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Simultaneously Tuning Charge Separation and Oxygen Reduction Pathway on Graphitic Carbon Nitride by Polyethylenimine for Boosted Photocatalytic Hydrogen Peroxide Production
Abstract
The synthesis of hydrogen peroxide (H 2 O 2 ) from H 2 O and O 2 by metal-free photocatalysts (e.g., graphitic carbon nitride, C 3 N 4 ) is a potentially promising approach to generate H 2 O 2 . However, the photocatalytic H 2 O 2 generation activity of the pristine C 3 N 4 in pure H 2 O is poor due to unpropitious rapid charge recombination and unfavorable selectivity. Herein, we report a facile method to boost the photocatalytic H 2 O 2 production by grafting cationic polyethylenimine (PEI) molecules onto C 3 N 4 . Experimental results and density functional theory (DFT) calculations demonstrate PEI can tune the local electronic environment of C 3 N 4 . The unique intermolecular electronic interaction in PEI/C 3 N 4 not only improves the electron–hole separation but also promotes the two-electron O 2 reduction to H 2 O 2 via the sequential two-step single-electron reduction route. With the synergy of improved charge separation and high selectivity of two-electron O 2 reduction, PEI/C 3 N 4 exhibits an unexpectedly high H 2 O 2 generation activity of 208.1 μmol g –1 h –1, which is 25-fold higher than that of pristine C 3 N 4 . This study establishes a paradigm of tuning the electronic property of C 3 N 4 via functional molecules for boosted photocatalysis activity and selectivity.
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Metadata
- Authors
- Zeng, X., Liu, Y., Kang, Y., Li, Q., Xia, Y., Zhu, Y., Hou, H., Uddin, M. H., Gengenbach, T. R., Xia, D., Sun, C., Mccarthy, D. T., Deletic, A., Yu, J., & Zhang, X.
- Venue
- ACS Catalysis
- Publisher
- American Chemical Society (ACS)
- Published
- 2020-02-25
- Volume
- 10
- Issue
- 6
- Pages
- 3697-3706
- ISSN
- 2155-5435 (ISSN-L)
- OpenAlex
- W3008097376
- Cited by
- 482
- References
- 46
- FWCI
- 12.05
- Type
- journal article
- Language
- en
- Open access
- closed
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