Photocatalytic H2O-to-H2O2 synchronized oxidation of an organic pollutant by carbon dot/g-C3N4 composites
Photocatalytic oxidation of organic pollutants using the solar energy is environmentally and economically attractive for developing an energy sustainable organic wastewater treatment process. Here, we employed the impregnation-thermal method to prepare novel carbon dot (CD) dispersed graphitic carbo...
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| Published in: | Journal of cleaner production Vol. 380; p. 134918 |
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| Main Authors: | , , , |
| Format: | Journal Article |
| Language: | English |
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Elsevier Ltd
20.12.2022
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| ISSN: | 0959-6526, 1879-1786 |
| Online Access: | Get full text |
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| Abstract | Photocatalytic oxidation of organic pollutants using the solar energy is environmentally and economically attractive for developing an energy sustainable organic wastewater treatment process. Here, we employed the impregnation-thermal method to prepare novel carbon dot (CD) dispersed graphitic carbon nitride (g-C3N4) (GCN)/pyromellitic dianhydride (PDI) (CD/GCN/PDI) composites for photocatalytic H2O-to-H2O2 and on-site oxidation of organic pollutants in contaminated or waste water. After a 5-h visible-light irradiation, 252 μM of H2O2 can be yielded by the CD/GCN/PDI composites. The CD, serving as an electron reservoir, dispersed on the GCN/PDI composite (i.e., CD0.003/GCN/PDI) facilitates the separation of photo-excited electrons to promote the two-electron reduction O2-to-H2O2 (O2→˙O2−→H2O2). Most importantly, it also on-site activates H2O2 to form ·OH radicals (H2O2→·OH) to enhance oxidation of organic pollutants (e.g., methylene blue and bisphenol A). The ·OH, ∙O2−, and photogenerated h+ account for 4–5%, 14–18%, and 20–25% oxidation of organic pollutants under visible-light irradiation for 3 h, respectively. The CD0.003/GCN/PDI composite was also tested for photocatalytic oxidation of the organic pollutant under visible-light irradiation for at least 12 h to demonstrate its photostability and reusability. This visible-light photocatalytic H2O-to-H2O2 for the enhanced oxidation of organic pollutants by the low-cost and metal-free CD/GCN/PDI composites using solar energy was developed to demonstrate the feasibility of an energy self-sufficient organic wastewater treatment process.
Photocatalytic H2O-to-H2O2 synchronized oxidation of an organic pollutant (R) by the CD/GCN/PDI composites. The CD, serving as an electron reservoir, dispersed on the GCN/PDI composite (i.e., CD0.003/GCN/PDI) facilitates the separation of photo-excited electrons to increase the two-electron reduction O2-to-H2O2 (O2→˙O2−→H2O2). Most importantly, it also on-site activates H2O2 to form ·OH radicals (H2O2→·OH) to enhance oxidation of organic pollutants (e.g., methylene blue and bisphenol A). Other on-site activated highly reactive species such as ∙O2− and photogenerated h+ also contribute to oxidation of organic pollutants in wastewater. [Display omitted]
•The novel CD/GCN/PDI can retard charge recombination for a high yield of H2O2.•The CD/GCN/PDI can induce highly reactive species to enhance organic pollutant oxidation.•The solar-driven H2O-to-H2O2 by CD/GCN/PDI shows energy self-sufficient water clean-up. |
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| AbstractList | Photocatalytic oxidation of organic pollutants using the solar energy is environmentally and economically attractive for developing an energy sustainable organic wastewater treatment process. Here, we employed the impregnation-thermal method to prepare novel carbon dot (CD) dispersed graphitic carbon nitride (g-C3N4) (GCN)/pyromellitic dianhydride (PDI) (CD/GCN/PDI) composites for photocatalytic H2O-to-H2O2 and on-site oxidation of organic pollutants in contaminated or waste water. After a 5-h visible-light irradiation, 252 μM of H2O2 can be yielded by the CD/GCN/PDI composites. The CD, serving as an electron reservoir, dispersed on the GCN/PDI composite (i.e., CD0.003/GCN/PDI) facilitates the separation of photo-excited electrons to promote the two-electron reduction O2-to-H2O2 (O2→˙O2−→H2O2). Most importantly, it also on-site activates H2O2 to form ·OH radicals (H2O2→·OH) to enhance oxidation of organic pollutants (e.g., methylene blue and bisphenol A). The ·OH, ∙O2−, and photogenerated h+ account for 4–5%, 14–18%, and 20–25% oxidation of organic pollutants under visible-light irradiation for 3 h, respectively. The CD0.003/GCN/PDI composite was also tested for photocatalytic oxidation of the organic pollutant under visible-light irradiation for at least 12 h to demonstrate its photostability and reusability. This visible-light photocatalytic H2O-to-H2O2 for the enhanced oxidation of organic pollutants by the low-cost and metal-free CD/GCN/PDI composites using solar energy was developed to demonstrate the feasibility of an energy self-sufficient organic wastewater treatment process.
Photocatalytic H2O-to-H2O2 synchronized oxidation of an organic pollutant (R) by the CD/GCN/PDI composites. The CD, serving as an electron reservoir, dispersed on the GCN/PDI composite (i.e., CD0.003/GCN/PDI) facilitates the separation of photo-excited electrons to increase the two-electron reduction O2-to-H2O2 (O2→˙O2−→H2O2). Most importantly, it also on-site activates H2O2 to form ·OH radicals (H2O2→·OH) to enhance oxidation of organic pollutants (e.g., methylene blue and bisphenol A). Other on-site activated highly reactive species such as ∙O2− and photogenerated h+ also contribute to oxidation of organic pollutants in wastewater. [Display omitted]
•The novel CD/GCN/PDI can retard charge recombination for a high yield of H2O2.•The CD/GCN/PDI can induce highly reactive species to enhance organic pollutant oxidation.•The solar-driven H2O-to-H2O2 by CD/GCN/PDI shows energy self-sufficient water clean-up. Photocatalytic oxidation of organic pollutants using the solar energy is environmentally and economically attractive for developing an energy sustainable organic wastewater treatment process. Here, we employed the impregnation-thermal method to prepare novel carbon dot (CD) dispersed graphitic carbon nitride (g-C₃N₄) (GCN)/pyromellitic dianhydride (PDI) (CD/GCN/PDI) composites for photocatalytic H₂O-to-H₂O₂ and on-site oxidation of organic pollutants in contaminated or waste water. After a 5-h visible-light irradiation, 252 μM of H₂O₂ can be yielded by the CD/GCN/PDI composites. The CD, serving as an electron reservoir, dispersed on the GCN/PDI composite (i.e., CD₀.₀₀₃/GCN/PDI) facilitates the separation of photo-excited electrons to promote the two-electron reduction O₂-to-H₂O₂ (O₂→˙O₂⁻→H₂O₂). Most importantly, it also on-site activates H₂O₂ to form ·OH radicals (H₂O₂→·OH) to enhance oxidation of organic pollutants (e.g., methylene blue and bisphenol A). The ·OH, ∙O₂⁻, and photogenerated h⁺ account for 4–5%, 14–18%, and 20–25% oxidation of organic pollutants under visible-light irradiation for 3 h, respectively. The CD₀.₀₀₃/GCN/PDI composite was also tested for photocatalytic oxidation of the organic pollutant under visible-light irradiation for at least 12 h to demonstrate its photostability and reusability. This visible-light photocatalytic H₂O-to-H₂O₂ for the enhanced oxidation of organic pollutants by the low-cost and metal-free CD/GCN/PDI composites using solar energy was developed to demonstrate the feasibility of an energy self-sufficient organic wastewater treatment process. |
| ArticleNumber | 134918 |
| Author | Chen, Chiaying Wang, H. Paul Hsu, Je-Wei Wei, Ling-Wei |
| Author_xml | – sequence: 1 givenname: Je-Wei surname: Hsu fullname: Hsu, Je-Wei organization: Department of Environmental Engineering, National Cheng Kung University, Tainan, 70101, Taiwan – sequence: 2 givenname: Ling-Wei surname: Wei fullname: Wei, Ling-Wei organization: Department of Environmental Engineering, National Cheng Kung University, Tainan, 70101, Taiwan – sequence: 3 givenname: Chiaying surname: Chen fullname: Chen, Chiaying organization: Department of Environmental Engineering, National Chung Hsing University, Taichung, 40227, Taiwan – sequence: 4 givenname: H. Paul orcidid: 0000-0001-7272-8031 surname: Wang fullname: Wang, H. Paul email: wanghp@ncku.edu.tw organization: Department of Environmental Engineering, National Cheng Kung University, Tainan, 70101, Taiwan |
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| Keywords | Advance oxidation processes Hydrogen peroxide Carbon dots Photocatalysis Graphitic carbon nitride |
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