氯苯低压热解的原位同步辐射光电离质谱研究

大气与环境光学学报 ›› 2022, Vol. 17 ›› Issue (4): 442-452.

氯苯低压热解的原位同步辐射光电离质谱研究

许鸣皋1, 文武2, 赵龙2, 杨玖重2, 朱宝忠1;3, 孙运兰1;3∗, 潘洋2∗

1 安徽工业大学冶金工程学院, 安徽马鞍山 243032; 2 中国科学技术大学国家同步辐射实验室, 安徽合肥 230026; 3 常州大学石油工程学院, 江苏常州 213164

收稿日期:2021-04-13 修回日期:2022-04-26 出版日期:2022-07-28 发布日期:2022-07-28
通讯作者: E-mail: ylsun@cczu.edu.cn;E-mail: panyang@ustc.edu.cn E-mail:panyang@ustc.edu.cn
作者简介:许鸣皋 (1988 - ), 安徽安庆人, 博士研究生, 主要从事冶金工程节能减排方面的研究。 E-mail: mgxu@ustc.edu.cn
基金资助:
Supported by National Natural Science Foundation of China (国家自然科学基金, 52076016, 91845203, 91945302), Key Technical Talent Programme of Chinese Academy of Sciences (中国科学院关键技术人才项目)

Chlorobenzene pyrolysis at low pressure by in-situ synchrotron radiation photoionization mass spectrometry

XU Minggao1, WEN Wu2, ZHAO Long2, YANG Jiuzhong2, ZHU Baozhong1;3, SUN Yunnan1;3∗, PAN Yang2∗

1 School of Metallurgical Engineering, Anhui University of Technology, Maanshan 243032, China; 2 National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230026, China; 3 School of Petroleum Engineering, Changzhou University, Changzhou 213164, China

Received:2021-04-13 Revised:2022-04-26 Published:2022-07-28 Online:2022-07-28

摘要/Abstract

摘要： 氯苯类化合物及其高温热解产物是大气中重要的一类污染物, 对氯苯热解路径的研究可为防止或减少相关污染物的排放提供基础理论指导。利用原位同步辐射光电离质谱技术 (SR-PIMS) 在 4 kPa 和 873∼1373 K 条件下开展了氯苯流动管反应器低压热解研究, 实时鉴定了包括烯烃、芳烃和氯化芳烃等 16 种热解产物, 获得了这些产物的摩尔分数随热解温度的变化规律。研究表明: 苯炔 (o-C6H4) 是氯苯热解形成小分子路径的关键中间体。对比本组之前氯苯常压流动管热解的实验结果, 发现低压减弱了氯化芳烃等含氯有机物的形成途径, 表明压力条件会影响氯苯重要次级热解产物氯化芳烃的形成。

关键词: 氯苯, 流动管热解, 原位同步辐射光电离质谱, 中间体

Abstract: Chlorobenzene compounds and their high-temperature pyrolysis products are one kind of the important pollutants in the atmosphere. The research on the pyrolysis path of chlorobenzene can provide basic theoretical guidance for preventing or reducing the emission of related pollutants. The pyrolysis of chlorobenzene in a flow tube reactor was studied at 4 kPa and 873∼1373 K by in-situ synchrotron radiation photoionization mass spectrometry (SR-PIMS). 16 products including olefin, aromatic hydrocarbons, and chlorinated aromatic hydrocarbons were detected in real time. Mole fractions of these products were obtained as function of pyrolysis temperature. The results show that o-benzyne is a key intermediate for the formation of small molecules in the pyrolysis of chlorobenzene. Besides, compared with the pyrolysis results of chlorobenzene at atmospheric-pressure observed before in this group, it was found that low pressure can reduce the formation pathways of chlorine-containing organics such as chlorinated aromatic hydrocarbons, an important secondary pyrolysis product of chlorobenzene, which indicates that pressure conditions can affect the formation and the following atmospheric emission of chlorinated aromatic hydrocarbons.

Key words: chlorobenzene, flow reactor pyrolysis, synchrotron radiation photoionization mass spectrometry; intermediate

中图分类号:

O657.63

许鸣皋, 文武, 赵龙, 杨玖重, 朱宝忠, 孙运兰, ∗, 潘洋∗. 氯苯低压热解的原位同步辐射光电离质谱研究[J]. 大气与环境光学学报, 2022, 17(4): 442-452.

XU Minggao, WEN Wu, ZHAO Long, YANG Jiuzhong, ZHU Baozhong, SUN Yunnan, ∗, PAN Yang∗. Chlorobenzene pyrolysis at low pressure by in-situ synchrotron radiation photoionization mass spectrometry[J]. Journal of Atmospheric and Environmental Optics, 2022, 17(4): 442-452.

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