Reactivity and reaction mechanisms of sulfate radicals with lindane: An experimental and theoretical study

被引:14
作者
He, Lei [1 ,2 ,3 ]
Bu, Lingjun [4 ]
Spinney, Richard [5 ]
Dionysiou, Dionysios D. [6 ]
Xiao, Ruiyang [1 ,2 ,3 ]
机构
[1] Cent South Univ, Sch Met & Environm, Inst Environm Engn, Changsha 410083, Peoples R China
[2] Chinese Natl Engn Res Ctr Control & Treatment Hea, Changsha, Peoples R China
[3] Water Pollut Control Technol Key Lab Hunan Prov, Changsha 410004, Peoples R China
[4] Hunan Univ, Coll Civil Engn, Key Lab Bldg Safety & Energy Efficiency, Minist Educ,Dept Water Engn & Sci, Changsha 410082, Peoples R China
[5] Ohio State Univ, Dept Chem & Biochem, Columbus, OH 43210 USA
[6] Univ Cincinnati, Dept Chem & Environm Engn ChEE, Environm Engn & Sci Program, Cincinnati, OH 45221 USA
基金
中国国家自然科学基金;
关键词
Lindane; Sulfate radicals; Advanced oxidation technologies; Reactivity; Mechanisms; ADVANCED OXIDATION TECHNOLOGIES; HYDROXYL RADICALS; RATE CONSTANTS; DEGRADATION; IBUPROFEN; KINETICS; PHARMACEUTICALS; PERFORMANCE; PHOTOLYSIS;
D O I
10.1016/j.envres.2021.111523
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Advanced oxidation technologies (AOTs) have been intensely used to eliminate various organic pollutants in engineering waters. In this context, we investigated the kinetics and mechanisms of the sulfate radical (SO4 center dot-)mediated degradation of lindane in UV/peroxydisulfate system, and compared results with previous studies on SO4 center dot--based AOTs for destruction of lindane. The second order rate constant (k) value between SO4 center dot- and lindane was determined to be (8.95 +/- 0.29) x 106 M-1 s-1 via competition kinetics using p-cyanobenzoic acid as reference compound, which is close to the theoretically calculated value of 4.41 x 107 M-1 s-1, that was performed at SMD/M05- 2X/6-311++G**//M05- 2X/6-31+G** level of theory using density functional theory (DFT) approach. H-atom abstraction pathway was calculated to be thermodynamically favorable and kinetically dominant. In the combined experimental and theoretical study, we aim for a better understanding on the degradation kinetics and mechanisms of lindane, serving as a starting point for more attention to SO4 center dot-- mediated degradation kinetics of cycloaliphatic compounds in future.
引用
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页数:5
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