Incorporation of Pd Single‐Atom Sites in Perovskite with an Excellent Selectivity toward Photocatalytic Semihydrogenation of Alkynes

• Published in: Angewandte Chemie International Edition Vol. 63; no. 42; pp. e202410394 - n/a
• Main Authors: Yang, Baoying, Liu, Kunlong, Ma, Yuhui, Ma, Jian‐Jie, Chen, Yi‐Yu, Huang, Meirong, Yang, Can, Hou, Yidong, Hung, Sung‐Fu, Yu, Jimmy C., Zhang, Jinshui, Wang, Xinchen
• Format: Journal Article
• Language: English
• Published: Germany Wiley Subscription Services, Inc 14.10.2024
• Edition: International ed. in English
• Subjects: Alkanes; Alkenes; Alkynes; Catalytic activity; Electronic structure; Hydrogenation; Incorporation; Lattices; Metal-substituted perovskites; Metals; Noble metals; Pd single sites; Perovskites; Phases; Phenylacetylene; Photocatalysis; Selectivity; Semihydrogenation; SrTiO3; Strontium titanates; Styrene; SrTiO3; Pd single sites; Metal-substituted perovskites; Photocatalysis; semihydrogenation
• ISSN: 1433-7851; 1521-3773; 1521-3773
• DOI: 10.1002/anie.202410394

Semihydrogenation is a crucial industrial process. Noble metals such as Pd have been extensively studied in semihydrogenation reactions, owing to their unique catalytic activity toward hydrogen activation. However, the overhydrogenation of alkenes to alkanes often happens due to the rather strong adsorption of alkenes on Pd active phases. Herein, we demonstrate that the incorporation of Pd active phases as single‐atom sites in perovskite lattices such as SrTiO3 can greatly alternate the electronic structure and coordination environment of Pd active phases to facilitate the desorption of alkenes rather than further hydrogenation. Furthermore, the incorporated Pd sites can be well stabilized without sintering by a strong host–guest interaction with SrTiO3 during the activation of H species in hydrogenation reactions. As a result, the Pd incorporated SrTiO3 (Pd‐SrTiO3) exhibits an excellent time‐independent selectivity (>99.9 %) and robust durability for the photocatalytic semihydrogenation of phenylacetylene to styrene. This strategy based on incorporation of active phases in perovskite lattices will have broad implications in the development of high‐performance photocatalysts for selective hydrogenation reactions. Pd active phases have been successfully incorporated in the lattices of SrTiO3 as single‐atom sites (Pd‐SrTiO3) for the semihydrogenation of alkynes. The Pd atoms with an optimized electronic structure and coordination environment facilitate the desorption of alkenes, thereby exhibiting an excellent time‐independent selectivity (>99.9 %) and robust durability.