Modulation of d-orbital to realize enriched electronic cobalt sites in cobalt sulfide for enhanced hydrogen evolution in electrocatalytic water/seawater splitting  

作　　者：Jian-Peng Sun Yu Zheng Zi-Sheng Zhang Xiang-Chao Meng Zi-Zhen Li 

机构地区：[1]Key Laboratory of Marine Chemistry Theory and Technology(Ministry of Education),College of Chemistry and Chemical Engineering,Ocean University of China,Qingdao,266100,China [2]Shanxi Institute of Energy,Taiyuan,030600,China [3]Department of Chemical and Biological Engineering,Faculty of Engineering,University of Ottawa,Ottawa,ON,K1N6 N5,Canada

出　　处：《Rare Metals》2024年第2期511-521,共11页稀有金属（英文版）

基　　金：This work was financially supported by Shandong Provincial Natural Science Foundation(No.ZR2021QB056);Taishan Scholars Foundation of Shandong province(No.tsqn201909058).

摘　　要：Herein,a novel single-atomic Pt doping and interface-rich CoS/Co(OH)_(2)(Pt-CoS/Co(OH)_(2)/C)electrocatalyst has been successfully prepared.Benefiting from precise regulation of d-orbital electronic structure modulation on Co site,Pt-CoS/Co(OH)_(2)/C exhibited remarkable HER activity and high stability for hydrogen evolution in splitting both water(73 mV@10 mA·cm^(−2)) and seawater(87 mV@10 mA·cm^(−2)).Notably,atomic Pt doping was introduced into CoS/Co(OH)_(2),which could produce local unbalanced Coulombic force and significantly increased the number of S vacancies,and then expose abundant Co sites.Meantime,Co(OH)_(2) in Pt-CoS/Co(OH)_(2)/C could act as the adsorption sites for H_(2)O in hydrogen evolution reaction process.Density functional theory results also proved that atomic Pt doping,S vacancies and Co(OH)_(2) coupling could result in the formation of enriched electronic Co sites and optimize d_(z2) orbital electronic structure,and then realize the depth upward shift of d-band center and enhance the adsorption of H*on Co sites.

关 键 词：ELECTROCATALYSTS Hydrogen evolution reaction Pt-CoS/Co(OH)_(2) d-band center Electronic structure Water/seawater electrolysis 

分 类 号：TQ116.2[化学工程—无机化工] TQ426