Application of high-resolution time-of-flight chemical ionization mass spectrometry measurements to estimate volatility distributions of α-pinene and naphthalene oxidation products

Chhabra, P. S.; Lambe, A. T.; Canagaratna, M. R.; Stark, H.; Jayne, J. T.; Onasch, T. B.; Davidovits, P.; Kimmel, J. R.; Worsnop, D. R.

doi:10.5194/amt-8-1-2015

Title: Application of high-resolution time-of-flight chemical ionization mass spectrometry measurements to estimate volatility distributions of α-pinene and naphthalene oxidation products

Journal Article · 05 January 2015 · Atmospheric Measurement Techniques (Online)

DOI: https://doi.org/10.5194/amt-8-1-2015 · OSTI ID:1197858

Chhabra, P. S. ^[1]; Lambe, A. T. ^[2]; Canagaratna, M. R. ^[1]; Stark, H. ^[3]; Jayne, J. T. ^[1]; Onasch, T. B. ^[2]; Davidovits, P. ^[4]; Kimmel, J. R. ^[5]; Worsnop, D. R. ^[1]

Aerodyne Research, Inc., Billerica, MA (United States)
Aerodyne Research, Inc., Billerica, MA (United States); Boston College, Chestnut Hill, MA (United States)
Aerodyne Research, Inc., Billerica, MA (United States); Univ. of Colorado, Boulder, CO (United States)
Boston College, Chestnut Hill, MA (United States)
Aerodyne Research, Inc., Billerica, MA (United States); Univ. of Colorado, Boulder, CO (United States); TOFWERK AG, Thun (Switzerland)

Recent developments in high-resolution time-of-flight chemical ionization mass spectrometry (HR-ToF-CIMS) have made it possible to directly detect atmospheric organic compounds in real time with high sensitivity and with little or no fragmentation, including low-volatility, highly oxygenated organic vapors that are precursors to secondary organic aerosol formation. Here, using ions identified by high-resolution spectra from an HR-ToF-CIMS with acetate reagent ion chemistry, we develop an algorithm to estimate the vapor pressures of measured organic acids. The algorithm uses identified ion formulas and calculated double bond equivalencies, information unavailable in quadrupole CIMS technology, as constraints for the number of possible oxygen-containing functional groups. The algorithm is tested with acetate chemical ionization mass spectrometry (acetate-CIMS) spectra of O₃ and OH oxidation products of α-pinene and naphthalene formed in a flow reactor with integrated OH exposures ranged from 1.2 × 10¹¹ to 9.7 × 10¹¹ molec s cm⁻³, corresponding to approximately 1.0 to 7.5 days of equivalent atmospheric oxidation. Measured gas-phase organic acids are similar to those previously observed in environmental chamber studies. For both precursors, we find that acetate-CIMS spectra capture both functionalization (oxygen addition) and fragmentation (carbon loss) as a function of OH exposure. The level of fragmentation is observed to increase with increased oxidation. The predicted condensed-phase secondary organic aerosol (SOA) average acid yields and O/C and H/C ratios agree within uncertainties with previous chamber and flow reactor measurements and ambient CIMS results. Furthermore, while acetate reagent ion chemistry is used to selectively measure organic acids, in principle this method can be applied to additional reagent ion chemistries depending on the application.

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Research Organization:: Boston College, Chestnut Hill, MA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: SC0006980; SC0004577; FG02-05ER63995

OSTI ID:: 1197858

Alternate ID(s):: OSTI ID: 1455196

Journal Information:: Atmospheric Measurement Techniques (Online), Vol. 8, Issue 1; ISSN 1867-8548

Publisher:: European Geosciences UnionCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 35 works

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Clustering, methodology, and mechanistic insights into acetate chemical ionization using high-resolution time-of-flight mass spectrometry Brophy, Patrick; Farmer, Delphine K. Atmospheric Measurement Techniques, Vol. 9, Issue 8 https://doi.org/10.5194/amt-9-3969-2016	journal	January 2016
Multi-generational oxidation model to simulate secondary organic aerosol in a 3-D air quality model Jathar, S. H.; Cappa, C. D.; Wexler, A. S. Geoscientific Model Development, Vol. 8, Issue 8 https://doi.org/10.5194/gmd-8-2553-2015	journal	January 2015
Technical Note: Relating functional group measurements to carbon types for improved model-measurement comparisons of organic aerosol composition Takahama, Satoshi; Ruggeri, Giulia Atmospheric Chemistry and Physics https://doi.org/10.5194/acp-2016-926	posted_content	October 2016
A Novel High-Volume Photochemical Emission Aging Flow Tube Reactor (PEAR) Ihalainen, Mika; Tiitta, Petri; Czech, Hendryk Taylor & Francis https://doi.org/10.6084/m9.figshare.7525424.v1	text	January 2018
Technical Note: Development of chemoinformatic tools to enumerate functional groups in molecules for organic aerosol characterization Ruggeri, G.; Takahama, S. Atmospheric Chemistry and Physics Discussions https://doi.org/10.5194/acpd-15-33631-2015	journal	November 2015
A switchable reagent ion high resolution time-of-flight chemical ionization mass spectrometer for real-time measurement of gas phase oxidized species: characterization from the 2013 Southern Oxidant and Aerosol Study Brophy, P.; Farmer, D. K. Atmospheric Measurement Techniques Discussions, Vol. 8, Issue 3 https://doi.org/10.5194/amtd-8-3199-2015	journal	January 2015
A novel high-volume Photochemical Emission Aging flow tube Reactor (PEAR) Ihalainen, Mika; Tiitta, Petri; Czech, Hendryk Taylor & Francis https://doi.org/10.6084/m9.figshare.7525424.v2	text	January 2019
Application of a FIGAERO ToF CIMS for on-line characterization of real-world fresh and aged particle emissions from buses Breton, M. Le; Psichoudaki, M.; Hallquist, M. Figshare https://doi.org/10.6084/m9.figshare.7560371	text	January 2019
Assessing the degree of plug flow in oxidation flow reactors (OFRs): a study on a potential aerosol mass (PAM) reactor Mitroo, Dhruv; Sun, Yujian; Combest, Daniel P. Atmospheric Measurement Techniques, Vol. 11, Issue 3 https://doi.org/10.5194/amt-11-1741-2018	journal	January 2018
A novel high-volume Photochemical Emission Aging flow tube Reactor (PEAR) Ihalainen, Mika; Tiitta, Petri; Czech, Hendryk Taylor & Francis https://doi.org/10.6084/m9.figshare.7525424	text	January 2019
Application of a FIGAERO ToF CIMS for on-line characterization of real-world fresh and aged particle emissions from buses Breton, M. Le; Psichoudaki, M.; Hallquist, M. Figshare https://doi.org/10.6084/m9.figshare.7560371.v1	text	January 2019
Secondary Organic Aerosol Formation from Healthy and Aphid-Stressed Scots Pine Emissions Faiola, Celia L.; Pullinen, Iida; Buchholz, Angela ACS Earth and Space Chemistry, Vol. 3, Issue 9 https://doi.org/10.1021/acsearthspacechem.9b00118	journal	August 2019

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