Significant role of UV and carbonate radical on the degradation of oxytetracycline in UV-AOPs: Kinetics and mechanism
Open accessAbstract
Carbonate radical (CO3(•-)), a selective oxidant, reacts readily with electron-rich compounds through electron transfer and/or hydrogen abstraction. In this study, the role of CO3(•-) in degrading oxytetracycline (OTC) by UV only, UV/H2O2 and UV/persulfate (UV/PS) advanced oxidation processes (AOPs) in the presence of HCO3(-) or CO3(2-) was investigated. For UV only process, the presence of photosensitizers, i.e., nitrate (NO3(-)) and natural organic matter (NOM), had different impacts on OTC degradation, i.e., an enhancing effect by NO3(-) due to the generation of HO(•) and a slight inhibiting effect by NOM possibly due to a light scattering effect. Differently for UV/H2O2 and UV/PS processes, the presence of NO3(-) hardly influenced the destruction of OTC. Generation of CO3(•-) presented a positive role on OTC degradation by UV/NO3(-)/HCO3(-). Such influence was also observed in the two studied AOPs in the presence of both bicarbonate and other natural water constituents. When various natural water samples from different sources were used as reaction matrices, UV only and UV/H2O2 showed an inhibiting effect while UV/PS demonstrated a comparable or even promoting effect in OTC decomposition. After elucidating the potential contribution of UV direct photolysis via excited state OTC* at an elevated reaction pH condition, putative OTC transformation byproducts via CO3(•-) reaction were identified by ultra-high definition accurate-mass quadrupole time-of-flight tandem mass spectrometry (QTOF/MS). Five different reaction pathways were subsequently proposed, including hydroxylation (+16 Da), quinonization (+14 Da), demethylation (-14 Da), decarbonylation (-28 Da) and dehydration (-18 Da). The significant role of UV at high pH and CO3(•-) on OTC removal from contaminated water was therefore demonstrated both kinetically and mechanistically.
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The pH change increases the electron density around the compound and facilitates the reaction of carbonate radical.
“The pH change increases the electron density around the compound and facilitates the reaction of carbonate radical.”
From Advanced Oxidation Processes for Degradation of Water Pollutants—Ambivalent Impact of Carbonate Species: A Review (2023) · cites this paper as [67]
The Introduction (page unavailable) says carbonate radical reacts mainly with electron-rich compounds, and Section 3.4.3 proposes that excited oxytetracycline may transfer an electron to it more easily. The paper does not say that a pH change increases electron density around oxytetracycline; its discussion of faster degradation at high pH proposes a different, still uncertain mechanism involving excited oxytetracycline. (LLM, conf=0.82)
Experimental — accuracy not yet measuredIn UV/H2O2 photolysis, the rate constant was 4.8 × 10-3 cm2 mJ-1, which is increased to 6 × 10-3 cm2 mJ-1 with the increase in CO3 2-/HCO3- concentration.
“In UV/H2O2 photolysis, the rate constant was 4.8 × 10 -3 cm 2 mJ -1 , which is increased to 6 × 10 -3 cm 2 mJ -1 with the increase in CO3 2 -/HCO3 -concentration.”
From Advanced Oxidation Processes for Degradation of Water Pollutants—Ambivalent Impact of Carbonate Species: A Review (2023) · cites this paper as [67]
Section 3.2 (page unavailable) reports that adding NaHCO₃ promoted oxytetracycline degradation in the studied UV/H₂O₂ conditions, supporting the claimed direction of change. The passages in our copy do not give the stated rate constants of 4.8 × 10⁻³ and 6 × 10⁻³ cm² mJ⁻¹, so those numerical values are not verified. (LLM, conf=0.84)
Experimental — accuracy not yet measuredThe degradation of oxytetracycline in the UV/H2O2 system in carbonate solution was promoted with the addition of CO3 2-.
“Liu et al. investigated the transformation of oxytetracycline in the UV/H2O2 system in carbonate solution. The degradation was promoted with the addition of CO3 2 -.”
From Advanced Oxidation Processes for Degradation of Water Pollutants—Ambivalent Impact of Carbonate Species: A Review (2023) · cites this paper as [67]
The Results and discussion (section 3.2; page unavailable) report that adding NaHCO₃ promoted oxytetracycline degradation under the studied UV/H₂O₂ conditions. The claim instead specifies addition of CO₃²⁻. Section 3.4 uses Na₂CO₃ in a UV/H₂O₂ experiment with tert-butanol, but does not establish the claimed promoting effect from adding CO₃²⁻. (LLM, conf=0.83)
Experimental — accuracy not yet measured90% degradation of oxytetracycline was observed with a lower UV fluence of 80 mJ/cm2 in the UV/PS process.
“However, the 90% degradation was observed with a lower UV fluence of 80 mJ/cm 2 in the UV/PS process.”
From Advanced Oxidation Processes for Degradation of Water Pollutants—Ambivalent Impact of Carbonate Species: A Review (2023) · cites this paper as [67]
Section 3.3 reports oxytetracycline removal by UV/PS and says it was more effective than UV/H₂O₂ or UV alone in the natural waters tested. Section 2.3 describes sampling at given UV fluences, but the passages found do not report 90% degradation at 80 mJ/cm²; searches for both numbers found no matching result. Page numbers were not available in our copy. (LLM, conf=0.83)
Experimental — accuracy not yet measuredThe degradation efficiency for oxytetracycline in UV/NO3- was 30%, and that in UV/H2O2 was 90% with UV fluence of 320 mJ/cm2.
“The degradation efficiency for oxytetracycline in UV/NO3 -was 30%, and that in UV/H2O2 was 90% with UV fluence of 320 mJ/cm 2 .”
From Advanced Oxidation Processes for Degradation of Water Pollutants—Ambivalent Impact of Carbonate Species: A Review (2023) · cites this paper as [67]
The Results and discussion section (page unavailable) reports that nitrate enhanced oxytetracycline degradation under UV and discusses degradation in the UV/H₂O₂ system. Neither that section nor the Photochemical experiments section (page unavailable) states 30% and 90% degradation at a UV fluence of 320 mJ/cm²; searches for the fluence and percentages did not verify those figures. (LLM, conf=0.78)
Experimental — accuracy not yet measured
Adding HCO3- had a positive effect in all the above UV-activated systems.
“On the other hand, adding HCO3 -had a positive effect in all the above UV-activated systems.”
From Advanced Oxidation Processes for Degradation of Water Pollutants—Ambivalent Impact of Carbonate Species: A Review (2023) · cites this paper as [67]
UV/PS was revealed to be effective in natural water.
“Moreover, the UV/PS was also revealed to be effective in natural water [67].”
From Advanced Oxidation Processes for Degradation of Water Pollutants—Ambivalent Impact of Carbonate Species: A Review (2023) · cites this paper as [67]
The addition of NO3- had a negligible effect in both UV/oxidant systems.
“The addition of NO3 -had a negligible effect in both UV/oxidant systems.”
From Advanced Oxidation Processes for Degradation of Water Pollutants—Ambivalent Impact of Carbonate Species: A Review (2023) · cites this paper as [67]
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- Authors
- Liu, Y., He, X., Duan, X., Fu, Y., Fatta-Kassinos, D., & Dionysiou, D. D.
- Affiliations
- Southwest Jiaotong University (CN)
- University of Cincinnati (US)
- University of Cyprus (CY)
- Corresponding author
- Fu, Yongsheng
- Dionysiou, Dionysios D.
- Venue
- Water Research
- Publisher
- Elsevier BV
- Published
- 2016-05
- Volume
- 95
- Pages
- 195-204
- ISSN
- 0043-1354 (ISSN-L)
- OpenAlex
- W2299532793
- Cited by
- 317
- References
- 65
- Citations by year
- 2026: 25 · 2025: 27 · 2024: 25 · 2023: 41 · 2022: 50 · 2021: 32 · 2020: 39 · 2019: 28 · 2018: 33 · 2017: 11 · 2016: 6
- FWCI
- 15.42
- Type
- journal article
- Language
- en
- Open access
- bronze
- doi.org
- Locations
- Water Research (publishedVersion)
- PubMed (publishedVersion)
- Zenodo (CERN European Organization for Nuclear Research) (submittedVersion, cc-by)
- Funders
- Cyprus Research Promotion Foundation
- Republic of Cyprus
- European Regional Development Fund
- EU (NEA IPODOMI/STRATH/0308/09)
- China Scholarship Council (201307000035)
- University of Cincinnati
- UNESCO
- Topics
- Physical Sciences › Environmental Science › Water Science and Technology › Advanced oxidation water treatment
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Advanced Photocatalysis Techniques
- Physical Sciences › Environmental Science › Health, Toxicology and Mutagenesis › Water Treatment and Disinfection
- Keywords
- oxytetracycline, carbonate radical, UV/H2O2, UV/persulfate, antibiotic degradation, degradation kinetics, degradation pathways, nitrate, natural organic matter, bicarbonate, hydroxyl radicals, decarbonylation
- MeSH terms
- Carbonates, Hydrogen Peroxide, Kinetics, Oxytetracycline, Ultraviolet Rays, Water Pollutants, Chemical
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