Acetone in the atmosphere: Distribution, sources, and sinks

Singh, H. B.; O'Hara, D.; Herlth, D.; Sachse, W.; Blake, D. R.; Bradshaw, J. D.; Kanakidou, Maria; Crutzen, Paul J.

doi:10.1029/93jd00764

Cited by 366 publications

(299 citation statements)

References 32 publications

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“…The global budget of acetone has been apportioned (Jacob et al, 2002) to 1% primary anthropogenic emissions (from solvents and vehicle emissions), 35% primary biogenic emissions, 22% secondary production from propane oxidation, 5% biomass burning, with most of the rest emitted from oceans. Sinks are photolysis (65%), OH oxidation (25%), and 10% due to wet and dry deposition (Singh et al, 1994(Singh et al, , 1995. Deposition velocities of ∼0.17-0.36 cm s −1 have been reported for the ocean (Mao et al, 2006;Warneke and de Gouw, 2001).…”

Section: Ovocs -Acetone (Ch 3 Coch 3 M/z 59)mentioning

confidence: 99%

Long-term study of VOCs measured with PTR-MS at a rural site in New Hampshire with urban influences

et al. 2009

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Abstract.A long-term, high time-resolution volatile organic compound (VOC) data set from a ground site that experiences urban, rural, and marine influences in the Northeastern United States is presented. A proton-transfer-reaction mass spectrometer (PTR-MS) was used to quantify 15 VOCs: a marine tracer dimethyl sulfide (DMS), a biomass burning tracer acetonitrile, biogenic compounds (monoterpenes, isoprene), oxygenated VOCs (OVOCs: methyl vinyl ketone (MVK) plus methacrolein (MACR), methanol, acetone, methyl ethyl ketone (MEK), acetaldehyde, and acetic acid), and aromatic compounds (benzene, toluene, C 8 and C 9 aromatics). Time series, overall and seasonal medians, with 10th and 90th percentiles, seasonal mean diurnal profiles, and inter-annual comparisons of mean summer and winter diurnal profiles are shown. Methanol and acetone exhibit the highest overall median mixing ratios 1.44 and 1.02 ppbv, respectively. Comparing the mean diurnal profiles of less well understood compounds (e.g., MEK) with better known compounds (e.g., isoprene, monoterpenes, and MVK + MACR) that undergo various controls on their atmospheric mixing ratios provides insight into possible sources of the lesser known compounds. The constant diurnal value of ∼0.7 for the toluene:benzene ratio in winter, may possibly indicate the influence of wood-based heating systems in this region. Methanol exhibits an initial early morning release in summer unlike any other OVOC (or isoprene) and a dramatic late afternoon mixing ratio increase in spring. Although several of the OVOCs appear to have biogenic sources, differences in features observed between isoprene, methanol, acetone, acetaldehyde, and MEK suggest they are produced or emitted in unique ways.

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Section: Ovocs -Acetone (Ch 3 Coch 3 M/z 59)mentioning

confidence: 99%

Long-term study of VOCs measured with PTR-MS at a rural site in New Hampshire with urban influences

et al. 2009

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“…The first one is that acetone and formaldehyde, which are important for tropospheric chemistry, are produced by both reactions studied in this work. Acetone is involved in radical generation and NOx cycles of the background troposphere [Singh et al, 1994[Singh et al, , 1995 Reissel et al, 1999] suggests that altogether, terpene oxidation accounts for a significant fraction of the global acetone sources. In addition, because of their high reactivity, the oxidation of terpenes is a faster source of acetone and formaldehyde than the oxidation of many other compounds (in particular methane), so their impact on the chemistry at regional scale should be even more important than at global scale.…”

Section: Atmospheric Implicationsmentioning

confidence: 99%

Product study and mechanisms of the reactions of α‐pinene and of pinonaldehyde with OH radicals

Nozière¹,

Barnes²,

Becker³

1999

J. Geophys. Res.

177

192

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Abstract. The reactions of a-pinene and of its main oxidation product, pinonaldehyde (3-acetyl-2,2-dimethyl-cyclobutyl-ethanal), with OH radicals have been studied in the laboratory using Fourier transform infrared spectroscopy for real-time monitoring of the gas-phase chemical species and a Scanning Mobility Particle Sizer system (3071 A, TSI) for the study of the secondary aerosol formation. All gas-phase molar yields were quantified using calibrated reference of the pure compound, except for the nitrates products. The results were: for the a-pinene experiments in the presence of NOx, pinonaldehyde, (87 _ 20)%; total nitrates (18 _+ 9)%; formaldehyde, (23 +_ 9)%; acetone (9 _ 6)%; for the a-pinene experiments in the absence of NOx: pinonaldehyde, (37 _+ 7)%; formaldehyde, (8 _ 1)%; acetone, (7 _+ 2)%; for the pinonaldehyde experiments in the presence of NO, formaldehyde (152 _ 56)% and acetone (15 _+ 7)%. The aerosol measurements showed that the condensed products accounted for the missing carbon in the gas-phase balance. The partitioning of the products into the condensed phase was found to be potentially .significant under experimental conditions but less than 10% for initial a-pinene concentrations lower than 1013 molecule cm -3 and hence negligible under atmospheric conditions in the absence of aerosol seeds. On the basis of these results a comprehensive mechanism for the gas-phase reaction of a-pinene with OH in the presence of NOx has been proposed, including quantitative values for all the involved branching ratios. al., 1998], have been studied in laboratory. These studies have generally focused on the first oxidation step and only a few products have been quantified. Pinonaldehyde (3-acetyl-2,2-dimethyl-cyclobutyl-ethanal) was found to be the main product but has never been quantified on an absolute basis by means of a calibrated sample of the pure compound. The only other reaction product identified and quantified is acetone. Moreover, most of the studies have not taken into account the condensed products formed by these reactions, which may represent a significant fraction of the carbon balance under laboratory conditions as it will be shown in the present work. As a result, the understanding of the mechanism for the reaction of a-pinene with OH radicals remained difficult. Furthermore, secondary oxidation steps such as the further reactions of pinonaldehyde, which are important to assess the overall effect of a-pinene on tropospheric chemistry, have never been studied.In the present work, the mechanism of the reaction of a-pinene with OH radicals has been studied. Several gas-phase products such as pinonaldehyde, alkyl nitrates, acetone, and formaldehyde, have been identified and, except for the alkyInitrates, quantified using calibrated reference samples. This work also gives a first insight into the oxidation mechanism beyond the initial oxidation step by studying the reaction of pinonaldehyde with OH radicals. A quantification of the condensed products formed in these reactions has been performe...

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“…Acetone photolysis is a significant source of PAN, especially in the mid-and upper troposphere (Singh et al, 1994):…”

Section: Sensitivity Of Acetone and Pan To Shifts In North American Amentioning

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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Acetone in the atmosphere: Distribution, sources, and sinks

Cited by 366 publications

References 32 publications

Long-term study of VOCs measured with PTR-MS at a rural site in New Hampshire with urban influences

Long-term study of VOCs measured with PTR-MS at a rural site in New Hampshire with urban influences

Product study and mechanisms of the reactions of α‐pinene and of pinonaldehyde with OH radicals

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

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