Unsaturated bi-heterometal clusters in metal-vacancy sites of 2D MoS2 for efficient hydrogen evolution  

作　　者：Gonglei Shao Jie Xu Shasha Gao Zhang Zhang Song Liu Xu Zhang Zhen Zhou 

机构地区：[1]Interdisciplinary Research Center for Sustainable Energy Science and Engineering(IRC4SE2),School of Chemical Engineering,Zhengzhou University,Zhengzhou,Henan,China [2]College of Chemistry and Materials Engineering,Wenzhou University,Wenzhou,Zhejiang,China [3]Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education),College of Chemistry,Nankai University,Tianjin,China [4]State Key Laboratory of Chemo/Biosensing and Chemometrics,Institute of Chemical Biology and Nanomedicine(ICBN),College of Chemistry and Chemical Engineering,Hunan University,Changsha,Hunan,China [5]Institute of New Energy Material Chemistry,School of Materials Science and Engineering,Nankai University,Tianjin,China

出　　处：《Carbon Energy》2024年第3期264-275,共12页碳能源（英文）

基　　金：supported by the National Natural Science Foundation of China(22205209,52202373 and U21A200972);China Postdoctoral Science Foundation(2022M722867);Key Research Project of Higher Education Institutions in Henan Province(23A530001)。

摘　　要：The valence states and coordination structures of doped heterometal atoms in two-dimensional(2D)nanomaterials lack predictable regulation strategies.Hence,a robust method is proposed to form unsaturated heteroatom clusters via the metal-vacancy restraint mechanism,which can precisely regulate the bonding and valence state of heterometal atoms doped in 2D molybdenum disulfide.The unsaturated valence state of heterometal Pt and Ru cluster atoms form a spatial coordination structure with Pt–S and Ru–O–S as catalytically active sites.Among them,the strong binding energy of negatively charged suspended S and O sites for H+,as well as the weak adsorption of positively charged unsaturated heterometal atoms for H*,reduces the energy barrier of the hydrogen evolution reaction proved by theoretical calculation.Whereupon,the electrocatalytic hydrogen evolution performance is markedly improved by the ensemble effect of unsaturated heterometal atoms and highlighted with an overpotential of 84 mV and Tafel slope of 68.5 mV dec^(−1).In brief,this metal vacancy-induced valence state regulation of heterometal can manipulate the coordination structure and catalytic activity of heterometal atoms doped in the 2D atomic lattice but not limited to 2D nanomaterials.

关 键 词：CLUSTERS hydrogen evolution reaction metal vacancy MOS2 unsaturated heterometal 

分 类 号：TQ116.2[化学工程—无机化工] TB33[一般工业技术—材料科学与工程]