Theoretical screening of the transition metal heteronuclear dimer anchored graphdiyne for electrocatalytic nitrogen reduction

作     者：Dongwei Ma Zaiping Zeng Liangliang Liu Yu Jia Dongwei Ma;Zaiping Zeng;Liangliang Liu;Yu Jia

作者机构：Key Laboratory for Special Functional Materials of Ministry of Educationand School of Materials Science and EngineeringHenan UniversityKaifeng 475004HenanChina International Laboratory for Quantum Functional Materials of Henanand School of Physics and EngineeringZhengzhou UniversityZhengzhou 450001HenanChina 

出 版 物：《Journal of Energy Chemistry》 (能源化学（英文版）)

年 卷 期：2021年第30卷第3期

页      面：501-509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）] 

基　　金：supported by the National Natural Science Foundation of China(Grant Nos.11704005 and 11774078) the Program for Science&Technology Innovation Talents in Universities of Henan Province(Grant No.20HASTIT028) 

主　　题：Nitrogen reduction reaction Graphdiyne Double-atom catalyst First Principles calculation 

摘      要：Developing efficient electrocatalysts for nitrogen reduction reaction(NRR)is crucial to replace the both energy-intensive and environment-malignant Haber-Bosch *** using density functional theory calculations,we systematically studied the potential of the heteronuclear 3 d transition metal dimers anchored graphdiyne monolayers(FeM@and NiM@GDY,M=Ti,V,Cr,Mn,Fe,Co,Ni,and Cu)as efficient NRR *** all the studied double-atom catalysts(DACs),FeCo@and NiCo@GDY are the most promising with excellent NRR catalytic activity,high ability to suppress the competing hydrogen evolution reaction(HER),and good *** both FeCo@and NiCo@GDY,NRR prefers to the distal pathway with the calculated onset potentials of -0.44 and -0.36 V,respectively,which are comparable and even better than their homonuclear ***,FeCo@and NiCo@GDY have higher ability to suppress HER than Fe_(2)@ and Co_(2)@GDY,which may result from the modulated d state electronic structure due to the synergy effect of the heteronuclear atoms in the *** work not only suggests that FeCo@and NiCo@GDY hold great promises as efficient,low-cost,and stable DACs for NRR,but also further provides a strategy,*** the atomic metal catalysts,to improve the NRR catalytic activity and/or selectivity.