密度泛函理论
过渡金属
氨
兴奋剂
金属
化学
材料科学
无机化学
计算化学
化学物理
物理化学
催化作用
有机化学
光电子学
作者
Xiaoling Liang,Shuirong Gu,Zufan Yang,Bo Xie,Shengjie Xia
标识
DOI:10.1016/j.cplett.2024.141461
摘要
Electrocatalytic nitrogen reduction reaction (NRR) represents a promising approach for the sustainable production of ammonia (NH3). However, current electrocatalysts exhibit limitations in terms of active sites, high reaction potential, and poor reaction selectivity. Consequently, there is a pressing need for the development of NRR electrocatalysts with high activity and selectivity under mild conditions. Among them, defect engineering and transition metal doping are two effective methods to improve the electronic structure of catalysts. In this paper, density functional theory was used to study the activity of electrocatalytic NRR on Molybdenum disulfide (MoS2) surfaces with 1–4 S vacancy numbers (VSx–MoS2, x = 1–4) and transition metal (TM)-doped VS3–MoS2 (TM@VS3–MoS2). Both VSx–MoS2 showed better structural stability, with S vacancy defects altering the electronic structure of the surface. As more Mo atoms were exposed on the surface of the structure, the adsorption of N2 gradually enhanced and the reaction was more inclined to undergo NRR. Further investigation of 18 TM-doped VS3–MoS2 revealed that the doping of Sc, Ti, V, Y, Zr and Nb atoms effectively inhibits the hydrogen precipitation reaction and reduced the energy of NH3 desorption, which contributed to the continuation of the reaction. Therefore, the improvement of MoS2 electrocatalytic NRR performance can be achieved by constructing S vacancies and TM doping to provide a better basis and reference for experimental exploration.
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