Edge-Rich Bicrystalline 1T/2H-MoS<sub>2</sub> Cocatalyst-Decorated {110} Terminated CeO<sub>2</sub> Nanorods for Photocatalytic Hydrogen Evolution
Chengzhang Zhu, Qiming Xian, Qiuying He, Chuanxiang Chen, Weixin Zou, Cheng Sun, Shaobin Wang, Xiaoguang Duan
Abstract
Developing all-solid-state Z-scheme systems with highly active photocatalysts are of huge interest in realizing long-term solar-to-fuel conversion. Here we reported an innovative hybrid of {110}-oriented CeO2 nanorods with edge-enriched bicrystalline 1T/2H-MoS2 coupling as efficient photocatalysts for water splitting. In the composites, the metallic 1T phase acts as an excellent solid state electron mediator in the Z-scheme, while the 2H phase and CeO2 are the adsorption sites of the photosensitizer and reactant (H2O), respectively. Through optimal structure and phase engineering, 1T/2H-MoS2@CeO2 heterojunctions simultaneously achieve high charge separation efficiency, proliferated density of exposed active sites, and excellent affinity to reactant molecules, reaching a superior hydrogen evolution rate of 73.1 μmol/h with an apparent quantum yield of 8.2% at 420 nm. Furthermore, density functional theory calculations show that 1T/2H-MoS2@CeO2 possesses the advantages of intensive electronic interaction from the built-in electric field (negative MoS2 and positive charged CeO2) and reduced H2O adsorption/dissociation energies. This work sheds light on the design of on-demand noble-metal-free Z-scheme heterostructures for solar energy conversion.