First-principles insights into the direct synthesis of acetic acid from CH ₄ and CO ₂ over TM–Si@2D catalysts

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 <i>via</i> 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.