文献类型：期刊文献

英文题名：Electronegativity-Induced Charge Balancing to Boost Stability and Activity of Amorphous Electrocatalysts

作者：Zhou, Yao[1,7,8];Hao, Wei[2];Zhao, Xiaoxu[2];Zhou, Jiadong[2];Yu, Huimei[3];Lin, Bo[4];Liu, Zheng[2,5];Pennycook, Stephen J.[6];Li, Shuzhou[2];Fan, Hong Jin[1]

机构：[1]Nanyang Technol Univ, Sch Phys & Math Sci, Singapore 637371, Singapore;[2]Nanyang Technol Univ, Sch Mat Sci & Engn, Singapore 639798, Singapore;[3]East China Univ Sci & Technol, Testing Platform, Sch Mat Sci & Engn, Shanghai 200237, Peoples R China;[4]Univ Elect Sci & Technol China, Sch Optoelect Sci & Engn, Chengdu 610054, Sichuan, Peoples R China;[5]Nanyang Technol Univ, Sch Elect & Elect Engn, Singapore 639798, Singapore;[6]Natl Univ Singapore, Dept Mat Sci & Engn, Singapore 117543, Singapore;[7]Beijing Inst Technol, Adv Res Inst Multidisciplinary Sci, Beijing 100081, Peoples R China;[8]Beijing Inst Technol, Sch Chem & Chem Engn, Beijing 100081, Peoples R China

年份：2022

卷号：34

期号：11

外文期刊名：ADVANCED MATERIALS

收录：;EI(收录号：20220611602691);WOS:【SCI-EXPANDED(收录号:WOS:000750344600001)】；

基金：Y.Z. and W.H. contributed equally to this work. H.J.F. and Y.Z. thank the financial support from Agency for Science, Technology and Research (A*STAR), Singapore by AME Individual Research Grants (A1983c0026), and from Singapore Ministry of Education by Tier 2 grant (MOE2017-T2-1-073). Y.Z. appreciates the support from Science and Technology Commission of Shanghai Municipality (19ZR1465100). S.Z.L. and H.W. appreciate the financial support from Singapore Ministry of Education by Tier 1 (RG8/20) and the computing resources from National Supercomputing Centre Singapore. X.X.Z. thanks the support from the Presidential Postdoctoral Fellowship, NTU, Singapore. Z.L., J.D.Z., and X.X.Z. thank the support from Singapore Ministry of Education via AcRF Tier 2 (MOE2019-T2-2-105 and MOE2016-T2-1-131) and AcRF Tier 1 (RG7/18).

语种：英文

外文关键词：amorphous catalysts; aqueous stability; charge transfer; electronegativity; hydrogen evolution reaction

摘要：Amorphization is an efficient strategy to activate intrinsically inert catalysts. However, the low crystallinity of amorphous catalysts often causes high solubility and poor electrochemical stability in aqueous solution. Here, a different mechanism is developed to simultaneously stabilize and activate the water-soluble amorphous MoSxOy via a charge-balancing strategy, which is induced by different electronegativity between the co-dopants Rh (2.28) and Sn (1.96). The electron-rich Sn prefers to stabilize the unstable apical O sites in MoSxOy through charge transfer, which can prevent the H from attacking. Meanwhile, the Rh, as the charge regulator, shifts the main active sites on the basal plane from inert Sn to active apical Rh sites. As a result, the amorphous RhSn-MoSxOy exhibits drastic enhancement in electrochemical stability (eta(10) increases only by 12 mV) after 1000 cycles and a distinct activity (eta(10): 26 mV and Tafel: 30.8 mV dec(-1)) for the hydrogen evolution reaction in acidic solution. This work paves a route for turning impracticably water-soluble catalysts into treasure and inspires new ideas to design high-performance amorphous electrocatalysts.