advanced Energy Technology School of Materials Science and Engineering Shaanxi Normal University Xi’an 710062 PR China State Key Laboratory of Marine Resource Utilization in South China Sea Hainan Provincial Key Lab of Fine Chemistry School of Chemical Engineering and Technology Hainan University Haikou 570228 PR China MOE Key Laboratory of New Processing Technology for Non-ferrous Metals and Materials Guangxi Key Laboratory of Processing for Non-ferrous Metals and Featured Materials Guangxi University Nanning Guangxi 530004 PR China

Noble metal based one-dimensionally (1D) bimetallic nanostructures are attracting increasing interest in energy conversion field because of their structural advantages and tunable chemical composition. At present, the facile and efficient synthesis of high-quality Au-core noble metal-shell nanowires still maintains the challenge. Herein, we develop a feasible one-pot chemical-reduction strategy to rapidly synthesize high-quality [email protected] core–shell nanowires ( [email protected] CSNWs) in 1-naphthol ethanol solution and explore their potential application in electrocatalysis. Expermattial results show the formation core–shell structure originates from the deposition-growth of Ir atoms at preferentially generated Au nanowires surface. When using as an electrocatalyst towards oxygen reduction reaction (ORR) in alkaline media, [email protected] CSNWs show Pt-like ORR electroactivity due to the compositional synergism effect and structural advantages of 1D nanowires, accompanying with excellent durability and extremely enhanced methanol tolerance towards ORR.

关键词： Low temperature fuel cells Pt-free electrocatalyst Core-shell structure Methanol tolerance Oxygen reduction reaction

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Enhancement of the Critical Temperature of HgBa2CuO4+δ by Applying Uniaxial and Hydrostatic Pressure: Implications for a Universal Trend in Cuprate Superconductors

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Physical Review Letters 2010年第16期105卷 167002-167002页

作者： F. Hardy N. J. Hillier C. Meingast D. Colson Y. Li N. Barišić G. Yu X. Zhao M. Greven J. S. Schilling Institute for Solid State Physics Karlsruhe Institute of Technology P.O. Box 3640 76021 Karlsruhe Germany Department of Physics Washington University CB 1105 One Brookings Drive St. Louis Missouri 63130 USA Service de Physique de l’Etat Condensé Orme des Merisiers CEA Saclay CNRS URA 2464 91195 Gif-Sur-Yvette Cedex France Department of Physics Stanford University Stanford California 94305 USA T.H. Geballe Laboratory for Advanced Materials Stanford University Stanford California 94305 USA I. Physikaliches Institut Universität Stuttgart 70550 Stuttgart Germany School of Physics and Astronomy University of Minnesota Minneapolis Minnesota 55455 USA State Key Lab of Inorganic Synthesis and Preparative Chemistry College of Chemistry Jilin University Changchun 130012 China

It is well known that the superconducting transition temperature (Tc) of cuprate superconductors can be enhanced by varying certain structural and electronic parameters, such as the flatness of the CuO2 planes or their doping level. We determine the uniaxial and hydrostatic pressure derivatives of Tc in the structurally simple tetragonal compound HgBa2CuO4+δ near optimal doping. Our results provide experimental evidence for two further methods to enhance Tc: (i) reducing the area of the CuO2 planes, and (ii) increasing the separation of the CuO2 planar groups. Tc is found to couple much more strongly to the ratio c/a of the lattice constants than to the unit cell volume. A comparison with prior results for structurally more complicated cuprates reveals a general trend of uniaxial pressure derivatives with Tc.

关键词： Hydrostatic pressure

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Front Cover: Highly Dispersed Pt Nanoparticles Embedded in N-Doped Porous Carbon for Efficient Hydrogen Evolution (Chem. Asian J. 14/2021)

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Chemistry – An Asian Journal 2021年第14期16卷

作者： Yuan Dong Dr. Jie Ying Yu-Xuan Xiao Jiang-Bo Chen Prof. Xiao-Yu Yang State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 122 Luoshi Road Wuhan 430070 P. R. China School of Chemical Engineering and Technology Sun Yat-sen University Zhuhai 519082 P. R. China School of Engineering and Applied Sciences Harvard University Cambridge Massachusetts 02138 USA

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Author Correction: Chemical fixation of carbon dioxide catalyzed via cobalt (III) ONO pincer ligated complexes

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Communications Chemistry 2019年第1期2卷 1页

作者： Habib Ullah Bibimaryam Mousavi Hussein A. Younus Zafar A. K. Khattak Somboon Chaemchuen Suleman Suleman Francis Verpoort State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan China Chemistry Department Faculty of Science Fayoum University Fayoum Egypt National Research Tomsk Polytechnic University Tomsk Russian Federation Ghent University Global Campus Songdo Incheon South Korea College of Arts and Sciences Khalifa University of Science and Technology Abu Dhabi UAE

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Electrophilically Trapping Water for Preventing Polymerization of Cyclic Ether Towards Low-Temperature Li Metal Battery

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Angewandte Chemie 2023年第14期135卷

作者： Hai-Zhen Jiang Chao Yang Prof. Min Chen Xiao-Wei Liu Lu-Ming Yin Prof. Ya You Prof. Jun Lu State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Hubei Wuhan 430070 China School of Chemistry Chemical Engineering and Life Sciences Wuhan University of Technology Hubei Wuhan 430070 P. R. China International School of Materials Science and Engineering School of Materials Science and Microelectronics Wuhan University of Technology Hubei Wuhan 430070 P. R. China College of Chemical and Biological Engineering Zhejiang University Hangzhou Zhejiang Province 310027 China

Cyclic ether, such as 1,3-dioxolane (DOL), are promising solvent for low-temperature electrolytes because of the low freezing point. Their use in electrolytes, however, is severely limited since it easily polymerizes in the presence of lithium inorganic salts. The trace water plays a key role via providing the source (proton) for chain initiation, which has, unfortunately, been neglected in most cases. In this work, we present an electrophile, trimethylsilyl isocyanate (Si−NCO), as the water scavenger, which eliminates moisture by a nucleophilic addition reaction. Si−NCO allows DOL to maintain liquid over a wide temperature range even in high-concentration electrolyte. Electrolyte with Si−NCO additive shows promising low-temperature performance. Our finding expands the use of cyclic ether solvents in the presence of inorganic salts and highlights a large space for unexplored design of water scavenger with electrophilic feature for low-temperature electrolytes.

关键词： Cationic Ring-Opening Polymerization Cyclic Ether Li-Metal Battery Low Temperature Electrolyte Water Scavenger

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Hydrogen/Electron Amphiphilic Bi-Functional Water Molecular Inactivator-Assisted Interface Stabilization in Highly Reversible Zn Metal Batteries

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Angewandte Chemie 2024年第7期137卷

作者： Wenwei Zhang Dr. Shaohua Zhu Tong Yang Lu Wu Jinghao Li Jiang Liang Dr. Yu Liu Lianmeng Cui Chen Tang Xinran Chen Huiqing Zhou Fan Qiao Min Zhou Prof. Ping Luo Fengtong Chi Dr. Xiaobin Liao Prof. Lei Zhang Prof. Qinyou An State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China The State Key Laboratory of Refractories and Metallurgy and Institute of Advanced Materials and Nanotechnology Wuhan University of Science and Technology Wuhan 430081 China School of Chemistry and Chemical Engineering Shanghai Jiao Tong University 800 Dongchuan Road Shanghai 200240 China School of Materials and Chemical Engineering Hubei University of Technology Wuhan 430068 China Hubei Longzhong Laboratory Wuhan University of Technology (Xiangyang Demonstration Zone) Xiangyang Hubei 441000 China Zhongyu Feima New Material Technology Innovation Center (Zhengzhou) Co. Ltd. High Technology Industrial Development Zone Zhengzhou 450001 China

Continuous hydrogen-bond-network in aqueous electrolytes can lead to uncontrollable hydrogen transfer, and combining the interfacial parasitic electron consumption cause the side reaction in aqueous zinc metal batteries (AZMBs). Herein, hydrogen/electron amphiphilic bi-functional 1,5-Pentanediol (PD) molecule was introduced to stabilize the electrode/electrolyte interface. Stronger proton affinity of -OH in PD can break bulk-H 2 O hydrogen-bond-network to inhibit the activity of water, and electron affinity can enhance electron acceptation capability, which ensures that PD is preferentially bound to electrode material over H 2 O. Besides, the participation of PD in the Zn 2+ solvation structure reduces water content at the solid–liquid interface and promotes uniform deposition process by optimizing Zn 2+ de-solvation energy. Accordingly, dense and vertical zinc texture based on intrinsic steric hindrance effect of PD and formed SEI protective layer to induce stable Zinc anode-electrolyte interface. Moreover, an organic–inorganic shielding water layer was formed at the cathode side to suppress vanadium dissolution in vanadium Oxide. Consequently, Zn//Zn symmetric cell could cycle for more than 5600 hours at 1 mAh cm −2 @1 mA cm −2 (more than 250 hours at 50 °C). Besides, the VO 2 and I 2 cathode all achieved stable cycling performance and former pouch cell could reach average capacity of 0.13 Ah.

关键词： Electrode/electrolyte interface Active-water SEI Electron and proton affinity Cathode dissolution

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Ethanol-Selectivity: AuCu Alloy Nanoparticle Embedded Cu Submicrocone Arrays for Selective Conversion of CO2to Ethanol (Small 37/2019)

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Small 2019年第37期15卷

作者： Sibo Shen Xianyun Peng Lida Song Yuan Qiu Chao Li Longchao Zhuo Jia He Junqiang Ren Xijun Liu Jun Luo Center for Electron Microscopy and Tianjin Key Lab of Advanced Functional Porous Materials Institute for New Energy Materials & Low-Carbon Technologies School of Materials Science and Engineering Tianjin University of Technology Tianjin 300384 China Hebei Key Laboratory of Active Components and Functions in Natural Products (under planning) College of Chemical Engineering Hebei Normal University of Science and Technology Qinhuangdao 066600 China School of Materials Science and Engineering Xi'an University of Technology Xi'an 710048 China State Key Laboratory of Advanced Processing and Recycling of Nonferrous Metals Lanzhou University of Technology Lanzhou 730050 China

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High-Performance Microbatteries: Recent Advances in High-Performance Microbatteries: Construction, Application, and Perspective (Small 39/2020)

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Small 2020年第39期16卷

作者： Zhe Zhu Ruyu Kan Song Hu Liang He Xufeng Hong Hui Tang Wen Luo State Key Laboratory of Advanced Technology for Materials Synthesis and Processing International School of Materials Science and Engineering Wuhan University of Technology Wuhan Hubei 430070 P. R. China Department of Materials Science and NanoEngineering Rice University Houston TX 77005 USA School of Materials and Energy University of Electronic Science and Technology of China Chengdu Sichuan 611731 P. R. China Department of Physics School of Science Wuhan University of Technology Wuhan Hubei 430070 P. R. China

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