文献类型：期刊文献

英文题名：Computational screening of transition metal atom doped C3N as electrocatalysts for nitrogen fixation

作者：Song, Wei[1];Li, Chensi[1];Ma, Pengfei[2];Liu, Xiao[1];Guo, Yongliang[1];Jia, Meng[3];Zhang, Wei[4];He, Chaozheng[5,6]

第一作者：Song, Wei

通讯作者：Zhang, W[1];He, CZ[2];He, CZ[3]

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;[5]Xian Technol Univ, Sch Mat Sci & Chem Engn, Xian 710021, Peoples R China;[6]Xian Technol Univ, Inst Environm & Energy Catalysis, Sch Mat Sci & Chem Engn, Xian 710021, Peoples R China

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

通讯机构：[1]corresponding author), Jilin Univ, Coll Phys, Int Ctr Computat Method & Software, Changchun 130012, Peoples R China;[2]corresponding author), Xian Technol Univ, Sch Mat Sci & Chem Engn, Xian 710021, Peoples R China;[3]corresponding author), Xian Technol Univ, Inst Environm & Energy Catalysis, Sch Mat Sci & Chem Engn, Xian 710021, Peoples R China.

年份：2023

卷号：535

外文期刊名：MOLECULAR CATALYSIS

收录：;EI(收录号：20225213318174);Scopus(收录号：2-s2.0-85144851960);WOS:【SCI-EXPANDED(收录号:WOS:000917457900001)】；

基金：The authors thank the National Natural Science Foundation of China for financial support (Nos. 21603109 and 11904081) . This research is also supported by Natural Science Foundation of Henan Department of Education (Nos. 22A150009 and 22B430013) , the Doctor Initial Research Program of Henan Institute of Technology (No. KQ2006) , the Science and Technology Innovation Talents Project of Henan Province (No. 21HASTIT021) , the Major Science and Technology Project of Xin- xiang City (No. 21ZD009) and the Education Department of Jilin Province and Science and Technology Plan (No. JJKH20211042KJ) .

语种：英文

外文关键词：Nitrogen reduction reaction; Electrocatalysts; DFT calculations; Dope; C3N surface

摘要：NH3 is the main product of nitrogen reduction and is not only an indispensable fertilizer component but also a promising clean energy carrier. The electrocatalytic nitrogen reduction reaction (NRR) can reduce N2 to NH3 under ambient conditions and is one of the most promising technologies to replace the traditional Haber-Bosch process. The careful choice and design of electrocatalysts are both key to achieving an efficient electrocatalytic reaction. In this study, using density functional theory calculations, the catalytic performance of a series of 3d transition metal (TM = Cr, Mn, Fe, Co) single-atom catalysts supported on C3N (TM@C3N) was systematically investigated. The best NRR performance was achieved for the Fe-C@C3N catalyst, and the reaction follows the enzymatic mechanism. Crucially, at a limiting potential of -0.49 V, the competitive hydrogen evolution reaction was effectively inhibited. Furthermore, the electronic properties of the reaction intermediates and Fe-C@C3N were analyzed to reveal the reasons for its high activity. The results of this study will help us understand the catalytic performance of TM-atom-doped C3N and aid the design of more active C3N-based NRR catalysts.