Boosting charge transfer at inorganic/organic S-scheme interface for photo-Fenton degradation of antibiotics and bacterial inactivation

doi:10.1016/S1872-2067(24)60265-2

Abstract

Abstract:

Solar-driven Fenton-like reactions are promising strategies for degrading pharmaceutical wastewater to address environmental challenges and antibiotic pollution. However, its efficacy is limited by suboptimal light absorption efficiency, rapid charge recombination, and inadequate interfacial charge transfer. In this study, an inorganic/organic S-scheme photo-Fenton system of pseudobrookite/carbon nitride (FTOCN) was synthesized via a hydrothermally coupled calcination process for the effective purification of tetracycline antibiotics under visible-light irradiation. The optimized FTOCN-2 heterostructure exhibits a significantly enhanced TC degradation capacity of 90% within 60 min. The rate constant of FTOCN-2 is 1.6 and 5.2 times greater than those of FTO and CN, respectively. Furthermore, FTOCN exhibits high antibacterial efficacy, highlighting its potential application in the purification of natural water. Measurements via a range of analytical techniques, including Kelvin probe force microscopy, density functional theory calculations, in situ X-ray photoelectron spectroscopy, and femtosecond transient absorption spectroscopy, corroborate the S-scheme mechanism. This study provides a novel perspective for the development of photo-Fenton systems with S-scheme heterojunctions for water purification.

Key words: Photo-Fenton reaction, Inorganic/organic heterojunction, Antibiotics degradation, Bacterial inactivation, S-scheme mechanism

Haotian Qin, Yuxin Huang, Qiang Cheng, Suding Yan, Kai Wang. Boosting charge transfer at inorganic/organic S-scheme interface for photo-Fenton degradation of antibiotics and bacterial inactivation[J]. Chinese Journal of Catalysis, 2025, 72: 106-117.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(24)60265-2

https://www.cjcatal.com/EN/Y2025/V72/I5/106

Figures/Tables 8

Fig. 1. (a) Synthesis procedure for FTOCN composites. TEM images of FTO (b) and FTOCN-2 (c). HRTEM (d) and elemental mapping (e) images of FTOCN-2.

Fig. 2. XRD patterns (a), TG curves (b), and UV-vis DRS spectra (c) of FTO, CN, and FTOCN-X (X = 1, 2, or 3) composites. (d) Calculated PDOS plots of FTO, CN, and FTOCN. (e) Zoomed-in PDOS plots of FTOCN. (f) Band structure diagrams of FTO and CN.

Fig. 3. Photocatalytic degradation curves (a) and pseudo-first-order kinetics (b) of TC over various catalysts under visible light irradiation. Influence of catalyst dosage (c), anions (d), pH (e), and recycling runs (f) on the TC degradation efficiency of FTOCN-2. (g) Photo-Fenton degradation of different pollutants over FTOCN-2. (h) Photocatalytic antibacterial properties of FTO, CN, and FTOCN-2 on samples from the Yangtze River.

Fig. 4. Photocurrent curves (a) and EIS plots (b) of FTO, CN, and FTOCN-2. (c) Photoluminescence spectra of FTO, CN, and FTOCN-X (X = 1, 2, or 3) samples. AFM images, KPFM potential images, and corresponding potential difference curves along the lines in under dark conditions and illumination for FTO (d) and FTOCN-2 (e).

Fig. 5. Work functions of FTO (a) and CN (b). 3D (c) and planar (d) averaged charge for the FTOCN composite (Fe: gold; Ti: blue; O: red; C: brown; and N: silver).

Fig. 6. High-resolution XPS spectra of Fe 2p (a), Ti 3d (b), C 1s (c), and N 1s (d) for FTO, CN, and FTOCN-2. In situ XPS measurements were performed under UV light illumination. (e) Schematic illustration of the charge transfer and separation mechanisms over FTOCN heterojunctions.

Fig. 7. 2D pseudocolor TA spectra of FTO (a) and FTOCN-2 (b) using a 400-nm pump pulse. TA spectra of FTO (c) and FTOCN-2 (d) at indicated time delays. (e) TA kinetics of FTO and FTOCN-2 probed at 650 nm. (f) Schematic of electron quenching pathways in a FTOCN heterojunction.

Fig. 8. (a) Effects of scavengers on photo-Fenton degradation over FTOCN-2. EPR spectra of DMPO-?O2- (b) and DMPO-?OH (c) for FTO, CN, and FTOCN-2. (d) Mechanism of the photo-Fenton reaction at the FTOCN heterojunction.

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