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[3]; Liu, Xiao[1]; Guo, Yongliang[1]; Jia, Meng[2]; Wei, Zhang[4]; He, Chaozheng[5]

第一作者：Song, Wei

机构：[1] School of Science, Henan Institute of Technology, Xinxiang, 453003, China; [2] School of Mechnical and Electrical Engineering, Xinxiang University, Xinxiang, 453003, China; [3] School of 3D Printing, Xinxiang University, Xinxiang, 453003, China; [4] Institute of Theoretical Chemistry, College of Chemistry, Jilin University, Changchun, 130012, China; [5] Shaanxi Key Laboratory of Green Preparation and Functionalization for Inorganic Materials, China

第一机构：School of Science, Henan Institute of Technology, Xinxiang, 453003, China

年份：2022

外文期刊名：SSRN

收录：EI(收录号：20220440149)

语种：英文

外文关键词：Ammonia - Atoms - Computation theory - Density functional theory - Design for testability - Electrocatalysis - Electrolysis - Electronic properties - Iron compounds - Nitrogen fixation - Reaction intermediates - Transition metals

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. ? 2022, The Authors. All rights reserved.