Ultrathin nitrogen-doped perovskite nanosheets LaTaON have been fabricated by exfoliating Dion-Jacobson-type layered perovskite RbLaTaON. These nanosheets demonstrate superior photocatalytic activities for water splitting into hydrogen and oxygen and remain active with photon wavelengths as far as 600 nm. Their apparent quantum efficiency under visible-light illumination (λ ≥ 420 nm) approaches 1.29% and 3.27% for photocatalytic hydrogen and oxygen production, being almost 4-fold and 8-fold higher than bulk RbLaTaON. Their outstanding performance likely stems from their tiny thickness (single perovskite slab) that essentially removes bulk charge diffusion steps and extends the lifetime of photogenerated charges. Theoretical calculations reveal a peculiar 2D charge transportation phenomenon in RbLaTaON; thus, exfoliating RbLaTaON into LaTaON nanosheets has limited impact on charge transportation properties but significantly enhances the surface areas which contributes to more reaction sites.
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