基于真空紫外光电离质谱的氯原子引发诺蒎酮氧化反应研究

引用本文: 胡荣荣, 马子吉, 岳浩, 林晓晓, 温作赢, 张为俊, 顾学军, 唐小锋. 基于真空紫外光电离质谱的氯原子引发诺蒎酮氧化反应研究[J]. 分析化学, 2022, 50(6): 948-956. doi: 10.19756/j.issn.0253-3820.221081 shu

Citation: HU Rong-Rong, MA Zi-Ji, YUE Hao, LIN Xiao-Xiao, WEN Zuo-Ying, ZHANG Wei-Jun, GU Xue-Jun, TANG Xiao-Feng. Investigation of Chlorine-initiated Oxidation Reactions of Nopinone by Vacuum Ultraviolet Photoionization Mass Spectrometry[J]. Chinese Journal of Analytical Chemistry, 2022, 50(6): 948-956. doi: 10.19756/j.issn.0253-3820.221081 shu

基于真空紫外光电离质谱的氯原子引发诺蒎酮氧化反应研究

胡荣荣 ^1,2, ,
马子吉 ^1,2, ,
岳浩 ^1,2, ,
林晓晓 ^{1,
,} ,
温作赢 ^1, ,
张为俊 ^1, ,
顾学军 ^1, ,
唐小锋 ^1,

1.
中国科学院合肥物质科学研究院安徽光学精密机械研究所, 合肥 230031;
2.
中国科学技术大学研究生院科学岛分院, 合肥 230026

通讯作者: 林晓晓,E-mail:lxx1989@aiofm.ac.cn

基金项目:
国家自然科学基金项目（Nos.42075113，42120104007，91961123）资助。

摘要: 采用微波放电流动管反应器模拟大气中氯原子（Cl）引发的诺蒎酮（C₉H₁₄O）氧化反应，结合自行研制的真空紫外光电离飞行时间质谱仪，在线检测获得反应中的关键物种，包含反应物、自由基和产物，并开展其反应动力学研究，通过比较关键物种的动力学实验与模拟计算结果，探讨了反应中关键物种的反应路径。结果表明，Cl原子和诺蒎酮分子之间的反应经夺氢通道生成自由基C₉H₁₃O，产生的自由基C₉H₁₃O与O₂分子反应主要生成过氧自由基C₉H₁₃OO₂，并且新生成的C₉H₁₃OO₂在无NO或NO₂条件下进一步与HO₂自由基反应生成氢过氧化物C₉H₁₃OO₂H，以及与自身发生双分子反应生成自由基C₉H₁₃OO、羰基化合物C₉H₁₂O₂和C₉H₁₃OOH。本研究通过实验研究和模拟计算揭示了Cl原子引发的诺蒎酮大气氧化反应机理。

关键词:

English

Investigation of Chlorine-initiated Oxidation Reactions of Nopinone by Vacuum Ultraviolet Photoionization Mass Spectrometry

1.
Anhui Institute of Optics&Fine Mechanics, Hefei Institutes of Physical Science, Chinese Academy of Sciences, Hefei 230031, China;
2.
Science Island Branch, Graduate School, University of Science and Technology of China, Hefei 230026, China

Corresponding author: LIN Xiao-Xiao, lxx1989@aiofm.ac.cn

Received Date: 18 February 2022
Revised Date: 04 April 2022
Fund Project:
Supported by the National Natural Science Foundation of China(Nos. 42075113, 42120104007, 91961123).

Abstract: A microwave discharge fast flow tube reactor was used to simulate chlorine-initiated oxidation of nopinone(C₉H₁₄O). The chemical compositions of radicals and stable products from the oxidation reactions were measured via a home-made vacuum ultraviolet photoionization time of flight mass spectrometer(VUVPI-TOFMS). The kinetic experiments of main radicals and products were also performed. By comparing the results of kinetic experiments and simulation calculations of key species,the reaction pathways of key species in the reaction were further explored. This study showed that the reaction of nopinone with Cl produced radical C₉H₁₃O via the hydrogen abstraction pathway. The radical C₉H₁₃O reacted with O₂ to mainly generate peroxy radical C₉H₁₃OO₂. Under NOx(NO and NO₂) free condition, peroxy radical C₉H₁₃OO₂ reacted with itself to produce radical C₉H₁₃OO, carbonyl compounds C₉H₁₂O₂ and C₉H₁₃OOH. In addition, the peroxy radical C₉H₁₃OO₂ could also react with HO₂ to produce hydroperoxide C₉H₁₃OO₂H. The mechanism of chlorine-initiated oxidation reactions of nopinone was also revealed through experimental studies and simulation calculations.

Key words:

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

基于真空紫外光电离质谱的氯原子引发诺蒎酮氧化反应研究

通讯作者: 林晓晓,E-mail:lxx1989@aiofm.ac.cn

English

Investigation of Chlorine-initiated Oxidation Reactions of Nopinone by Vacuum Ultraviolet Photoionization Mass Spectrometry

Corresponding author: LIN Xiao-Xiao, lxx1989@aiofm.ac.cn

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

基于真空紫外光电离质谱的氯原子引发诺蒎酮氧化反应研究

通讯作者: 林晓晓,E-mail:lxx1989@aiofm.ac.cn

English

Investigation of Chlorine-initiated Oxidation Reactions of Nopinone by Vacuum Ultraviolet Photoionization Mass Spectrometry

Corresponding author: LIN Xiao-Xiao, lxx1989@aiofm.ac.cn

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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