DOI: 10.1016/j.watres.2019.01.023
Scopus记录号: 2-s2.0-85060766821
论文题名: Photochemical behavior of benzophenone sunscreens induced by nitrate in aquatic environments
作者: Ge J. ; Huang D. ; Han Z. ; Wang X. ; Wang X. ; Wang Z.
刊名: Water Research
ISSN: 431354
出版年: 2019
起始页码: 178
结束页码: 186
语种: 英语
英文关键词: Benzophenones
; Kinetics
; Nitrate
; Phototransformation
; Product identification
Scopus关键词: Alkalinity
; Density functional theory
; Design for testability
; Dissolved oxygen
; Endocrine disrupters
; Enzyme kinetics
; Fighter aircraft
; Irradiation
; Liquid chromatography
; Mass spectrometry
; Photolysis
; Polypropylenes
; Reaction kinetics
; Toxicity
; Benzophenones
; Endocrine disrupting activity
; Liquid chromatography-quadrupole time-of-flight mass spectrometries
; Photobacterium phosphoreum
; Phototransformations
; Potential ecological risk
; Product identification
; Transformation pathways
; Nitrates
; 2,4 dihydroxybenzophenone
; benzophenone derivative
; dissolved oxygen
; nitrate
; reactive oxygen metabolite
; sunscreen
; unclassified drug
; benzene
; concentration (composition)
; dissolved oxygen
; endocrine disruptor
; irradiation
; photochemistry
; PPCP
; reaction kinetics
; reactive oxygen species
; toxicity test
; aquatic environment
; Article
; biotransformation
; chemical reaction kinetics
; concentration (parameter)
; controlled study
; degradation
; density functional theory
; dimerization
; ecotoxicity
; electron spin resonance
; hydroxylation
; liquid chromatography
; mineralization
; nitration
; nitrosylation
; nonhuman
; pH
; Photobacterium phosphoreum
; photochemistry
; photolysis
; priority journal
; reaction analysis
; sunlight
; time of flight mass spectrometry
; toxicity testing
; ultraviolet radiation
; Kobus
; Photobacterium phosphoreum
英文摘要: Benzophenones (BPs), which are widely used UV filters, have aroused considerable public concern owing to their potential endocrine-disrupting activities. Herein, we systematically investigated their photochemical behavior and fate, which is mediated by nitrate in aquatic environments. The results showed that 10 μM of 3 BPs can be completely degraded within 4 h of simulated sunlight irradiation in a 10 mM nitrate solution at pH 8.0, and 2,4-dihydroxybenzophenone (BP-1) has a 31.6% mineralization rate after 12 h irradiation. Their photolytic rates (k obs ) presented a significant linear correlation with the logarithmic values of the nitrate concentration for 0.1–10 mM (R 2 > 0.98), and in three actual waters, the rates of BP-1 were also positively related to the intrinsic nitrate concentration. Furthermore, higher transformation rates under alkaline condition were observed, especially for BP-1, with its k obs at pH 10 being 8.3-fold higher than that at pH 6.0. Moreover, dissolved oxygen (DO) also has an impact on the reaction kinetics to some degree. According to the quenching experiments, we found that three reactive oxygen species (ROS), namely, •OH, •NO, and •NO 2 , participated in this photolysis of BPs, and the contribution of •OH accounted for 32.1%. Furthermore, we selected BP-1 as the model molecule to study the transformation pathways and toxicity changes in this system. Four main transformation pathways including hydroxylation, nitrosylation, nitration, and dimerization were proposed, based on liquid chromatography quadrupole time-of-flight mass spectrometry (LC-Q-TOF-MS) analysis and density functional theory (DFT). According to the toxicity test, the formed intermediates were more toxic to Photobacterium phosphoreum than the parent BP-1. Therefore, these results can help reveal primary phototransformation mechanisms and evaluate the potential ecological risks of BPs in aquatic environments. © 2019 Elsevier Ltd Citation statistics:
资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/121984
Appears in Collections: 气候变化事实与影响
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作者单位: State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing, Jiangsu 210023, China
Recommended Citation:
Ge J.,Huang D.,Han Z.,et al. Photochemical behavior of benzophenone sunscreens induced by nitrate in aquatic environments[J]. Water Research,2019-01-01