Constant-potential simulation of electrocatalytic N_(2) reduction over atomic metal-N-graphene catalysts  

作　　者：Sanmei Wang Yong Zhou Hengxin Fang Chunyang Nie Chang Q Sun Biao Wang 

机构地区：[1]Research Institute of Interdisciplinary Sciences(RISE)and School of Materials Science&Engineering,Dongguan University of Technology,Dongguan 523808,China [2]Sino-French Institute of Nuclear Engineering and Technology,Sun Yat-sen University,Zhuhai 519082,China [3]Guangdong Provincial Key Laboratory of Extreme Conditions,Dongguan 523803,China [4]School of Science,Nanyang Technological University,Singapore 639798,Singapore

出　　处：《Chinese Chemical Letters》2025年第3期439-443,共5页中国化学快报(英文版)

基　　金：Natural Science Foundation of Guangdong Province(No.2024A1515011094(C.Q Sun));National Natural Science Foundation of China(Nos.12304243(H.X.Fang),12150100(B.Wang))is gratefully acknowledged。

摘　　要：Charge-neutral method(CNM)is extensively used in investigating the performance of catalysts and the mechanism of N_(2)electrochemical reduction(NRR).However,disparities remain between the predicted potentials required for NRR by the CNM methods and those observed experimentally,as the CNM method neglects the charge effect from the electrode potential.To address this issue,we employed the constant electrode potential(CEP)method to screen atomic transition metal-N-graphene(M_(1)/N-graphene)as NRR electrocatalysts and systematically investigated the underlying catalytic mechanism.Among eight types of M_(1)/N-graphene(M_(1)=Mo,W,Fe,Re,Ni,Co,V,Cr),W_(1)/N-graphene emerges as the most promising NRR electrocatalyst with a limiting potential as low as−0.13 V.Additionally,the W_(1)/N-graphene system consistently maintains a positive charge during the reaction due to its Fermi level being higher than that of the electrode.These results better match with the actual circumstances compared to those calculated by conventional CNM method.Thus,our work not only develops a promising electrocatalyst for NRR but also deepens the understanding of the intrinsic electrocatalytic mechanism.

关 键 词：N_(2) reduction Single-atom catalysts Constant potential GRAPHENE DFT 

分 类 号：O643.36[理学—物理化学]