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Title: Ion mobility spectrometry–mass spectrometry (IMS–MS) for on- and offline analysis of atmospheric gas and aerosol species

Abstract

Abstract. Measurement techniques that provide molecular-level information are needed to elucidate the multiphase processes that produce secondary organic aerosol (SOA) species in the atmosphere. Here we demonstrate the application of ion mobility spectrometry-mass spectrometry (IMS–MS) to the simultaneous characterization of the elemental composition and molecular structures of organic species in the gas and particulate phases. Molecular ions of gas-phase organic species are measured online with IMS–MS after ionization with a custom-built nitrate chemical ionization (CI) source. This CI–IMS–MS technique is used to obtain time-resolved measurements (5 min) of highly oxidized organic molecules during the 2013 Southern Oxidant and Aerosol Study (SOAS) ambient field campaign in the forested SE US. The ambient IMS–MS signals are consistent with laboratory IMS–MS spectra obtained from single-component carboxylic acids and multicomponent mixtures of isoprene and monoterpene oxidation products. Mass-mobility correlations in the 2-D IMS–MS space provide a means of identifying ions with similar molecular structures within complex mass spectra and are used to separate and identify monoterpene oxidation products in the ambient data that are produced from different chemical pathways. Water-soluble organic carbon (WSOC) constituents of fine aerosol particles that are not resolvable with standard analytical separation methods, such as liquid chromatography (LC), are shown tomore » be separable with IMS–MS coupled to an electrospray ionization (ESI) source. The capability to use ion mobility to differentiate between isomers is demonstrated for organosulfates derived from the reactive uptake of isomers of isoprene epoxydiols (IEPOX) onto wet acidic sulfate aerosol. Controlled fragmentation of precursor ions by collisionally induced dissociation (CID) in the transfer region between the IMS and the MS is used to validate MS peak assignments, elucidate structures of oligomers, and confirm the presence of the organosulfate functional group.« less

Authors:
ORCiD logo; ; ORCiD logo; ; ; ; ; ; ; ; ORCiD logo; ; ORCiD logo; ; ; ; ;
Publication Date:
Research Org.:
Boston College, Chestnut Hill, MA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1271467
Alternate Identifier(s):
OSTI ID: 1360128
Grant/Contract Number:  
SC001110; SC0011935
Resource Type:
Published Article
Journal Name:
Atmospheric Measurement Techniques (Online)
Additional Journal Information:
Journal Name: Atmospheric Measurement Techniques (Online) Journal Volume: 9 Journal Issue: 7; Journal ID: ISSN 1867-8548
Publisher:
Copernicus Publications, EGU
Country of Publication:
Germany
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Krechmer, Jordan E., Groessl, Michael, Zhang, Xuan, Junninen, Heikki, Massoli, Paola, Lambe, Andrew T., Kimmel, Joel R., Cubison, Michael J., Graf, Stephan, Lin, Ying-Hsuan, Budisulistiorini, Sri H., Zhang, Haofei, Surratt, Jason D., Knochenmuss, Richard, Jayne, John T., Worsnop, Douglas R., Jimenez, Jose-Luis, and Canagaratna, Manjula R. Ion mobility spectrometry–mass spectrometry (IMS–MS) for on- and offline analysis of atmospheric gas and aerosol species. Germany: N. p., 2016. Web. doi:10.5194/amt-9-3245-2016.
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Krechmer, Jordan E., Groessl, Michael, Zhang, Xuan, Junninen, Heikki, Massoli, Paola, Lambe, Andrew T., Kimmel, Joel R., Cubison, Michael J., Graf, Stephan, Lin, Ying-Hsuan, Budisulistiorini, Sri H., Zhang, Haofei, Surratt, Jason D., Knochenmuss, Richard, Jayne, John T., Worsnop, Douglas R., Jimenez, Jose-Luis, & Canagaratna, Manjula R. Ion mobility spectrometry–mass spectrometry (IMS–MS) for on- and offline analysis of atmospheric gas and aerosol species. Germany. https://doi.org/10.5194/amt-9-3245-2016
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Krechmer, Jordan E., Groessl, Michael, Zhang, Xuan, Junninen, Heikki, Massoli, Paola, Lambe, Andrew T., Kimmel, Joel R., Cubison, Michael J., Graf, Stephan, Lin, Ying-Hsuan, Budisulistiorini, Sri H., Zhang, Haofei, Surratt, Jason D., Knochenmuss, Richard, Jayne, John T., Worsnop, Douglas R., Jimenez, Jose-Luis, and Canagaratna, Manjula R. Mon . "Ion mobility spectrometry–mass spectrometry (IMS–MS) for on- and offline analysis of atmospheric gas and aerosol species". Germany. https://doi.org/10.5194/amt-9-3245-2016.
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@article{osti_1271467,
title = {Ion mobility spectrometry–mass spectrometry (IMS–MS) for on- and offline analysis of atmospheric gas and aerosol species},
author = {Krechmer, Jordan E. and Groessl, Michael and Zhang, Xuan and Junninen, Heikki and Massoli, Paola and Lambe, Andrew T. and Kimmel, Joel R. and Cubison, Michael J. and Graf, Stephan and Lin, Ying-Hsuan and Budisulistiorini, Sri H. and Zhang, Haofei and Surratt, Jason D. and Knochenmuss, Richard and Jayne, John T. and Worsnop, Douglas R. and Jimenez, Jose-Luis and Canagaratna, Manjula R.},
abstractNote = {Abstract. Measurement techniques that provide molecular-level information are needed to elucidate the multiphase processes that produce secondary organic aerosol (SOA) species in the atmosphere. Here we demonstrate the application of ion mobility spectrometry-mass spectrometry (IMS–MS) to the simultaneous characterization of the elemental composition and molecular structures of organic species in the gas and particulate phases. Molecular ions of gas-phase organic species are measured online with IMS–MS after ionization with a custom-built nitrate chemical ionization (CI) source. This CI–IMS–MS technique is used to obtain time-resolved measurements (5 min) of highly oxidized organic molecules during the 2013 Southern Oxidant and Aerosol Study (SOAS) ambient field campaign in the forested SE US. The ambient IMS–MS signals are consistent with laboratory IMS–MS spectra obtained from single-component carboxylic acids and multicomponent mixtures of isoprene and monoterpene oxidation products. Mass-mobility correlations in the 2-D IMS–MS space provide a means of identifying ions with similar molecular structures within complex mass spectra and are used to separate and identify monoterpene oxidation products in the ambient data that are produced from different chemical pathways. Water-soluble organic carbon (WSOC) constituents of fine aerosol particles that are not resolvable with standard analytical separation methods, such as liquid chromatography (LC), are shown to be separable with IMS–MS coupled to an electrospray ionization (ESI) source. The capability to use ion mobility to differentiate between isomers is demonstrated for organosulfates derived from the reactive uptake of isomers of isoprene epoxydiols (IEPOX) onto wet acidic sulfate aerosol. Controlled fragmentation of precursor ions by collisionally induced dissociation (CID) in the transfer region between the IMS and the MS is used to validate MS peak assignments, elucidate structures of oligomers, and confirm the presence of the organosulfate functional group.},
doi = {10.5194/amt-9-3245-2016},
journal = {Atmospheric Measurement Techniques (Online)},
number = 7,
volume = 9,
place = {Germany},
year = {Mon Jul 25 00:00:00 EDT 2016},
month = {Mon Jul 25 00:00:00 EDT 2016}
}
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https://doi.org/10.5194/amt-9-3245-2016
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Figures / Tables:

Figure 1 Figure 1: A schematic diagram of the IMS–TOF (a). The instrument can be used with different ionization sources, including the ESI source shown in (a) and the custom-built nitrate-ion chemical ionization source (NO$^{-}_{3}$ -CI) attached to the front end of the desolvation region shown in (b). The diagram is notmore » drawn to scale.« less
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