Welcome to Journal of Synthetic Crystals! Today is Jun. 8, 2025 Share:

Journal of Synthetic Crystals ›› 2025, Vol. 54 ›› Issue (4): 708-716.DOI: 10.16553/j.cnki.issn1000-985x.2024.0242

• Research Articles • Previous Articles     Next Articles

Theoretical Study of Ni-MoTiNO for Electrochemical N2 Reduction Reaction

CAO Qi, CUI Luyao   

  1. College of Chemistry and Chemical Engineering, Taiyuan University of Technology, Taiyuan 030024, China
  • Received:2024-10-10 Online:2025-04-15 Published:2025-04-28

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.

Key words: ammonia synthesis, MvK mechanism, electrocatalysis, nitrogen vacancy, MoTiNO, loading

CLC Number: