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In-Situ Integration of a Hydrophobic and Fast-Zn2+-Conductive Inorganic Interphase to Stabilize Zn Metal Anodes

Angewandte Chemie 2023年第27期135卷

作者： Mengyu Liu Wentao Yuan Dr. Guoqiang Ma Kaiyue Qiu Dr. Xueyu Nie Prof. Yongchang Liu Prof. Shigang Shen Prof. Ning Zhang College of Chemistry and Materials Science Key Laboratory of Analytical Science and Technology of Hebei Province Hebei University Baoding 071002 P. R. China Contribution: Conceptualization (equal) Data curation (lead) Formal analysis (lead) Investigation (lead) Methodology (equal) Writing - original draft (equal) Contribution: Data curation (equal) Formal analysis (equal) Investigation (equal) Methodology (equal) Software (lead) Validation (equal) Contribution: Formal analysis (equal) Validation (equal) Contribution: Formal analysis (equal) Beijing Advanced Innovation Center for Materials Genome Engineering Institute for Advanced Materials and Technology State Key Laboratory for Advanced Metals and Materials University of Science and Technology Beijing Beijing 100083 P. R. China Contribution: Conceptualization (equal) Formal analysis (equal) Funding acquisition (supporting) Resources (equal) Supervision (equal) Writing - review & editing (equal) Contribution: Formal analysis (equal) Resources (equal) Supervision (supporting) Contribution: Conceptualization (lead) Formal analysis (equal) Funding acquisition (lead) Investigation (equal) Methodology (equal) Resources (lead) Supervision (lead) Writing - original draft (lead) Writing - review & editing (lead)

The irreversible issues of Zn anode stemming from dendrite growth and water-induced erosion have severely hindered the commercialization of rechargeable aqueous Zn batteries. Herein, a hydrophobic and fast-Zn 2+ -conductive zinc hexacyanoferrate (HB-ZnHCF) interphase layer is in situ integrated on Zn by a rapid room-temperature wet-chemistry method to address these dilemmas. Different from currently proposed hydrophilic inorganic cases, the hydrophobic and compact HB-ZnHCF interphase effectively prevents the access of water molecules to Zn surface, thus avoiding H 2 evolution and Zn corrosion. Moreover, the HB-ZnHCF with large internal ion channels, strong zincophilicity, and high Zn 2+ transference number (0.86) permits fast Zn 2+ transport and enables smooth Zn deposition. Remarkably, the resultant HB-ZnHCF@Zn electrode delivers unprecedented reversibility with 99.88 % Coulombic efficiency over 3000 cycles, realizes long-term cycling over 5800 h (>8 months, 1 mA cm −2 ) and 1000 h (10 mA cm −2 ), and assures the stable operation of full Zn battery with both coin- and pouch-type configurations.

关键词： Aqueous Zn Battery Hydrophobic Interphase Inorganic Interphase Zinc Hexacyanoferrate Zn Metal Anode

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Wide Band-Gap Polymer Donors Functionalized with Unconventional Carbamate Side Chains for Polymer Solar Cells

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Angewandte Chemie 2022年第50期134卷

作者： Jie Tang Chentong Liao Yuwei Duan Xiaopeng Xu Min Deng Liyang Yu Ruipeng Li Qiang Peng School of Chemical Engineering College of Chemistry and State Key Laboratory of Polymer Materials Engineering Sichuan University Chengdu 610065 P. R. China Contribution: Conceptualization (equal) Data curation (lead) Formal analysis (lead) Methodology (lead) Contribution: Data curation (equal) Formal analysis (equal) Methodology (equal) Key Laboratory of Applied Surface and Colloid Chemistry of Ministry of Education Shaanxi Key Laboratory for Advanced Energy Devices Shaanxi Engineering Lab for Advanced Energy Technology School of Materials Science & Engineering Shaanxi Normal University Xi'an 710119 P. R. China Contribution: Data curation (supporting) Formal analysis (supporting) Contribution: Conceptualization (supporting) Data curation (supporting) Formal analysis (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Methodology (supporting) Contribution: Conceptualization (supporting) Formal analysis (supporting) Investigation (supporting) Supervision (supporting) Writing - original draft (lead) Writing - review & editing (supporting) National Synchrotron Light Source II Brookhaven National Lab Suffolk Upton NY 11973 USA Contribution: Conceptualization (lead) Project administration (lead) Supervision (lead) Validation (lead) Writing - review & editing (lead)

Side-chain engineering with heteroatoms is not only effective in tuning frontier molecular orbitals, but also possible for forming secondary bonds which can be utilized to planarize the molecular backbone, hence, improving the photon absorption as well as charge-transport abilities of polymer solar-cell (PSC) materials. Herein, two types of unconventional side chains, namely carboxylate and carbamate, containing various heteroatoms are introduced to the thiophene bridges in high performance benzodithiophene (BDT) based donor polymers to from the novel polymers PTzTz-C and PTzTz-N, respectively. In these polymers, non-covalent O⋅⋅⋅S and N⋅⋅⋅H interactions induce a high tendency to aggregation. In a ternary-blend PSC with PTzTz-N added to the high-performance D18 : BTP-eC9 blend, complimentary absorption and improved thin-film morphology were observed with a top power conversion efficiency of 18.76 %, which is an improvement of almost 5 % over the D18 : BTP-eC9 binary blends.

关键词： Carbamate Conformation Locks Donor Polymer Solar Cells

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H2-free Semi-hydrogenation of Butadiene by the Atomic Sieving Effect of Pd Membrane with Tree-like Pd Dendrites Array

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Angewandte Chemie 2023年第38期135卷

作者： Yong-Qing Yan Zhao Wei Prof. Zhao Wang Yao Li Wei-Hao Wang Bo Jiang Prof. Bao-Lian Su Laboratory of Living Materials the State Key Laboratory of Advanced Technology for Material Synthesis and Processing Wuhan University of Technology Wuhan 430070 Hubei China Contribution: Data curation (lead) Formal analysis (lead) Investigation (lead) Methodology (lead) Writing - original draft (lead) Writing - review & editing (supporting) Contribution: Conceptualization (equal) Data curation (equal) Formal analysis (equal) Investigation (equal) Methodology (equal) Validation (equal) Writing - original draft (equal) Writing - review & editing (equal) Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory Guangdong Laboratory Xianhu Hydrogen Valley Foshan 528200 P. R. China Contribution: Conceptualization (lead) Data curation (lead) Formal analysis (lead) Funding acquisition (lead) Investigation (lead) Methodology (lead) Project administration (lead) Resources (lead) Supervision (lead) Validation (lead) Visualization (lead) Writing - original draft (lead) Writing - review & editing (lead) Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) Writing - original draft (supporting) Writing - review & editing (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) Writing - original draft (supporting) Laboratory of Inorganic Materials Chemistry (CMI) University of Namur 61 rue de Bruxelles 5000 Namur Belgium

H 2 -free semi-hydrogenation at room temperature shows great advantage for replacing the thermocatalytic process in industry owing to the high energy and resource saving, however, remains great challenges. Herein, a tree-like Pd dendrites array decorated Pd membrane was constructed as the core device in an electrochemistry assisted gas-fed membrane reactor for butadiene semi-hydrogenation. It reveals that hydrogen atomic sieving effect of this Pd-based membrane under electrochemical condition was the key for semi-hydrogenation. The configuration study of Pd nanostructured membrane demonstrates that the penetration of hydrogen atoms through Pd membrane from electrochemical side to chemical side is affected by the consumption of hydrogen atom in semi-hydrogenation step. Such atomic sieving property of nanostructured Pd membrane with 5.1 times increase in catalytic active surface area brings above 14 times higher in butadiene conversion than that of bare Pd foil, with ≈90 % of butenes selectivity at butadiene conversion ≈98 % over 300 h of H 2 -free reaction under 15 mA cm −2 .

关键词： 1,3-Butadiene Pd Membrane Semi-Hydrogenation Unsaturated Hydrocarbons Water Electrolysis

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Self-Assembly of Peapod-like Micrometer Tubes from a Planet-Satellite-type Supramolecular Megamer

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Angewandte Chemie 2022年第46期134卷

作者： Dr. Fugui Xu Dr. Ke Li Dr. Shanlong Li Chen Li Dr. Chunyang Yu Dr. Yuling Wang Dr. Wenfeng Jiang Prof. Shaoliang Lin Prof. Yiyong Mai Prof. Yongfeng Zhou School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative Molecules State Key Laboratory of Metal Matrix Composites Shanghai Key Laboratory of Electrical Insulation and Thermal Ageing Shanghai Jiao Tong University 800 Dongchuan Road Shanghai 200240 China Contribution: Data curation (lead) Formal analysis (lead) Investigation (lead) Methodology (lead) Writing - original draft (equal) Writing - review & editing (equal) Contribution: Data curation (equal) Formal analysis (equal) Investigation (equal) Methodology (equal) Writing - original draft (equal) Writing - review & editing (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Methodology (supporting) Software (lead) Writing - original draft (supporting) Writing - review & editing (supporting) Contribution: Methodology (supporting) Software (supporting) Writing - original draft (supporting) Writing - review & editing (supporting) Contribution: Formal analysis (supporting) Software (supporting) Writing - original draft (supporting) Contribution: Data curation (supporting) Project administration (supporting) Contribution: Formal analysis (supporting) Methodology (supporting) Project administration (supporting) Shanghai Key Laboratory of Advanced Polymeric Materials Key Laboratory for Ultrafine Materials of Ministry of Education School of Materials Science and Engineering East China University of Science and Technology 130 Meilong Road Shanghai 200237 China Contribution: Conceptualization (equal) Methodology (supporting) Project administration (equal) Supervision (equal) Writing - original draft (equal) Writing - review & editing (equal) Contribution: Conceptualization (lead) Formal analysis (lead) Funding acquisition (lead) Project administration (lead) Supervision (lead) Writing - original draft (lead) Writing - review & editing (lead) Contribution: Conceptualization (lead) Formal analysis (equal) Funding acquisition (lead) Methodology (equal) Project

This study presents interesting self-assembly of peapod-like micrometer tubes from a planet-satellite-type supramolecular megamer, which was constructed through the specific host–guest molecular recognition between azobenzene (AZO)-functionalized hyperbranched poly(ethyl-3-oxetanemethanol)- star -poly(ethylene oxide) (HSP-AZO) and β -cyclodextrin(CD)-based hydrophilic hyperbranched polyglycerol (CD- g -HPG). A peapod-like structure with micrometer-sized tube as the pod and vesicles encapsulated inside as the peas was formed through sequential vesicle entosis, linear association, and fusion processes. Dissipative particle dynamics (DPD) simulations support the structural possibility of the supramolecular peapod formation and its mechanism. UV light irradiation could lead to the disassembly of the peapod-like structure. This study expands the family of supramolecular polymers and opens a new avenue to develop bioinspired complex hierarchical nanoarchitectures at the microscopic level.

关键词： Host–Guest Interaction Hyperbranched Polymers Self-Assembly Supramolecular Polymers Vesicles

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Annealing in Argon Universally Upgrades the Na-Storage Performance of Mn-Based Layered Oxide Cathodes by Creating Bulk Oxygen Vacancies

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Angewandte Chemie 2023年第15期135卷

作者： Dr. Junteng Jin Prof. Yongchang Liu Dr. Xudong Zhao Prof. Hui Liu Prof. Shiqing Deng Dr. Qiuyu Shen Ying Hou Prof. He Qi Prof. Xianran Xing Prof. Lifang Jiao Prof. Jun Chen Beijing Advanced Innovation Center for Materials Genome Engineering Department of Physical Chemistry University of Science and Technology Beijing Beijing 100083 China Contribution: Data curation (lead) Investigation (lead) Methodology (lead) Validation (lead) Writing - original draft (lead) Institute for Advanced Materials and Technology State Key Laboratory for Advanced Metals and Materials University of Science and Technology Beijing Beijing 100083 China Contribution: Conceptualization (lead) Formal analysis (lead) Funding acquisition (lead) Methodology (lead) Resources (lead) Supervision (lead) Validation (lead) Writing - original draft (lead) Writing - review & editing (lead) Contribution: Software (lead) Contribution: Formal analysis (equal) Contribution: Formal analysis (equal) Investigation (supporting) Contribution: Formal analysis (supporting) Contribution: Writing - review & editing (supporting) Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Nankai University Tianjin 300071 China Contribution: Supervision (supporting) Writing - review & editing (supporting) Contribution: Conceptualization (lead) Formal analysis (equal) Funding acquisition (lead) Investigation (equal) Methodology (equal) Resources (lead) Supervision (lead) Validation (lead) Writing - review & editing (lead)

Manganese-rich layered oxide cathodes of sodium-ion batteries (SIBs) are extremely promising for large-scale energy storage owing to their high capacities and cost effectiveness, while the Jahn–Teller (J–T) distortion and low operating potential of Mn redox largely hinder their practical applications. Herein, we reveal that annealing in argon rather than conventional air is a universal strategy to comprehensively upgrade the Na-storage performance of Mn-based oxide cathodes. Bulk oxygen vacancies are introduced via this method, leading to reduced Mn valence, lowered Mn 3 d- orbital energy level, and formation of the new-concept Mn domains. As a result, the energy density of the model P2-Na 0.75 Mg 0.25 Mn 0.75 O 2 cathode increases by ≈50 % benefiting from the improved specific capacity and operating potential of Mn redox. The Mn domains can disrupt the cooperative J–T distortion, greatly promoting the cycling stability. This exciting finding opens a new avenue towards high-performance Mn-based oxide cathodes for SIBs.

关键词： Cathode DFT Computations Mn-Based Layered Oxides Oxygen Vacancy Sodium-Ion Batteries

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Grain-growth Inhibitor with Three-section-sintering for Highly Dispersed Single-crystal NCM90 Cubes

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Angewandte Chemie 2023年第2期136卷

作者： Dr. Hao Huang Hongjian Zhu Dr. Jian Gao Dr. Jiantao Wang Prof. Minhua Shao Prof. Weidong Zhou Beijing Advanced Innovation Center for Soft Matter Science and Engineering State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical Technology Beijing 100029 China Contribution: Data curation (lead) Investigation (lead) Writing - original draft (lead) Contribution: Investigation (supporting) China Automotive Battery Research Institute Co. Ltd. Beijing 101407 China Contribution: Methodology (supporting) Supervision (supporting) Department of Chemical and Biological Engineering The Hong Kong University of Science and Technology Hong Kong 999077 China Contribution: Methodology (supporting) Software (supporting) Writing - review & editing (supporting) Contribution: Conceptualization (lead) Supervision (lead) Writing - original draft (equal) Writing - review & editing (lead)

Single crystallization of LiNi x Co y Mn 1-x-y O 2 (NCM) is currently an effective strategy to improve the cycling life of NCM cathode, owing to the reduced surface area and enhanced mechanical strength, but the application of single crystal NCM(SC-NCM) is being hindered by severe particle agglomeration and poor C-rate performance. Here, a strategy of three-section-sintering(TSS) with the presence of grain-growth inhibitor was proposed, in which, the TSS includes three sections of phase-formation, grain-growth and phase-preservation. While, the addition of MoO 3 inhibits the grain growth and restrains the particle agglomeration. With the help of TSS and 1 mol % of MoO 3 , highly dispersed surface Mo-doped SC-NCM(MSC-NCM) cubes are obtained with the average diameter of 1.3 μm. Benefiting from the surface Mo-doping and the reduced surface energy, the Li + -migration preferred (1 0 4) crystalline facet is exposed as the dominant plane in MSC-NCM cubes, because of which, C-rate performance is significantly improved compared with the regular SC-NCM. Furthermore, this preparation strategy is compatible well with the current industrial production line, providing an easy way for the large-scale production of SC-NCM.

关键词： Cathode Cube Grain Growth Inhibitor Lithium-Ion Batteries Single Crystal

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Bi-affinity Electrolyte Optimizing High-Voltage Lithium-Rich Manganese Oxide Battery via Interface Modulation Strategy

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Angewandte Chemie 2023年第30期135卷

作者： Xuedi Yuan Dr. Tao Dong Jiaxin Liu Dr. Yingyue Cui Haotian Dong Dr. Du Yuan Prof. Haitao Zhang Beijing Key Laboratory of Ionic Liquids Clean Process Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 P. R. China School of Henan Institute of Advanced Technology Zhengzhou University Zhengzhou 450002 P. R. China Contribution: Data curation (lead) Formal analysis (lead) Methodology (lead) Writing - original draft (lead) Contribution: Methodology (supporting) Supervision (lead) Contribution: Methodology (supporting) College of Materials Science and Engineering Changsha University of Science and Technology 960 2nd Section Changsha Hunan 410004 P. R. China Henan Key Laboratory of Energy Storage Materials and Processes Zhengzhou Institute of Emerging Industrial Technology Zhengzhou 450003 P. R. China Contribution: Conceptualization (lead) Funding acquisition (lead) Resources (lead) Supervision (lead) Writing - review & editing (lead)

The practical implementation of high-voltage lithium-rich manganese oxide (LRMO) cathode is limited by the unanticipated electrolyte decomposition and dissolution of transition metal ions. The present study proposes a bi-affinity electrolyte formulation, wherein the sulfonyl group of ethyl vinyl sulfone (EVS) imparts a highly adsorptive nature to LRMO, while fluoroethylene carbonate (FEC) exhibits a reductive nature towards Li metal. This interface modulation strategy involves the synergistic use of EVS and FEC as additives to form robust interphase layers on the electrode. As-formed S-endorsed but LiF-assisted configuration cathode electrolyte interphase with a more dominant −SO 2 − component may promote the interface transport kinetics and prevent the dissolution of transition metal ions. Furthermore, the incorporation of S component into the solid electrolyte interphase and the reduction of its poorly conducting component can effectively inhibit the growth of lithium dendrites. Therefore, a 4.8 V LRMO/Li cell with optimized electrolyte may demonstrate a remarkable retention capacity of 97 % even after undergoing 300 cycles at 1 C.

关键词： Bi-Affinity Electrolyte Ethyl Vinyl Sulfone Fluoroethylene Carbonate Interphase Modulation Strategy Lithium Rich Manganese Oxide Cathode

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New Anderson-Based Polyoxometalate Covalent Organic Frameworks as Electrodes for Energy Storage Boosted Through Keto-Enol Tautomerization

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Angewandte Chemie 2023年第32期135卷

作者： Dr. Dawid Pakulski Dr. Adam Gorczyński Daria Brykczyńska Dr. Verónica Montes-García Włodzimierz Czepa Dr. Iwona Janica Dr. Michał Bielejewski Prof. Maciej Kubicki Prof. Violetta Patroniak Prof. Paolo Samorì Dr. Artur Ciesielski Adam Mickiewicz University Foundation Poznań Science and Technology Park Rubież 46 61-612 Poznań Poland Centre for Advanced Technologies Adam Mickiewicz University Uniwersytetu Poznańskiego 10 61-614 Poznań Poland Contribution: Conceptualization (lead) Investigation (lead) Methodology (lead) Writing - original draft (lead) Writing - review & editing (equal) Faculty of Chemistry Adam Mickiewicz University Uniwersytetu Poznańskiego 8 61-614 Poznań Poland Contribution: Investigation (equal) Methodology (equal) Writing - original draft (equal) Contribution: Investigation (equal) Methodology (equal) Université de Strasbourg CNRS Institut de Science et d'Ingénierie Supramoléculaires 8 allée Gaspard Monge 67000 Strasbourg France Institute of Molecular Physics Polish Academy of Sciences M. Smoluchowskiego 17 60-179 Poznań Poland Contribution: Investigation (equal) Contribution: Conceptualization (equal) Data curation (equal) Contribution: Conceptualization (equal) Data curation (equal) Writing - review & editing (lead) Contribution: Data curation (lead) Writing - original draft (equal) Writing - review & editing (lead)

The unique electrochemical properties of polyoxometalates (POMs) render them ideal components for the fabrication of next-generation high-performance energy storage systems. However, their practical applications have been hindered by their high solubility in common electrolytes. This problem can be overcome by the effective hybridization of POMs with other materials. Here we present the design and synthesis of two novel polyoxometalate-covalent organic frameworks (POCOF) via one-pot solvothermal strategy between an amino-functionalized Anderson-type POM and a trialdehyde-based building unit. We show that structural and functional complexity can be enriched by adding hydroxyl groups in the 2,4,6 position to the benzene-1,3,5-tricarbaldehyde allowing to exploit for the first time in POCOFs the keto-enol tautomerization as additional feature to impart greater chemical stability to the COFs and enhanced properties leading to large specific surface area (347 m 2 /g) and superior electrochemical performance of the POCOF-1 electrodes, when compared with POCOF-2 electrodes that possess only imine-type linkage and with pristine POM electrodes. Specifically, POCOF-1 electrodes display remarkable specific, areal, and volumetric capacitance (125 F/g, 248 mF/cm 2 and 41.9 mF/cm 3 , respectively) at a current density of 0.5 A/g, a maximum energy density (56.2 Wh/kg), a maximum power density (3.7 kW/kg) and an outstanding cyclability (90 % capacitance retention after 5000 cycles).

关键词： Covalent Organic Framework Energy Storage Devices Functional Porous Materials Hybrid Materials Polyoxometalate

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Single Atom Bi Decorated Copper Alloy Enables C−C Coupling for Electrocatalytic Reduction of CO2into C2+Products**

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Angewandte Chemie 2023年第30期135卷

作者： Yucheng Cao Suya Chen Shuowen Bo Dr. Wenjun Fan Jiangnan Li Dr. Chunmei Jia Prof. Dr. Zhen Zhou Prof. Dr. Qinghua Liu Dr. Lirong Zheng Prof. Dr. Fuxiang Zhang State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian National Laboratory for Clean Energy Dalian 116023 Liaoning China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences Beijing 100049 China Contribution: Formal analysis (lead) Investigation (lead) Methodology (lead) Writing - original draft (lead) School of Materials Science and Engineering Institute of New Energy Material Chemistry Renewable Energy Conversion and Storage Center (ReCast) Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Nankai University Tianjin 300350 China Contribution: Data curation (equal) Formal analysis (equal) Investigation (equal) Methodology (equal) National Synchrotron Radiation Laboratory University of Science and Technology of China Hefei 230029 Anhui China Contribution: Investigation (supporting) Methodology (supporting) Beijing Synchrotron Radiation Facility Institute of High Energy Physics Chinese Academy of Sciences Beijing 100049 China

Single atom alloy (SAA) catalysts have been recently explored for promotion of various heterogeneous catalysis, but it remains unexplored for selective electrocatalytic reduction of carbon dioxide (CO 2 ) into multi-carbon (C 2+ ) products involving C−C coupling. Herein we report a single-atomic Bi decorated Cu alloy (denoted as BiCu-SAA) electrocatalyst that could effectively modulate selectivity of CO 2 reduction into C 2+ products instead of previous C 1 ones. The BiCu-SAA catalyst exhibits remarkably superior selectivity of C 2+ products with optimal Faradaic efficiency (FE) of 73.4 % compared to the pure copper nanoparticle or Bi nanoparticles-decorated Cu nanocomposites, and its structure and performance can be well maintained at current density of 400 mA cm −2 under the flow cell system. Based on our in situ characterizations and density functional theory calculations, the BiCu-SAA is found to favor the activation of CO 2 and subsequent C−C coupling during the electrocatalytic reaction, as should be responsible for its extraordinary C 2+ selectivity.

关键词： C−C Coupling CO2 Reduction Electrocatalyst Selectivity Single Atom Catalyst

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Amorphous Mo-doped NiS0.5Se0.5Nanosheets@Crystalline NiS0.5Se0.5Nanorods for High Current-density Electrocatalytic Water Splitting in Neutral Media

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Angewandte Chemie 2022年第6期135卷

作者： Dr. Yang Wang Dr. Xiaopeng Li Dr. Zhong Huang Dr. Haozhi Wang Dr. Zelin Chen Dr. Jinfeng Zhang Prof. Xuerong Zheng Prof. Yida Deng Prof. Wenbin Hu State Key Laboratory of Marine Resource Utilization in South China Sea School of Materials Science and Engineering Hainan University Haikou 570228 P. R. China Contribution: Data curation (lead) Investigation (lead) Methodology (lead) Validation (lead) Writing - original draft (lead) School of Materials Science and Engineering Tianjin Key Laboratory of Building Green Functional Materials Tianjin Chengjian University Tianjin 300384 China Contribution: Formal analysis (equal) State Key Laboratory of Marine Resource Utilization in South China Sea College of Information and Communication Engineering Hainan University Haikou 570228 P. R. China Contribution: Methodology (equal) Software (equal) Validation (equal) Contribution: Methodology (equal) Software (equal) School of Materials Science and Engineering Tianjin Key Laboratory of Composite and Functional Materials Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of Education Tianjin University Tianjin 300072 P. R. China Contribution: Methodology (equal) Contribution: Conceptualization (equal) Investigation (equal) Supervision (equal) Contribution: Funding acquisition (lead) Supervision (equal) Contribution: Funding acquisition (supporting)

It is vitally important to develop highly active, robust and low-cost transition metal-based electrocatalysts for overall water splitting in neutral solution especially at large current density. In this work, amorphous Mo-doped NiS 0.5 Se 0.5 nanosheets@crystalline NiS 0.5 Se 0.5 nanorods (Am−Mo−NiS 0.5 Se 0.5 ) was synthesized using a facil one-step strategy. In phosphate buffer saline solution, the Am−Mo−NiS 0.5 Se 0.5 shows tiny overpotentials of 48 and 209 mV for hydrogen evolution reaction (HER), 238 and 514 mV for oxygen evolution reaction (OER) at 10 and 1000 mA cm −2 , respectively. Moreover, Am−Mo−NiS 0.5 Se 0.5 delivers excellent stability for at least 300 h without obvious degradation. Theoretical calculations revealed that the Ni sites in the defect-rich amorphous structure of Am−Mo−NiS 0.5 Se 0.5 owns higher electron state density and strengthened the binding energy of H 2 O, which will optimize H adsorption/desorption energy barriers and reduce the adsorption energy of OER determining step.

关键词： Amorphous Crystalline High-Current-Density Neutral Environment Water Splitting

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