Computational prediction of Mo_(2)@g-C_(6)N_(6) monolayer as an efficient electrocatalyst for N_(2) reduction

作     者：Jiajun Wang Mengyao Shi Guolin Yi Lu Wang Shulai Lei Ke Xu Shujuan Li Jianshuai Mu Jiajun Wang;Mengyao Shi;Guolin Yi;Lu Wang;Shulai Lei;Ke Xu;Shujuan Li;Jianshuai Mu

作者机构：Tianjin Key Laboratory of Structure and Performance for Functional MoleculesCollege of ChemistryTianjin Normal UniversityTianjin 300387China Hubei Key Laboratory of Low Dimensional Optoelectronic Materials and DevicesHubei University of Arts and ScienceXiangyang 441053China Institute of MathematicsFree University of BerlinBerlin D-14195Germany 

出 版 物：《Chinese Chemical Letters》 (中国化学快报（英文版）)

年 卷 期：2022年第33卷第10期

页      面：4623-4627页

核心收录：

学科分类：081702[工学-化学工艺] 081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 080502[工学-材料学] 0805[工学-材料科学与工程（可授工学、理学学位）] 0703[理学-化学] 

基　　金：supported by the Science&Technology Development Fund of Tianjin Education Commission for Higher Education(No.2020KJ008) the Natural Science Foundation of Tianjin(No.18JCQNJC76000) the College Students'Innovation and Entrepreneurship Training Program of Tianjin(No.202110065112) Science and Technology Research Project of Hubei Provincial De-partment of Education(No.D20212603) Hubei University of Arts and Science(Nos.2020kypytd002,XK2021024) China Scholarship Council 

主　　题：g-C_(6)N_(6)monolayer Double-atom catalysts Nitrogen reduction reaction Hydrogen evolution reaction Limiting potential Density functional theory 

摘      要：Electrocatalytic nitrogen reduction reaction(NRR)is an environmentally friendly method for sustainable ammonia synthesis under ambient *** for efficient NRR electrocatalysts with high activity and selectivity is currently urgent but remains great ***,we systematically investigate the NRR catalytic activities of single and double transition metal atoms(TM=Fe,Co,Ni and Mo)anchored on g-C_(6)N_(6) monolayers by performing first-principles *** on the stability,activity,and selectivity analysis,Mo_(2)@g-C_(6)N_(6) monolayer is screened out as the most promising candidate for *** exploration of the reaction mechanism demonstrates that the Mo dimer anchored on g-C_(6)N_(6) can sufficiently activate and efficiently reduce the inert nitrogen molecule to ammonia through a preferred distal pathway with a particularly low limiting potential of -0.06 *** addition,we find that Mo_(2)@g-C_(6)N_(6) has excellent NRR selectivity over the competing hydrogen evolution reaction,with the Faradaic efficiency being 100%.Our work not only predicts a kind of ideal NRR electrocatalyst but also encouraging more experimental and theoretical efforts to develop novel double-atom catalysts(DACs)for NRR.