LAUSR

Abstract The Zn-catalyzed acetylene hydration reaction is an important process to produce acetaldehyde in the chemical industry. Heteroatom-doped Zn catalyst has emerged as one of the most promising candidates to replace noble metal-based catalysts for highly efficient acetylene hydration reaction. Single atom catalyst (SAC) has unique performance due to its maximum atomic efficiency, unsaturated metal coordination and electron confinement effect. In this work, geometric and electronic structures of defective graphene supported Zn single atom catalysts with N/S-doping have been systematically studied. The reaction mechanism and activity of acetylene hydration catalyzed by ZnNx (x = 1, 2, 3, 4) and ZnN4S2 are investigated with DFT calculation. Studies have shown that, due to the addition of S atoms, the electronic structure of acetylene is changed when acetylene is adsorbed, which makes the reaction easier. The energy barrier of the ZnN4S2 catalyst is only 11.17 kcal/mol, which is a potential single atom catalyst for acetylene hydration. These results provide insights for the development of highly efficient SACs for acetylene hydration with non-noble single atom metal.