Global S&T Development Trend Analysis Platform of Resources and Environment
DOI | 10.5194/acp-18-12969-2018 |
Gas-to-particle partitioning of major biogenic oxidation products: a study on freshly formed and aged biogenic SOA | |
Gkatzelis, Georgios I.1; Hohaus, Thorsten1; Tillmann, Ralf1; Gensch, Iulia1; Mueller, Markus2,4; Eichler, Philipp2,6; Xu, Kang-Ming3; Schlag, Patrick1,7; Schmitt, Sebastian H.1; Yu, Zhujun1; Wegener, Robert1; Kaminski, Martin1; Holzinger, Rupert3; Wisthaler, Armin2,5; Kiendler-Scharr, Astrid1 | |
2018-09-10 | |
发表期刊 | ATMOSPHERIC CHEMISTRY AND PHYSICS
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ISSN | 1680-7316 |
EISSN | 1680-7324 |
出版年 | 2018 |
卷号 | 18期号:17页码:12969-12989 |
文章类型 | Article |
语种 | 英语 |
国家 | Germany; Austria; Netherlands; Norway; Brazil |
英文摘要 | Secondary organic aerosols (SOAs) play a key role in climate change and air quality. Determining the fundamental parameters that distribute organic compounds between the phases is essential, as atmospheric lifetime and impacts change drastically between the gas and particle phase. In this work, gas-to-particle partitioning of major biogenic oxidation products was investigated using three different aerosol chemical characterization techniques. The aerosol collection module, the collection thermal desorption unit, and the chemical analysis of aerosols online are different aerosol sampling inlets connected to a proton-transfer reaction time-of-flight mass spectrometer (ACM-PTR-ToF-MS, TD-PTR-ToF-MS, and CHARON-PTR-ToF-MS, respectively, referred to hereafter as ACM, TD, and CHARON). These techniques were deployed at the atmosphere simulation chamber SAPHIR to perform experiments on the SOA formation and aging from different monoterpenes (beta-pinene, limonene) and real plant emissions (Pinus sylvestris L.). The saturation mass concentration C* and thus the volatility of the individual ions was determined based on the simultaneous measurement of their signal in the gas and particle phase. A method to identify and exclude ions affected by thermal dissociation during desorption and ionic dissociation in the ionization chamber of the proton-transfer reaction mass spectrometer (PTR-MS) was developed and tested for each technique. Narrow volatility distributions with organic compounds in the semi-volatile (SVOCs - semi-volatile organic compounds) to intermediate-volatility (IVOCs -intermediate-volatility organic compounds) regime were found for all systems studied. Despite significant differences in the aerosol collection and desorption methods of the proton-transfer-reaction (PTR)-based techniques, a comparison of the C* values obtained with different techniques was found to be in good agreement (within 1 order of magnitude) with deviations explained by the different operating conditions of the PTR-MS. The C* of the identified organic compounds were mapped onto the two-dimensional volatility basis set (2D-VBS), and results showed a decrease in C* with increasing oxidation state. For all experiments conducted in this study, identified partitioning organic compounds accounted for 20-30% of the total organic mass measured from an aerosol mass spectrometer (AMS). Further comparison between observations and theoretical calculations was performed for species found in our experiments that were also identified in previous publications. Theoretical calculations based on the molecular structure of the compounds showed, within the uncertainties ranges, good agreement with the experimental C* for most SVOCs, while IVOCs deviated by up to a factor of 300. These latter differences are discussed in relation to two main processes affecting these systems: (i) possible interferences by thermal and ionic fragmentation of higher molecular-weight compounds, produced by accretion and oligomerization reactions, that fragment in the m/z range detected by the PTR-MS and (ii) kinetic influences in the distribution between the gas and particle phase with gas-phase condensation, diffusion in the particle phase, and irreversible uptake. |
领域 | 地球科学 |
收录类别 | SCI-E |
WOS记录号 | WOS:000444187300002 |
WOS关键词 | SECONDARY ORGANIC AEROSOL ; VOLATILITY BASIS-SET ; MASS-SPECTROMETRY CHARACTERIZATION ; SIMULATION CHAMBER SAPHIR ; PURE-COMPONENT PROPERTIES ; ALPHA-PINENE OZONOLYSIS ; THERMAL-DESORPTION ; VAPOR-PRESSURE ; D-LIMONENE ; BETA-PINENE |
WOS类目 | Environmental Sciences ; Meteorology & Atmospheric Sciences |
WOS研究方向 | Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/27307 |
专题 | 地球科学 |
作者单位 | 1.Forschungszentrum Julich, IEK Troposphere 8, Inst Energy & Climate Res, Julich, Germany; 2.Univ Innsbruck, Inst Ionenphys & Angew Phys, Innsbruck, Austria; 3.Inst Marine & Atmospher Res Utrecht, Princetonpl 5, NL-3584 CC Utrecht, Netherlands; 4.Ionicon Analyt GmbH, Innsbruck, Austria; 5.Univ Oslo, Dept Chem, Oslo, Norway; 6.German Environm Agcy, Dessau Rosslau, Germany; 7.Univ Sao Paulo, Inst Phys, Sao Paulo, Brazil |
推荐引用方式 GB/T 7714 | Gkatzelis, Georgios I.,Hohaus, Thorsten,Tillmann, Ralf,et al. Gas-to-particle partitioning of major biogenic oxidation products: a study on freshly formed and aged biogenic SOA[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2018,18(17):12969-12989. |
APA | Gkatzelis, Georgios I..,Hohaus, Thorsten.,Tillmann, Ralf.,Gensch, Iulia.,Mueller, Markus.,...&Kiendler-Scharr, Astrid.(2018).Gas-to-particle partitioning of major biogenic oxidation products: a study on freshly formed and aged biogenic SOA.ATMOSPHERIC CHEMISTRY AND PHYSICS,18(17),12969-12989. |
MLA | Gkatzelis, Georgios I.,et al."Gas-to-particle partitioning of major biogenic oxidation products: a study on freshly formed and aged biogenic SOA".ATMOSPHERIC CHEMISTRY AND PHYSICS 18.17(2018):12969-12989. |
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