Few-Layered 1T-MoS2-Modified ZnCoS Solid-Solution Hollow Dodecahedra for Enhanced Photocatalytic Hydrogen Evolution

摘要： Enhancing solar hydrogen production efficiency essentially relies on the modification of low-cost and highly stable photocatalysts with enhanced light-harvesting ability and promoted charge transfer kinetics. Herein, we report a facile synthetic route to modify the performance of a low-cost metal sulfide semiconductor, consisting of the bimetallic metal-organic frameworks (MOFs)-templating and the simultaneous sulfidation of the photocatalyst and loading of MoS2 co-catalyst. The mutual sulfur atom shared by all the transition metal sulfides allowed the formation of ZnCoS solid-solution structure and the stabilization of the metallic 1T-MoS2 phase, contributing to the photocatalytic activity enhancement from several aspects: i) extending the light absorption region from UV to visible and near-infrared light by the incorporation of another transition metal sulfide species, i.e., CoS; ii) achieving abundant catalytically active sites, and high electronic conductivity between the intimately contacted ZnCoS and MoS2 by loading few-layered 1T-MoS2; and iii) further increasing its capability of utilizing the single-photon with relatively higher energy in the UV-visible region by the involvement of a metal-free photosensitizer–Eosin Y (EY). As a consequence, the novel few-layered 1T MoS2-modified hollow Zn0.5Co0.5S rhombic dodecahedra exhibited a high photocatalytic H2 production activity of 15.47 mmol h-1 g-1 with an apparent quantum efficiency of 30.3% at 420 nm and stability with 90% H2 evolution retention even after seven consecutive runs for total 35 h irradiation. This novel approach to prepare advanced materials could be further extended to the phase-controllable preparation of MoS2 and the discovery of other transition metal chalcogenides with high activity and stability in various applications.