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Br-对UV/PDS去除对乙酰氨基酚过程的影响及其转化规律 被引量:2

Effect and conversion of Br-during acetaminophen removal in UV/PDS process
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摘要 以对乙酰氨基酚(Acetaminophen,AAP)为目标污染物,结合降解动力学、密度泛函理论(Density Functional Theory,DFT)计算及毒性模拟,从有机和无机两个方面研究了UV/PDS氧化AAP过程中Br-的转化规律.结果表明,低浓度的Br-(≤0.1 mmol·L^(-1))使AAP的降解速率从0.0895min^(-1)降至0.0645 min^(-1),而高浓度的Br-(0.5~2 mmol·L^(-1))使其增至0.1052~0.1583 min^(-1);与溴相关的物种对AAP降解的贡献率达到46.80%.低PDS浓度、低pH值、低AAP浓度和高Br-浓度会促进Br-向HOBr转化.AAP浓度对HOBr转化为溴酸盐(BrO3-)和总有机溴(Total Organic Bromine,TOBr)的影响显著.TOBr的形成是HOBr、活性溴物种(RBS,如Br_(2)^(·-))和自由基(如SO_(4)^(·-)和OH·)联合作用于AAP及其中间产物的结果.此外,通过DFT计算和HPLC/MS分析,提出了Br-转化机制和AAP降解途径.毒性模拟表明,形成的大部分溴代有机物的毒性高于AAP的毒性. The Br-conversion and effects during the oxidation of acetaminophen(AAP)by UV/PDS were investigated from both organic and inorganic aspects based on the kinetics analysis,density functional theory(DFT)calculation and ecotoxicity simulation.The results showed that low concentrations of Br-(≤0.1 mmol·L^(-1))decreased the AAP degradation rate from 0.0895 min^(-1) to 0.0645 min-1,whereas relatively high concentrations(0.5~2 mmol·L^(-1))increased it to 0.1052~0.1583 min^(-1),and Br-related species accounted for 46.80%of AAP degradation.The conversion from Br-to HOBr was promoted with lower PDS concentration,lower pH,lower AAP concentration,and higher Br-concentration.HOBr was then converted into bromate(BrO_(3)^(-))and total organic bromine(TOBr),these processes were significantly affected by AAP concentration.The formation of TOBr resulted from the combined effect of HOBr,reactive brominated species(RBS)such as Br_(2)^(•-),and radicals such as SO_(4)^(•-)and OH•on AAP and its intermediates.Additionally,the Br-conversion mechanism and AAP degradation pathways were proposed based on DFT calculations and HPLC/MS analysis.Toxicity simulation indicated that the majority of the formed brominated organic products exhibited higher toxicity than that of AAP.
作者 颉亚玮 汪伟 陈吕军 刘锐 刘宏远 XIE Yawei;WANG Wei;CHEN Lujun;LIU Rui;LIU Hongyuan(College of Civil Engineering,Zhejiang University of Technology,Hangzhou 310023;Hangzhou Urban&Rural Construction Design Institute Co.,Ltd,Hangzhou 310023;School of Environment,Tsinghua University,Beijing 100084;Yangtze Delta Region Institute of Tsinghua University,Zhejiang,Zhejiang Provincial Key Laboratory of Water Science and Technology,Jiaxing 314006)
出处 《环境科学学报》 CAS CSCD 北大核心 2023年第9期57-67,共11页 Acta Scientiae Circumstantiae
基金 国家自然科学基金(No.52070111,52170093) 浙江省自然科学基金(No.LY22E080010)。
关键词 对乙酰氨基酚(AAP) UV/PDS Br-转化 转化驱动因素 降解途径 理论计算 acetaminophen(AAP) UV/PDS Br-conversion conversion drivers degradation pathways theoretical calculation
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