Abstract
Polymeric carbon nitride (C3N4) with atomic thick layers has displayed ultrashort carrier transfer and ion/molecule migration path for enhancement of photocatalytic performance. However, rational modulation towards electron configurations of ultra-thin C3N4 nanosheets is still a challenge, because the existing exfoliation strategies suffer from uncontrollable atom-defects and edge functional groups, leading to poor solar-to-fuel conversion efficiency. Herein, a post-redox method is developed to form atomic thick C3N4 nanosheets with optimized electron configurations through liquid exfoliation and C-reduction. The as-prepared carbon-reduced atomic thick C3N4 (CRed-AT-C3N4) expose more active sites, greatly enhance charge carrier mobility and distinctly reduce the optical band gap, thus leading to a remarkably improved photocatalytic hydrogen evolution rate of 246.2 μmol h−1 under visible light irradiation (λ > 420 nm), which is 17-fold higher than that of the pristine counterpart. The apparent quantum efficiency reaches 18.52 % at 420 nm and surpasses most of existing C3N4-based photocatalysts.
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