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Atmospheric Measurement Techniques An interactive open-access journal of the European Geosciences Union
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Volume 10, issue 4 | Copyright
Atmos. Meas. Tech., 10, 1373-1386, 2017
https://doi.org/10.5194/amt-10-1373-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.

Research article 11 Apr 2017

Research article | 11 Apr 2017

New insights into atmospherically relevant reaction systems using direct analysis in real-time mass spectrometry (DART-MS)

Yue Zhao1,a, Michelle C. Fairhurst1, Lisa M. Wingen1, Véronique Perraud1, Michael J. Ezell1, and Barbara J. Finlayson-Pitts1 Yue Zhao et al.
  • 1Department of Chemistry, University of California, Irvine, CA 92697, USA
  • acurrently at: Department of Atmospheric Sciences, University of Washington, Seattle, WA 98195, USA

Abstract. The application of direct analysis in real-time mass spectrometry (DART-MS), which is finding increasing use in atmospheric chemistry, to two different laboratory model systems for airborne particles is investigated: (1) submicron C3–C7 dicarboxylic acid (diacid) particles reacted with gas-phase trimethylamine (TMA) or butylamine (BA) and (2) secondary organic aerosol (SOA) particles from the ozonolysis of α-cedrene. The diacid particles exhibit a clear odd–even pattern in their chemical reactivity toward TMA and BA, with the odd-carbon diacid particles being substantially more reactive than even ones. The ratio of base to diacid in reacted particles, determined using known diacid–base mixtures, was compared to that measured by high-resolution time-of-flight aerosol mass spectrometry (HR-ToF-AMS), which vaporizes the whole particle. Results show that DART-MS probes  ∼ 30nm of the surface layer, consistent with other studies on different systems. For α-cedrene SOA particles, it is shown that varying the temperature of the particle stream as it enters the DART-MS ionization region can distinguish between specific components with the same molecular mass but different vapor pressures. These results demonstrate the utility of DART-MS for (1) examining reactivity of heterogeneous model systems for atmospheric particles and (2) probing components of SOA particles based on volatility.

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Two model systems are studied: dicarboxylic acid particles with gaseous amines and α-cedrene ozonolysis particles. Measurements by direct analysis in real-time mass spectrometry and high-resolution time-of-flight aerosol mass spectrometry show that the reaction of the amines with the acid particles is restricted to the surface layer, with an odd–even alternating pattern. Furthermore, in the α-cedrene study, DART-MS is able to differentiate isomers based on their volatility.
Two model systems are studied: dicarboxylic acid particles with gaseous amines and α-cedrene...
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