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O3和ClO2氧化NDMA前体的动力学和产物生成规律

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王小凤, 周北海, 杨宏伟, 王小??. O3和ClO2氧化NDMA前体的动力学和产物生成规律[J]. 环境工程学报, 2018, 12(5): 1452-1461. doi: 10.12030/j.cjee.201710019
引用本文: 王小凤, 周北海, 杨宏伟, 王小??. O3和ClO2氧化NDMA前体的动力学和产物生成规律[J]. 环境工程学报, 2018, 12(5): 1452-1461. doi: 10.12030/j.cjee.201710019
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WANG Xiaofeng, ZHOU Beihai, YANG Hongwei, WANG Xiaomao. Reaction kinetic and product formation of NDMA precursor oxidized by O3 and ClO2[J]. Chinese Journal of Environmental Engineering, 2018, 12(5): 1452-1461. doi: 10.12030/j.cjee.201710019
Citation: WANG Xiaofeng, ZHOU Beihai, YANG Hongwei, WANG Xiaomao. Reaction kinetic and product formation of NDMA precursor oxidized by O3 and ClO2[J]. Chinese Journal of Environmental Engineering, 2018, 12(5): 1452-1461. doi: 10.12030/j.cjee.201710019
shu

O3和ClO2氧化NDMA前体的动力学和产物生成规律

  • 1.

    北京科技大学能源与环境工程学院，北京 100083

  • 2.

    清华大学环境学院，北京 100084

  • 基金项目:

    国家自然科学基金资助项目（51278268）

Reaction kinetic and product formation of NDMA precursor oxidized by O3 and ClO2

  • 1.

    School of Energy and Environmental Engineering, University of Science Technology Beijing, Beijing 100083, China

  • 2.

    School of Environment, Tsinghua University, Beijing 100084, China

  • Fund Project:

  • 摘要: 以4种含有二甲胺（DMA）官能团的药物和个人护理品（PPCPs）为研究对象，通过研究其降解反应动力学和氧化产物生成规律，确定臭氧（O3）和二氧化氯（ClO2）对N-亚硝基二甲胺（NDMA）生成势的控制效果。O3氧化PPCPs的二级反应速率常数（k）为105~106（mol·s）-1，ClO2氧化PPCPs的k为101~102（mol·s）-1，ClO2与O3均可去除PPCP类NDMA前体。O3与PPCP反应生成氮加氧产物，加氧在DMA官能团的氮上，该氮加氧产物不再具有NDMA生成势，且O3与PPCP摩尔比为1:1时，加一氧产物的生成量最大。ClO2与PPCPs反应时生成去DMA基产物，脱落的DMA也具有NDMA生成势，ClO2氧化产物仍具有NDMA生成势，且ClO2与PPCPs的摩尔比为3:1时，去DMA基产物生成量最大。O3氧化可满足对NDMA生成势的控制，但ClO2氧化不能满足对NDMA生成势的控制。
    Abstract: The effect of N-nitrosodimethlymine (NDMA) formation potential by ozone (O3) or chlorine dioxide (ClO2) oxidation was assessed through investigating reaction kinetics and product formation patterns of model precursors. Four pharmaceutical and personal care products (PPCPs) containing dimethylamine (DMA) functional groups were selected as model precursors. The kinetic results showed that the second-order reaction kinetic constants (k) were from 105 to 106(mol·s)-1 for the model PPCPs oxidized by O3, while the k were from 101 to 102(mol·s)-1 oxidized by ClO2. Model PPCPs could be removed by both O3 and ClO2. The formation patterns of oxidation products showed that products adding oxygen at nitrogen in DMA group formed after ozonation. The adding oxygen products have no NDMA formation potential. And the highest yields of products adding oxygen at nitrogen in DMA group were observed when the molecular ratio of O3 to PPCP was from 1 to 1. However, products dropping DMA group off formed after oxidized by ClO2. The dropped DMA group still has NDMA formation potential. The highest yields of products dropping DMA group off were observed when the molecular ratio of ClO2 to PPCP was from 3 to 1. It was concluded that NDMA formation could be controlled by O3 but not by ClO2.
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  • 刊出日期:  2018-05-19

O3和ClO2氧化NDMA前体的动力学和产物生成规律

  • 1. 北京科技大学能源与环境工程学院，北京 100083
  • 2. 清华大学环境学院，北京 100084
基金项目:

国家自然科学基金资助项目（51278268）

摘要: 以4种含有二甲胺（DMA）官能团的药物和个人护理品（PPCPs）为研究对象，通过研究其降解反应动力学和氧化产物生成规律，确定臭氧（O3）和二氧化氯（ClO2）对N-亚硝基二甲胺（NDMA）生成势的控制效果。O3氧化PPCPs的二级反应速率常数（k）为105~106（mol·s）-1，ClO2氧化PPCPs的k为101~102（mol·s）-1，ClO2与O3均可去除PPCP类NDMA前体。O3与PPCP反应生成氮加氧产物，加氧在DMA官能团的氮上，该氮加氧产物不再具有NDMA生成势，且O3与PPCP摩尔比为1:1时，加一氧产物的生成量最大。ClO2与PPCPs反应时生成去DMA基产物，脱落的DMA也具有NDMA生成势，ClO2氧化产物仍具有NDMA生成势，且ClO2与PPCPs的摩尔比为3:1时，去DMA基产物生成量最大。O3氧化可满足对NDMA生成势的控制，但ClO2氧化不能满足对NDMA生成势的控制。

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