Solution-Processable Microstructuring of 1T′-Phase Janus MoSSe Monolayers for Boosted Hydrogen Production

Janus monolayers of transition metal dichalcogenides (TMDs) offer versatile applications due to their tunable polymorphisms. While previous studies focused on conventional 2H-phase Janus monolayers, the scalable synthesis of an unconventional 1T' phase remains challenging. We present a novel solution strategy for fabricating Janus 1T'-MoOSe and MoSSe monolayers by growing sandwiched Se-Mo-O/S shells onto Au nanocores. The Janus Au@1T'-MoSSe catalyst exhibits superior electrocatalytic hydrogen evolution reaction (HER) activity compared to 1T'-MoS₂, -MoSe₂, and -MoOSe, attributed to its unique electronic structure and intrinsic strain. Remarkably, photoexciting the nanoplasmonic Au cores further enhances the HER via a localized surface plasmon (LSP) effect that drives hot electron injection into surface sulfur vacancies of 1T'-MoSSe monolayer shells, accelerating proton reduction. This synergistic activation of anion vacancies by internal strain and external light-induced Au LSPs, coupled with our scalable synthesis, provides a pathway for developing tailorable polymorphic Janus TMDs for specific applications.