Edge‐Enriched Ultrathin MoS2 Embedded Yolk‐Shell TiO2 with Boosted Charge Transfer for Superior Photocatalytic H2 Evolution

Exploring TiO₂‐photocatalysts for sunlight conversion has high demand in artificial photosynthesis. In this work, edge‐enriched ultrathin molybdenum disulfide (MoS₂) flakes are uniformly embedded into the bulk of yolk‐shell TiO₂ as a cocatalyst to accelerate photogenerated‐electron transfer from the bulk to the surface of TiO₂. The as‐formed MoS₂/TiO₂ (0.14 wt%) hybrids exhibit a high hydrogen evolution rate (HER) of 2443 µmol g^?1 h^?1, about 1000% and 470% of that of pristine TiO₂ (247 µmol g^?1 h^?1) and bulk MoS₂ decorated TiO₂ (513 µmol g^?1 h^?1). Such a greatly enhanced HER is attributed to the exposed catalytic edges of the ultrathin MoS₂ flakes with a robust chemical linkage (Ti? S bond), providing rapid charge transfer channels between TiO₂ and MoS₂. The catalytic stability is promoted by the antiaggregation of the highly dispersed MoS₂ flakes in the bulk of yolk‐shell TiO₂. The exponential fitted decay kinetics of time‐resolved photoluminescence (ns‐PL) spectra illustrates that embedding ultrathin MoS₂ flakes in TiO₂ effectively decreases the average lifetime of PL in the MoS₂/TiO₂ hybrids (τ_ave = 4.55 ns), faster than that of pristine TiO₂ (≈7.17 ns) and the bulk MoS₂/TiO₂ (≈6.13 ns), allowing a superior charge separation and charge trapping process for reducing water.