Ru‐RuO ₂ Coordinated with Si‐Supported GaN Nanowires for Light‐Driven Simultaneous Activation of CO ₂ and H ₂ to Achieve Exceptional Reverse Water–Gas Shift Reaction

Abstract

Abstract The reverse water–gas shift (RWGS) reaction presents an industrial promise for carbon dioxide valorization. In this work, a dual‐site Ru‐RuO 2 cocatalyst anchored on Si‐supported GaN nanowires (NWs) is developed for solar‐powered CO 2 ‐to‐CO conversion. The assembled Si‐supported GaN NWs/Ru‐RuO 2 delivers a considerable CO rate of 57.89 mmol·cm −2 ·h −1 with nearly 100% selectivity under illumination at 5.5 W·cm −2 without external heating, along with a remarkable turnover frequency of 2.28 × 10 5 h −1 . The temperature‐programmed desorption, in situ spectroscopic characterization, and DFT calculations collectively reveal that the Si‐supported GaN NWs/Ru‐RuO 2 enables simultaneous activation of CO 2 and H 2 . Moreover, the synergy between Ru‐RuO 2 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 2 ‐to‐CO conversion and opens avenues for downstream synthetic applications.