Observations of gas-phase products from the nitrate-radical-initiated oxidation of four monoterpenes
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Published:2022-07-13
Issue:13
Volume:22
Page:9017-9031
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ISSN:1680-7324
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Container-title:Atmospheric Chemistry and Physics
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language:en
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Short-container-title:Atmos. Chem. Phys.
Author:
Dam Michelia, Draper Danielle C., Marsavin Andrey, Fry Juliane L.ORCID, Smith James N.ORCID
Abstract
Abstract. Chemical ionization mass spectrometry with the nitrate reagent ion (NO3- CIMS) was used to investigate the products of the nitrate radical
(NO3) initiated oxidation of four monoterpenes in laboratory chamber experiments. α-Pinene, β-pinene, Δ-3-carene, and
α-thujene were studied. The major gas-phase species produced in each system were distinctly different, showing the effect of monoterpene
structure on the oxidation mechanism and further elucidating the contributions of these species to particle formation and growth. By comparing
groupings of products based on the ratios of elements in the general formula CwHxNyOz, the
relative importance of specific mechanistic pathways (fragmentation, termination, and radical rearrangement) can be assessed for each
system. Additionally, the measured time series of the highly oxidized reaction products provide insights into the ratio of relative production and
loss rates of the high-molecular-weight products of the Δ-3-carene system. The measured effective O:C ratios of reaction products were
anticorrelated with new particle formation intensity and number concentration for each system; however, the monomer : dimer ratios of products had a small
positive trend. Gas-phase yields of oxidation products measured by NO3- CIMS correlated with particle number concentrations for each
monoterpene system, with the exception of α-thujene, which produced a considerable amount of low-volatility products but no
particles. Species-resolved wall loss was measured with NO3- CIMS and found to be highly variable among oxidized reaction products in our
stainless steel chamber.
Funder
National Science Foundation U.S. Department of Energy
Publisher
Copernicus GmbH
Subject
Atmospheric Science
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