Hydrogen evolution reaction activity enhancement from active site turnover mechanism  

作　　者：Jiacheng Wang Tongqing Yang Xiyue Li Haiqin Zhang Yixue Zhang Yan He Hongyao Xue 

机构地区：[1]College of Electromechanical Engineering,Qingdao University of Science and Technology,Qingdao 266061,Shandong,China

出　　处：《Journal of Energy Chemistry》2024年第5期629-638,共10页能源化学（英文版）

基　　金：financial support from the National Natural Science Foundation of China(No.52302098,52336003,52176076,51676103);China Postdoctoral Science Foundation(2023M731855);Taishan Scholar Project of Shandong Province(China)(No.ts20190937);Natural Science Foundation of Shandong Province(China)(No.ZR2023QE344,ZR2021LFG003);Qingdao Postdoctoral Science Foundation(No.QDBSH20220201021,QDBSH20220202084);The Youth Innovation Project for Universities of Shandong Province(2023KJ102)。

摘　　要：Although heteroatom doping is an effective way to improve the catalytic activity of transition metal phosphides(TMPs),the mechanism of activity enhancement needs to be further refined.To this end,we synthesized a Co-doped Ni_(2)P catalyst as a research model and found that the introduction of heterogeneous Co reconstructed the charge distribution around the P site,which effectively enhanced the hydrogen evolution reaction(HER)activity of the pure Ni_(2)P.Based on in-situ Raman real-time monitoring technology,we monitored for the first time that Co doping triggered a switch of the active site(from the original Co-active site to the P-active site),which promoted the adsorption of H_(2)O to enhance the HER activity.The density functional theory(DFT)calculations indicated that the P site of Co-Ni_(2)P expressed the highest activity and the Ni site of pure Ni_(2)P expressed the highest activity,which further confirms the in-situ Raman monitoring results.The active site turnover mechanism discovered in this study will undoubtedly provide more rational and targeted ideas for future catalyst design.

关 键 词：In-situ Raman observation Heteroatom doping Activesites turnover Hydrogen production 

分 类 号：TQ116.2[化学工程—无机化工] TQ426