Development of a hydrophilic interaction liquid chromatography (HILIC) method for the chemical characterization of water-soluble isoprene epoxydiol (IEPOX)-derived secondary organic aerosol.
Development of a hydrophilic interaction liquid chromatography (HILIC) method for the chemical characterization of water-soluble isoprene epoxydiol (IEPOX)-derived secondary organic aerosol.
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DOI：
10.1039/c8em00308d
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发表时间：
2018-11-14
影响因子：
5.5
通讯作者：
Surratt, Jason D.
中科院分区：
文献类型：
--
作者：
Cui, Tianqu;Zeng, Zhexi;dos Santos, Erickson O.;Zhang, Zhenfa;Chen, Yuzhi;Zhang, Yue;Rose, Caitlin A.;Budisulistiorini, Sri H.;Collins, Leonard B.;Bodnar, Wanda M.;de Souza, Rodrigo A. F.;Martin, Scot T.;Machado, Cristine M. D.;Turpin, Barbara J.;Gold, Avram;Ault, Andrew P.;Surratt, Jason D.
异戊二烯环氧二醇（IEPOX）对硫酸盐气溶胶的酸催化多相化学反应产生大量的水溶性二次有机气溶胶（SOA）成分，包括大气细颗粒物（PM2.5）中的2-甲基四醇、甲基四醇硫酸盐及其低聚物。这些成分通常通过气相色谱法与电子电离质谱法（GC/EI-MS）连接并预先衍生化或通过反相液相色谱法与电喷雾电离高分辨率质谱法（RPLC/ESI-HR-MS）连接进行测量。然而，这两种技术在明确解析和量化极性SOA成分方面都有局限性，这是由于热降解或分离不良。与真实的2-甲基四醇和甲基四醇硫酸盐标准合成的内部，我们开发了一种亲水相互作用液相色谱（HILIC）/ESI-HR-四极杆飞行时间质谱（QTOFMS）协议，可以色谱解析和准确测量主要IEPOX衍生SOA成分在实验室产生的SOA和大气PM2.5。2-甲基四醇同时解决沿着与4-6个非对映异构体的甲基四醇硫酸盐，允许有效的定量两个主要类别的SOA成分通过一个单一的非热分析方法。在美国东南部，2-甲基四醇和甲基四醇硫酸盐的总和分别占实验室产生的β-IEPOX气溶胶质量、实验室产生的δ-IEPOX气溶胶质量和有机气溶胶质量的约92%、62%和21%，其中甲基四醇硫酸盐的质量浓度为甲基四醇质量浓度的171-271%。从亚马逊中部和美国东南部收集的PM2.5样本中，甲基四醇硫酸盐的质量浓度分别为0.39和2.33 μg m-3，分别改进的分辨率清楚地揭示了来自β-和δ-IEPOX的酸催化多相化学的甲基四醇硫酸盐的特定异构体模式。我们还表明，传统的GC/EI-MS分析高估2-甲基四醇高达188%，导致（部分）从甲基四醇硫酸盐的热降解。最后，发现C5-烯烃三醇和3-甲基四氢呋喃-3，4-二醇主要是分别由2-甲基四醇硫酸盐和3-甲基乙基四醇硫酸盐的热降解形成的GC/EI-MS伪影，并且用HILIC/ESI-HR-QTOFMS未检测到。
Acid-catalyzed multiphase chemistry of isoprene epoxydiols (IEPOX) on sulfate aerosol produces substantial amounts of water-soluble secondary organic aerosol (SOA) constituents, including 2-methyltetrols, methyltetrol sulfates, and oligomers thereof in atmospheric fine particulate matter (PM2.5). These constituents have commonly been measured by gas chromatography interfaced to electron ionization mass spectrometry (GC/EI-MS) with prior derivatization or by reverse-phase liquid chromatography interfaced to electrospray ionization high-resolution mass spectrometry (RPLC/ESI-HR-MS). However, both techniques have limitations in explicitly resolving and quantifying polar SOA constituents due either to thermal degradation or poor separation. With authentic 2-methyltetrol and methyltetrol sulfate standards synthesized in-house, we developed a hydrophilic interaction liquid chromatography (HILIC)/ESI-HR-quadrupole time-of-flight mass spectrometry (QTOFMS) protocol that can chromatographically resolve and accurately measure the major IEPOX-derived SOA constituents in both laboratory-generated SOA and atmospheric PM2.5. 2-Methyltetrols were simultaneously resolved along with 4–6 diastereomers of methyltetrol sulfate, allowing efficient quantification of both major classes of SOA constituents by a single non-thermal analytical method. The sum of 2-methyltetrols and methyltetrol sulfates accounted for approximately 92%, 62%, and 21% of the laboratory-generated β-IEPOX aerosol mass, laboratory-generated δ-IEPOX aerosol mass, and organic aerosol mass in the southeastern U.S., respectively, where the mass concentration of methyltetrol sulfates was 171–271% the mass concentration of methyltetrol. Mass concentrations of methyltetrol sulfates were 0.39 and 2.33 μg m−3 in a PM2.5 sample collected from central Amazonia and the southeastern U.S., respectively. The improved resolution clearly reveals isomeric patterns specific to methyltetrol sulfates from acid-catalyzed multiphase chemistry of β- and δ-IEPOX. We also demonstrate that conventional GC/EI-MS analyses overestimate 2-methyltetrols by up to 188%, resulting (in part) from the thermal degradation of methyltetrol sulfates. Lastly, C5-alkene triols and 3-methyltetrahydrofuran-3,4-diols are found to be largely GC/EI-MS artifacts formed from thermal degradation of 2-methyltetrol sulfates and 3-methyletrol sulfates, respectively, and are not detected with HILIC/ESI-HR-QTOFMS.
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DOI：
10.1016/s0021-9673(00)96972-3
发表时间：
1990-01-19
期刊：
JOURNAL OF CHROMATOGRAPHY
影响因子：
--
作者：
ALPERT, AJ
通讯作者：
ALPERT, AJ
影响因子：
3.8
作者：
Isaacman, G.;Kreisberg, N. M.;Goldstein, A. H.
通讯作者：
Goldstein, A. H.
影响因子：
11.4
作者：
Lin, Ying-Hsuan;Zhang, Zhenfa;Docherty, Kenneth S.;Zhang, Haofei;Budisulistiorini, Sri Hapsari;Rubitschun, Caitlin L.;Shaw, Stephanie L.;Knipping, Eladio M.;Edgerton, Eric S.;Kleindienst, Tadeusz E.;Gold, Avram;Surratt, Jason D.
通讯作者：
Surratt, Jason D.
影响因子：
6.3
作者：
de Sa, Suzane S.;Palm, Brett B.;Martin, Scot T.
通讯作者：
Martin, Scot T.
影响因子：
5.2
作者：
Davidson, CI;Phalen, RF;Solomon, PA
通讯作者：
Solomon, PA