The electrocatalytic nitrogen reduction reaction(e-NRR)is a promising alternative method for the Haber–Bosch process.However,it still faces many challenges in searching for high activity,stability,and selectivity cat...The electrocatalytic nitrogen reduction reaction(e-NRR)is a promising alternative method for the Haber–Bosch process.However,it still faces many challenges in searching for high activity,stability,and selectivity catalysts and ascertaining the catalytic mechanism with complete insight.Here,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 strategy.The 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,respectively.Furthermore,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 mechanism.This 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.展开更多
Ultrathin transition metal dichalcogenides(TMDs)are of particular interest as low-cost alternatives to highly active electrocatalysts because of their high surface activation energy.However,their striking structural c...Ultrathin transition metal dichalcogenides(TMDs)are of particular interest as low-cost alternatives to highly active electrocatalysts because of their high surface activation energy.However,their striking structural characteristics cause chemical instability and undergo oxidation easily.展开更多
基金supported by the National Natural Science Foundation of China(No.21971002)the Natural Science Foundation of Anhui province(Nos.2008085QB81 and 2208085QA11).
文摘The electrocatalytic nitrogen reduction reaction(e-NRR)is a promising alternative method for the Haber–Bosch process.However,it still faces many challenges in searching for high activity,stability,and selectivity catalysts and ascertaining the catalytic mechanism with complete insight.Here,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 strategy.The 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,respectively.Furthermore,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 mechanism.This 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.
基金This work was supported financially by the National Natural Science Foundation of China(21805102,21825103,and 51727809)the National Basic Research Program of China(973 Program,2015CB932600).
文摘Ultrathin transition metal dichalcogenides(TMDs)are of particular interest as low-cost alternatives to highly active electrocatalysts because of their high surface activation energy.However,their striking structural characteristics cause chemical instability and undergo oxidation easily.
