First-principles insights into the direct synthesis of acetic acid from CH4 and CO2 over TM–Si@2D catalysts

Abstract

The direct synthesis of acetic acid from natural gases has attracted great attention. However, achieving selective C–C coupling remains a major challenge. We designed doped single-atom transition metal catalysts on 2D materials, guided by DFT calculations on the reaction pathways for acetic acid synthesis via CH₄/CO₂ coupling. Among the catalysts examined, Ni–Si@h-BN shows strong electron synergy in CH₄ activation and C–C coupling under the E–R mechanism, confirmed by kinetics.