Near-Atomic Indium Catalysts Enable Cost-Efficient High-Pressure Reverse Water–Gas Shift

Abstract The reverse water–gas shift (RWGS) reaction is a pivotal step for converting CO2 into value-added chemical intermediates, yet its implementation under industrially relevant high-pressure conditions remains limited by catalyst deactivation, insufficient productivity, and prohibitive material costs. Here, we report a near-atomic indium catalyst supported on monoclinic ZrO2 that addresses these challenges. Strong In–O–Zr interfacial interactions formed at low indium loadings promote oxygen-vacancy formation while suppressing the over-reduction and sintering of indium oxide, enabling stable operation at temperatures up to 500 °C and pressures of 20 bar. Under these demanding conditions, a catalyst containing only 2.5 wt % In2O3 achieves a CO yield of 42.2 ± 1.9% with a CO productivity of 1305 ± 58 mmol gcat–1 h–1, exceeding previously reported high-pressure RWGS catalysts. Importantly, the low indium content translates into an estimated metal cost of the catalyst of around 12 USD kg–1, comparable to conventional RWGS catalysts while delivering substantially higher performance. These results demonstrate that interface-engineered, low-loading oxide catalysts provide a cost-effective and scalable pathway for high-pressure RWGS, enabling further advancement toward industrial deployment.