Theoretical screening of cooperative N-bridged dual-atom sites for efficient electrocatalytic nitrogen reduction with remolding insight

作     者：Huimei Chen Yan Yang Chi Jiao Zhiwen Zhuo Junjie Mao Yan Liu Huimei Chen;Yan Yang;Chi Jiao;Zhiwen Zhuo;Junjie Mao;Yan Liu

作者机构：Key Laboratory of Functional Molecular SolidsMinistry of EducationCollege of Chemistry and Materials ScienceAnhui Normal UniversityWuhu 241002China 

出 版 物：《Nano Research》 (纳米研究（英文版）)

年 卷 期：2024年第17卷第4期

页      面：3413-3422页

核心收录：

学科分类：081704[工学-应用化学] 07[理学] 070304[理学-物理化学(含∶化学物理)] 08[工学] 0817[工学-化学工程与技术] 0805[工学-材料科学与工程（可授工学、理学学位）] 0703[理学-化学] 0702[理学-物理学] 

基　　金：supported by the National Natural Science Foundation of China(No.21971002) the Natural Science Foundation of Anhui province(Nos.2008085QB81 and 2208085QA11) 

主　　题：nitrogen reduction dual-atom catalysts high-throughput screening hydrogen evolution reaction density functional theory calculations 

摘      要：The electrocatalytic nitrogen reduction reaction(e-NRR)is a promising alternative method for the Haber–Bosch ***,it still faces many challenges in searching for high activity,stability,and selectivity catalysts and ascertaining the catalytic mechanism with complete ***,a series of graphene-based N-bridged dual-atom catalysts(M1-N-M2/NC)are systematically investigated via first-principle calculation and a high-throughput screening *** result unveils that N_(2) adsorption on M1-N-M2/NC in bridge-on adsorption mode can effectively break the scaling relationship on single-atom catalysts(SACs).Moreover,V-N-Ru/NC and V-N-Os/NC are systematically screened out as promising e-NRR catalysts,with extremely low limiting potentials of-0.20 and-0.18 V,***,the adsorption site competition between*N_(2) and*H,as well as the competitive twin reactions of hydrogen evolution reaction(HER)on intermediates(N_(n)H_(m))during the e-NRR process,is systematically evaluated to form a remodeling insight for the reactions in mechanism,and the e-NRR of new proposed dual-atom catalysts(DACs)is strategically optimized for its high-efficiency performance potential via our remolding insight in e-NRR *** work provides new ideas and insights for the design and mechanism of e-NRR catalysts and an effective strategy for rapidly screening highly efficient e-NRR catalysts.