Kinetics, SOA yields, and chemical composition of seconaary organic aerosol from beta-caryophyllene ozonolysis with and without nitrogen oxides between 213 and 313 K

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dc.contributor.author Gao, Linyu
dc.contributor.author Song, Junwei
dc.contributor.author Mohr, Claudia
dc.contributor.author Huang, Wei
dc.contributor.author Vallon, Magdalena
dc.contributor.author Jiang, Feng
dc.contributor.author Leisner, Thomas
dc.contributor.author Saathoff, Harald
dc.date.accessioned 2022-06-27T10:56:02Z
dc.date.available 2022-06-27T10:56:02Z
dc.date.issued 2022-05-06
dc.identifier.citation Gao , L , Song , J , Mohr , C , Huang , W , Vallon , M , Jiang , F , Leisner , T & Saathoff , H 2022 , ' Kinetics, SOA yields, and chemical composition of seconaary organic aerosol from beta-caryophyllene ozonolysis with and without nitrogen oxides between 213 and 313 K ' , Atmospheric Chemistry and Physics , vol. 22 , no. 9 , pp. 6001-6020 . https://doi.org/10.5194/acp-22-6001-2022
dc.identifier.other PURE: 214221698
dc.identifier.other PURE UUID: b1fcc861-29ec-4059-b683-5785cf7128ab
dc.identifier.other WOS: 000791462500001
dc.identifier.other Scopus: 85129790701
dc.identifier.other ORCID: /0000-0002-5049-2117/work/115271061
dc.identifier.uri http://hdl.handle.net/10138/345513
dc.description.abstract beta-caryophyllene (BCP) is one of the most important sesquiterpenes (SQTs) in the atmosphere, with a large potential contribution to secondary organic aerosol (SOA) formation mainly from reactions with ozone (O-3) and nitrate radicals (NO3). In this work, we study the temperature dependence of the kinetics of BCP ozonolysis, SOA yields, and SOA chemical composition in the dark and in the absence and presence of nitrogen oxides including nitrate radicals (NO3). We cover a temperature range of 213-313 K, representative of tropospheric conditions. The oxidized components in both gas and particle phases were characterized on a molecular level by a chemical ionization mass spectrometer equipped with a filter inlet for gases and aerosols using iodide as the reagent ion (FIGAERO-iodide-CIMS). The batch mode experiments were conducted in the 84.5 m(3) aluminium simulation chamber AIDA at the Karlsruhe Institute of Technology (KIT). In the absence of nitrogen oxides, the temperature-dependent rate coefficient of the endocyclic double bond in BCP reacting with ozone between 243-313 K is negatively correlated with temperature, corresponding to the following Arrhenius equation: k = (1.6 +/- 0.4) x 10(-15) x exp((559 +/- 97)/ T). The SOA yields increase from 16 +/- 5 % to 37 +/- 11 %, with temperatures decreasing from 313 to 243 K at a total organic particle mass of 10 mu g m(-3). The variation in the ozonolysis temperature leads to a substantial impact on the abundance of individual organic molecules. In the absence of nitrogen oxides, monomers C14-15H22-24O3-7 (37.4 %), dimers C28-30H44-48O5-9 (53.7 %), and timers C41_44H62_6609_11 (8.6 %) are abundant in the particle phase at 213 K. At 313 K, we observed more oxidized monomers (mainly C14-15H22-24O6-9, 67.5 %) and dimers (mainly C27-29H42-44O9-11, 27.6 %), including highly oxidized molecules (HOMs; C14H22O7,9C15H22O7,9C15H24O7,9), which can be formed via hydrogen shift mechanisms, but no significant timers. In the presence of nitrogen oxides, the organonitrate fraction increased from 3 % at 213 K to 12 % and 49 % at 243 and 313 K, respectively. Most of the organonitrates were monomers with Cis skeletons and only one nitrate group. More highly oxygenated organonitrates were observed at higher temperatures, with their signal-weighted O : C atomic ratio increasing from 0.41 to 0.51 from 213 to 313 K. New dimeric and timeric organic species without nitrogen atoms (C-20, C-35) were formed in the presence of nitrogen oxides at 298-313 K, indicating potential new reaction pathways. Overall, our results show that increasing temperatures lead to a relatively small decrease in the rate coefficient of the endocyclic double bond in BCP reacting with ozone but to a strong decrease in SOA yields. In contrast, the formation of HOMs and organonitrates increases significantly with temperature. en
dc.format.extent 20
dc.language.iso eng
dc.relation.ispartof Atmospheric Chemistry and Physics
dc.rights cc_by
dc.rights.uri info:eu-repo/semantics/openAccess
dc.subject 1172 Environmental sciences
dc.title Kinetics, SOA yields, and chemical composition of seconaary organic aerosol from beta-caryophyllene ozonolysis with and without nitrogen oxides between 213 and 313 K en
dc.type Article
dc.contributor.organization Institute for Atmospheric and Earth System Research (INAR)
dc.description.reviewstatus Peer reviewed
dc.relation.doi https://doi.org/10.5194/acp-22-6001-2022
dc.relation.issn 1680-7316
dc.rights.accesslevel openAccess
dc.type.version publishedVersion

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