Low efficient transfer of photogenerated charge carriers to redox sites along with high surface reaction barrier is a bottleneck problem of photocatalytic H2O overall splitting. Here, in the absence of cocatalysts, H2O overall splitting has been achieved by single-atomic S vacancy hexagonal CdS with a spin polarization electric field (PEF). Theoretical and experimental results confirm that single-atomic S vacancy-induced spin PEF with opposite direction to the Coulomb field accelerates charge carrier transport dynamics from the bulk phase to surface-redox sites. By systematically tuning the spin PEF intensity with single-atomic S vacancy content, common pristine CdS is converted to a photocatalyst that can efficiently complete H2O overall splitting by releasing a great number of H2 bubbles under natural solar light. This work solves the bottleneck of solar energy conversion in essence by single atom vacancy engineering, which will promote significant photocatalytic performance enhancement for commercialization.

Fast recombination of charges in bulk or on the surface of semiconductors seriously hinders the conversion efficiency of solar energy due to the inherent challenge of transferring two opposite charges to redox sites separately and simultaneously. Intrinsic spontaneous polarization electric fields (ISPEFs) are considered a promising strategy to solve these challenges, thereby significantly boosting the solar photocatalytic conversion efficiency. In this article, developments for solar energy conversion efficiency under the action of an ISPEF are concluded and reviewed. The key points are the recent research progress on spatial separation and directional transfer under an ISPEF induced by macroscopic, piezoelectric, ferroelectric, and surface or interfacial polarization. Particularly, basic principles of ISPEFs over different types of polarization materials are systematically discussed. Ultimately, future research directions and opportunities for polarization photocatalyst materials with an ISPEF are proposed.

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Defect engineering and cocatalyst loading are effective methods to modify semiconductors to improve their catalytic activity and stability. Herein, sulfur vacancies and dislocations in Mn0.3Cd0.7S nanorods are manipulated by regulating the amount of the sulfur source. After the introduction of Co2P, the maximum H2 production rate for Co2P/Mn0.3Cd0.7S can reach up to 245.3 μmol h−1, ≈2,700 times higher than that of Mn0.3Cd0.7S at the optimal contents of sulfur vacancies and dislocations. The sulfur vacancies serve as the trap sites of electrons and the dislocations might create new transfer channels for carriers, inducing the improvement of catalytic activity and stability.