Detection of atmospheric gaseous amines and amides by a high-resolution time-of-flight chemical ionization mass spectrometer with protonated ethanol reagent ions
Detection of atmospheric gaseous amines and amides by a high-resolution time-of-flight chemical ionization mass spectrometer with protonated ethanol reagent ions
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使用质子化乙醇试剂离子的高分辨率飞行时间化学电离质谱仪检测大气中的气态胺和酰胺
DOI：
10.5194/acp-16-14527-2016
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发表时间：
2016-11
期刊：
影响因子：
--
通讯作者：
Wang Lin
中科院分区：
文献类型：
--
作者：
Wang D. F.;Chen J. M.;Worsnop D. R.;Wang Lin
抽象的。胺和酰胺是重要的大气有机氮化合物，但对这些物种的高时间分辨率、高灵敏度和同时环境测量相当稀少。本文介绍了一种高分辨率飞行时间化学电离质谱仪(HR-ToF-CIMS)的研制，该方法利用质子化乙醇作为试剂离子同时检测大气中的气态胺(C_1~C_6)和酰胺(C_1~C_6)。该方法对胺的灵敏度为5.6~19.4 HzPPTV−1，对酰胺的灵敏度为3.8~38 HZ PPTV−1，总试剂离子信号为 ∼ 0.32 MHz。在背景信号为3 、积分时间为1 的条件下，对胺类化合物的检出限为0.10~0.50σ，对酰胺类化合物的检出限为0.29~1.95 。实验室的受控表征表明，相对湿度对胺和酰胺的检测有显著影响，而有机物的存在对检测没有明显影响。中国，2015年7月25日至8月25日，利用该方法在上海市区进行了胺和酰胺类化合物的环境测量。胺的浓度从万亿分之几到万亿分之数百不等，而酰胺的浓度从万亿分之几十到万亿亿分之几不等。在C_1-~C_6-胺中，C_2-胺是优势物种，其浓度高达130PPTV。对于酰胺，C3-酰胺(高达8.7ppb)是最丰富的物种。胺化物的日轨迹和反向轨迹分析表明，除了大气中二次形成的酰胺外，工业排放可能是上海市区酰胺的重要来源。在活动期间，胺和酰胺的光氧化可能是它们在白天损失的主要途径，湿沉积也是一个重要的汇。
Abstract. Amines and amides are important atmospheric organic-nitrogen compounds but high time resolution, highly sensitive, and simultaneous ambient measurements of these species are rather sparse. Here, we present the development of a high-resolution time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) method, utilizing protonated ethanol as reagent ions to simultaneously detect atmospheric gaseous amines (C1 to C6) and amides (C1 to C6). This method possesses sensitivities of 5.6–19.4 Hz pptv−1 for amines and 3.8–38.0 Hz pptv−1 for amides under total reagent ion signals of ∼ 0.32 MHz. Meanwhile, the detection limits were 0.10–0.50 pptv for amines and 0.29–1.95 pptv for amides at 3σ of the background signal for a 1 min integration time. Controlled characterization in the laboratory indicates that relative humidity has significant influences on the detection of amines and amides, whereas the presence of organics has no obvious effects. Ambient measurements of amines and amides utilizing this method were conducted from 25 July to 25 August 2015 in urban Shanghai, China. While the concentrations of amines ranged from a few parts per trillion by volume to hundreds of parts per trillion by volume, concentrations of amides varied from tens of parts per trillion by volume to a few parts per billion by volume. Among the C1- to C6-amines, the C2-amines were the dominant species with concentrations up to 130 pptv. For amides, the C3-amides (up to 8.7 ppb) were the most abundant species. The diurnal and backward trajectory analysis profiles of amides suggest that in addition to the secondary formation of amides in the atmosphere, industrial emissions could be important sources of amides in urban Shanghai. During the campaign, photo-oxidation of amines and amides might be a main loss pathway for them in daytime, and wet deposition was also an important sink.
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影响因子：
5
作者：
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通讯作者：
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影响因子：
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作者：
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作者：
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DOI：
10.1073/pnas.1103352108
发表时间：
2011-05-31
影响因子：
11.1
作者：
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通讯作者：
de Gouw, Joost
DOI：
10.1073/pnas.1404853111
发表时间：
2014-10-21
影响因子：
11.1
作者：
Kuerten, Andreas;Jokinen, Tuija;Curtius, Joachim
通讯作者：
Curtius, Joachim