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

Abstract 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 (RuN 5 ) onto the surface of the NRs. The CdS NRs decorated with plasmonic Au nanoparticles and RuN 5 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−RuN 5 can act as an efficient dual‐function photocatalyst for simultaneous H 2 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−RuN 5 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.