Importance of secondary sources in the atmospheric budgets of formic and acetic acids

被引：263

作者：

Paulot, F. ^{[1
]}

Wunch, D. ^{[1
]}

Crounse, J. D. ^{[2
]}

Toon, G. C. ^{[3
]}

Millet, D. B. ^{[4
]}

DeCarlo, P. F. ^{[5
,12
]}

Vigouroux, C. ^{[6
]}

Deutscher, N. M. ^{[7
]}

Abad, G. Gonzalez ^{[8
]}

Notholt, J. ^{[9
]}

Warneke, T. ^{[9
]}

Hannigan, J. W. ^{[10
]}

Warneke, C. ^{[11
,12
]}

de Gouw, J. A. ^{[11
,12
]}

Dunlea, E. J. ^{[12
,13
]}

De Maziere, M. ^{[6
]}

Griffith, D. W. T. ^{[7
]}

Bernath, P. ^{[8
]}

Jimenez, J. L. ^{[12
,13
]}

Wennberg, P. O. ^{[1
]}

机构：

[1] CALTECH, Div Engn & Appl Sci, Pasadena, CA 91125 USA

[2] CALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USA

[3] CALTECH, Jet Prop Lab, Pasadena, CA USA

[4] Univ Minnesota, Dept Soil Water & Climate, St Paul, MN 55108 USA

[5] Univ Colorado, Dept Atmospher & Ocean Sci, Boulder, CO 80309 USA

[6] Belgian Inst Space Aeron, Brussels, Belgium

[7] Univ Wollongong, Sch Chem, Wollongong, NSW, Australia

[8] Univ York, Dept Chem, York YO10 5DD, N Yorkshire, England

[9] Inst Environm Phys, Bremen, Germany

[10] Natl Ctr Atmospher Res, Boulder, CO 80307 USA

[11] NOAA, Earth Syst Res Lab, Div Chem Sci, Boulder, CO USA

[12] Univ Colorado, Cooperat Inst Res Environm Sci, Boulder, CO 80309 USA

[13] Univ Colorado, Dept Chem & Biochem, Boulder, CO 80309 USA

来源：

ATMOSPHERIC CHEMISTRY AND PHYSICS | 2011年 / 11卷 / 05期

基金：

美国国家航空航天局; 美国国家科学基金会; 英国自然环境研究理事会;

关键词：

VOLATILE ORGANIC-COMPOUNDS; OH-INITIATED OXIDATION; KNUDSEN CELL REACTOR; GAS-PHASE REACTIONS; HETEROGENEOUS UPTAKE; TEMPERATURE-RANGE; CARBOXYLIC-ACIDS; TROPOSPHERIC CHEMISTRY; TRANSPACIFIC TRANSPORT; PHOTOCHEMICAL DATA;

D O I：

10.5194/acp-11-1989-2011

中图分类号：

X [环境科学、安全科学];

学科分类号：

08 ; 0830 ;

摘要：

We present a detailed budget of formic and acetic acids, two of the most abundant trace gases in the atmosphere. Our bottom-up estimate of the global source of formic and acetic acids are similar to 1200 and similar to 1400 Gmol yr(-1), dominated by photochemical oxidation of biogenic volatile organic compounds, in particular isoprene. Their sinks are dominated by wet and dry deposition. We use the GEOS-Chem chemical transport model to evaluate this budget against an extensive suite of measurements from ground, ship and satellite-based Fourier transform spectrometers, as well as from several aircraft campaigns over North America. The model captures the seasonality of formic and acetic acids well but generally underestimates their concentration, particularly in the Northern midlatitudes. We infer that the source of both carboxylic acids may be up to 50% greater than our estimate and report evidence for a long-lived missing secondary source of carboxylic acids that may be associated with the aging of organic aerosols. Vertical profiles of formic acid in the upper troposphere support a negative temperature dependence of the reaction between formic acid and the hydroxyl radical as suggested by several theoretical studies.

引用

页码：1989 / 2013

页数：25

共 156 条

[41] Evolution of Asian aerosols during transpacific transport in INTEX-B [J].