Computer-aided design of Pt/In2O3 single-atom catalysts for CO2 hydrogenation to methanol†

Abstract

Methanol (CH3OH) synthesis from carbon dioxide (CO2) hydrogenation is an industrially viable approach to CO2 utilization. For the recently developed indium oxide (In2O3) catalyst, higher performance may be achieved by introducing transition metal promoters, although recent studies suggest that single atom sites favour CO formation. Here, by density functional theory-based microkinetic simulations, bulk-doped Pt/In2O3 single atom catalysts (SACs) with much higher CO2 reactivity than the In2O3 catalyst while maintaining CH3OH selectivity were designed. Several Pt/In2O3 SACs were synthesized to confirm our theoretical predictions. The synthesized Pt/In2O3 SAC in the predominantly bulk-doped form exhibits much higher CO2 reactivity than the In2O3 catalyst with high stability and similar CH3OH selectivity, yielding a CH3OH productivity of 1.25 g gcat-1 h-1. This study demonstrates the power of computational methods in designing oxide-based catalysts for industrial reactions and reveals a bulk-doped SAC with high performance.