Ultrasonic cavitation-induced radical processes for tetracycline degradation and Cr(VI) reduction: Highlighting the pivotal role of Cr(V) intermediates.

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Názov: Ultrasonic cavitation-induced radical processes for tetracycline degradation and Cr(VI) reduction: Highlighting the pivotal role of Cr(V) intermediates.
Autori: Li D; College of Hydraulic and Environmental Engineering, China Three Gorges University, Yichang 443002 Hubei, China; Engineering Research Center of Eco-environment in Three Gorges Reservoir Region of Ministry of Education, China Three Gorges University, Yichang 443002 Hubei, China., Luo B; Engineering Research Center of Eco-environment in Three Gorges Reservoir Region of Ministry of Education, China Three Gorges University, Yichang 443002 Hubei, China., Hong F; Engineering Research Center of Eco-environment in Three Gorges Reservoir Region of Ministry of Education, China Three Gorges University, Yichang 443002 Hubei, China., Li R; College of Hydraulic and Environmental Engineering, China Three Gorges University, Yichang 443002 Hubei, China; Engineering Research Center of Eco-environment in Three Gorges Reservoir Region of Ministry of Education, China Three Gorges University, Yichang 443002 Hubei, China., Lv Y; College of Civil Engineering & Architecture, China Three Gorges University, Yichang 443002 Hubei, China; Engineering Research Center of Eco-environment in Three Gorges Reservoir Region of Ministry of Education, China Three Gorges University, Yichang 443002 Hubei, China. Electronic address: yuanfei@whu.edu.cn., Huang Y; College of Hydraulic and Environmental Engineering, China Three Gorges University, Yichang 443002 Hubei, China; Engineering Research Center of Eco-environment in Three Gorges Reservoir Region of Ministry of Education, China Three Gorges University, Yichang 443002 Hubei, China., Huang D; Engineering Research Center of Eco-environment in Three Gorges Reservoir Region of Ministry of Education, China Three Gorges University, Yichang 443002 Hubei, China. Electronic address: huangdi@ctgu.edu.cn.
Zdroj: Ultrasonics sonochemistry [Ultrason Sonochem] 2026 Jan; Vol. 124, pp. 107713. Date of Electronic Publication: 2025 Dec 09.
Spôsob vydávania: Journal Article
Jazyk: English
Informácie o časopise: Publisher: Elsevier Science Country of Publication: Netherlands NLM ID: 9433356 Publication Model: Print-Electronic Cited Medium: Internet ISSN: 1873-2828 (Electronic) Linking ISSN: 13504177 NLM ISO Abbreviation: Ultrason Sonochem Subsets: MEDLINE
Imprint Name(s): Publication: Amsterdam : Elsevier Science
Original Publication: Oxford : Butterworth Heinemann, c1994-
Výrazy zo slovníka MeSH: Ultrasonics*/methods , Tetracycline*/metabolism , Chromium*/metabolism , Water Pollutants, Chemical*/metabolism, Water Purification/methods ; Free Radicals/metabolism ; Temperature
Abstrakt: Tetracycline (TC) and Cr(VI) often co-occur in wastewaters, where their synergistic toxicity and contrasting redox behaviors complicate remediation. In this study, ultrasonic cavitation was employed as a employed as a green and efficient process to simultaneously degrade TC and reduce Cr(VI). Under optimal conditions (20 kHz, 12 mm probe, 131 μm amplitude, 308 K), TC and Cr(VI) removal reached 62.9 % and 70.8 % within 2 h, respectively. The synergistic mechanism was elucidated through radical quenching, electron paramagnetic resonance (EPR) spectroscopy, and complementary computational fluid dynamics (CFD) simulations and density functional theory (DFT) calculations. Cavitation bubble collapse generated both oxidative and reductive radicals, enabling concurrent oxidation and reduction. Radical identification showed that ·O2- and ·H were the dominant reductants responsible for Cr(VI) reduction, whereas 1O2 and ·OH primarily controlled TC degradation. CFD simulations further demonstrated that mechanical energy, internal energy, and bubble growth rate during cavitation were positively correlated with radical generation. Importantly, experimental evidence suggested that Cr(VI) promoted the conversion of ·O2- into 1O2, establishing a coupled radical pathway that linked metal detoxification with antibiotic degradation. Furthermore, Cr(V) intermediates were detected as key transient species, exhibiting strong oxidative capacity toward TC and accelerating Cr(VI) reduction. Complementary DFT calculations confirmed that the coexistence of TC and ·H markedly lowered the energy barrier of Cr(VI) reduction. Overall, this work provides new mechanistic insight into radical transformation and metal-organic coupling under ultrasonic cavitation, and highlights its potential as a sustainable strategy for treating waters co-contaminated with metals and antibiotics.
(Copyright © 2025 The Author(s). Published by Elsevier B.V. All rights reserved.)
Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
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Contributed Indexing: Keywords: (1)O(2) generation; CFD simulation; Cr(V) intermediate; EPR-spin trapping analysis; Simultaneous redox transformation; Ultrasonic cavitation
Substance Nomenclature: F8VB5M810T (Tetracycline)
0R0008Q3JB (Chromium)
0 (Water Pollutants, Chemical)
0 (Free Radicals)
Entry Date(s): Date Created: 20251211 Date Completed: 20260306 Latest Revision: 20260306
Update Code: 20260306
PubMed Central ID: PMC12753498
DOI: 10.1016/j.ultsonch.2025.107713
PMID: 41380544
Databáza: MEDLINE
Popis
Abstrakt:Tetracycline (TC) and Cr(VI) often co-occur in wastewaters, where their synergistic toxicity and contrasting redox behaviors complicate remediation. In this study, ultrasonic cavitation was employed as a employed as a green and efficient process to simultaneously degrade TC and reduce Cr(VI). Under optimal conditions (20 kHz, 12 mm probe, 131 μm amplitude, 308 K), TC and Cr(VI) removal reached 62.9 % and 70.8 % within 2 h, respectively. The synergistic mechanism was elucidated through radical quenching, electron paramagnetic resonance (EPR) spectroscopy, and complementary computational fluid dynamics (CFD) simulations and density functional theory (DFT) calculations. Cavitation bubble collapse generated both oxidative and reductive radicals, enabling concurrent oxidation and reduction. Radical identification showed that ·O<subscript>2</subscript><sup>-</sup> and ·H were the dominant reductants responsible for Cr(VI) reduction, whereas <sup>1</sup>O<subscript>2</subscript> and ·OH primarily controlled TC degradation. CFD simulations further demonstrated that mechanical energy, internal energy, and bubble growth rate during cavitation were positively correlated with radical generation. Importantly, experimental evidence suggested that Cr(VI) promoted the conversion of ·O<subscript>2</subscript><sup>-</sup> into <sup>1</sup>O<subscript>2</subscript>, establishing a coupled radical pathway that linked metal detoxification with antibiotic degradation. Furthermore, Cr(V) intermediates were detected as key transient species, exhibiting strong oxidative capacity toward TC and accelerating Cr(VI) reduction. Complementary DFT calculations confirmed that the coexistence of TC and ·H markedly lowered the energy barrier of Cr(VI) reduction. Overall, this work provides new mechanistic insight into radical transformation and metal-organic coupling under ultrasonic cavitation, and highlights its potential as a sustainable strategy for treating waters co-contaminated with metals and antibiotics.<br /> (Copyright © 2025 The Author(s). Published by Elsevier B.V. All rights reserved.)
ISSN:1873-2828
DOI:10.1016/j.ultsonch.2025.107713