Computational Screening of Single Atoms Anchored on Defective Mo ₂ CO ₂ MXene Nanosheet as Efficient Electrocatalysts for the Synthesis of Ammonia

The electrochemical nitrogen reduction reaction (NRR) over single-atom catalysts (SACs) anchored on Mo vacancies of Mo2CO2 MXene nanosheets under ambient conditions suffers from poor selectivity, low yield, and Faradaic efficiency because their sluggish kinetics the competing hydrogen evolution reaction. Herein, density functional theory calculations are performed to improve understanding selectivity yielding ammonia through NRR various isolated SACs, that is, Sc Au, vacancy nanosheet (denoted as MO2CO2-MSA). potential-determining step shows eight candidates (i.e., Y, Zr, Nb, Hf, Ta, W, Re, Os) confined defective layer could promote electroreduction N2 NH3. Among these, Mo2CO2-YSA presented lowest reported Presents energy barrier (0.08 eV) distal pathway high compared with previously synthesized Mo2CO2-RuSA a relatively (0.65 selectivity. In addition, formation is more negative than catalyst, suggesting experimental preparation catalyst highly feasible. This work lays solid foundation for improving rational design MXene-based systems efficient electrocatalysts synthesis ammonia.