Computer-aided design of Pt/In 2 O 3 single-atom catalysts for CO 2 hydrogenation to methanol

Methanol (CH 3 OH) synthesis from carbon dioxide (CO 2 ) hydrogenation is an industrially viable approach to CO 2 utilization. For the recently developed indium oxide (In 2 O 3 ) 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/In 2 O 3 single atom catalysts (SACs) with much higher CO 2 reactivity than the In 2 O 3 catalyst while maintaining CH 3 OH selectivity were designed. Several Pt/In 2 O 3 SACs were synthesized to confirm our theoretical predictions. The synthesized Pt/In 2 O 3 SAC in the predominantly bulk-doped form exhibits much higher CO 2 reactivity than the In 2 O 3 catalyst with high stability and similar CH 3 OH selectivity, yielding a CH 3 OH productivity of 1.25 g g cat −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.