Spatiotemporal photon distribution control on active sites enables bio-inspired methane-to-methanol conversion.

Abstract

Direct catalytic conversion of methane to methanol offers a pathway for transforming a potent greenhouse gas into a portable clean liquid fuel, thereby mitigating carbon emissions and supporting sustainable energy. However, this process faces challenges from thermodynamically favorable methanol overoxidation. Here, we show that spatiotemporal regulation of photogenerated charge carriers on engineered catalytic sites enables a bio-inspired ordered two-step photocatalytic process that imitates methane monooxygenase. In a platinum-loaded cadmium sulfide photocatalyst, unsaturated sulfur sites modulate hole migration while platinum sites modulate electron migration, ensuring their concurrent surface arrival within picoseconds and prolonged localization. This dynamics temporarily anchors methane at hole-enriched sulfur sites while hydroxyl radical generation occurs at electron-rich platinum sites, decoupling hydroxyl radical formation from methane dehydrogenation to suppress overoxidation. The approach achieves methane-to-methanol conversion with selectivity of 83.5%, offering a bio-inspired solar-driven strategy for C₁ valorization.