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

F. Paulot; D. Wunch; J. D. Crounse; G. C. Toon; D. B. Millet; P. F. DeCarlo; C. Vigouroux; N. M. Deutscher; G. Gonzalez Abad; J. Notholt; T. Warneke; J. W. Hannigan; C. Warneke; J. A. de Gouw; E. J. Dunlea; M. De Maziere; D. W. T. Griffith; P. Bernath; J. L. Jimenez; P. O. Wennberg

doi:10.5194/acp-11-1989-2011

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

F. Paulot, D. Wunch, J. D. Crounse, G. C. Toon, D. B. Millet, P. F. DeCarlo, C. Vigouroux, N. M. Deutscher, G. Gonzalez Abad, J. Notholt, T. Warneke, J. W. Hannigan, C. Warneke, J. A. de Gouw, E. J. Dunlea, M. De Maziere, D. W. T. Griffith, P. Bernath, J. L. Jimenez, P. O. Wennberg

Chemistry

Research output: Contribution to journal › Article › peer-review

Abstract

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.

Original language	English
Pages (from-to)	1989-2013
Number of pages	25
Journal	Atmospheric Chemistry and Physics
Volume	11
Issue number	5
DOIs	https://doi.org/10.5194/acp-11-1989-2011
Publication status	Published - 2011

Keywords

VOLATILE ORGANIC-COMPOUNDS
GAS-PHASE OH
IONIZATION MASS-SPECTROMETRY
INFRARED-SPECTROSCOPY AFTIR
KNUDSEN CELL REACTOR
HETEROGENEOUS UPTAKE
INITIATED OXIDATION
HYDROXYL RADICALS
TEMPERATURE-RANGE
CARBOXYLIC-ACIDS

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10.5194/acp-11-1989-2011

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Paulot, F., Wunch, D., Crounse, J. D., Toon, G. C., Millet, D. B., DeCarlo, P. F., Vigouroux, C., Deutscher, N. M., Abad, G. G., Notholt, J., Warneke, T., Hannigan, J. W., Warneke, C., de Gouw, J. A., Dunlea, E. J., De Maziere, M., Griffith, D. W. T., Bernath, P., Jimenez, J. L., & Wennberg, P. O. (2011). Importance of secondary sources in the atmospheric budgets of formic and acetic acids. Atmospheric Chemistry and Physics, 11(5), 1989-2013. https://doi.org/10.5194/acp-11-1989-2011

@article{fc3b774ac9904c99809aa012602f1913,

title = "Importance of secondary sources in the atmospheric budgets of formic and acetic acids",

abstract = "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.",

keywords = "VOLATILE ORGANIC-COMPOUNDS, GAS-PHASE OH, IONIZATION MASS-SPECTROMETRY, INFRARED-SPECTROSCOPY AFTIR, KNUDSEN CELL REACTOR, HETEROGENEOUS UPTAKE, INITIATED OXIDATION, HYDROXYL RADICALS, TEMPERATURE-RANGE, CARBOXYLIC-ACIDS",

author = "F. Paulot and D. Wunch and Crounse, {J. D.} and Toon, {G. C.} and Millet, {D. B.} and DeCarlo, {P. F.} and C. Vigouroux and Deutscher, {N. M.} and Abad, {G. Gonzalez} and J. Notholt and T. Warneke and Hannigan, {J. W.} and C. Warneke and {de Gouw}, {J. A.} and Dunlea, {E. J.} and {De Maziere}, M. and Griffith, {D. W. T.} and P. Bernath and Jimenez, {J. L.} and Wennberg, {P. O.}",

year = "2011",

doi = "10.5194/acp-11-1989-2011",

language = "English",

volume = "11",

pages = "1989--2013",

journal = "Atmospheric Chemistry and Physics",

issn = "1680-7316",

publisher = "Copernicus Publications",

number = "5",

}

Paulot, F, Wunch, D, Crounse, JD, Toon, GC, Millet, DB, DeCarlo, PF, Vigouroux, C, Deutscher, NM, Abad, GG, Notholt, J, Warneke, T, Hannigan, JW, Warneke, C, de Gouw, JA, Dunlea, EJ, De Maziere, M, Griffith, DWT, Bernath, P, Jimenez, JL & Wennberg, PO 2011, 'Importance of secondary sources in the atmospheric budgets of formic and acetic acids', Atmospheric Chemistry and Physics, vol. 11, no. 5, pp. 1989-2013. https://doi.org/10.5194/acp-11-1989-2011

TY - JOUR

T1 - Importance of secondary sources in the atmospheric budgets of formic and acetic acids

AU - Paulot, F.

AU - Wunch, D.

AU - Crounse, J. D.

AU - Toon, G. C.

AU - Millet, D. B.

AU - DeCarlo, P. F.

AU - Vigouroux, C.

AU - Deutscher, N. M.

AU - Abad, G. Gonzalez

AU - Notholt, J.

AU - Warneke, T.

AU - Hannigan, J. W.

AU - Warneke, C.

AU - de Gouw, J. A.

AU - Dunlea, E. J.

AU - De Maziere, M.

AU - Griffith, D. W. T.

AU - Bernath, P.

AU - Jimenez, J. L.

AU - Wennberg, P. O.

PY - 2011

Y1 - 2011

N2 - 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.

AB - 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.

KW - VOLATILE ORGANIC-COMPOUNDS

KW - GAS-PHASE OH

KW - IONIZATION MASS-SPECTROMETRY

KW - INFRARED-SPECTROSCOPY AFTIR

KW - KNUDSEN CELL REACTOR

KW - HETEROGENEOUS UPTAKE

KW - INITIATED OXIDATION

KW - HYDROXYL RADICALS

KW - TEMPERATURE-RANGE

KW - CARBOXYLIC-ACIDS

UR - http://www.scopus.com/inward/record.url?scp=79952342467&partnerID=8YFLogxK

U2 - 10.5194/acp-11-1989-2011

DO - 10.5194/acp-11-1989-2011

M3 - Article

SN - 1680-7316

VL - 11

SP - 1989

EP - 2013

JO - Atmospheric Chemistry and Physics

JF - Atmospheric Chemistry and Physics

IS - 5

ER -

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

Abstract

Keywords

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