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Coupling Filter-Based Thermal Desorption Chemical Ionization Mass Spectrometry with Liquid Chromatography/Electrospray Ionization Mass Spectrometry for Molecular Analysis of Secondary Organic Aerosol

Huang, Yuanlong and Kenseth, Christopher M. and Dalleska, Nathan F. and Seinfeld, John H. (2020) Coupling Filter-Based Thermal Desorption Chemical Ionization Mass Spectrometry with Liquid Chromatography/Electrospray Ionization Mass Spectrometry for Molecular Analysis of Secondary Organic Aerosol. Environmental Science and Technology, 54 (20). pp. 13238-13248. ISSN 0013-936X. https://resolver.caltech.edu/CaltechAUTHORS:20200615-111229578

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Abstract

Filter-based thermal desorption (F-TD) techniques, such as the filter inlet for gases and aerosols, are widely employed to investigate the molecular composition and physicochemical properties of secondary organic aerosol (SOA). Here, we introduce an enhanced capability of F-TD through the combination of a customized F-TD inlet with chemical ionization mass spectrometry (CIMS) and ultraperformance liquid chromatography/electrospray ionization mass spectrometry (UPLC/ESI-MS). The utility of F-TD/CIMS + UPLC/ESI-MS is demonstrated by application to α-pinene ozonolysis SOA for which increased filter aerosol mass loading is shown to slow the evaporation rates of deposited compounds. Evidence for oligomer decomposition producing multimode F-TD/CIMS thermograms is provided by the measurement of the mass fraction remaining of monomeric and dimeric α-pinene oxidation products on the filter via UPLC/ESI-MS. In situ evaporation of aerosol particles suggests that α-pinene-derived hydroperoxides are thermally labile; thus, analysis of particle-phase (hydro)peroxides via F-TD may not be appropriate. A synthesized pinene-derived dimer ester (C₂₀H₃₂O₅) is found to be thermally stable up to 200 °C, whereas particle-phase dimers (C₁₉H₃₀O₅) are observed to form during F-TD analysis via thermally induced condensation of synthesized pinene-derived alcohols and diacids. The complementary F-TD/CIMS + UPLC/ESI-MS method offers previously inaccessible insight into the molecular composition and thermal desorption behavior of SOA that both clarifies and expands on analysis via traditional F-TD techniques.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/acs.est.0c01779DOIArticle
ORCID:
AuthorORCID
Huang, Yuanlong0000-0002-6726-8904
Kenseth, Christopher M.0000-0003-3188-2336
Dalleska, Nathan F.0000-0002-2059-1587
Seinfeld, John H.0000-0003-1344-4068
Additional Information:© 2020 American Chemical Society. Received: March 21, 2020; Revised: June 11, 2020; Accepted: June 12, 2020; Published: June 12, 2020. We appreciate insightful discussions with John D. Crounse and Lu Xu. We acknowledge generous support from Dwight and Christine Landis. UPLC/(−)ESI-Q-TOF-MS was performed in the Caltech Environmental Analysis Center (EAC). The EAC is supported by the Linde Center and Beckman Institute at Caltech. The authors declare no competing financial interest.
Funders:
Funding AgencyGrant Number
Ronald And Maxine Linde Center for Global Environmental ScienceUNSPECIFIED
Caltech Beckman InstituteUNSPECIFIED
Issue or Number:20
Record Number:CaltechAUTHORS:20200615-111229578
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20200615-111229578
Official Citation:Coupling Filter-Based Thermal Desorption Chemical Ionization Mass Spectrometry with Liquid Chromatography/Electrospray Ionization Mass Spectrometry for Molecular Analysis of Secondary Organic Aerosol. Yuanlong Huang, Christopher M. Kenseth, Nathan F. Dalleska, and John H. Seinfeld. Environmental Science & Technology 2020 54 (20), 13238-13248; DOI: 10.1021/acs.est.0c01779
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:103917
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:15 Jun 2020 18:19
Last Modified:21 Oct 2020 22:45

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