Atmos. Chem. Phys. Discuss., 13, 28225-28278, 2013
www.atmos-chem-phys-discuss.net/13/28225/2013/
doi:10.5194/acpd-13-28225-2013
© Author(s) 2013. This work is distributed
under the Creative Commons Attribution 3.0 License.
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This discussion paper has been under review for the journal Atmospheric Chemistry and Physics (ACP). Please refer to the corresponding final paper in ACP.
Emissions of organic carbon and methane from petroleum and dairy operations in California's San Joaquin Valley
D. R. Gentner1, T. B. Ford2, A. Guha3, K. Boulanger1,*, J. Brioude4,5, W. M. Angevine4,5, J. A. de Gouw4,5, C. Warneke4,5, J. B. Gilman4,5, T. B. Ryerson4,5, J. Peischl4,5, S. Meinardi6, D. R. Blake6, E. Atlas7, W. A. Lonneman8, T. E. Kleindienst8, M. R. Beaver9,**, J. M. St. Clair9, P. O. Wennberg9, T. C. VandenBoer10,***, M. Z. Markovic10,****, J. G. Murphy10, R. A. Harley1, and A. H. Goldstein1,3
1Department of Civil and Environmental Engineering, University of California, Berkeley, CA 94720, USA
2Department of Chemistry, University of California, Berkeley, CA, 94720, USA
3Department of Environmental Science, Policy and Management, University of California, Berkeley, CA, 94720, USA
4Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO 80309, USA
5Chemical Sciences Division, Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO 80305, USA
6Department of Chemistry, University of California, Irvine, CA, 92697, USA
7Rosenstiel School of Marine and Atmospheric Science, University of Miami, Miami, FL, 33149, USA
8National Exposure Research Laboratory, Environmental Protection Agency, Research Triangle Park, NC, USA
9California Institute of Technology, Pasadena, CA, USA
10Department of Chemistry, University of Toronto, Toronto, ON, CA
*now at: Department of Civil and Environmental Engineering, Massachusetts Institute of Technology, Cambridge, MA 02139, USA
**now at: National Exposure Research Laboratory, Environmental Protection Agency, Research Triangle Park, NC, USA
***now at: Department of Chemistry, Memorial University of Newfoundland, NL, CA
****now at: Chemical Sciences Division, Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO 80305, USA; Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO 80309, USA

Abstract. Petroleum and dairy operations are prominent sources of gas-phase organic compounds in California's San Joaquin Valley. Ground site measurements in Bakersfield and aircraft measurements of reactive gas-phase organic compounds were made in this region as part of the CalNex (California Research at the Nexus of Air Quality and Climate Change) project to determine the sources contributing to regional gas-phase organic carbon emissions. Using a combination of near-source and downwind data, we assess the composition and magnitude of emissions from these prominent sources that are relatively understudied compared to motor vehicles We also developed a statistical modeling method with the FLEXPART-WRF transport and meteorological model using ground-based data to assess the spatial distribution of emissions in the San Joaquin Valley. We present evidence for large sources of paraffinic hydrocarbons from petroleum extraction/processing operations and oxygenated compounds from dairy (and other cattle) operations. In addition to the small straight-chain alkanes typically associated with petroleum operations, we observed a wide range of branched and cyclic alkanes that have limited previous in situ measurements or characterization in emissions from petroleum operations. Observed dairy emissions were dominated by ethanol, methanol, and acetic acid, and methane. Dairy operations were responsible for the vast majority of methane emissions in the San Joaquin Valley; observations of methane were well-correlated with non-vehicular ethanol, and multiple assessments of the spatial distribution of emissions in the San Joaquin Valley highlight the dominance of dairy operations for methane emissions. The good agreement of the observed petroleum operations source profile with the measured composition of non-methane hydrocarbons in unrefined natural gas associated with crude oil suggests a fugitive emissions pathway during petroleum extraction, storage, or processing with negligible coincident methane emissions Aircraft observations of emission hotspots from operations at oil wells and dairies are consistent with the statistical source footprint determined via transport modeling and ground-based data. At Bakersfield, petroleum and dairy operations each comprised 22–23% of anthropogenic non-methane organic carbon and were each responsible for ~12% of potential precursors to ozone, but their direct impacts as potential SOA precursors were estimated to be minor. A comparison with the California Air Resources Board emission inventory supports the current relative emission rates of reactive organic gases from these sources in the region.

Citation: Gentner, D. R., Ford, T. B., Guha, A., Boulanger, K., Brioude, J., Angevine, W. M., de Gouw, J. A., Warneke, C., Gilman, J. B., Ryerson, T. B., Peischl, J., Meinardi, S., Blake, D. R., Atlas, E., Lonneman, W. A., Kleindienst, T. E., Beaver, M. R., Clair, J. M. St., Wennberg, P. O., VandenBoer, T. C., Markovic, M. Z., Murphy, J. G., Harley, R. A., and Goldstein, A. H.: Emissions of organic carbon and methane from petroleum and dairy operations in California's San Joaquin Valley, Atmos. Chem. Phys. Discuss., 13, 28225-28278, doi:10.5194/acpd-13-28225-2013, 2013.
 
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