人工晶体学报2025，Vol.54Issue(4)：708-716,9.DOI:10.16553/j.cnki.issn1000-985x.2024.0242
Ni-MoTiNO用于电化学N2还原反应的理论研究
Theoretical Study of Ni-MoTiNO for Electrochemical N2 Reduction Reaction
摘要
Abstract
The electrochemical nitrogen reduction reaction(ENRR)is one of the sustainable development technologies for the synthesis of NH3 to replace the Haber-Bosch process.The core issue is to find stable electrocatalysts with high catalytic activity and selectivity.Since the transition metal oxynitrides(TMNO)surface follows the Mars-van Krevelen(MvK)mechanism pathway for ammonia synthesis reaction,it exhibits more favorable N2 adsorption and activation than the conventional association mechanism.Based on this,Ni was selected to be loaded on dual-sites MoTiNO with the best ENRR performance,and the Ni-MoTiNO structure was constructed as an electrochemical N2 reduction catalyst by the density function theory(DFT)calculation method,and four aspects,including the structural stability,two-site adsorption behaviors,ENRR catalytic activity based on the *H-migration-assisted MvK mechanism,and the analysis of the electronic properties,were investigated.Results show that the synergistic action of the dual sites(Ni and Nv)on the surface of Ni-MoTiNO both promotes *H migration and effectively breaks the linear proportionality between the strong adsorption of *N-related intermediates and the difficulty in resolving the products in ENRR.Experiments have proved that the synthesized Ni-MoTiNO can effectively achieve ammonia synthesis and has a relatively high selectivity.关键词
合成氨/MvK机理/电催化/氮空位/MoTiNO/负载Key words
ammonia synthesis/MvK mechanism/electrocatalysis/nitrogen vacancy/MoTiNO/loading分类
化学引用本文复制引用
曹琦,崔璐瑶..Ni-MoTiNO用于电化学N2还原反应的理论研究[J].人工晶体学报,2025,54(4):708-716,9.基金项目
国家自然科学基金(21978187) （21978187）
山西省自然科学基金(202203021221058) （202203021221058）
