| Summary: | Electrocatalytic reduction of CO<sub>2</sub> to valuable fuels and chemicals can not only alleviate the energy crisis but also improve the atmospheric environment. The key is to develop electrocatalysts that are extremely stable, efficient, selective, and reasonably priced. In this study, spin-polarized density function theory (DFT) calculations were used to comprehensively examine the catalytic efficacy of transition metal-hexaaminobenzene (TM-HAB) monolayers as single-atom catalysts for the electroreduction of CO<sub>2</sub>. In the modified two-dimensional TM-HAB monolayer, our findings demonstrate that the binding of individual metal atoms to HAB can be strong enough for the atoms to be evenly disseminated and immobilized. In light of the conflicting hydrogen evolution processes, TM-HAB effectively inhibits hydrogen evolution. CH<sub>4</sub> dominates the reduction byproducts of Sc, Ti, V, Cr, and Cu. HCOOH makes up the majority of Zn’s reduction products. Co’s primary reduction products are CH<sub>3</sub>OH and CH<sub>4</sub>, whereas Mn and Fe’s primary reduction products are HCHO, CH<sub>3</sub>OH, and CH<sub>4</sub>. Among these, the Ti-HAB reduction products have a 1.14 eV limiting potential and a 1.31 V overpotential. The other monolayers have relatively low overpotentials between 0.01 V and 0.7 V; therefore, we predict that TM-HAB monolayers will exhibit strong catalytic activity in the electrocatalytic reduction of CO<sub>2</sub>, making them promising electrocatalysts for CO<sub>2</sub> reduction.
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