The dual-transition-metal dichalcogenide monolayers anchored with Mn dimer: Promising electrocatalysts for efficient nitrogen reduction reaction

Abstract

Due to its great efficiency, the electrocatalytic nitrogen reduction reaction (NRR) presents itself as a viable and eco-friendly substitute for the traditional Haber-Bosch ammonia production process. However, it is still a formidable task to find electrocatalysts with high activity and selectivity. In this study, a series of transition metals (TM = Ti–Ni, Zr–Mo, Ru–Pd, and Hf–Pt) anchored on 1T′-dual-transition-metal dichalcogenides (1T′-d-TMDs) monolayers (TM2@1T′-CrCoS4) were systematically investigated as electrocatalysts for NRR using first-principles calculations based on density functional theory. Based on a thorough examination of selectivity, high activity, and stability, Mn2@1T′-CrCoS4 and Co2@1T′-CrCoS4 demonstrate exceptional NRR performance. With a limiting potential of −0.11 V, Mn2@1T′-CrCoS4 stood out among them in terms of catalytic activity, favoring the enzymatic pathway. Furthermore, ab initio molecular dynamics (AIMD) simulations were used to assess the dynamic stability of Mn2@1T′-CrCoS4 and Co2@1T′-CrCoS4. To determine the source of increased activities, the density of states (DOS), charge density difference, and crystal orbital Hamilton population analysis were used. According to our research, the 1T′-d-TMDS is a viable substrate for the development of effective NRR catalysts and offers a platform for electrocatalyst experimentation.