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Development of a hydrophilic interaction liquid chromatography (HILIC) method for the chemical characterization of water-soluble isoprene epoxydiol (IEPOX)-derived secondary organic aerosol.
Environ Sci Process Impacts. 2018 Nov 14; 20(11):1524-1536.ES

Abstract

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.

Authors+Show Affiliations

Department of Environmental Sciences and Engineering, Gillings School of Global Public Health, The University of North Carolina at Chapel Hill, Chapel Hill, North Carolina, USA. surratt@unc.edu.No affiliation info availableNo affiliation info availableNo affiliation info availableNo affiliation info availableNo affiliation info availableNo affiliation info availableNo affiliation info availableNo affiliation info availableNo affiliation info availableNo affiliation info availableNo affiliation info availableNo affiliation info availableNo affiliation info availableNo affiliation info availableNo affiliation info availableNo affiliation info available

Pub Type(s)

Journal Article

Language

eng

PubMed ID

30259953

Citation

Cui, Tianqu, et al. "Development of a Hydrophilic Interaction Liquid Chromatography (HILIC) Method for the Chemical Characterization of Water-soluble Isoprene Epoxydiol (IEPOX)-derived Secondary Organic Aerosol." Environmental Science. Processes & Impacts, vol. 20, no. 11, 2018, pp. 1524-1536.
Cui T, Zeng Z, Dos Santos EO, et al. Development of a hydrophilic interaction liquid chromatography (HILIC) method for the chemical characterization of water-soluble isoprene epoxydiol (IEPOX)-derived secondary organic aerosol. Environ Sci Process Impacts. 2018;20(11):1524-1536.
Cui, T., Zeng, Z., Dos Santos, E. O., Zhang, Z., Chen, Y., Zhang, Y., Rose, C. A., Budisulistiorini, S. H., Collins, L. B., Bodnar, W. M., de Souza, R. A. F., Martin, S. T., Machado, C. M. D., Turpin, B. J., Gold, A., Ault, A. P., & Surratt, J. D. (2018). Development of a hydrophilic interaction liquid chromatography (HILIC) method for the chemical characterization of water-soluble isoprene epoxydiol (IEPOX)-derived secondary organic aerosol. Environmental Science. Processes & Impacts, 20(11), 1524-1536. https://doi.org/10.1039/c8em00308d
Cui T, et al. Development of a Hydrophilic Interaction Liquid Chromatography (HILIC) Method for the Chemical Characterization of Water-soluble Isoprene Epoxydiol (IEPOX)-derived Secondary Organic Aerosol. Environ Sci Process Impacts. 2018 Nov 14;20(11):1524-1536. PubMed PMID: 30259953.
* Article titles in AMA citation format should be in sentence-case
TY - JOUR T1 - Development of a hydrophilic interaction liquid chromatography (HILIC) method for the chemical characterization of water-soluble isoprene epoxydiol (IEPOX)-derived secondary organic aerosol. AU - Cui,Tianqu, AU - Zeng,Zhexi, AU - Dos Santos,Erickson O, AU - Zhang,Zhenfa, AU - Chen,Yuzhi, AU - Zhang,Yue, AU - Rose,Caitlin A, AU - Budisulistiorini,Sri H, AU - Collins,Leonard B, AU - Bodnar,Wanda M, AU - de Souza,Rodrigo A F, AU - Martin,Scot T, AU - Machado,Cristine M D, AU - Turpin,Barbara J, AU - Gold,Avram, AU - Ault,Andrew P, AU - Surratt,Jason D, PY - 2018/9/28/pubmed PY - 2019/2/12/medline PY - 2018/9/28/entrez SP - 1524 EP - 1536 JF - Environmental science. Processes & impacts JO - Environ Sci Process Impacts VL - 20 IS - 11 N2 - 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. SN - 2050-7895 UR - https://www.unboundmedicine.com/medline/citation/30259953/Development_of_a_hydrophilic_interaction_liquid_chromatography__HILIC__method_for_the_chemical_characterization_of_water_soluble_isoprene_epoxydiol__IEPOX__derived_secondary_organic_aerosol_ L2 - https://doi.org/10.1039/c8em00308d DB - PRIME DP - Unbound Medicine ER -