<p>Propane dehydrogenation is an energy-intensive industrial reaction that requires high temperatures (550–750 °C) to overcome thermodynamic barriers. Here we overcome these limits and demonstrate that near-ambient propane dehydrogenation can be achieved through photo-thermo-catalysis in a water-vapour environment. We reduce the reaction temperature to 50–80 °C using a single-atom catalyst of copper supported on TiO<sub>2</sub> and a continuous-flow fixed-bed reactor. The mechanism differs from conventional propane dehydrogenation in that hydrogen is produced from the photocatalytic splitting of water vapour, surface-bound hydroxyl radicals extract propane hydrogen atoms to form propylene without over-oxidation, and water serves as a catalyst. This route also works for the dehydrogenation of other small alkanes. Moreover, we demonstrate sunlight-driven water-catalysed propane dehydrogenation operating at reaction temperatures as low as 10 °C. We anticipate that this work will be a starting point for integrating solar energy usage into a wide range of high-temperature industrial reactions.</p><p></p>

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Light-driven propane dehydrogenation by a single-atom catalyst under near-ambient conditions

  • Leilei Kang,
  • Beien Zhu,
  • Qingqing Gu,
  • Xinyi Duan,
  • Lei Ying,
  • Guodong Qi,
  • Jun Xu,
  • Lin Li,
  • Yang Su,
  • Yanan Xing,
  • Yanlong Wang,
  • Gang Li,
  • Rengui Li,
  • Yi Gao,
  • Bing Yang,
  • Xiao Yan Liu,
  • Aiqin Wang,
  • Tao Zhang

摘要

Propane dehydrogenation is an energy-intensive industrial reaction that requires high temperatures (550–750 °C) to overcome thermodynamic barriers. Here we overcome these limits and demonstrate that near-ambient propane dehydrogenation can be achieved through photo-thermo-catalysis in a water-vapour environment. We reduce the reaction temperature to 50–80 °C using a single-atom catalyst of copper supported on TiO2 and a continuous-flow fixed-bed reactor. The mechanism differs from conventional propane dehydrogenation in that hydrogen is produced from the photocatalytic splitting of water vapour, surface-bound hydroxyl radicals extract propane hydrogen atoms to form propylene without over-oxidation, and water serves as a catalyst. This route also works for the dehydrogenation of other small alkanes. Moreover, we demonstrate sunlight-driven water-catalysed propane dehydrogenation operating at reaction temperatures as low as 10 °C. We anticipate that this work will be a starting point for integrating solar energy usage into a wide range of high-temperature industrial reactions.