Gas-phase products and secondary aerosol yields from the ozonolysis of ten different terpenes

被引:63
作者
Lee, A [1 ]
Goldstein, AH
Keywood, MD
Gao, S
Varutbangkul, V
Bahreini, R
Ng, NL
Flagan, RC
Seinfeld, JH
机构
[1] Univ Calif Berkeley, Dept Environm Sci Policy & Management, Berkeley, CA 94720 USA
[2] CALTECH, Dept Environm Sci & Engn, Pasadena, CA 91125 USA
[3] CALTECH, Dept Chem Engn, Pasadena, CA 91125 USA
关键词
D O I
10.1029/2005JD006437
中图分类号
P4 [大气科学(气象学)];
学科分类号
0706 ; 070601 ;
摘要
[1] The ozonolyses of six monoterpenes (alpha-pinene, beta-pinene, 3-carene, terpinolene, alpha-terpinene, and myrcene), two sesquiterpenes (alpha-humulene and beta-caryophyllene), and two oxygenated terpenes ( methyl chavicol and linalool) were conducted individually in Teflon chambers to examine the gas-phase oxidation product and secondary organic aerosol (SOA) yields from these reactions. Particle size distribution and number concentration were monitored and allowed for the calculation of the SOA yield from each experiment, which ranged from 1 to 54%. A proton transfer reaction mass spectrometer (PTR-MS) was used to monitor the evolution of gas-phase products, identified by their mass to charge ratio (m/z). Several gas-phase oxidation products, formaldehyde, acetaldehyde, formic acid, acetone, acetic acid, and nopinone, were identified and calibrated. Aerosol yields, and the yields of these identified and calibrated oxidation products, as well as many higher m/z oxidation products observed with the PTR-MS, varied significantly between the different parent terpene compounds. The sum of measured oxidation products in the gas and particle phase ranged from 33 to 77% of the carbon in the reacted terpenes, suggesting there are still unmeasured products from these reactions. The observations of the higher molecular weight oxidation product ions provide evidence of previously unreported compounds and their temporal evolution in the smog chamber from multistep oxidation processes. Many of the observed ions, including m/z 111 and 113, have also been observed in ambient air above a Ponderosa pine forest canopy, and our results confirm they are consistent with products from terpene + O-3 reactions. Many of these products are stable on the timescale of our experiments and can therefore be monitored in field campaigns as evidence for ozone oxidative chemistry.
引用
收藏
页数:18
相关论文
共 58 条
[11]   Emission of reactive terpene compounds from orange orchards and their removal by within-canopy processes [J].
Ciccioli, P ;
Brancaleoni, E ;
Frattoni, M ;
Di Palo, V ;
Valentini, R ;
Tirone, G ;
Seufert, G ;
Bertin, N ;
Hansen, U ;
Csiky, O ;
Lenz, R ;
Sharma, M .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1999, 104 (D7) :8077-8094
[12]   State-of-the-art chamber facility for studying atmospheric aerosol chemistry [J].
Cocker, DR ;
Flagan, RC ;
Seinfeld, JH .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2001, 35 (12) :2594-2601
[13]   Missing OH reactivity in a forest: Evidence for unknown reactive biogenic VOCs [J].
Di Carlo, P ;
Brune, WH ;
Martinez, M ;
Harder, H ;
Lesher, R ;
Ren, XR ;
Thornberry, T ;
Carroll, MA ;
Young, V ;
Shepson, PB ;
Riemer, D ;
Apel, E ;
Campbell, C .
SCIENCE, 2004, 304 (5671) :722-725
[14]   Contributions of organic peroxides to secondary aerosol formed from reactions of monoterpenes with O3 [J].
Docherty, KS ;
Wu, W ;
Lim, YB ;
Ziemann, PJ .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2005, 39 (11) :4049-4059
[15]   Effects of stabilized Criegee intermediate and OH radical scavengers on aerosol formation from reactions of β-pinene with O3 [J].
Docherty, KS ;
Ziemann, PJ .
AEROSOL SCIENCE AND TECHNOLOGY, 2003, 37 (11) :877-891
[16]  
Faloona I, 2001, J GEOPHYS RES-ATMOS, V106, P24315, DOI 10.1029/2000JD900691
[17]  
Fuentes JD, 2000, B AM METEOROL SOC, V81, P1537, DOI 10.1175/1520-0477(2000)081<1537:BHITAB>2.3.CO
[18]  
2
[19]   A review and synthesis of monoterpene speciation from forests in the United States [J].
Geron, C ;
Rasmussen, R ;
Arnts, RR ;
Guenther, A .
ATMOSPHERIC ENVIRONMENT, 2000, 34 (11) :1761-1781
[20]   Forest thinning experiment confirms ozone deposition to forest canopy is dominated by reaction with biogenic VOCs [J].
Goldstein, AH ;
McKay, M ;
Kurpius, MR ;
Schade, GW ;
Lee, A ;
Holzinger, R ;
Rasmussen, RA .
GEOPHYSICAL RESEARCH LETTERS, 2004, 31 (22) :1-4