Solar-driven dry reforming of methane (DRM) offers an energy-saving and environmentally sustainable route for syngas production. Nevertheless, this technology still suffers from insufficient production rates, especially under high gas hourly space velocity (GHSV). In this work, we design an electron pump catalyst with an asymmetric light-responsive architecture, comprising Ru nanoclusters and Ni single atoms, to boost syngas production rates. Under illumination without external heating, Ruac-Nisa/NC achieves a remarkable syngas production of 4.70 mol·gcat -1·h-1 at 500°C and a GHSV of 288 000 h- 1, outperforming state-of-the-art benchmarks by five times, and maintained excellent stability over 1500 min. Experimental and computational studies disclose that the asymmetric architecture enables directional electron transfer and suppresses electron-hole recombination, as an electron pump, creating electron-enriched Ru sites and electron-deficient Ni sites. This interfacial electron configuration furnishes favorable active sites for reactant activation and *CH3O formation, thereby improving DRM kinetics. This work unlocks a design strategy for catalysts in solar-driven reactions and provides a mechanistic lever for enhancing electron-transfer efficiency and reactant activation.
Si‐ma et al. (Tue,) studied this question.