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<p>Spillover hydrogenation—a process by which reduction occurs via spilled hydrogen species—is an emerging strategy for selective hydrogenation reactions. Methods to promote spillover hydrogenation on supported Pd nanocatalysts, such as encapsulating Pd nanoparticles or using porous channels, often reduce the availability of Pd sites or increase mass transfer resistance. Here we show that light irradiation can directly induce site separation to enable spillover hydrogenation over semiconductor-supported Pd nanocatalysts, without impairing catalytic activity. Photogenerated electrons accumulated on Pd nanoparticles suppress unsaturated substrate adsorption, ensuring that the Pd exclusively facilitates H<sub>2</sub> dissociation. Photogenerated holes left on the support enhance substrate adsorption and active hydrogen migration. Here, this photo-enhanced spillover hydrogenation is validated across multiple catalytic systems (Pd/SrTiO<sub>3</sub>, Pd/ZnO, Pd/PCN and Ru/MnO<sub><i>x</i></sub>), demonstrating that this effect is not material-specific, but is a generalizable interfacial phenomenon. These findings suggest that light irradiation is a widely applicable methodology for improving spillover hydrogenation efficiency.</p><p></p>

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Photo-enhanced spillover hydrogenation over semiconductor-supported Pd nanocatalysts

  • 期刊论文

  • 发表日期：

    2026年3月9日

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  • Baoying Yang,
  • Kunlong Liu,
  • Shengyang Zhong,
  • Meirong Huang,
  • Jian-Jie Ma,
  • Yi-Yu Chen,
  • Sung-Fu Hung,
  • Yidong Hou,
  • Masakazu Anpo,
  • Jimmy C. Yu,
  • Jinshui Zhang,
  • Xinchen Wang

摘要

Spillover hydrogenation—a process by which reduction occurs via spilled hydrogen species—is an emerging strategy for selective hydrogenation reactions. Methods to promote spillover hydrogenation on supported Pd nanocatalysts, such as encapsulating Pd nanoparticles or using porous channels, often reduce the availability of Pd sites or increase mass transfer resistance. Here we show that light irradiation can directly induce site separation to enable spillover hydrogenation over semiconductor-supported Pd nanocatalysts, without impairing catalytic activity. Photogenerated electrons accumulated on Pd nanoparticles suppress unsaturated substrate adsorption, ensuring that the Pd exclusively facilitates H2 dissociation. Photogenerated holes left on the support enhance substrate adsorption and active hydrogen migration. Here, this photo-enhanced spillover hydrogenation is validated across multiple catalytic systems (Pd/SrTiO3, Pd/ZnO, Pd/PCN and Ru/MnOx), demonstrating that this effect is not material-specific, but is a generalizable interfacial phenomenon. These findings suggest that light irradiation is a widely applicable methodology for improving spillover hydrogenation efficiency.