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Article Abstract
Photosynthesis of HO from earth-abundant O and HO molecules offers an eco-friendly route for solar-to-chemical conversion. The persistent challenge is to tune the photo-/thermo- dynamics of a photocatalyst toward efficient electron-hole separation while maintaining an effective driving force for charge transfer. Such a case is achieved here by way of a synergetic strategy of sub-band-assisted Z-Scheme for effective HO photosynthesis via direct O reduction and HO oxidation without a sacrificial agent. The optimized SnS/g-CN heterojunction shows a high reactivity of 623.0 µmol g h for HO production under visible-light irradiation (λ > 400 nm) in pure water, ≈6 times higher than pristine g-CN (100.5 µmol g h). Photodynamic characterizations and theoretical calculations reveal that the enhanced photoactivity is due to a markedly promoted lifetime of trapped active electrons (204.9 ps in the sub-band and >2.0 ns in a shallow band) and highly improved O activation, as a result of the formation of a suitable sub-band and catalytic sites along with a low Gibbs-free energy for charge transfer. Moreover, the Z-Scheme heterojunction creates and sustains a large driving force for O and HO conversion to high value-added HO.
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