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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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Cover Feature: Fabrication of Efficient and Stable Perovskite Solar Cells in High-Humidity Environment through Trace-Doping of Large-Sized Cations (ChemSusChem 11/2019)

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ChemSusChem 2019年第11期12卷 2328-2328页

作者： Xueping Liu Jiang He Pengfei Wang Yuhao Liu Junyan Xiao Dr. Zhiliang Ku Prof. Yong Peng Prof. Fuzhi Huang Prof. Yi-Bing Cheng Dr. Jie Zhong State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 P.R. China Wuhan National Laboratory for Optoelectronics Huazhong University of Science and Technology Wuhan 430074 P.R. China School of Materials Science and Engineering Wuhan University of Technology Wuhan 430070 P.R. China Department of Materials Science and Engineering Monash University VIC 3800 Australia ARC Centre of Excellence in Exciton Science Monash University Clayton VIC 3800 Australia

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Dual-Anionic Coordination Manipulation Induces Phosphorus and Boron-Rich Gradient Interphase Towards Stable and Safe Sodium Metal Batteries

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Angewandte Chemie 2024年第3期137卷

作者： Yi-Hu Feng Dr. Mengting Liu Wenli Qi Haoliang Liu Qiang Liu Dr. Chao Yang Yongwei Tang Xu Zhu Shuai Sun Yuan-Meng Li Tian-Ling Chen Bing Xiao Prof. Xiao Ji Prof. Ya You Prof. Peng-Fei Wang Center of Nanomaterials for Renewable Energy State Key Laboratory of Electrical Insulation and Power Equipment School of Electrical Engineering Xi'an Jiaotong University Xi'an Shaanxi 710049 P. R. China School of Optical and Electronic Information-Wuhan National Laboratory for Optoelectronics Huazhong University of Science and Technology Wuhan Hubei 430074 P. R. China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan Hubei 430070 P. R. China Jiangsu Jufeng New Energy Technology Co. Ltd. Changzhou Jiangsu 213166 P. R. China

High-voltage sodium metal batteries (SMBs) present a viable pathway towards high-energy-density sodium-based batteries due to the competitive cost advantage and abundant supply of sodium resources. However, they still suffer from severe capacity decay induced by the notorious decomposition of the electrolyte under high voltage and unstable cathode/electrolyte interphase (CEI). In addition, the high reactivity of Na metal and flammable electrolytes push SMBs to their safety limits. Herein, a special dual-anion aggregated Na + solvation structure is designed in a nonflammable trimethyl phosphate-based localized high-concentration electrolyte, and a gradient CEI enriched with phosphorus and boron compounds is formed on the cathode. This thin and stable interphase effectively suppresses the parasitic reaction, improves the interfacial stability of the cathode, and facilitates Na + transport through the interface by the synergistic effect of multi-components, thus optimizing the cycling stability and safety of SMBs. The Na 0.95 Ni 0.4 Fe 0.15 Mn 0.3 Ti 0.15 O 2 //Na batteries employing such electrolyte provide a discharge capacity of 167.5 mAh g −1 and high retention in the capacity of 85.2 % after 800 cycles at 1 C. This approach offers a general strategy for the design of flame-retardant high-voltage electrolytes and the practical application of SMBs.

关键词： sodium metal batteries electrolyte non-flammable cathode/electrolyte interphase solvation structure

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Naphthyl Substituted Impurities Induce Efficient Room Temperature Phosphorescence

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Angewandte Chemie 2023年第50期135卷

作者： Weiguo Qiao Ming Yao Jingwen Xu Haiyan Peng Jianlong Xia Xiaolin Xie Zhong'an Li Key Laboratory for Material Chemistry of Energy Conversion and Storage Ministry of Education School of Chemistry and Chemical Engineering State Key Laboratory of Materials Processing and Die & Mould Technology Huazhong University of Science and Technology Wuhan 430074 China Contribution: Conceptualization (supporting) Investigation (lead) Methodology (equal) Resources (lead) Writing - original draft (lead) Writing - review & editing (supporting) Contribution: Investigation (supporting) Methodology (supporting) Resources (supporting) Writing - review & editing (supporting) School of Chemistry Chemical Engineering and Life Science State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China Contribution: Investigation (supporting) Methodology (supporting) Writing - review & editing (supporting) Contribution: Investigation (supporting) Project administration (supporting) Supervision (supporting) Writing - review & editing (supporting) Contribution: Investigation (supporting) Project administration (supporting) Writing - review & editing (supporting) Contribution: Project administration (supporting) Resources (supporting) Writing - review & editing (supporting)

Accidentally, it was found that triphenylamine (TPA) from commercial sources shows ultralong yellow-green room temperature phosphorescence (RTP) like commercial carbazole, which however disappears for lab-synthesized TPA with high purity. Herein, we for the first time identify the impurity types that cause RTP of commercial TPA, which are two N , N -diphenyl-naphthylamine isomers. Due to similar molecular polarity and very trace amount (≈0.8 ‰, molar ratio), these naphthyl substituted impurities can be easily overlooked. We further show that even at an extremely low amount (1000000 : 1, mass ratio) of impurities, RTP emission is still generated, attributed to the triplet-to-triplet energy transfer mechanism. Notably, this doping strategy is also applicable to the triphenylphosphine and benzophenone host systems, of which strong RTP emission can be activated by simply doping the corresponding naphthyl substituted analogues into them. This work therefore provides a general and efficient host/guest strategy toward high performance and diverse organic RTP materials.

关键词： Host-Guest System Impurities Room Temperature Phosphorescence Triphenylamine Triplet-to-Triplet Energy Transfer

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Ultra-High Proportion of Grain Boundaries in Zinc Metal Anode Spontaneously Inhibiting Dendrites Growth

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Angewandte Chemie 2024年第32期136卷

作者： Sitian Lian Zhijun Cai Prof. Mengyu Yan Prof. Congli Sun Nianyao Chai Bomian Zhang Kesong Yu Ming Xu Dr. Jiexin Zhu Dr. Xuelei Pan Dr. Yuhang Dai Jiazhao Huang Bo Mai Ling Qin Wenchao Shi Qiqi Xin Xiangyu Chen Dr. Kai Fu Prof. Qinyou An Dr. Qiang Yu Prof. Liang Zhou Dr. Wen Luo Dr. Kangning Zhao Prof. Xuewen Wang Prof. Liqiang Mai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 P. R. China Department of Physics The Chinese University of Hong Kong Shatin New Territories Hong Kong 999077 P. R. China Advanced Technology Institute University of Surrey Guildford Surrey GU2 7XH UK State Key Laboratory of Materials Processing and Die & Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan Hubei 430074 P. R. China Minhang Hospital Shanghai Medical College of Fudan University Shanghai 201199 P. R. China Laoshan Laboratory Qingdao 266237 P. R. China School of Physical Sciences Great Bay University Dongguan 523808 P. R. China

Aqueous Zn-ion batteries are an attractive electrochemical energy storage solution for their budget and safe properties. However, dendrites and uncontrolled side reactions in anodes detract the cycle life and energy density of the batteries. Grain boundaries in metals are generally considered as the source of the above problems but we present a diverse result. This study introduces an ultra-high proportion of grain boundaries on zinc electrodes through femtosecond laser bombardment to enhance stability of zinc metal/electrolyte interface. The ultra-high proportion of grain boundaries promotes the homogenization of zinc growth potential, to achieve uniform nucleation and growth, thereby suppressing dendrite formation. Additionally, the abundant active sites mitigate the side reactions during the electrochemical process. Consequently, the 15 μm Fs−Zn||MnO 2 pouch cell achieves an energy density of 249.4 Wh kg −1 and operates for over 60 cycles at a depth-of-discharge of 23 %. The recognition of the favorable influence exerted by UP-GBs paves a new way for other metal batteries.

关键词： zinc anode grain boundary femtosecond laser aqueous battery nucleation mode

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TiO 2 -rGO-Cu complex: A photocatalyst possessing an interfacial electron transport mechanism to enhance hydrogen production from seawater

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Chemical Physics Letters 2023年 822卷

作者： Lei Xia Yi Lu Yuan-Zhou Li Zhi-Yi Hu Xiao-Yu Yang State Key Laboratory of Advanced Technology for Materials Synthesis and Processing & School of Materials Science and Engineering Wuhan University of Technology 122 Luoshi Road Wuhan 430070 China Nanostructure Research Centre (NRC) Wuhan University of Technology 122 Luoshi Road 430070 Wuhan Hubei China Institut für Anorganische Chemie und Strukturchemie Heinrich-Heine-Universität Düsseldorf Universitätsstraße 1 Düsseldorf 40225 Germany

Photocatalytic hydrogen production from seawater has great prospects for generating clean energy from renewable resources. We designed a TiO 2 -rGO-Cu photocatalyst that possesses a pathway for directed electron transfer from nitrogen-doped TiO 2 to rGO and then to Cu nanoparticles, which leads to efficient electron-hole pairs separation. Results show that TiO 2 -rGO-Cu has a hydrogen production rate of 16.08 mmol h −1 g −1 in simulated seawater, which is as much as 25 times higher than that of TiO 2 . The mechanism for a highly efficient directional interfacial electron transport is proposed. The strategy could be effective for designing new photocatalysts for hydrogen production from seawater.

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Strong and Tough MXene Bridging-induced Conductive Nacre

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Angewandte Chemie 2024年第30期136卷

作者： Jia Yan Dr. Tianzhu Zhou Xinyu Yang Zejun Zhang Lei Li Prof. Zhaoyong Zou Prof. Zhengyi Fu Prof. Qunfeng Cheng School of Chemistry Key Laboratory of Bio-inspired Smart Interfacial Science and Technology of Ministry of Education Beihang University Beijing 100191 P. R. China School of Chemistry and Materials Science University of Science and Technology of China Hefei 230026 P. R. China Suzhou Institute for Advanced Research University of Science and Technology of China Suzhou 215123 P. R. China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 P. R. China Institute of Energy Materials Science (IEMS) University of Shanghai for Science and Technology Shanghai 200093 P. R. China

Nacre is a classic model, providing an inspiration for fabricating high-performance bulk nanocomposites with the two-dimensional platelets. However, the “brick” of nacre, aragonite platelet, is an ideal building block for making high-performance bulk nanocomposites. Herein, we demonstrated a strong and tough conductive nacre through reassembling aragonite platelets with bridged by MXene nanosheets and hydrogen bonding, not only providing high mechanical properties but also excellent electrical conductivity. The flexural strength and fracture toughness of the obtained conductive nacre reach ~282 MPa and ~6.3 MPa m 1/2 , which is 1.6 and 1.6 times higher than that of natural nacre, respectively. These properties are attributed to densification and high orientation degree of the conductive nacre, which is effectively induced by the combined interactions of hydrogen bonding and MXene nanosheets bridging. The crack propagations in conductive nacre are effectively inhibited through crack deflection with hydrogen bonding, and MXene nanosheets bridging between aragonite platelets. In addition, our conductive nacre also provides a self-monitoring function for structural damage and offers exceptional electromagnetic interference shielding performance. Our strategy of reassembling the aragonite platelets exfoliated from waste nacre into high-performance artificial nacre, provides an avenue for fabricating high-performance bulk nanocomposites through the sustainable reutilization of shell resources.

关键词： aragonite platelet MXene mechanical properties electrical conductivity

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Frontispiece: Hybrid Hydrogen-Bonded Organic Frameworks: Structures and Functional Applications

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Chemistry – A European Journal 2023年第14期29卷

作者： Ying Liu Prof. Ganggang Chang Dr. Fang Zheng Dr. Lihang Chen Prof. Qiwei Yang Prof. Qilong Ren Prof. Zongbi Bao Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological Engineering Zhejiang University 38 Zheda Road Hangzhou Zhejiang Province 310027 P.R. China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing School of Chemistry Chemical Engineering and Life Science Wuhan University of Technology 122 Luoshi Road Wuhan Hubei Province 430070 P.R. China Institute of Zhejiang University-Quzhou 99 Zheda Road Quzhou Zhejiang Province 324000 P.R. China

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Continuous Modulation of Electrocatalytic Oxygen Reduction Activities of Single-Atom Catalysts throughp-nJunction Rectification

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Angewandte Chemie 2022年第5期135卷

作者： Dr. Zechao Zhuang Lixue Xia Jiazhao Huang Dr. Peng Zhu Dr. Yong Li Dr. Chenliang Ye Prof. Minggang Xia Ruohan Yu Zhiquan Lang Jiexin Zhu Prof. Lirong Zheng Prof. Yu Wang Prof. Tianyou Zhai Prof. Yan Zhao Prof. Shiqiang Wei Prof. Jun Li Prof. Dingsheng Wang Prof. Yadong Li Department of Chemistry Tsinghua University Beijing 100084 China State Key Laboratory of Silicate Materials for Architectures International School of Materials Science and Engineering Wuhan University of Technology Wuhan 430070 China State Key Laboratory of Material Processing and Die & Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan 430074 China Institute of Applied and Physical Chemistry and Center for Environmental Research and Sustainable Technology University of Bremen 28359 Bremen Germany Department of Photoelectronic Information Science and Engineering School of Science Xi'an Jiaotong University Xi'an 710049 China Nanostructure Research Centre Wuhan University of Technology Wuhan 430070 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China Beijing Synchrotron Radiation Facility Institute of High Energy Physics Chinese Academy of Sciences Beijing 100049 China Shanghai Synchrotron Radiation Facility Shanghai Institute of Applied Physics Chinese Academy of Sciences Shanghai 201204 China The Institute of Technological Sciences Wuhan University Wuhan 430072 China National Synchrotron Radiation Laboratory University of Science and Technology of China Hefei 230026 China

Fine-tuning single-atom catalysts (SACs) to surpass their activity limit remains challenging at their atomic scale. Herein, we exploit p -type semiconducting character of SACs having a metal center coordinated to nitrogen donors (MeN x ) and rectify their local charge density by an n -type semiconductor support. With iron phthalocyanine (FePc) as a model SAC, introducing an n -type gallium monosulfide that features a low work function generates a space-charged region across the junction interface, and causes distortion of the FeN 4 moiety and spin-state transition in the Fe II center. This catalyst shows an over two-fold higher specific oxygen-reduction activity than that of pristine FePc. We further employ three other n -type metal chalcogenides of varying work function as supports, and discover a linear correlation between the activities of the supported FeN 4 and the rectification degrees, which clearly indicates that SACs can be continuously tuned by this rectification strategy.

关键词： Diode Rectification Oxygen Reduction Reaction Single-Atom Catalysis Two-Dimensional Metal Chalcogenide p-n Junction

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Corrigendum to “Silica coating with well-defined micro-nano hierarchy for universal and stable surface superhydrophobicity” [Chem. Phys. Lett. 730 (2019) 594–599]

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Chemical Physics Letters 2019年 735卷

作者： Huan Liu Wei Geng Cheng-Jing Jin Si-Ming Wu Yi Lu Jie Hu Hao-Zheng Yu Gang-Gang Chang Tian Zhao Ying Wan Zhi-Qiang Luo Ge Tian Xiao-Yu Yang State Key Laboratory Advanced Technology for Materials Synthesis and Processing & School of Materials Science and Engineering Wuhan University of Technology 122 Luoshi Road Wuhan 430070 China Chemical Engineering and Life Science School of Chemistry Wuhan University of Technology 122 Luoshi Road Wuhan 430070 China College of Life Science and Technology Huazhong University of Science and Technology 1037 Luoyu Road Wuhan 430074 China School of Engineering and Applied Sciences Harvard University Cambridge MA 02138 USA Southern Marine Science and Engineer Guangdong Laboratory (Zhuhai) Zhuhai 51900 China

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