DOI: 10.1016/j.watres.2018.11.009
Scopus记录号: 2-s2.0-85056608546
论文题名: The importance of reactive oxygen species on the aqueous phototransformation of sulfonamide antibiotics: kinetics, pathways, and comparisons with direct photolysis
作者: Ge L. ; Zhang P. ; Halsall C. ; Li Y. ; Chen C.-E. ; Li J. ; Sun H. ; Yao Z.
刊名: Water Research
ISSN: 431354
出版年: 2019
起始页码: 243
结束页码: 250
语种: 英语
英文关键词: Dissociated forms
; Oxidation kinetics
; Photodegradation
; Sulfonamides
; Transformation products
Scopus关键词: Amides
; Antibiotics
; Kinetics
; Mass spectrometry
; Oxygen
; Photodegradation
; Photolysis
; Photooxidation
; Reaction intermediates
; Reaction rates
; Risk assessment
; Sulfur compounds
; Surface waters
; Antimicrobial potency
; Oxidation kinetics
; Photochemical transformations
; Reactive oxygen species
; Sulfonamide antibiotics
; Sulfonamides
; Tandem mass spectrometry
; Transformation products
; Oxidation
; hydroxyl radical
; reactive oxygen metabolite
; singlet oxygen
; sulfachlorpyridazine
; sulfadiazine
; sulfadimethoxine
; sulfadimidine
; sulfafurazole
; sulfamerazine
; sulfamethizole
; sulfamethoxazole
; sulfathiazole
; sulfonamide
; antibiotics
; chemical pollutant
; chemical reaction
; comparative study
; hydroxyl radical
; oxidation
; photolysis
; photooxidation
; pollutant removal
; reaction kinetics
; surface water
; transformation
; Article
; controlled study
; hydroxylation
; oxidation kinetics
; pH
; photodegradation
; photolysis
; photooxidation
; priority journal
; tandem mass spectrometry
英文摘要: Sulfonamide antibiotics (SAs) are increasingly detected as aquatic contaminants and exist as different dissociated species depending on the pH of the water. Their removal in sunlit surface waters is governed by photochemical transformation. Here we report a detailed examination of the hydroxyl radical (•OH) and singlet oxygen ( 1 O 2 ) mediated photooxidation of nine SAs: sulfamethoxazole, sulfisoxazole, sulfamethizole, sulfathiazole, sulfamethazine, sulfamerazine, sulfadiazine, sulfachloropyridazine and sulfadimethoxine. Both •OH and 1 O 2 oxidation kinetics varied depending on the dominant protonated states of the SA in question (H 2 SAs + , HSAs 0 and SAs − ) as a function of pH. Based on competition kinetic experiments and matrix deconvolution calculations, HSAs 0 or SAs − (pH ∼5–8) were observed to be more highly reactive towards •OH, while SAs − (pH ∼8) react the fastest with 1 O 2 for most of the SAs tested. Using the empirically derived rates of reaction for the speciated forms at different pHs, the environmental half-lives were determined using typical 1 O 2 and •OH concentrations observed in the environment. This approach suggests that photochemical 1 O 2 oxidation contributes more than •OH oxidation and direct photolysis to the overall phototransformation of SAs in sunlit waters. Based on the identification of key photointermediates using tandem mass spectrometry, 1 O 2 oxidation generally occurred at the amino moiety on the molecule, whereas •OH reaction experienced multi-site hydroxylation. Both these reactions preserve the basic parent structure of the compounds and raise concerns that the routes of phototransformation give rise to intermediates with similar antimicrobial potency as the parent SAs. We therefore recommend that these phototransformation pathways are included in risk assessments concerning the presence and fate of SAs in waste and surface waters. © 2018 The Authors Citation statistics:
资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/122156
Appears in Collections: 气候变化事实与影响
There are no files associated with this item.
作者单位: Key Laboratory for Ecological Environment in Coastal Areas (SOA), National Marine Environmental Monitoring Center, Dalian, 116023, China; Lancaster Environment Centre, Lancaster University, Lancaster, LA1 4YQ, United Kingdom; Environmental Research Institute, MOE Key Laboratory of Environmental Theoretical Chemistry, South China Normal University, Guangzhou, 510006, China
Recommended Citation:
Ge L.,Zhang P.,Halsall C.,et al. The importance of reactive oxygen species on the aqueous phototransformation of sulfonamide antibiotics: kinetics, pathways, and comparisons with direct photolysis[J]. Water Research,2019-01-01