Insights into electrochemical nitrogen reduction reaction mechanisms:Combined effect of single transition-metal and boron atom

作     者：Xingzhu Chen Wee-Jun Ong Xiujian Zhao Peng Zhang Neng Li Xingzhu Chen;Wee-Jun Ong;Xiujian Zhao;Peng Zhang;Neng Li

作者机构：State Key Laboratory of Silicate Materials for ArchitecturesWuhan University of TechnologyWuhan 430070HubeiChina School of Energy and Chemical EngineeringXiamen University MalaysiaSelangor Darul Ehsan 43900Malaysia College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005FujianChina State Center for International Cooperation on Designer Low-Carbon&Environmental Materials(CDLCEM)School of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450001HenanChina Shenzhen Research Institute of Wuhan University of TechnologyShenzhen 518000GuangdongChina 

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

年 卷 期：2021年第30卷第7期

页      面：577-585页

核心收录：

学科分类：0820[工学-石油与天然气工程] 081702[工学-化学工艺] 0808[工学-电气工程] 081705[工学-工业催化] 0817[工学-化学工程与技术] 08[工学] 0807[工学-动力工程及工程热物理] 0827[工学-核科学与技术] 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：the Fok Ying-Tong Education Foundation for Young Teachers in the Higher Education Institutions of China(grant number 161008) the Basic Research Program of Shenzhen(grant number JCYJ20190809120015163) the Key R&D Program of Hubei province(grant number 2020CFA087) the Fundamental Research Funds for the Central Universities(grant number 2019III-034) the Xiamen University Malaysia Research Fund(grant number XMUMRF/2019-C3/IENG/0013) the Ministry of Higher Education(MOHE)Malaysia under the Fundamental Research Grant Scheme(FRGS)(grant number FRGS/1/2020/TK02/XMU/02/1) the Overseas Expertise Introduction Project(111 project)for Discipline Innovation of China(grant number B18038) 

主　　题：Boron-carbon–nitrogen(BCN) Single-atom catalysts Electrocatalytic nitrogen reduction reaction Density functional theory Combined effect 

摘      要：Developing single-atom catalysts(SACs) for electrochemical devices is a frontier in energy *** comparison of stability,activity and selectivity between various single atoms is one of the main research focuses in ***,the in-depth understanding of the role that the coordination atoms of single atom play in the catalytic process is ***,we proposed a graphene-like boroncarbon-nitride(BCN) monolayer as the support of single metal *** electrocatalytic nitrogen reduction reaction(eNRR) performances of 3 d,4 d transition metal(TM) atoms embedded in defective BCN were systematically investigated by means of density functional theory(DFT) *** study shows that the TM-to-N and B-to-N π-back bonding can contribute to the activation of N_(2).Importantly,a combined effect is revealed between single TM atom and boron atom on eNRR:TM atom enhances the nitrogen reduction process especially in facilitating the N_(2) adsorption and the NH3 desorption,while boron atom modulates the bonding strength of key intermediates by balancing the charged ***,Nb@BN3 possesses the highest electrocata lytic activity with limiting potential of-0.49 V,and exhibits a high selectivity for nitrogen reduction reaction(NRR) to ammonia compared with hydrogen evolution reaction(HER).As such,this work can stimulate a research doorway for designing multi-active sites of the anchored single atoms and the innate atoms of substrate based on the mechanistic insights to guide future eNRR research.