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题名: VOCs 的质子化增强检测技术研究
作者: 许策1
学位类别: 硕士
答辩日期: 2017-05
授予单位: 中国科学院大学
授予地点: 北京
导师: 束继年
关键词: 挥发性有机物 ; 醛类 ; VOCs ; 光电离 ; aldehydes ; 掺杂 ; photoionization ; 低气压电离 ; dopping ; LPPI
其他题名: Protonation-enhanced detecton of VOCs by vacuumultraviolet mass spectrometre
学位专业: 环境工程
中文摘要: 随着工业化进程的推进和加快,汽车数目的增多和其他燃烧过程中使用化 石燃料的不断增长给环境带来的压力越来越大,如今环境问题已经影响到了人 们的生活和健康,并已发展成为制约经济发展的重要因素。在众多污染源中, 挥发性有机化合物(VOCs) 是其中的一个重要组分,它不仅是室内污染的主要成 分,而且也是室外污染与雾霾的重要成因之一。高效灵敏的分析检测方法对于 分析VOCs 成分并对其实施有效监控及采取针对性地防控措施具有重要意义。 本论文主要以乙醛、正丙醛、正丁醛以及其他VOCs 为研究对象,研究了通过 二氯甲烷和二溴甲烷掺杂,促进待测物质质子化来提高自主研发的高灵敏度低 气压光电离质谱(LPPI-MS)对醛类等VOCs 的检测灵敏度的可行性。主要研究 成果如下: (1)应用LPPI-MS 技术以二氯甲烷作为掺杂物(dopant),将二氯甲烷掺 杂于乙醛、正丙醛和正丁醛样品中,结果显示,自主研发的LPPI-MS 技术对于 乙醛和正丙醛的检测效率分别增长了390 倍和530 倍。乙醛和正丙醛的标定灵 敏度分别达到了2207 counts/ppbv 和1238 counts/ppbv,同时计算出的两种醛类 的2σ LODs 分别为43 pptv 和35 pptv。由于质子化正丁醛的质谱峰(m/z 73)与 水团簇(H2O)4H+重叠,在实验中尚不能很好的辨别二氯甲烷对正丁醛质子化的增 强效应以及在LPPI-MS 检测过程中对正丁醛检测信号的影响。 (2)基于在LPPI-MS 中二氯甲烷掺杂对检测灵敏度的提高研究,将二溴甲 烷作为掺杂剂,应用在LPPI-MS 技术电离过程中,探讨了二溴甲烷对乙醛、正 丙醛和正丁醛的质子化促进作用。实验结果显示自主研发的LPPI-MS 技术对于 乙醛和正丙醛的检测效率分别增长了33 倍和60 倍。在二溴甲烷掺杂条件下, 丁醛质谱峰受水团簇(H2O)4H+影响不明显,可清楚观察到LPPI-MS 对正丁醛检 测灵敏度的提高。所以可以看到,质子化丁醛的信号强度增长了21 倍,LPPI-MS 对正丁醛的检测灵敏度达到337 counts/ppbv。 (3)以醛类的质子化增强检测为基础,将二溴甲烷作为掺杂剂,探究通过 二溴甲烷掺杂,提高LPPI-MS 对非极性有机物苯,醇类有机物甲醇,有机羧酸 甲酸的检测效率,进一步拓展了质子化增强技术在VOCs 检测领域的应用。研 究结果表明,LPPI-MS 对苯、甲醇和甲酸的检测灵敏度分别提高4 倍、126 倍和 204 倍。
英文摘要: Nowadays, fast industrial development is advancing at a staggering rate, the increasing number of automobiles and the increasing consumption of fossil fuels during the productive processes has brought much more press to the environment than ever before. On the other hand, today’s environmental problems are also upsetting citizens’ normal life and undermining people’s health and are becoming a serious issue hindering economic development. Volatile organic compounds (VOCs) are important part among these numerous pollutants. It is not only a major pollutant in indoor environment, but also a pollutant causing outdoor air pollution and haze. High sensitive online detection methods play a pivotal role in the analysis of components of VOCs and provide valuable support to effective control and targeted prevention. In this paper, the optimization of a laboratory-built high-sensitive low pressure photoionization mass spectrometer (LPPI-MS) has been mainly illustrated, attempting to realize the high sensitive detection of acetaldehyde, propionaldehyde and butyaldehyde via doping dichlromethane and dibromomethane. Main results are illustrated as follows: (1) Via using dichloromethane as dopant for LPPI-MS and doping it into alcetaldehyde, propionaldehyde and butyaldehyde samples, the detection sensitivity of LPPI-MS towards acetaldehyde and propionaldehyde increased 390 times and 530 times, reaching reaching 2207 counts/ppbv and 1238 counts/ppbv, respectively. The corresponding 2σ LODs of acetaldehyde and propionaldehyde is 43 pptv and 35 pptv, respectively. Overlapped by the mass peak of water cluster ((H2O)4H+), the enhancement of protonation of butyaldehyde and the consequent influence on the detection sensitivity of LPPI-MS towards butyaldehyde by dichloromethane doping can not be clearly identified. (2) Based on the study of the improvement of LPPI-MS detection ability by dichloromethane doping, we applied dibromomethane as dopant to LPPI-MS detection to further explore the application doping technique in the enhancement of the protonation of acetaldehyde, propionaldehyde and butyaldehyde. As the results showed, the detection sensitivity of LPPI-MS towards acetaldehyde and propionaldehyde increased 33 times and 60 times, reaching 452 and 337 counts/ppbv, respectively. During dibromomethane doping process, the mass peak of protonated butyaldehyde was little affected by water cluster ((H2O)4H+), so the improvement of the detection sensitivity of LPPI-MS towards butyaldehyde can be easily identified.So we can see the signal intensity of protonated butyaldehyde increased 21 times, the detection sensitivity of LPPI-MS towards butyaldehyde reached 337 counts/ppbv. (3) Based on the study of photoionization enhancement of aldehydes, we used dibromomethane as dopant, trying to improve detection sensitivity of LPPI-MS towards benzene, carbinol and methanoic acid to further apply this method in the detection of VOCs. As the results showed, the detection sensitivity of LPPI-MS towards benzene, methanol and methanoic acid increased 4 times, 126 times and 204 times.
内容类型: 学位论文
URI标识: http://ir.rcees.ac.cn/handle/311016/38721
Appears in Collections:大气环境研究室_学位论文

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作者单位: 1.中国科学院生态环境研究中心

Recommended Citation:
许策. VOCs 的质子化增强检测技术研究[D]. 北京. 中国科学院大学. 2017.
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