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Graphitic Carbon Nitride Doped with Biphenyl Diimide: Efficient Photocatalyst for Hydrogen Peroxide Production from Water and Molecular Oxygen by Sunlight
Abstract
Photocatalytic hydrogen peroxide (H 2 O 2 ) production from water and molecular oxygen (O 2 ) by sunlight is a promising strategy for green, safe, and sustainable H 2 O 2 synthesis. We prepared graphitic carbon nitride (g-C 3 N 4 ) doped with electron-deficient biphenyl diimide (BDI) units by a simple calcination procedure. The g-C 3 N 4 /BDI catalyst, when photoirradiated by visible light (λ >420 nm) in pure water with O 2, successfully promotes water oxidation by the photogenerated valence band holes and selective two-electron reduction of O 2 by the conduction band electrons, resulting in successful production of millimolar levels of H 2 O 2 . Electrochemical analysis, Raman spectroscopy, and ab initio calculation results revealed that, upon photoexcitation of the catalyst, the photogenerated positive holes are localized on the BDI unit while the conduction band electrons are localized on the melem unit. This spatial charge separation suppresses rapid recombination of the hole–electron pairs and facilitates efficient H 2 O 2 production. The solar-to-chemical energy conversion efficiency for H 2 O 2 production is 0.13%, which is comparable to that for photosynthetic plants. This metal-free photocatalysis therefore shows potential as an artificial photosynthesis for clean solar fuel production.
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Cites
Abe, R. (2010) · Journal of Photochemistry and Photobiology C: Photochemistry Reviews · doi:10.1016/j.jphotochemrev.2011.02.003 · Cited by 1,223
Cited by
Zeng, X., Liu, Y., Kang, Y., Li, Q., Xia, Y., Zhu, Y., Hou, H., Uddin, M. H., Gengenbach, T. R., Xia, D., et al. (2020) · ACS Catalysis · doi:10.1021/acscatal.9b05247 · Cited by 482
Yang, Y., Zeng, G., Huang, D., Zhang, C., He, D., Zhou, C., Wang, W., Xiong, W., Li, X., Li, B., et al. (2020) · Applied Catalysis B: Environmental · doi:10.1016/j.apcatb.2020.118970 · Cited by 412
Teng, Z., Yang, N., Lv, H., Wang, S., Hu, M., Wang, C., Wang, D., & Wang, G. (2019) · Chem · doi:10.1016/j.chempr.2018.12.009 · Cited by 328
Bao, Y., Zou, P., Liu, H., & Zheng, A. (2026) · Chemical Communications · doi:10.1039/d5cc05594f · Cited by 1
Metadata
- Authors
- Kofuji, Y., Ohkita, S., Shiraishi, Y., Sakamoto, H., Tanaka, S., Ichikawa, S., & Hirai, T.
- Venue
- ACS Catalysis
- Publisher
- American Chemical Society (ACS)
- Published
- 2016-09-20
- Volume
- 6
- Issue
- 10
- Pages
- 7021-7029
- ISSN
- 2155-5435 (ISSN-L)
- OpenAlex
- W2514219918
- Cited by
- 376
- References
- 1
- FWCI
- 7.42
- Type
- journal article
- Language
- en
- Open access
- closed
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- Kofuji, Y., Ohkita, S., Shiraishi, Y., Sakamoto, H., Tanaka, S., Ichikawa, S., & Hirai, T. (2016). Graphitic Carbon Nitride Doped with Biphenyl Diimide: Efficient Photocatalyst for Hydrogen Peroxide Production from Water and Molecular Oxygen by Sunlight. ACS Catalysis. https://doi.org/10.1021/acscatal.6b02367
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