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Kinetic and mechanistic investigations of the degradation of sulfamethazine in heat-activated persulfate oxidation process.
J Hazard Mater. 2015 Dec 30; 300:39-47.JH

Abstract

Sulfamethazine (SMZ) is widely used in livestock feeding and aquaculture as an antibiotic agent and growth promoter. Widespread occurrence of SMZ in surface water, groundwater, soil and sediment has been reported. In this study, degradation of SMZ by heat-activated persulfate (PS) oxidation was investigated in aqueous solution. Experimental results demonstrated that SMZ degradation followed pseudo-first-order reaction kinetics. The pseudo-first-order rate constant (kobs) was increased markedly with increasing concentration of PS and temperature. Radical scavenging tests revealed that the predominant oxidizing species was SO4·(-) with HO playing a less important role. Aniline moiety in SMZ molecule was confirmed to be the reactive site for SO4·(-) attack by comparison with substructural analogs. Nontarget natural water constituents affected SMZ removal significantly, e.g., Cl(-) and HCO3(-) improved the degradation while fulvic acid reduced it. Reaction products were enriched by solid phase extraction (SPE) and analyzed by liquid chromatography-electrospray ionization-triple quadrupole mass spectrometry (LC-ESI-MS/MS). 6 products derived from sulfonamide S--N bond cleavage, aniline moiety oxidation and Smiles-type rearrangement were identified, and transformation pathways of SMZ oxidation were proposed. Results reveal that heat-activated PS oxidation could be an efficient approach for remediation of water contaminated by SMZ and related sulfonamides.

Authors+Show Affiliations

College of Resources and Environmental Science, Nanjing Agricultural University, Nanjing 210095, China.College of Resources and Environmental Science, Nanjing Agricultural University, Nanjing 210095, China. Electronic address: yuefeiji@njau.edu.cn.Nanjing Institute of Environmental Science, Ministry of Environmental Protection of PRC, Nanjing 210042, China.College of Resources and Environmental Science, Nanjing Agricultural University, Nanjing 210095, China. Electronic address: jhlu@njau.edu.cn.College of Resources and Environmental Science, Nanjing Agricultural University, Nanjing 210095, China.

Pub Type(s)

Journal Article
Research Support, Non-U.S. Gov't

Language

eng

PubMed ID

26151383

Citation

Fan, Yan, et al. "Kinetic and Mechanistic Investigations of the Degradation of Sulfamethazine in Heat-activated Persulfate Oxidation Process." Journal of Hazardous Materials, vol. 300, 2015, pp. 39-47.
Fan Y, Ji Y, Kong D, et al. Kinetic and mechanistic investigations of the degradation of sulfamethazine in heat-activated persulfate oxidation process. J Hazard Mater. 2015;300:39-47.
Fan, Y., Ji, Y., Kong, D., Lu, J., & Zhou, Q. (2015). Kinetic and mechanistic investigations of the degradation of sulfamethazine in heat-activated persulfate oxidation process. Journal of Hazardous Materials, 300, 39-47. https://doi.org/10.1016/j.jhazmat.2015.06.058
Fan Y, et al. Kinetic and Mechanistic Investigations of the Degradation of Sulfamethazine in Heat-activated Persulfate Oxidation Process. J Hazard Mater. 2015 Dec 30;300:39-47. PubMed PMID: 26151383.
* Article titles in AMA citation format should be in sentence-case
TY - JOUR T1 - Kinetic and mechanistic investigations of the degradation of sulfamethazine in heat-activated persulfate oxidation process. AU - Fan,Yan, AU - Ji,Yuefei, AU - Kong,Deyang, AU - Lu,Junhe, AU - Zhou,Quansuo, Y1 - 2015/06/27/ PY - 2015/05/05/received PY - 2015/06/23/revised PY - 2015/06/24/accepted PY - 2015/7/8/entrez PY - 2015/7/8/pubmed PY - 2016/8/31/medline KW - Heat-activated persulfate oxidation KW - Reaction products KW - Sulfamethazine KW - Sulfate radical KW - Transformation mechanisms SP - 39 EP - 47 JF - Journal of hazardous materials JO - J. Hazard. Mater. VL - 300 N2 - Sulfamethazine (SMZ) is widely used in livestock feeding and aquaculture as an antibiotic agent and growth promoter. Widespread occurrence of SMZ in surface water, groundwater, soil and sediment has been reported. In this study, degradation of SMZ by heat-activated persulfate (PS) oxidation was investigated in aqueous solution. Experimental results demonstrated that SMZ degradation followed pseudo-first-order reaction kinetics. The pseudo-first-order rate constant (kobs) was increased markedly with increasing concentration of PS and temperature. Radical scavenging tests revealed that the predominant oxidizing species was SO4·(-) with HO playing a less important role. Aniline moiety in SMZ molecule was confirmed to be the reactive site for SO4·(-) attack by comparison with substructural analogs. Nontarget natural water constituents affected SMZ removal significantly, e.g., Cl(-) and HCO3(-) improved the degradation while fulvic acid reduced it. Reaction products were enriched by solid phase extraction (SPE) and analyzed by liquid chromatography-electrospray ionization-triple quadrupole mass spectrometry (LC-ESI-MS/MS). 6 products derived from sulfonamide S--N bond cleavage, aniline moiety oxidation and Smiles-type rearrangement were identified, and transformation pathways of SMZ oxidation were proposed. Results reveal that heat-activated PS oxidation could be an efficient approach for remediation of water contaminated by SMZ and related sulfonamides. SN - 1873-3336 UR - https://www.unboundmedicine.com/medline/citation/26151383/Kinetic_and_mechanistic_investigations_of_the_degradation_of_sulfamethazine_in_heat_activated_persulfate_oxidation_process_ L2 - https://linkinghub.elsevier.com/retrieve/pii/S0304-3894(15)00515-4 DB - PRIME DP - Unbound Medicine ER -