文献类型：期刊文献

英文题名：A DFT Investigation of B-Doped C3N as Single Atom Electrocatalysts for N2-to-NH3 Conversion

作者：Ma P.; Du P.; Song W.; Wang J.

第一作者：Ma P.

机构：[1]School of 3D Printing, Xinxiang University, Henan, Xinxiang, 453003, China;[2]School of Electronic Engineering, Tongling University, Anhui, Tongling, 244061, China;[3]Institute of Plasma Physics, Chinese Academy of Sciences, Anhui, Hefei, 230000, China;[4]School of Science, Henan Institute of Technology, Henan, Xinxiang, 453003, China

第一机构：新乡学院3D打印学院

年份：2024

卷号：25

期号：2

外文期刊名：ChemPhysChem

收录：Scopus(收录号：2-s2.0-85178114551)

语种：英文

外文关键词：B-doped; C₃N; DFT calculations; Nitrogen reduction reaction; Single-atom catalysts

摘要：The NH3 synthesis from N2 plays an important role in the ecological cycle and industrial production. Different from industrial NH3 synthesis with high pollution and energy consumption, electrocatalytic NH3 synthesis is favored because of its environmental protection, energy saving, ambient reaction conditions and other characteristics. However, due to the low efficiency and poor reaction selectivity of the existing electrocatalysts, which can not be used actually, the development of new electrocatalysts for nitrogen reduction reaction (NRR) is particularly urgent. Herein, we designed a series of transition metal atoms anchored B-doped defective C3N surface (TM@B2C3N) as single-atom catalysts. Through the screening process of N2 adsorption activation, N2H formation and NH3 desorption, finally the excellent electrocatalysts with strong stability and high activity (Cr@B2C3N and Mn@B2C3N) were obtained. After simulating the entire pathway, it was found that the NRR process on Cr@B2C3N and Mn@B2C3N via consecutive and distal pathways with the lowest limiting potential of ?0.42 and ?0.52 V, which have the good ability to inhibit hydrogen evolution reaction. Finally, the electronic properties were analyzed, and the reason for their high catalytic activity was summarized. This work provides a new idea for the rational design of NRR electrocatalysts and promotes the practical application of electrocatalysts. ? 2023 Wiley-VCH GmbH.