Boosting CO2 Hydrogenation to Methanol via Enriching the Cu─ZnO Interface on Layered Double Oxides

Abstract The controlled creation, selective exposure, and activation of more Cu─ZnO interface while simultaneously minimizing copper usage are crucial for accelerating methanol synthesis from CO 2 hydrogenation over Cu─ZnO‐Al 2 O 3 catalysts. Employing layered double oxides (LDO) as the support with intrinsically structured ZnAl, herein, an efficient triphasic catalyst bearing extrinsically deposited ultrafine Cu nanoparticles derived from metal–organic framework (MOF), manifesting a rich Cu─ZnO interface when compared to identically synthesized counterparts with limited and regular interfaces is presented. The resulting 2D catalyst with the maximized interface between Cu crystallites and LDO gallery (C/ZALDO) dramatically raises the rate of CO 2 hydrogenation to methanol with a remarkable methanol space‐time yield of 1612 g MeOH ·kg Cu −1 ·h −1 at 260 °C and 30 bar. Ex situ characterizations and in situ spectroscopy results confirm that methanol is produced from the hydrogenation of carbon monoxide (CO*) intermediate (via RWGS+CO‐hydro pathway) which is stably adsorbed on the Cu─ZnO interface.