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

L. Hu, D. B. Millet, S. Y. Kim, K. C. Wells, T. J. Griffis, E. V. Fischer, D. Helmig, J. Hueber, A. J. Curtis

Research output: Contribution to journalArticlepeer-review

20 Scopus citations

Abstract

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 Combining double low line 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.

Original languageEnglish (US)
Pages (from-to)3379-3392
Number of pages14
JournalAtmospheric Chemistry and Physics
Volume13
Issue number6
DOIs
StatePublished - 2013

Fingerprint Dive into the research topics of 'North American acetone sources determined from tall tower measurements and inverse modeling'. Together they form a unique fingerprint.

Cite this