High-resolution chemical ionization mass spectrometry (ToF-CIMS): application to study SOA composition and processing

Aljawhary, D.; Lee, Alex K. Y.; Abbatt, Jonathan P. D.

doi:10.5194/amt-6-3211-2013

Cited by 130 publications

(213 citation statements)

References 52 publications

(81 reference statements)

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“…The relatively minor changes in O : C of SOA, despite modest changes in the SOA composition, suggest that there could be compensating effects, i.e., differences in SOA composition are offset by differences in the O : C of the SOA arising from low yield versus high yield pathways. Recently, high-resolution time-of-flight chemical ionization mass spectrometry (HRToF-CIMS) has been used to resolve the composition of SOA in carbon and oxidation state space (for ambient OA that is dominated by carbon, hydrogen and oxygen, oxidation state = 2× O : C − H : C) (Chhabra et al, 2015;Aljawhary et al, 2013). The SOM enables us to visualize the product distribution of SOA in carbon and oxygen space and allows for a direct comparison with the measurements.…”

Section: Soa In Carbon-oxygen Spacementioning

confidence: 99%

Multi-generational oxidation model to simulate secondary organic aerosol in a 3-D air quality model

et al. 2015

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Abstract. Multi-generational gas-phase oxidation of organic vapors can influence the abundance, composition and properties of secondary organic aerosol (SOA). Only recently have SOA models been developed that explicitly represent multigenerational SOA formation. In this work, we integrated the statistical oxidation model (SOM) into SAPRC-11 to simulate the multi-generational oxidation and gas/particle partitioning of SOA in the regional UCD/CIT (University of California, Davis/California Institute of Technology) air quality model. In the SOM, evolution of organic vapors by reaction with the hydroxyl radical is defined by (1) the number of oxygen atoms added per reaction, (2) the decrease in volatility upon addition of an oxygen atom and (3) the probability that a given reaction leads to fragmentation of the organic molecule. These SOM parameter values were fit to laboratory smog chamber data for each precursor/compound class. SOM was installed in the UCD/CIT model, which simulated air quality over 2-week periods in the South Coast Air Basin of California and the eastern United States. For the regions and episodes tested, the two-product SOA model and SOM produce similar SOA concentrations but a modestly different SOA chemical composition. Predictions of the oxygen-tocarbon ratio qualitatively agree with those measured globally using aerosol mass spectrometers. Overall, the implementation of the SOM in a 3-D model provides a comprehensive framework to simulate the atmospheric evolution of organic aerosol.

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Section: Soa In Carbon-oxygen Spacementioning

confidence: 99%

Multi-generational oxidation model to simulate secondary organic aerosol in a 3-D air quality model

et al. 2015

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“…Acetate (CH 3 COO À ) reagent ions was used to ionize and detect acids, including peroxyacids [Veres et al, 2008;Lopez-Hilfiker et al, 2015]. Recent studies have also shown that this reagent ion can be used to measure polyphenols and nitrated phenols, benzoyl peroxide by proton abstraction with similar sensitivity as carboxylic acids [Mohr et al, 2013;Lopez-Hilfiker et al, 2015], and glyoxal, methylglyoxal, and levoglucosan, with far lower sensitivity, via clustering reactions [Veres et al, 2010;Aljawhary et al, 2013]. Since there was no biomass burning influence during BEACHON-RoMBAS, we assume that the contribution of phenols and levoglucosan to the particle-phase acid signal calculated here is minimal.…”

Section: Instrumentation 221 Movi-hrtof-cimsmentioning

confidence: 99%

Estimating the contribution of organic acids to northern hemispheric continental organic aerosol

Yatavelli

Mohr

Stark

et al. 2015

Geophysical Research Letters

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Using chemical ionization mass spectrometry to detect particle‐phase acids and aerosol mass spectrometry (AMS) measurements from Colorado, USA, and two studies in Hyytiälä, Finland, we quantify the fraction of organic aerosol (OA) mass that is composed of molecules with acid functional groups (facid). Molecules containing one or more carboxylic acid functionality contributed approximately 29% (45–51%) of the OA mass in Colorado (Finland). Organic acid mass concentration correlates well with AMS m/z 44 (primarily CO2+), a commonly used marker for highly oxidized aerosol. Using the average empirical relationship between AMS m/z 44 and organic acids in these three studies, together with m/z 44 data from 29 continental northern hemispheric (NH) AMS data sets, we estimate that molecules containing carboxylic acid functionality constitute on average 28% (range 10–50%) of NH continental OA mass with typically higher values at rural/remote sites and during summer and lower values at urban sites and during winter.

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“…The recent coupling of chemical ionization to high-resolution time-of-flight mass spectrometers (HR-ToF-MS) enables the simultaneous determination of the abundance and molecular composition of a wide array of atmospheric inorganic and organic compounds with fast time response and high sensitivity (Junninen et al, 2010;Bertram et al, 2011;Yatavelli et al, 2012;Aljawhary et al, 2013;Lee et al, 2014;Lopez-Hilfiker et al, 2014, 2016aFarmer, 2015, 2016;Yuan et al, 2016). The use of HR-ToF-CIMS has allowed for groundbreaking progress in atmospheric organic chemistry, such as the observation of 3610 Y.…”

Section: Introductionmentioning

confidence: 99%

“…On the other hand, many atmospheric organic systems consist of a wide range of organic compounds with different functionality and polarity. Therefore, multiple complementary ionization schemes are needed to obtain a broad view of these systems (Aljawhary et al, 2013;Praplan et al, 2015).…”

Section: Introductionmentioning

confidence: 99%

“…In CIMS, the analyte molecule reacts with a specific reagent ion via one or more mechanisms, including ligand switching reaction forming an ion-molecule adduct (Huey et al, 1995;Kercher et al, 2009;Aljawhary et al, 2013;Lee et al, 2014;Farmer, 2015, 2016), proton addition (abstraction) forming a protonated (de-protonated) ion (Nowak et al, 2002;Veres et al, 2008;Yatavelli et al, 2012;Aljawhary et al, 2013;Farmer, 2015, 2016;Yuan et al, 2016), or by direct charge transfer forming a molecular ion (Huey et al, 1995;Kim et al, 2016). The reagent ions used mainly include I − , NO − 3 , acetate, CF 3 O − , and SF − 6 for negative ion CIMS, and H 3 O + , NO + , protonated ethanol, and benzene cation for positive ion CIMS.…”

Section: Introductionmentioning

confidence: 99%

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An electrospray chemical ionization source for real-time measurement of atmospheric organic and inorganic vapors

et al. 2017

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Abstract. We present an electrospray ion source coupled to an orthogonal continuous-flow atmospheric pressure chemical ionization region. The source can generate intense and stable currents of several specific reagent ions using a range of salt solutions prepared in methanol, thereby providing both an alternative to more common radioactive ion sources and allowing for the generation of reagent ions that are not available in current chemical ionization mass spectrometry (CIMS) techniques, such as alkaline cations. We couple the orthogonal electrospray chemical ionization (ESCI) source to a high-resolution time-of-flight mass spectrometer (HRToF-MS), and assess instrument performance through calibrations using nitric acid (HNO 3 ), formic acid (HCOOH), and isoprene epoxydiol (trans-β-IEPOX) gas standards, and through measurements of oxidized organic compounds formed from ozonolysis of α-pinene in a continuous-flow reaction chamber. When using iodide as the reagent ion, the HR-ToF-ESCIMS prototype has a sensitivity of 11, 2.4, and 10 cps pptv −1 per million counts per second (cps) of reagent ions and a detection limit (3σ , 5 s averaging) of 4.9, 12.5, and 1.4 pptv to HNO 3 , HCOOH, and IEPOX, respectively. These values are comparable to those obtained using an iodide-adduct HR-ToF-CIMS with a radioactive ion source and low-pressure ion-molecule reaction region. Applications to the α-pinene ozonolysis system demonstrates that HRToF-ESCIMS can generate multiple reagent ions (e.g., I − , NO − 3 , acetate, Li + , Na + , K + , and NH + 4 ) having different selectivity to provide a comprehensive molecular description of a complex organic system.

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High-resolution chemical ionization mass spectrometry (ToF-CIMS): application to study SOA composition and processing

Cited by 130 publications

References 52 publications

Multi-generational oxidation model to simulate secondary organic aerosol in a 3-D air quality model

Multi-generational oxidation model to simulate secondary organic aerosol in a 3-D air quality model

Estimating the contribution of organic acids to northern hemispheric continental organic aerosol

An electrospray chemical ionization source for real-time measurement of atmospheric organic and inorganic vapors

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