Enhancing Oxygen Reduction Reaction Electrocatalytic Performance of Nickel-Nitrogen-Carbon Catalysts through Coordination Environment Engineering  

作　　者：Hui-Jian Zou Yan Leng Chen-Shuang Yin Xikun Yang Chun-Gang Min Feng Tan Ai-Min Ren 

机构地区：[1]School of Materials Science and Engineering,Kunming University of Science and Technology,Kunming,Yunnan,650093 China [2]Research Center for Analysis and Measurement,Kunming University of Science and Technology,Kunming,Yunnan,650093 China [3]Kunming Sino-Platinum Metals Catalyst Co.,Ltd.,Kunming,Yunnan,650106 China [4]Yunnan Precious Metals Lab.Co.,Ltd.,Kunming,Yunnan,650106 China [5]Institute of Theoretical Chemistry,College of Chemistry,Jilin University,Changchun,Jilin,130023 China

出　　处：《Chinese Journal of Chemistry》2025年第3期297-307,共11页中国化学(英文版)

基　　金：supported by Scientific and Technological Project of Yunnan Precious Metals Laboratory(No.YPML-2023050234);Major Science and Technology Programs of Yunnan(Nos.202302AH360001 and 202307AC110005).

摘　　要：Single-atom catalysts(SACs)have attracted significant attention due to their high atomic utilization and tunable coordination environment.However,the catalytic mechanisms related to the active center and coordination environment remain unclear.In this study,we systematically investigated the oxygen evolution reaction(OER)and oxygen reduction reaction(ORR)catalytic activities of NiN_(4),NiN_(3),NiN_(3)H_(2),NiN_(4)X,NiN_(3)X,and NiN_(3)H_(2)X(X denotes axial ligand)through density functional theory(DFT)calculations.This study unveils two distinct reaction pathways for ORR and OER,involving proton-electron pairs adsorbed from both the solution and the catalyst surface.The overpotential is the key parameter to evaluate the catalytic performance when proton-electron pairs are adsorbed from the solution.NiN_(3)and NiN_(3)H_(2)show promise as pH-universal bifunctional electrocatalysts for both ORR and OER.On the other hand,when proton-electron pairs are adsorbed from the catalyst surface,the reaction energy barrier becomes the crucial metric for assessing catalytic activity.Our investigation reveals that NiN_(3)H_(2)consistently exhibits optimal ORR activity across a wide pH range,regardless of the source of proton-electron pair(solvent or catalyst surface).

关 键 词：Nickel-nitrogen-carbon Axial ligands N-defect FIRST-PRINCIPLES Oxygen evolution reaction Oxygen reduction reaction Local coordination environment ELECTROCATALYSIS 

分 类 号：O64[理学—物理化学]