Particle nucleation following the O3 and OH initiated oxidation of α-pinene and β-pinene between 278 and 320 K

被引:33
作者
Burkholder, James B.
Baynard, Tahllee
Ravishankara, A. R.
Lovejoy, Edward R.
机构
[1] Univ Colorado, Cooperat Inst Res Environm Sci, Boulder, CO 80309 USA
[2] Univ Colorado, Dept Chem & Biochem, Boulder, CO 80309 USA
关键词
D O I
10.1029/2006JD007783
中图分类号
P4 [大气科学(气象学)];
学科分类号
0706 ; 070601 ;
摘要
[1] Measurements of particle nucleation following the gas phase oxidation of alpha-pinene and beta-pinene are reported. Particle nucleation following ozonolysis and O-3 plus OH initiated monoterpene oxidation was measured in a 70-L Teflon bag reactor over the temperature range 278 to 320 K. Particle concentration temporal profiles were measured for a range of initial monoterpene and ozone concentrations using ultrafine condensation particle counters. Profiles were interpreted using a coupled gas phase chemistry and kinetic multicomponent nucleation model to determine the molar yield of the nucleating species in the ozonolysis experiments to be 1 x 10(-5) and 0.009, for alpha-pinene and beta-pinene, respectively. OH initiated oxidation was found to increase the nucleator yield for alpha-pinene, approximately a factor of three, but not for beta-pinene. The molar yield of condensable reaction products ( vapor pressure < 20 ppt at 296 K) was determined to be 0.06 for both alpha- pinene and beta-pinene and was independent of the oxidation source. Particle growth, which is determined by the condensable reaction products, was nearly temperature independent. Atmospheric box model calculations of nucleation and particle growth for alpha- pinene and beta-pinene oxidation under typical tropospheric conditions are presented and showed that ( 1) nucleation can be significant under favorable conditions, ( 2) nucleation is dominated by OH initiated oxidation, and ( 3) the partitioning of the condensable monoterpene oxidation products made a significant contribution to the growth of atmospheric aerosol and was capable of explaining the observed particle growth rates commonly observed in remote forests.
引用
收藏
页数:16
相关论文
共 63 条
[31]   Gaseous and particulate oxidation products analysis of a mixture of α-pinene plus β-pinene/O3/air in the absence of light and α-pinene plus β-pinene/NOx/air in the presence of natural sunlight [J].
Jaoui, M ;
Kamens, RM .
JOURNAL OF ATMOSPHERIC CHEMISTRY, 2003, 44 (03) :259-297
[32]  
Jenkin ME, 2000, ATMOS ENVIRON, V34, P2837
[33]   Impact of humidity on the ozone initiated oxidation of limonene, Δ3-carene, and α-pinene [J].
Jonsson, ÅM ;
Hallquist, M ;
Ljungström, E .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2006, 40 (01) :188-194
[34]   Identification of polymers as major components of atmospheric organic aerosols [J].
Kalberer, M ;
Paulsen, D ;
Sax, M ;
Steinbacher, M ;
Dommen, J ;
Prevot, ASH ;
Fisseha, R ;
Weingartner, E ;
Frankevich, V ;
Zenobi, R ;
Baltensperger, U .
SCIENCE, 2004, 303 (5664) :1659-1662
[35]   Formation and gas/particle partitioning of monoterpenes photo-oxidation products over forests [J].
Kavouras, IG ;
Mihalopoulos, N ;
Stephanou, EG .
GEOPHYSICAL RESEARCH LETTERS, 1999, 26 (01) :55-58
[36]   Secondary organic aerosol formation vs primary organic aerosol emission: In situ evidence for the chemical coupling between monoterpene acidic photooxidation products and new particle formation over forests [J].
Kavouras, IG ;
Mihalopoulos, N ;
Stephanou, EG .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 1999, 33 (07) :1028-1037
[37]   Formation of atmospheric particles from organic acids produced by forests [J].
Kavouras, IG ;
Mihalopoulos, N ;
Stephanou, EG .
NATURE, 1998, 395 (6703) :683-686
[38]   Secondary organic aerosol formation from the ozonolysis of cycloalkenes and related compounds [J].
Keywood, MD ;
Varutbangkul, V ;
Bahreini, R ;
Flagan, RC ;
Seinfeld, JH .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2004, 38 (15) :4157-4164
[39]   Secondary organic aerosol formation from cyclohexene ozonolysis: Effect of OH scavenger and the role of radical chemistry [J].
Keywood, MD ;
Kroll, JH ;
Varutbangkul, V ;
Bahreini, R ;
Flagan, RC ;
Seinfeld, JH .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2004, 38 (12) :3343-3350
[40]   Rate constants for the gas-phase reactions of ozone with isoprene, α- and β-pinene, and limonene as a function of temperature [J].
Khamaganov, VG ;
Hites, RA .
JOURNAL OF PHYSICAL CHEMISTRY A, 2001, 105 (05) :815-822