posted on 2024-05-08, 17:31authored byRuike Tan, Xinhui Wang, Yuxiang Kong, Qing Ji, Qingyun Zhan, Qingchuan Xiong, Xiaoyue Mu, Lu Li
The
technology of liquid organic hydrogen carriers presents great
promise for large-scale hydrogen storage. Nevertheless, the activation
of inert C(sp3)–H bonds in hydrocarbon carriers
poses formidable challenges, resulting in a sluggish dehydrogenation
process and necessitating high operating temperatures. Here, we break
the shackles of C–H bond activation under visible light irradiation
by fabricating subnanometer Pt clusters on defective Ce–Zr
solid solutions. We achieved an unprecedented hydrogen production
rate of 2601 mmol gcat.–1 h–1 (turnover frequency >50,000 molH2 molPt–1 h–1) from cyclohexane, surpassing
the most advanced thermo- and photocatalysts. By optimizing the temperature-dominated
hydrogen transfer process, achievable by harnessing hitherto wasted
infrared light in sunlight, an astonishing 56% apparent quantum efficiency
and a 5.2% solar-to-hydrogen efficiency are attained at 353 K. Our
research stands as one of the most effective photocatalytic processes
to date, holding profound practical significance in the utilization
of solar energy and the exploitation of alkanes.