Photocatalytic H2O Overall Splitting into H2 Bubbles by Single Atomic Sulfur Vacancy CdS with Spin Polarization Electric Field

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 H-2 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.