All‐in‐One: Plasmonic Janus Heterostructures for Efficient Cooperative Photoredox Catalysis

• Published in: Angewandte Chemie 2024-09, Vol.136 (38), p.n/a
• Main Authors: Han, Chuang, Zeng, Zikang, Zhang, Xiaorui, Liang, Yujun, Kundu, Bidyut Kumar, Yuan, Lan, Tan, Chang‐Long, Zhang, Yi, Xu, Yi‐Jun
• Format: Article
• Language: eng ; ger
• Subjects: Alcohols; Cadmium sulfide; Catalysis; Catalysts; charge decoupling; Charge transfer; Chemical bonds; Decoupling; dual-function catalyst; Electric fields; functional active site; Gold; Heterostructures; Hydrogen evolution; Janus structure; Nanoparticles; Nanorods; Photoredox catalysis; Plasmonics; selective photoredox
• ISSN: 0044-8249; 1521-3757
• DOI: 10.1002/ange.202408527

Janus heterostructures consisting of multiple jointed components with distinct properties have gained growing interest in the photoredox catalytic field. Herein, we have developed a facile low‐temperature method to gain anisotropic one‐dimensional Au‐tipped CdS (Au−CdS) nanorods (NRs), followed by assembling Ru molecular co‐catalyst (RuN5) onto the surface of the NRs. The CdS NRs decorated with plasmonic Au nanoparticles and RuN5 complex harness the virtues of metal‐semiconductor and inorganic‐organic interface, giving directional charge transfer channels, spatially separated reaction sites, and enhanced local electric field distribution. As a result, the Au−CdS−RuN5 can act as an efficient dual‐function photocatalyst for simultaneous H2 evolution and valorization of biomass‐derived alcohols. Benefiting from the interfacial charge decoupling and selective chemical bond activation, the optimal all‐in‐one Au−CdS−RuN5 heterostructure shows greatly enhanced photoactivity and selectivity as compared to bare CdS NRs, along with a remarkable apparent quantum yield of 40.2 % at 400 nm. The structural evolution and working mechanism of the heterostructures are systematically analyzed based on experimental and computational results. We report the design of a reduction co‐catalyst‐tipped and oxidation co‐catalyst‐capped Janus heterostructure, which reveals the benefits of efficient interfacial charge separation via transfer of photogenerated electrons and holes, respectively, to Au and RuN5 sites for selective organic synthesis and H2 production via photoredox paired reaction coupling.