Formation of new particles in the gas-phase ozonolysis of monoterpenes

被引:189
作者
Koch, S [1 ]
Winterhalter, R [1 ]
Uherek, E [1 ]
Kolloff, A [1 ]
Neeb, P [1 ]
Moortgat, GK [1 ]
机构
[1] Max Planck Inst Chem, Div Atmospher Chem, D-55020 Mainz, Germany
关键词
monoterpenes; ozone; organic acids; secondary organic aerosol; dicarboxylic acids;
D O I
10.1016/S1352-2310(00)00133-3
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
The formation of organic acids and secondary organic aerosol in the gas-phase ozonolysis was investigated by laboratory experiments at 295 +/- 2 K in the absence of seed aerosol for a series of monoterpenes (beta-pinene, sabinene, alpha-pinene, Delta(3)-carene, limonene, terpinolene) and methylene-cyclo-hexane and methyl-cyclo-hexene as model compounds. In the filter samples of the aerosol produced by ozonolysis series of organic acids were identified as methyl ester using GC/MS. In the ozonolysis of beta-pinene, sabinene, alpha-pinene, Delta(3)-carene and limonene the corresponding C-9-dicarboxylic acids were found as main products of the organic acid fraction. In case of terpinolene, methylene-cyclo-hexane and methyl-cyclo-hexene C-7- and C-6-dicarboxylic acids, respectively, were detected. The yields of these dicarboxylic acids were determined to range between 1 and 5 mol% using ion chromatography. Particle formation was observed with a 10 nm condensation nuclei counter after the consumption of (6.1 +/- 0.3) x 10(10) molecule cm(-3) of beta-pinene, sabinene, alpha-pinene, Delta(3)-carene and limonene, respectively. In case of terpinolene, methylene-cyclo-hexane and methyl-cyclo-hexene (1.8 +/- 0.1) x 10(11) molecule cm(-3) of the reactants were converted. Upper limits for the partial vapor pressures of the dicarboxylic acids in the aerosol were determined to be (5.6 +/- 4.0)x 10(-8) Torr for the Cg-dicarboxylic acids and (1.7 +/- 1.2)x 10(-7) Torr for the C7- and C-6-dicarboxylic acids. The formation of secondary organic aerosol by ozonolysis of terpenes under suitable atmospheric conditions has most likely to be taken into account. (C) 2000 Published by Elsevier Science Ltd.
引用
收藏
页码:4031 / 4042
页数:12
相关论文
共 41 条
  • [1] Atmospheric aerosols: Biogeochemical sources and role in atmospheric chemistry
    Andreae, MO
    Crutzen, PJ
    [J]. SCIENCE, 1997, 276 (5315) : 1052 - 1058
  • [2] ANDREAE MO, 1995, FUTURE CLIMATES WORL, P347
  • [3] [Anonymous], 1975, Angew. Chem, DOI [10.1002/ange.19750872104, DOI 10.1002/ANGE.19750872104]
  • [4] Gas-phase tropospheric chemistry of volatile organic compounds .1. Alkanes and alkenes
    Atkinson, R
    [J]. JOURNAL OF PHYSICAL AND CHEMICAL REFERENCE DATA, 1997, 26 (02) : 215 - 290
  • [5] FORMATION OF OH RADICALS IN THE GAS-PHASE REACTIONS OF O3 WITH A SERIES OF TERPENES
    ATKINSON, R
    ASCHMANN, SM
    AREY, J
    SHOREES, B
    [J]. JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1992, 97 (D5) : 6065 - 6073
  • [6] BLAU K, 1993, HDB DERIVATIVES CHRO, P15
  • [7] Gas-phase terpene oxidation products: a review
    Calogirou, A
    Larsen, BR
    Kotzias, D
    [J]. ATMOSPHERIC ENVIRONMENT, 1999, 33 (09) : 1423 - 1439
  • [8] cis-pinic acid, a possible precursor for organic aerosol formation from ozonolysis of α-pinene
    Christoffersen, TS
    Hjorth, J
    Horie, O
    Jensen, NR
    Kotzias, D
    Molander, LL
    Neeb, P
    Ruppert, L
    Winterhalter, R
    Virkkula, A
    Wirtz, K
    Larsen, BR
    [J]. ATMOSPHERIC ENVIRONMENT, 1998, 32 (10) : 1657 - 1661
  • [9] EMISSIONS OF VOLATILE ORGANIC COMPOUNDS FROM VEGETATION AND THE IMPLICATIONS FOR ATMOSPHERIC CHEMISTRY
    Fehsenfeld, Fred
    Calvert, Jack
    Fall, Ray
    Goldan, Paul
    Guenther, Alex
    Hewitt, C.
    Lamb, Brian
    Liu, Shaw
    Trainer, Michael
    Westberg, Hal
    Zimmerman, Pat
    [J]. GLOBAL BIOGEOCHEMICAL CYCLES, 1992, 6 (04) : 389 - 430
  • [10] Organic aerosol formation from the oxidation of biogenic hydrocarbons
    Griffin, RJ
    Cocker, DR
    Flagan, RC
    Seinfeld, JH
    [J]. JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1999, 104 (D3) : 3555 - 3567