Li, Ruitao; Gong, Kun; Zheng, Yihan; Wang, Yuxin; Yang, Haoran; Dai, Yuanyuan; Niu, Qiang; Lin, Tiejun; Zhong, Liangshu

NANO ENERGY

2025, ,

Li, Ruitao; Gong, Kun; Zheng, Yihan; Wang, Yuxin; Yang, Haoran; Dai, Yuanyuan; Niu, Qiang; Lin, Tiejun; Zhong, Liangshu

Solar-driven CO2/CH4 dry reforming (DRM) offers an energy-efficient and environmentally sustainable pathway to produce valuable syngas while mitigating greenhouse gas emissions. Although single-atom catalysts (SACs) have been investigated to improve stability in solar-driven DRM, the efficiency is persistently hampered by the intrinsic activity-stability trade-off. Herein, we presented a photo-tailored strategy to manipulate the local coordination environment of ceria-anchored Ni SACs, forming a Ni1-O2 configuration that enabled atomic-level control over reaction pathways for enhanced solar-driven DRM performance. As a result, a record-breaking CO yield of 1258.0 mol & sdot;gNi-1 & sdot;h-1 and a high light-to-fuel efficiency of 35.4 % were achieved, with exceptional stability maintained throughout the reaction. This photothermal performance significantly surpassed most stateof-the-art CO yield (<= 200 mol & sdot;gNi-1 & sdot;h-1) across all reported light-to-fuel efficiency levels. Mechanistic studies indicated that the Ni1-O2-CeOv coordination structure, which was stable after reaction, featuring an electron-rich Ni center, greatly enhanced optical absorption and promoted efficient separation of photogenerated charge carriers. Full-spectrum photon utilization also facilitated the generation of light-activated HCOO* and CH3O* intermediates, accelerating C-H cleavage and suppressing coke formation, respectively. The synergy between photo-generated hot carriers and localized thermal effects lowered activation barriers via tailoring critic reaction intermediates. This work establishes coordination microengineering as a universal strategy to decouple activity-stability correlation in SACs, offering new insights for advancing solar-driven DRM technologies.