Liu Zhengqing, Sun Zhehao, Qu Xiaoyan, Nie Kunkun, Yang Yawei, Li Binjie, Chong Shaokun, Yin Zongyou, Huang Wei
Frontiers Science Center for Flexible Electronics, Xi'an Institute of Flexible Electronics (IFE), Xi'an Institute of Biomedical Materials and Engineering, Northwestern Polytechnical University, Xi'an 710129, China.
Research School of Chemistry, The Australian National University, Canberra, Australian Capital Territory 2601, Australia.
J Am Chem Soc. 2024 Aug 21;146(33):23252-23264. doi: 10.1021/jacs.4c05692. Epub 2024 Aug 9.
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'-MoS, -MoSe, 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.
过渡金属二硫属化物（TMDs）的Janus单层由于其可调节的多态性而具有广泛的应用。虽然先前的研究集中在传统的2H相Janus单层，但非常规1T'相的可扩展合成仍然具有挑战性。我们提出了一种新颖的溶液策略，通过在金纳米核上生长夹心式Se-Mo-O/S壳层来制备Janus 1T'-MoOSe和MoSSe单层。与1T'-MoS、-MoSe和-MoOSe相比，Janus Au@1T'-MoSSe催化剂表现出优异的电催化析氢反应（HER）活性，这归因于其独特的电子结构和内在应变。值得注意的是，光激发纳米等离子体金核通过局部表面等离子体（LSP）效应进一步增强了HER，该效应将热电子注入1T'-MoSSe单层壳层的表面硫空位，加速质子还原。内部应变和外部光诱导的金LSP对阴离子空位的这种协同激活，再加上我们的可扩展合成，为开发用于特定应用的可定制多态Janus TMDs提供了一条途径。
