Tailoring Advanced CdS Anisotropy‐Driven Charge Spatial Vectorial Separation and Migration via In Situ Dual Co‐Catalyst Synergistic Layout

Abstract Tailoring advanced anisotropy‐driven efficient separation and migration of photogenerated carriers is a pivotal stride toward enhancing photocatalytic activity. Here, CdS‐MoS 2 binary photocatalysts are tailored into a dumbbell shape by leveraging the rod‐shaped morphology of CdS and employing an in situ tip‐induction strategy. To further enhance the photocatalytic activity, an in situ photo‐deposition strategy is incorporated to cultivate MnO x particles on the dumbbell‐shaped CdS‐MoS 2 . The in situ deposition of MnO x effectively isolated the oxidatively active sites on the CdS surface, emphasizing the reductively active crystalline face of CdS, specifically the (002) face. Benefiting from its robust activity as a reduction active site, MoS 2 adeptly captures photogenerated electrons, facilitating the reduction of H + to produce hydrogen. The anisotropically driven separation of CdS photogenerated carriers markedly mitigates the Coulomb force or binding force of the photogenerated electrons, thus promoting a smoother migration toward the active site for photocatalytic hydrogen evolution. The hydrogen evolution rate of 35MnO x ‐CdS‐MoS 2 ‐3 surpasses that of CdS by nearly an order of magnitude, achieving a quantum efficiency of 22.30% at 450 nm. Under simulated solar irradiation, it attains a rate of 42.86 mmol g −1 h −1 . This work imparts valuable insights for the design of dual co‐catalysts, anisotropy‐driven spatial vectorial charge separation and migration, and the analysis of migration pathways of photogenerated carriers.