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Heterojunction of (P, S) co-doped g-C3N4 and 2D TiO2 for improved carbamazepine and acetaminophen photocatalytic degradation
Abstract
Novel photocatalysts of phosphorus and sulfur co-doped graphitic carbon nitride incorporated in 2D TiO2 structure were successfully fabricated and applied for solar-driven degradation of emerging pollutants from the group of pharmaceuticals not susceptible to biodegradation. The hybrid photocatalysts with different loadings of (P, S)-doped g-C3N4 were characterized by X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), UV–vis diffuse reflectance spectroscopy (DR/UV–vis), photoluminescence (PL) spectroscopy, X-ray photoelectron spectroscopy (XPS), Raman spectroscopy, and transmission electron microscopy (TEM). The optimum (P, S)-doped g-C3N4/TiO2 (5 %) composite revealed improved photocatalytic activity towards the degradation of carbamazepine and acetaminophen. For CBZ, about 100 % degradation was achieved in less than 30 min of photodegradation, whereas for ACT, the complete removal was observed in 60 min of irradiation under simulated solar light. The multi-anion doped g-C3N4/2D TiO2 composite demonstrated an excellent synergy towards the degradation of CBZ and ACT with a synergy index of 1.35 and 1.62. Moreover, the mineralization efficiency measured as TOC removal was 76 % and 40 % for CBZ and ACT, respectively. The reactive oxygen species responsible for the degradation of selected pharmaceuticals are superoxide (•O2– ) and hydroxyl radicals (HO•), and the kinetics of reactions proved to fit the first-order kinetics with a rate constant of 0.21 min 1 for CBZ degradation and 0.074 min 1 for ACT degradation. Our results suggest that (P, S)-doped g-C3N4/ 2D TiO2 heterostructure is a Z-scheme heterojunction, which can effectively separate photogenerated charge carriers. The emissions and decay times analyzed for single components and the optimal (P, S)-doped g-C3N4/ 2D TiO2 (5 %) composite confirmed interfacial charge transfer between TiO2 nanosheets and (P, S)-g-C3N4 and more effective separation of electron-hole pairs. Identification of carbamazepine and acetaminophen intermediates was performed using LC-MS analysis in combination with additional DFT calculations of the possible by-products formation. Regarding reusability, the photocatalytic activity of (P, S)-doped g-C3N4/ 2D TiO2 (5 %) was stable after subsequent cycles of carbamazepine and acetaminophen degradation.
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Authors (8)
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Paweł Głuchowski
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Grzegorz Trykowski doktor
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Marcin Pisarek
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Karol Sikora
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- Accepted or Published Version
- DOI:
- Digital Object Identifier (open in new tab) 10.1016/j.seppur.2023.123320
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- Category:
- Articles
- Type:
- artykuły w czasopismach
- Published in:
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SEPARATION AND PURIFICATION TECHNOLOGY
no. 311,
ISSN: 1383-5866 - Language:
- English
- Publication year:
- 2023
- Bibliographic description:
- Çako E., Dudziak S., Głuchowski P., Trykowski G., Pisarek M., Fiszka Borzyszkowska A., Sikora K., Zielińska-Jurek A.: Heterojunction of (P, S) co-doped g-C3N4 and 2D TiO2 for improved carbamazepine and acetaminophen photocatalytic degradation// SEPARATION AND PURIFICATION TECHNOLOGY -Vol. 311, (2023), s.123320-
- DOI:
- Digital Object Identifier (open in new tab) 10.1016/j.seppur.2023.123320
- Sources of funding:
- Verified by:
- Gdańsk University of Technology
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