Dopant-vacancy activated tetragonal transition metal selenide for hydrogen evolution electrocatalysis  

作　　者：Qiuyan Huang Xin Liu Ze Zhang Lianli Wang Beibei Xiao Zhimin Ao 

机构地区：[1]School of Energy and Power Engineering,Jiangsu University of Science and Technology,Zhenjiang 212003,China [2]School of Materials Science and Engineering,Xi'an University of Science and Technology,Xi'an 710054,China [3]Advanced Interdisciplinary Institute of Environment and Ecology,Beijing Normal University,Zhuhai 519087,China

出　　处：《Chinese Chemical Letters》2023年第7期249-255,共7页中国化学快报（英文版）

基　　金：the supports from the National Natural Science Foundation of China (Nos. 21503097, 51631004, 51701152, 21806023, and 51702345);Natural Science Foundation of Shaanxi Province (No. 2018JQ5181)。

摘　　要：Hydrogen production from water electrolysis using renewable electricity is a highly promising route to solve the energy crisis of human society. The tetragonal 3d-transition metal selenide with metallic feature has been discovered to efficiently catalyze the hydrogen evolution electrocatalysis;however, its performance is still unsatisfactory and further improvement is necessary. Herein, the hydrogen evolution reaction of the functional tetragonal 3d-transition metal selenide with the heteroatom-dopant as well as cationic vacancy is fully investigated by means of density functional theory calculations. Our results identify 53 promising candidates endowed with good activity due to the absolute free energy of hydrogen adsorption |ΔGH| ≤ 0.30 eV wherein 15 candidates with |ΔG_H| ≤ 0.09 eV possess compelling performance in comparison with the benchmark Pt material. Interestingly, the functional CuSe systems account for 29out of 53 candidates, being high attractive for experimental synthesis. According to the analysis of electronic structure, the enhanced performance stems from the upshift of the sp orbitals, which benefits for the improved affinity toward hydrogen capture. This work provides new direction and guidance for the design of novel electrocatalysts.

关 键 词：Hydrogen evolution reaction Transition metal selenide Heteroatom-dopant Density functional theory calculations 

分 类 号：TQ116.2[化学工程—无机化工] TQ426