Acetone in the upper troposphere and lower stratosphere: Impact on trace gases and aerosols

Arnold, Frank; Bürger, V.; Droste-Fanke, B.; Grimm, F.; Krieger, Anna; Schneider, Johannes; Stilp, T.

doi:10.1029/97gl02974

Cited by 120 publications

(84 citation statements)

References 12 publications

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“…Acetone (CH 3 C(O)CH 3 ) is the simplest ketone and one of the most abundant volatile organic compounds (VOCs) in the atmosphere, with typical mixing ratios ranging from a few hundred parts per trillion (pptv) to several parts per billion (ppbv) or more (Chatfield et al, 1987;Singh et al, 1995;Arnold et al, 1997;Riemer et al, 1998;Goldstein and Schade, 2000;Karl et al, 2003;Lewis et al, 2005;Aiello and McLaren, 2009;Gao et al, 2013). It affects atmospheric chemistry as an important source of hydrogen oxide radicals (HO x = OH + HO 2 ) in the upper troposphere (Jaeglé et al, 1997(Jaeglé et al, , 2001McKeen et al, 1997;Wennberg et al, 1998;Folkins and Chatfield, 2000;Arnold et al, 2005), and as a precursor of peroxyacetyl nitrate (PAN, CH 3 C(O)OONO 2 ), which is a key reservoir for nitrogen oxides (NO x = NO Acetone is emitted by terrestrial vegetation as a by-product of plant metabolic processes, such as cyanogenesis and acetoacetate decarboxylation Jardine et al, 2010), and during plant decay (de Gouw et al, 1999;Warneke et al, 1999).…”

Section: Introductionmentioning

confidence: 99%

North American acetone sources determined from tall tower measurements and inverse modeling

Millet

Kim

et al. 2013

Atmos. Chem. Phys.

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We apply a full year of continuous atmospheric acetone measurements from the University of Minnesota tall tower Trace Gas Observatory (KCMP tall tower; 244 m a.g.l.), with a 0.5° × 0.667° GEOS-Chem nested grid simulation to develop quantitative new constraints on seasonal acetone sources over North America. Biogenic acetone emissions in the model are computed based on the MEGANv2.1 inventory. An inverse analysis of the tall tower observations implies a 37% underestimate of emissions from broadleaf trees, shrubs, and herbaceous plants, and an offsetting 40% overestimate of emissions from needleleaf trees plus secondary production from biogenic precursors. The overall result is a small (16%) model underestimate of the total primary + secondary biogenic acetone source in North America. Our analysis shows that North American primary + secondary anthropogenic acetone sources in the model (based on the EPA NEI 2005 inventory) are accurate to within approximately 20%. An optimized GEOS-Chem simulation incorporating the above findings captures 70% of the variance (R = 0.83) in the hourly measurements at the KCMP tall tower, with minimal bias. The resulting North American acetone source is 11 Tg a⁻¹, including both primary emissions (5.5 Tg a⁻¹) and secondary production (5.5 Tg a⁻¹), and with roughly equal contributions from anthropogenic and biogenic sources. The North American acetone source alone is nearly as large as the total continental volatile organic compound (VOC) source from fossil fuel combustion. Using our optimized source estimates as a baseline, we evaluate the sensitivity of atmospheric acetone and peroxyacetyl nitrate (PAN) to shifts in natural and anthropogenic acetone sources over North America. Increased biogenic acetone emissions due to surface warming are likely to provide a significant offset to any future decrease in anthropogenic acetone emissions, particularly during summer

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Section: Introductionmentioning

confidence: 99%

North American acetone sources determined from tall tower measurements and inverse modeling

Millet

Kim

et al. 2013

Atmos. Chem. Phys.

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“…Its background mixing ratio ranges between 200 ppt v in the southern hemisphere and 500 ppt v in the northern hemisphere (Singh et al, 1995). However, mixing ratios exceeding 2 ppb v in the free troposphere and 1 ppb v in the lower stratosphere have been observed (Wohlfrom et al, 1999;Arnold et al, 1997;Pöschl et al, 2001). The major anthropogenic sources of acetone in the atmosphere are direct emissions and secondary production by the oxidation of hydrocarbons (i.e.…”

Section: Introductionmentioning

confidence: 99%

On the relationship between acetone and carbon monoxide in different air masses

et al. 2003

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Abstract. Carbon monoxide and acetone measurements are presented for five aircraft measurement campaigns at midlatitudes, polar and tropical regions in the northern hemisphere. Throughout all campaigns, free tropospheric air masses, which were influenced by anthropogenic emissions, showed a similar linear relation between acetone and CO, with a slope of 21-25 ppt v acetone/ppb v CO. Measurements in the anthropogenically influenced marine boundary layer revealed a slope of 13-16 ppt v acetone/ppb v CO. The different slopes observed in the marine boundary layer and the free troposphere indicate that acetone is emitted by the ocean in relatively clean air masses and taken up by the ocean in polluted air masses. In the lowermost stratosphere, a good correlation between acetone and CO was observed as well, however, with a much smaller slope (∼5 ppt v acetone/ppb v CO) compared to the troposphere. This is caused by the longer photochemical lifetime of CO compared to acetone in the lower stratosphere, due to the increasing photolytic loss of acetone and the decreasing OH concentration with altitude. No significant correlation between acetone and CO was observed over the tropical rain forest due to the large direct and indirect biogenic emissions of acetone.The common slopes of the linear acetone-CO relation in various layers of the atmosphere, during five field experiments, makes them useful for model calculations. Often a single observation of the acetone-CO correlation, determined from stratospheric measurements, has been used in box model applications. This study shows that different slopes have to be considered for marine boundary layer, free tropospheric and stratospheric air masses, and that the acetone-CO relation cannot be used for air masses which are strongly influenced by biogenic emissions.Correspondence to: M. de Reus

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“…In the atmosphere the photolysis of acetone leads to the production of odd hydrogen (HOx) radicals. Particularly in the upper troposphere, acetone seems to be the most important precursor for HOx radicals [Arnold et al, 1997a;McKeen et al, 1997]. High concentrations of acetone have been observed in the upper troposphere over the North Atlantic Ocean [Arnold et al, 1997b], which presumably originated from industrial sources in North America.…”

Section: Introductionmentioning

confidence: 99%

Chemical characterization of pollution layers over the tropical Indian Ocean: Signatures of emissions from biomass and fossil fuel burning

et al. 2001

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On the other hand, high mixing ratios of sulfur dioxide (up to 1.5 ppb) and aerosol sulfate (up to 3 ppb) indicate the influence of fossil fuel burning. During most flights the contributions from these two sources were well mixed within the same air mass, suggesting that the sources on the ground are also close to each other. This is consistent with the assumption that biomass is mainly burnt as biofuel for domestic use in populated areas, where fossil fuel is also used. The ratios dX/dCO (X:acetone, acetonitrile, sulfur dioxide, potassium, or sulfate) measured during the flights indicate that most of the CO in the continental outflow is due to biomass or biofuel burning, whereas the majority of the aerosols results from fossil fuel burning.

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Acetone in the upper troposphere and lower stratosphere: Impact on trace gases and aerosols

Cited by 120 publications

References 12 publications

North American acetone sources determined from tall tower measurements and inverse modeling

North American acetone sources determined from tall tower measurements and inverse modeling

On the relationship between acetone and carbon monoxide in different air masses

Chemical characterization of pollution layers over the tropical Indian Ocean: Signatures of emissions from biomass and fossil fuel burning

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