Sulfur Vacancy and Ti(3)C(2)T (x) Cocatalyst Synergistically Boosting Interfacial Charge Transfer in 2D/2D Ti(3)C(2)T (x) /ZnIn(2)S(4) Heterostructure for Enhanced Photocatalytic Hydrogen Evolution

Constructing an efficient photoelectron transfer channel to promote the charge carrier separation is a great challenge for enhancing photocatalytic hydrogen evolution from water. In this work, an ultrathin 2D/2D Ti(3)C(2)T (x) /ZnIn(2)S(4) heterostructure is rationally designed by coupling the ultrathin ZnIn(2)S(4) with few‐layered Ti(3)C(2)T (x) via the electrostatic self‐assembly strategy. The 2D/2D Ti(3)C(2)T (x) /ZnIn(2)S(4) heterostructure possesses larger contact area and strong electronic interaction to promote the charge carrier transfer at the interface, and the sulfur vacancy on the ZnIn(2)S(4) acting as the electron trap further enhances the separation of the photoinduced electrons and holes. As a consequence, the optimal 2D/2D Ti(3)C(2)T (x) /ZnIn(2)S(4) composite exhibits a high photocatalytic hydrogen evolution rate of 148.4 µmol h(−1), which is 3.6 times and 9.2 times higher than that of ZnIn(2)S(4) nanosheet and flower‐like ZnIn(2)S(4), respectively. Moreover, the stability of the ZnIn(2)S(4) is significantly improved after coupling with the few‐layered Ti(3)C(2)T (x) . The characterizations and density functional theory calculation demonstrate that the synergistic effect of the sulfur vacancy and Ti(3)C(2)T (x) cocatalyst can greatly promote the electrons transfer from ZnIn(2)S(4) to Ti(3)C(2)T (x) and the separation of photogenerated charge carriers, thus enhancing the photocatalytic hydrogen evolution from water.