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DOI | 10.5194/acp-18-14757-2018 |
A model framework to retrieve thermodynamic and kinetic properties of organic aerosol from composition-resolved thermal desorption measurements | |
Schobesberger, Siegfried1; 39;Ambro, Emma L.2 | |
2018-10-15 | |
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:20页码:14757-14785 |
文章类型 | Article |
语种 | 英语 |
国家 | USA; Finland; Sweden; Switzerland |
英文摘要 | Chemical ionization mass spectrometer (CIMS) techniques have been developed that allow for quantitative and composition-resolved measurements of organic compounds as they desorb from secondary organic aerosol (SOA) particles, in particular during their heat-induced evaporation. One such technique employs the Filter Inlet for Gases and AEROsol (FIGAERO). Here, we present a newly developed model framework with the main aim of reproducing FIGAERO-CIMS thermograms: signal vs. ramped desorption temperature. The model simulates the desorption of organic compounds during controlled heating of filter-sampled SOA particles, plus the subsequent transport of these compounds through the FIGAERO manifold into an iodide-CIMS. Desorption is described by a modified Hertz-Knudsen equation and controlled chiefly by the temperature-dependent saturation concentration C*, mass accommodation (evaporation) coefficient, and particle surface area. Subsequent transport is governed by interactions with filter and manifold surfaces. Reversible accretion reactions (oligomer formation and decomposition) and thermal decomposition are formally described following the Arrhenius relation. We use calibration experiments to tune instrument-specific parameters and then apply the model to a test case: measurements of SOA generated from dark ozonolysis of alpha-pinene. We then discuss the ability of the model to describe thermograms from simple calibration experiments and from complex SOA, and the associated implications for the chemical and physical properties of the SOA. For major individual compositions observed in our SOA test case (#C = 8 to 10), the thermogram peaks can typically be described by assigning C*(25 degrees C) values in the range 0.05 to 5 mu g m(-3), leaving the larger, high-temperature fractions (> 50 %) of the thermograms to be described by thermal decomposition, with dissociation rates on the order of similar to 1 h 1 at 25 degrees C. We conclude with specific experimental designs to better constrain instrumental model parameters and to aid in resolving remaining ambiguities in the interpretation of more complex SOA thermogram behaviors. The model allows retrieval of quantitative volatility and mass transport information from FIGAERO thermograms, and for examining the effects of various environmental or chemical conditions on such properties. |
领域 | 地球科学 |
收录类别 | SCI-E |
WOS记录号 | WOS:000447403100001 |
WOS关键词 | IONIZATION-MASS-SPECTROMETRY ; ALPHA-PINENE OZONOLYSIS ; LOW VOLATILITY COMPOUNDS ; CHEMICAL-IONIZATION ; SOLID-STATE ; MOLECULAR COMPOSITION ; EVAPORATION KINETICS ; MULTILAYER MODEL ; OLIGOMER CONTENT ; VAPOR-PRESSURES |
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/20572 |
专题 | 地球科学 |
作者单位 | 1.Univ Washington, Dept Atmospher Sci, Seattle, WA 98195 USA; 2.Univ Eastern Finland, Dept Appl Phys, Kuopio 70211, Finland; 3.Univ Washington, Dept Chem, Seattle, WA 98195 USA; 4.Stockholm Univ, Dept Environm Sci & Analyt Chem, S-10691 Stockholm, Sweden; 5.Tofwerk AG, CH-3600 Thun, Switzerland |
推荐引用方式 GB/T 7714 | Schobesberger, Siegfried,39;Ambro, Emma L.. A model framework to retrieve thermodynamic and kinetic properties of organic aerosol from composition-resolved thermal desorption measurements[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2018,18(20):14757-14785. |
APA | Schobesberger, Siegfried,&39;Ambro, Emma L..(2018).A model framework to retrieve thermodynamic and kinetic properties of organic aerosol from composition-resolved thermal desorption measurements.ATMOSPHERIC CHEMISTRY AND PHYSICS,18(20),14757-14785. |
MLA | Schobesberger, Siegfried,et al."A model framework to retrieve thermodynamic and kinetic properties of organic aerosol from composition-resolved thermal desorption measurements".ATMOSPHERIC CHEMISTRY AND PHYSICS 18.20(2018):14757-14785. |
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