Degradation of three typical hydroxamic acids collectors via UVA-B activated H2O2 and persulfate: Kinetics, transformation pathway, DFT calculation and toxicity evaluation
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2023
Authors
Pang, WanchengYao, Jun
Šolević Knudsen, Tatjana

Cao, Ying
Liu, Bang
Li, Hao
Li, Miaomiao
Zhu, Junjie
Article (Published version)

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This work systematically studied the kinetics and mechanism of degradation of salicylhydroxamic acid (SHA), benzhydroxamic acid (BHA) and N-hydroxyphthalimide (NOP) by UVA-B/H2O2 and UVA-B/peroxodisulfate (PDS). UVA-B irradiation could induce a direct photolysis of SHA and dominated SHA destruction in both systems. BHA and NOP were effectively degraded via HO•- and SO4•−-mediated oxidation. UVA-B/PDS displayed a better degradation performance for HAAs investigated than UVA-B/H2O2. An acidic pH was more suitable for three HAAs removal in the UVA-B/H2O2 system. However, basic pH was more efficient for HAAs degradation in the UVA-B/PDS system. The degradation of BHA and NOP was predominantly driven by SO4•− at all pH levels used (5.0–9.0). The second-order rate constants for SHA, BHA and NOP reactions with HO• and SO4•− were calculated to be (4.16–5.22) × 109 M−1•s−1 and (1.19–7.22) × 109 M−1•s−1, respectively. Presence of various water constituents had different influence on HAA removal,... with a enhancement in the presence of HCO3–, Fe2+ and Cu2+. When real waters were used as a background, dissolved organic carbon and Cl− were the main factors that consumed radicals and affected the degradation performance of HAAs. Analysis of the transformation products and density functional theory revealed that all of the investigated HAAs first generated amidated products but the formation mechanisms might have been different. HAAs degradation pathways mainly included hydrolysis, hydroxylation, decarboxylation and ring opening processes. Toxicity evaluation showed that the UV/AOP degradation of HAAs generated some transformation products with higher acute toxicity than the parent compounds.
Keywords:
Degradation kinetics / Hydroxamic acid / Hydroxyl and sulfate radical / Transformation pathway / UVA-B irradiationSource:
Chemical Engineering Journal, 2023, 451, 138639-Publisher:
- Elsevier
Funding / projects:
- The Major National R & D Projects for Chinese Ministry of Science and Technology, Grant (2019YFC1803500)
- The National Science Foundation of China (41720104007)
- 111 Project (B21017)
- The Graduate Innovation Fund Project of China University of Geosciences, Beijing (YB2021YC016).
- Ministry of Education, Science and Technological Development, Republic of Serbia, Grant no. 200026 (University of Belgrade, Institute of Chemistry, Technology and Metallurgy - IChTM) (RS-200026)
- The International Joint Scientific and Technical Collaboration between the People’s Republic of China and the Republic of Serbia as part of the Project Number 4-18
Note:
- The peer-reviewed version: https://cer.ihtm.bg.ac.rs/handle/123456789/5546
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IHTMTY - JOUR AU - Pang, Wancheng AU - Yao, Jun AU - Šolević Knudsen, Tatjana AU - Cao, Ying AU - Liu, Bang AU - Li, Hao AU - Li, Miaomiao AU - Zhu, Junjie PY - 2023 UR - https://cer.ihtm.bg.ac.rs/handle/123456789/5331 AB - This work systematically studied the kinetics and mechanism of degradation of salicylhydroxamic acid (SHA), benzhydroxamic acid (BHA) and N-hydroxyphthalimide (NOP) by UVA-B/H2O2 and UVA-B/peroxodisulfate (PDS). UVA-B irradiation could induce a direct photolysis of SHA and dominated SHA destruction in both systems. BHA and NOP were effectively degraded via HO•- and SO4•−-mediated oxidation. UVA-B/PDS displayed a better degradation performance for HAAs investigated than UVA-B/H2O2. An acidic pH was more suitable for three HAAs removal in the UVA-B/H2O2 system. However, basic pH was more efficient for HAAs degradation in the UVA-B/PDS system. The degradation of BHA and NOP was predominantly driven by SO4•− at all pH levels used (5.0–9.0). The second-order rate constants for SHA, BHA and NOP reactions with HO• and SO4•− were calculated to be (4.16–5.22) × 109 M−1•s−1 and (1.19–7.22) × 109 M−1•s−1, respectively. Presence of various water constituents had different influence on HAA removal, with a enhancement in the presence of HCO3–, Fe2+ and Cu2+. When real waters were used as a background, dissolved organic carbon and Cl− were the main factors that consumed radicals and affected the degradation performance of HAAs. Analysis of the transformation products and density functional theory revealed that all of the investigated HAAs first generated amidated products but the formation mechanisms might have been different. HAAs degradation pathways mainly included hydrolysis, hydroxylation, decarboxylation and ring opening processes. Toxicity evaluation showed that the UV/AOP degradation of HAAs generated some transformation products with higher acute toxicity than the parent compounds. PB - Elsevier T2 - Chemical Engineering Journal T1 - Degradation of three typical hydroxamic acids collectors via UVA-B activated H2O2 and persulfate: Kinetics, transformation pathway, DFT calculation and toxicity evaluation VL - 451 SP - 138639 DO - 10.1016/j.cej.2022.138639 ER -
@article{ author = "Pang, Wancheng and Yao, Jun and Šolević Knudsen, Tatjana and Cao, Ying and Liu, Bang and Li, Hao and Li, Miaomiao and Zhu, Junjie", year = "2023", abstract = "This work systematically studied the kinetics and mechanism of degradation of salicylhydroxamic acid (SHA), benzhydroxamic acid (BHA) and N-hydroxyphthalimide (NOP) by UVA-B/H2O2 and UVA-B/peroxodisulfate (PDS). UVA-B irradiation could induce a direct photolysis of SHA and dominated SHA destruction in both systems. BHA and NOP were effectively degraded via HO•- and SO4•−-mediated oxidation. UVA-B/PDS displayed a better degradation performance for HAAs investigated than UVA-B/H2O2. An acidic pH was more suitable for three HAAs removal in the UVA-B/H2O2 system. However, basic pH was more efficient for HAAs degradation in the UVA-B/PDS system. The degradation of BHA and NOP was predominantly driven by SO4•− at all pH levels used (5.0–9.0). The second-order rate constants for SHA, BHA and NOP reactions with HO• and SO4•− were calculated to be (4.16–5.22) × 109 M−1•s−1 and (1.19–7.22) × 109 M−1•s−1, respectively. Presence of various water constituents had different influence on HAA removal, with a enhancement in the presence of HCO3–, Fe2+ and Cu2+. When real waters were used as a background, dissolved organic carbon and Cl− were the main factors that consumed radicals and affected the degradation performance of HAAs. Analysis of the transformation products and density functional theory revealed that all of the investigated HAAs first generated amidated products but the formation mechanisms might have been different. HAAs degradation pathways mainly included hydrolysis, hydroxylation, decarboxylation and ring opening processes. Toxicity evaluation showed that the UV/AOP degradation of HAAs generated some transformation products with higher acute toxicity than the parent compounds.", publisher = "Elsevier", journal = "Chemical Engineering Journal", title = "Degradation of three typical hydroxamic acids collectors via UVA-B activated H2O2 and persulfate: Kinetics, transformation pathway, DFT calculation and toxicity evaluation", volume = "451", pages = "138639", doi = "10.1016/j.cej.2022.138639" }
Pang, W., Yao, J., Šolević Knudsen, T., Cao, Y., Liu, B., Li, H., Li, M.,& Zhu, J.. (2023). Degradation of three typical hydroxamic acids collectors via UVA-B activated H2O2 and persulfate: Kinetics, transformation pathway, DFT calculation and toxicity evaluation. in Chemical Engineering Journal Elsevier., 451, 138639. https://doi.org/10.1016/j.cej.2022.138639
Pang W, Yao J, Šolević Knudsen T, Cao Y, Liu B, Li H, Li M, Zhu J. Degradation of three typical hydroxamic acids collectors via UVA-B activated H2O2 and persulfate: Kinetics, transformation pathway, DFT calculation and toxicity evaluation. in Chemical Engineering Journal. 2023;451:138639. doi:10.1016/j.cej.2022.138639 .
Pang, Wancheng, Yao, Jun, Šolević Knudsen, Tatjana, Cao, Ying, Liu, Bang, Li, Hao, Li, Miaomiao, Zhu, Junjie, "Degradation of three typical hydroxamic acids collectors via UVA-B activated H2O2 and persulfate: Kinetics, transformation pathway, DFT calculation and toxicity evaluation" in Chemical Engineering Journal, 451 (2023):138639, https://doi.org/10.1016/j.cej.2022.138639 . .