Fundamental Understanding of Hydrogen Evolution Reaction on Zinc Anode Surface:A First‑Principles Study  

作　　者：Xiaoyu Liu Yiming Guo Fanghua Ning Yuyu Liu Siqi Shi Qian Li Jiujun Zhang Shigang Lu Jin Yi 

机构地区：[1]Institute for Sustainable Energy&Department of Chemistry,Shanghai University,Shanghai 200444,People’s Republic of China [2]School of Materials Science and Engineering,Shanghai University,Shanghai 200444,People’s Republic of China [3]College of Materials Science and Engineering,National Engineering Research Center for Magnesium Alloys,Chongqing University,Chongqing 400044,People’s Republic of China

出　　处：《Nano-Micro Letters》2024年第6期180-191,共12页纳微快报（英文版）

基　　金：This work was financially supported by the National Natural Science Foundation of China(22075171);Natural Science Foundation of Shanghai(23ZR1423400);The firstprinciples calculations were supported by the High Performance Computing Center of Shanghai University.

摘　　要：Hydrogen evolution reaction(HER)has become a key factor affecting the cycling stability of aqueous Zn-ion batteries,while the corresponding fundamental issues involving HER are still unclear.Herein,the reaction mechanisms of HER on various crystalline surfaces have been investigated by first-principle calculations based on density functional theory.It is found that the Volmer step is the ratelimiting step of HER on the Zn(002)and(100)surfaces,while,the reaction rates of HER on the Zn(101),(102)and(103)surfaces are determined by the Tafel step.Moreover,the correlation between HER activity and the generalized coordination number(CN)of Zn at the surfaces has been revealed.The relatively weaker HER activity on Zn(002)surface can be attributed to the higher CN of surface Zn atom.The atomically uneven Zn(002)surface shows significantly higher HER activity than the flat Zn(002)surface as the CN of the surface Zn atom is lowered.The CN of surface Zn atom is proposed as a key descriptor of HER activity.Tuning the CN of surface Zn atom would be a vital strategy to inhibit HER on the Zn anode surface based on the presented theoretical studies.Furthermore,this work provides a theoretical basis for the in-depth understanding of HER on the Zn surface.

关 键 词：Aqueous Zn-ion battery Zn anode Hydrogen evolution reaction Coordination number First-principles calculation 

分 类 号：TM912[电气工程—电力电子与电力传动] O469[理学—凝聚态物理]