Kinetics and mechanism of triclocarban degradation by the chlorination process: Theoretical calculation and experimental verification
文献类型：期刊论文
| 作者 | Peng, Tao1,3,4; Xu, Chao2,3; Yang, Bin2,3; Gu, Feng-Long2,3; Ying, Guang-Guo2,3 |
| 刊名 | Chemosphere
 |
| 出版日期 | 2023 |
| 卷号 | 338页码:139551 |
| ISSN号 | 0045-6535 |
| DOI | 10.1016/j.chemosphere.2023.139551 |
| 英文摘要 | Triclocarban (TCC) is an antimicrobial agent commonly used in many household and personal care products, and has been found persistent in the aquatic environment. Here we elucidate the kinetics and mechanism of TCC degradation during chlorination process by density functional theory (DFT) calculation and experimental verification. Results showed that hypochlorous acid (HOCl)/hypochlorite (OCl?) reacted with TCC via Cl-substitution, OH-substitution and C–N bond cleavage pathways. The reactivity of OCl? (2.80 × 10?7 M?1 s?1) with TCC was extremely low and HOCl (1.96 M?1 s?1) played the dominant role in TCC chlorination process. The N site of TCC was the most reactive site for chlorination. The second-order rate constants, which are determined using density functional theory (DFT) (kTCC?chlorineC, 1.96 M?1 s?1), can be separated into reaction rate constants related to the reactions of HOCl and OCl? with different isomers of TCC (TCC2 and TCC6). The obtained kTCC?chlorineC was consistent with the experimental determined second-order rate constant (kTCC?chlorineE, 3.70 M?1 s?1) in chlorination process. Eight transformation products (TP348, TP382, TP127, TP161, TP195, TP330, TP204, and TP296) were experimentally detected for chlorination of TCC, which could also be predicted by DFT calculation. Explicit water molecules participated in the chlorination reaction by transmitting the proton and connecting with TCC, HOCl/OCl? and other H2O molecules, and obviously reduced the energy barrier of chlorination. ? 2023 Elsevier Ltd |
| 语种 | 英语 |
| 源URL | [http://ir.gig.ac.cn/handle/344008/80336]  |
| 专题 | 有机地球化学国家重点实验室 |
| 作者单位 | 1.University of Chinese Academy of Sciences, Beijing; 100049, China 2.School of Environment, South China Normal University, Guangzhou; 510006, China 3.SCNU Environmental Research Institute, Guangdong Provincial Key Laboratory of Chemical Pollution and Environmental Safety & MOE Key Laboratory of Theoretical Chemistry of Environment, South China Normal University, Guangzhou; 510006, China 4.State Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou; 510640, China |
| 推荐引用方式 GB/T 7714 | Peng, Tao,Xu, Chao,Yang, Bin,et al. Kinetics and mechanism of triclocarban degradation by the chlorination process: Theoretical calculation and experimental verification[J]. Chemosphere,2023,338:139551. |
| APA | Peng, Tao,Xu, Chao,Yang, Bin,Gu, Feng-Long,&Ying, Guang-Guo.(2023).Kinetics and mechanism of triclocarban degradation by the chlorination process: Theoretical calculation and experimental verification.Chemosphere,338,139551. |
| MLA | Peng, Tao,et al."Kinetics and mechanism of triclocarban degradation by the chlorination process: Theoretical calculation and experimental verification".Chemosphere 338(2023):139551. |
入库方式： OAI收割
来源：广州地球化学研究所
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