MoS2 and Ti3C2 Ensembles into TiO2 for Efficient Photocatalytic Hydrogen Evolution: Dual‐Bonding Interactions and Capacitive Effect Trigger the Intrinsic Activities

Photocatalytic hydrogen evolution provides a sustainable and environmentally benign approach for large‐scale solar energy conversion. How to substantially trigger the photocatalytic efficiency of semiconductor catalysts is still a challenging issue. Here, the sandwich‐like hierarchical Ti 3 C 2 –TiO 2 –MoS 2 (TM) composite is designed and synthesized by in situ growth of TiO 2 and MoS 2 nanosheets on MXene (Ti 3 C 2 ) nanosheets. Consequently, the dual‐cocatalyst‐modified TiO 2 photocatalyst can spark efficient photocatalytic H 2 evolution (4.3 times higher than pristine TiO 2 ) and maintain excellent stability (>30 h). Specifically, the enhancement of photocatalytic efficiency can be originated from the promoted charge separation and migration through TiOMo and COTi dual charge transfer channels and enriched reactive active sites for proton reduction. More importantly, the capacitive properties of MoS 2 and Ti 3 C 2 can retain the photogenerated electrons at a long‐lived charge‐separated state, further improving the activity and stability. The potential of earth‐abundant cocatalysts with capacitance effect to construct high‐efficiency and low‐cost photocatalysts is demonstrated.