Non-oxidative dehydrogenation of propane produces valuable propylene feedstocks and clean hydrogen fuel but, as an endothermic reaction, conventionally requires high temperatures. Here we report a photocatalyst that combines plasmonic Al@TiO₂ core–shell nanoparticles with Pt single atomic active sites and clusters, capable of efficient dehydrogenation of propane into propylene with high selectivity using visible light illumination. Through strong metal–support interactions, the reducible TiO₂ shell layer controls the nuclearity of the exposed Pt species, which in turn controls their photocatalytic reactivity. A comparison of reaction orders for the light-driven and the corresponding thermally driven process shows that hot carriers lower the apparent C−H activation energy barrier. Plasmon-generated hot carriers, along with the presence of low-coordination Pt sites, suppress further dehydrogenation of propylene and prevent coke formation that would otherwise occur on extended Pt islands. This work clearly demonstrates how plasmonics and single atom catalysts can be combined for high-specificity photocatalyst design.

中文翻译：

---

使用具有 Pt 单原子和团簇的等离子体Al@TiO2核壳纳米颗粒对丙烷进行光驱动脱氢


丙烷的非氧化脱氢可产生有价值的丙烯原料和清洁的氢燃料，但作为吸热反应，通常需要高温。在这里，我们报道了一种光催化剂，它将等离子体 Al@TiO₂ 核壳纳米颗粒与 Pt 单原子活性位点和团簇相结合，能够使用可见光照明将丙烷高效脱氢成具有高选择性的丙烯。通过强金属-载体相互作用，可还原的 TiO₂ 壳层控制暴露的 Pt 物质的核性，进而控制它们的光催化反应性。光驱动过程和相应的热驱动过程的反应顺序比较表明，热载流子降低了表观的 C-H 活化能势垒。等离激元生成的热载流子，以及低配位 Pt 位点的存在，抑制了丙烯的进一步脱氢，并防止了在扩展的 Pt 岛上发生的焦炭形成。这项工作清楚地展示了如何将等离激元和单原子催化剂相结合进行高特异性光催化剂设计。