Ru-RuO Coordinated with Si-Supported GaN Nanowires for Light-Driven Simultaneous Activation of CO and H to Achieve Exceptional Reverse Water-Gas Shift Reaction.

The reverse water-gas shift (RWGS) reaction presents an industrial promise for carbon dioxide valorization. In this work, a dual-site Ru-RuO cocatalyst anchored on Si-supported GaN nanowires (NWs) is developed for solar-powered CO-to-CO conversion. The assembled Si-supported GaN NWs/Ru-RuO delivers a considerable CO rate of 57.89 mmol·cm·h with nearly 100% selectivity under illumination at 5.5 W·cm without external heating, along with a remarkable turnover frequency of 2.28 × 10 h. The temperature-programmed desorption, in situ spectroscopic characterization, and DFT calculations collectively reveal that the Si-supported GaN NWs/Ru-RuO enables simultaneous activation of CO and H. Moreover, the synergy between Ru-RuO and GaN substantially reduces the reaction energy barrier from 0.83 to 0.64 eV via the key *COOH intermediate, thereby establishing a new benchmark for light-driven RWGS efficiency. This work provides a strategic design for high-performance CO-to-CO conversion and opens avenues for downstream synthetic applications.