Molecular characterisation of ambient aerosols by sequential solvent extractions and high-resolution mass spectrometry

Molecular characterisation of ambient aerosols by sequential solvent extractions and high-resolution mass spectrometry
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通过连续溶剂萃取和高分辨率质谱法对环境气溶胶进行分子表征

DOI:
10.1071/en17197
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发表时间:
2018-05
影响因子:
4.3
通讯作者:
Shi Quan
Shi Quan
中科院分区:
环境科学与生态学4区
文献类型:
--
作者:
Zhang Jingyi;Jiang Bin;Wang Zhiheng;Liang Yongmei;Zhang Yahe;Xu Chunming;Shi Quan

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环境背景有机化合物通常对环境气溶胶细颗粒物有很大的贡献,并且可以影响大气化学。质谱前的溶剂萃取被广泛用于气溶胶中有机化合物的测定,但不同溶剂的分子选择性尚不清楚。我们用各种溶剂提取了气溶胶样品,并显示了通过质谱法获得的有机化合物分布图如何根据提取溶剂而变化。摘要为了全面研究北京地区大气气溶胶中有机化合物的特征,采用傅里叶变换离子回旋共振质谱(FT-ICR MS)对北京地区一个雾霾天采集的大气气溶胶样品进行了连续提取和分析。电喷雾电离(ESI)用于MS分析。气溶胶样品在非极性至极性溶剂正己烷(n-C6)、二氯甲烷(DCM)、乙腈(ACN)和水的顺序中提取,也以相反的顺序提取。将分离的组分分别定义为非极性、低极性、中极性和高极性有机化合物。总有机碳(TOC)的70%左右为可提取的,其中水溶性有机碳(WSOC)和非极性有机碳分别占TOC的30%和25%。非极性和低极性的化合物,如氧化的多环芳烃(PAHs)和含氮化合物(CHN)的分子高度缩合的n-C6和DCM萃取。水溶性有机质(WSOM)占主导地位,脂肪族和芳香族有机硫酸盐(CHOS)和硝基氧有机硫酸盐(CHONS)。大多数含氧化合物(CHO)和含氧和氮的化合物(CHON)具有高双键当量(DBE)和长碳链倾向于被萃取到有机溶剂中。
Environmental context Organic compounds generally make a large contribution to ambient aerosol fine particles, and can influence atmospheric chemistry. Solvent extraction before mass spectrometry is widely used for the determination of organic compounds in aerosols, but the molecular selectivity of different solvents is unclear. We extracted an aerosol sample with various solvents and show how the organic compound profile obtained by mass spectrometry changes depending on the extracting solvent. Abstract For a comprehensive characterisation of organic compounds in aerosols, samples collected on a hazy day from Beijing were sequentially extracted with various solvents and analysed by Fourier-transform ion cyclotron resonance mass spectrometry (FT-ICR MS). Electrospray ionisation (ESI) was used for the MS analysis. Aerosol samples were extracted in an apolar-to-polar solvent order of n-hexane (n-C6), dichloromethane (DCM), acetonitrile (ACN) and water, and also extracted in reverse sequence. The separated fractions were defined as non-polar, low-polarity, mid-polarity and high-polarity organic compounds respectively. Approximately 70 % of the total organic carbon (TOC) was extractable, of which the water-soluble organic carbon (WSOC) and non-polar organic carbon accounted for 30 and 25 % of the TOC respectively. Non-polar and low-polarity compounds with a high degree of molecular condensation such as oxidised polycyclic aromatic hydrocarbons (PAHs) and nitrogen-containing compounds (CHN) were extracted by n-C6 and DCM. Water-soluble organic matter (WSOM) was predominant with aliphatic and aromatic organosulfates (CHOS) and nitrooxy-organosulfates (CHONS). Most oxygen-containing compounds (CHO) and oxygen- and nitrogen-containing compounds (CHON) with high double-bond equivalents (DBEs) and long carbon chains tended to be extracted into organic solvents.
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