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

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 '-dTMDs) monolayers (TM2@1T '-CrCoS4) were systematically investigated as electrocatalysts for NRR using firstprinciples 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.