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.
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共 63 条
[1]   Gas-phase tropospheric chemistry of volatile organic compounds .1. Alkanes and alkenes [J].
Atkinson, R .
JOURNAL OF PHYSICAL AND CHEMICAL REFERENCE DATA, 1997, 26 (02) :215-290
[2]   Gas-phase tropospheric chemistry of biogenic volatile organic compounds: a review [J].
Atkinson, R ;
Arey, J .
ATMOSPHERIC ENVIRONMENT, 2003, 37 :S197-S219
[3]   Laboratory studies of particle nucleation:: Initial results for H2SO4, H2O, and NH3 vapors [J].
Ball, SM ;
Hanson, DR ;
Eisele, FL ;
McMurry, PH .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1999, 104 (D19) :23709-23718
[4]   Thermodynamics of the formation of atmospheric organic particulate matter by accretion reactions - 2. Dialdehydes, methylglyoxal, and diketones [J].
Barsanti, KC ;
Pankow, JF .
ATMOSPHERIC ENVIRONMENT, 2005, 39 (35) :6597-6607
[5]   Thermodynamics of the formation of atmospheric organic particulate matter by accretion reactions - Part 1: aldehydes and ketones [J].
Barsanti, KC ;
Pankow, JF .
ATMOSPHERIC ENVIRONMENT, 2004, 38 (26) :4371-4382
[6]   Rapid formation of sulfuric acid particles at near-atmospheric conditions [J].
Berndt, T ;
Böge, O ;
Stratmann, F ;
Heintzenberg, J ;
Kulmala, M .
SCIENCE, 2005, 307 (5710) :698-700
[7]   Atmospheric particle formation from the ozonolysis of alkenes in the presence of SO2 [J].
Berndt, T ;
Böge, O ;
Stratmann, F .
ATMOSPHERIC ENVIRONMENT, 2004, 38 (14) :2145-2153
[8]   Evaporation rates and vapor pressures of individual aerosol species formed in the atmospheric oxidation of α- and β-pinene [J].
Bilde, M ;
Pandis, SN .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2001, 35 (16) :3344-3349
[9]   New particle formation during α- and β-pinene oxidation by O3, OH and NO3, and the influence of water vapour:: particle size distribution studies [J].
Bonn, B ;
Moortgat, GK .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2002, 2 :183-196
[10]   Influence of water vapor on the process of new particle formation during monoterpene ozonolysis [J].
Bonn, B ;
Schuster, G ;
Moortgat, GK .
JOURNAL OF PHYSICAL CHEMISTRY A, 2002, 106 (12) :2869-2881