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

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 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.