Stable carbon isotope composition of secondary organic aerosol from β-pinene oxidation

被引:51
|
作者
Fisseha, Rebeka [1 ]
Spahn, Holger [1 ]
Wegener, Robert [1 ]
Hohaus, Thorsten [1 ]
Brasse, Gregor [1 ]
Wissel, Holger [1 ]
Tillmann, Ralf [1 ]
Wahner, Andreas [1 ]
Koppmann, Ralf [2 ]
Kiendler-Scharr, Astrid [1 ]
机构
[1] Forschungszentrum Julich, Inst Chem & Dynam Geosphare, ICG Troposphare 2, D-52425 Julich, Germany
[2] Berg Univ Wuppertal, Fachgrp Phys, Fachbereich Math & Nat Wissensch, D-42119 Wuppertal, Germany
关键词
MASTER CHEMICAL MECHANISM; METHYL VINYL KETONE; GAS-PHASE REACTIONS; MCM V3 PART; TROPOSPHERIC DEGRADATION; LIGHT-HYDROCARBONS; MASS-SPECTROMETRY; OZONE; PRODUCTS; AIR;
D O I
10.1029/2008JD011326
中图分类号
P4 [大气科学(气象学)];
学科分类号
0706 ; 070601 ;
摘要
A chamber study was carried out to investigate the stable carbon isotopic composition (delta C-13) of secondary organic aerosol (SOA) formed from ozonolysis of beta-pinene. beta-Pinene (600 ppb) with a known delta C-13 value (-30.1%) and 500 ppb ozone were injected into the chamber in the absence of light and the resulting SOA was collected on preheated quartz fiber filters. Furthermore, delta C-13 values of the gas-phase beta-pinene and one of its oxidation products, nopinone, were measured using a gas chromatograph coupled to an isotope ratio mass spectrometer (GC-IRMS). beta-Pinene was progressively enriched with the heavy carbon isotope due to the kinetic isotope effect (KIE). The KIE of the reaction of beta-pinene with ozone was measured to be 1.0026 ((O3)epsilon 2.6 +/- 1.5 parts per thousand). The delta C-13 value of total secondary organic aerosol was very similar to that of its precursor (average = -29.6 +/- 0.2 parts per thousand) independent of experiment time. Nopinone, one of the major oxidation products of beta-pinene, was found in both the gas and aerosol phases. The gas-phase nopinone was heavier than the initial beta-pinene by 1.3 parts per thousand but lighter than the corresponding aerosol-phase nopinone. On average, the gas-phase nopinone was lighter by 2.3 parts per thousand than the corresponding aerosol- phase nopinone. The second product found in the SOA was detected as acetone, but it desorbed from the filter at a higher temperature than nopinone, which indicates that it is a pyrolysis product. The acetone showed a much lower delta C-13 (-36.6%) compared to the initial beta-pinene delta C-13.
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页数:8
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