文献类型：期刊文献

英文题名：A first-principles study of transition metal clusters supported on graphene as electrocatalysts for N2 to NH3 reaction

作者：Liu, Xiao[1];Li, Chensi[1];Ma, Pengfei[2];Zhang, Wei[4];Jia, Meng[3];Song, Wei[1]

第一作者：Liu, Xiao

通讯作者：Song, W[1];Jia, M[2]

机构：[1]Henan Inst Technol, Sch Sci, Xinxiang 453003, Peoples R China;[2]Xinxiang Univ, Sch 3D Printing, Xinxiang 453003, Peoples R China;[3]Xinxiang Univ, Sch Mech & Elect Engn, Xinxiang 453003, Peoples R China;[4]Jilin Univ, Coll Phys, Int Ctr Computat Method & Software, Changchun 130012, Peoples R China

第一机构：Henan Inst Technol, Sch Sci, Xinxiang 453003, Peoples R China

通讯机构：[1]corresponding author), Henan Inst Technol, Sch Sci, Xinxiang 453003, Peoples R China;[2]corresponding author), Xinxiang Univ, Sch Mech & Elect Engn, Xinxiang 453003, Peoples R China.|[1107111]新乡学院机电工程学院;[11071]新乡学院;

年份：2023

卷号：35

外文期刊名：MATERIALS TODAY COMMUNICATIONS

收录：;Scopus(收录号：2-s2.0-85161692450);WOS:【SCI-EXPANDED(收录号:WOS:001040505000001)】；

基金：Funding: This work was supported by the Natural Science Founda- tion of Henan Department of Education [grant number 22A150009, 22B430013] , the Science and Technology Innovation Talents Project of Henan Province [grant number 21HASTIT021] , the Major Science and Technology Project of Xinxiang City [grant number 21ZD009] .

语种：英文

外文关键词：Nitrogen reduction reaction; Electrocatalysts; DFT calculations; Single clusters catalyst; Graphene

摘要：NH3 is an important raw material for a variety of chemicals, but also an important carbon-free energy carrier. Currently, NH3 synthesis mainly relies on Habor-Bosch method with high energy consumption, high pollution and low efficiency. So it is urgent to develop a green process for NH3 synthesis. The electrochemical NH3 synthesis can be carried out under ambient conditions. Therefore, it is very important to find electrocatalysts with good stability, high activity and excellent selectivity. Here, we have designed homonuclear transition metal (TM = Fe, Co, Ni) clusters catalyst supported on graphene (TM3 @Gra) as electrocatalysts for nitrogen reduction reaction (NRR). The mechanism of electrocatalytic NRR on TM3 @Gra was investigated. The Fe3 @Gra, Co3 @Gra, and Ni3 @Gra showed high catalytic activity with corresponding limiting potential of -0.60, -0.64 and -0.45 V, respectively. Finally, the selectivity and thermal stability analysis confirmed that TM3 @Gra were the ideal NRR electrocatalysts. We hope that the results of this study will facilitate the design and development of NRR catalysts and provide theoretical reference for the rational design of cluster catalysts.