Post-redox engineering electron configurations of atomic thick C3N4 nanosheets for enhanced photocatalytic hydrogen evolution

[Display omitted] •Post-redox route is a potential strategy for rationally engineering electron configurations of ultrathin C3N4.•Pleasurable PHE efficiency with high AQE surpasses most of existing C3N4-based photocatalysts.•The optimized electron configurations of mesoporous atomic thick layers boo...

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Published in:Applied catalysis. B, Environmental Environmental, 2020-08, Vol.270, p.118855, Article 118855
Main Authors: Li, Yongli, Xu, Xiangfeng, Wang, Jinshu, Luo, Wei, Zhang, Zhipeng, Cheng, Xing, Wu, Junshu, Yang, Yilong, Chen, Ge, Sun, Shaorui, Wang, Lianzhou
Format: Article
Language:English
Subjects:
Atomic thick
Carbon
Carbon nitride
Carrier mobility
Configurations
Current carriers
Electron configurations
Electrons
Energy conversion efficiency
Exfoliation
Functional groups
Hydrogen evolution
Irradiation
Light irradiation
Nanosheets
Nuclear fuels
Photocatalysis
Photocatalytic hydrogen evolution
Post redox
Quantum efficiency
Radiation
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Summary:[Display omitted] •Post-redox route is a potential strategy for rationally engineering electron configurations of ultrathin C3N4.•Pleasurable PHE efficiency with high AQE surpasses most of existing C3N4-based photocatalysts.•The optimized electron configurations of mesoporous atomic thick layers boost the photocatalytic performance. 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.
ISSN:0926-3373
1873-3883
DOI:10.1016/j.apcatb.2020.118855