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Nitrogen Oxide Chemistry in an Urban Plume: Investigation of the Chemistry of Peroxy and Multifunctional Organic Nitrates with a Lagrangian Model : Volume 9, Issue 6 (16/12/2009)

By Pérez, I. M.

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Book Id: WPLBN0003993208
Format Type: PDF Article :
File Size: Pages 67
Reproduction Date: 2015

Title: Nitrogen Oxide Chemistry in an Urban Plume: Investigation of the Chemistry of Peroxy and Multifunctional Organic Nitrates with a Lagrangian Model : Volume 9, Issue 6 (16/12/2009)  
Author: Pérez, I. M.
Volume: Vol. 9, Issue 6
Language: English
Subject: Science, Atmospheric, Chemistry
Collections: Periodicals: Journal and Magazine Collection, Copernicus GmbH
Historic
Publication Date:
2009
Publisher: Copernicus Gmbh, Göttingen, Germany
Member Page: copernicus

Citation

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Cohen, R. C., Lafranchi, B. W., & Pérez, I. M. (2009). Nitrogen Oxide Chemistry in an Urban Plume: Investigation of the Chemistry of Peroxy and Multifunctional Organic Nitrates with a Lagrangian Model : Volume 9, Issue 6 (16/12/2009). Retrieved from http://www.ebooklibrary.org/


Description
Description: Dept. of Chemistry, University of California Berkeley, Berkeley, CA, USA. Air quality in the outflow from urban centers affects millions of people, as well as, natural and managed ecosystems downwind. In locations where there are large sources of biogenic VOCs downwind of urban centers, the outflow is characterized by a high VOC reactivity due to biogenic emissions and low NOx. However most field and chamber studies have focused on limiting cases of high NOx or of near zero NOx. Recent measurements of a wide suite of VOCs, O3 and meteorological parameters at several locations within the Sacramento urban plume have provided a detailed benchmark for testing our understanding of chemistry in a plume transitioning from high NOx to low NOx and high VOC reactivity. As an additional simplification, the strong mountain valley circulation in the region makes this urban plume a physical realization of a nearly idealized Lagrangian plume. Here, we describe a model of this plume. We use a Lagrangian model representing chemistry based on the Master Chemical Mechanism (MCM) v3.1 along with mixing and deposition. We discuss the effects of entrainment of background air, the branching ratio for the production of isoprene nitrates and the effects of soil NOx emissions on the composition of the evolving plume. The model predicts that after 2–3 h of chemical processing only 45% of the peroxynitrates (ΣPNs) are PAN and that most (69%) RONO2 are secondary alkyl nitrate products of the reaction of OH with RONO2. We find the model is more consistent with the observations if: a) the yield of ΣPNs from large and multi-functional aldehydes is close to zero; and b) the reaction between OH and RONO2 produces multifunctional nitrates as opposed to either HNO3 or NO2 as is typical in most currently adopted reaction mechanisms. Model results also show that adding NOx emissions throughout the transect increases the available NOx in the downwind regions, but modeled ozone concentrations were little affected by the increased NOx.

Summary
Nitrogen oxide chemistry in an urban plume: investigation of the chemistry of peroxy and multifunctional organic nitrates with a Lagrangian model

Excerpt
Atkinson, R. and Arey, J.: Gas-phase tropospheric chemistry of biogenic volatile organic compounds: a review, Atmos. Environ., 37, S197–S219, 2003.; Baker, B., Guenther, A., Greenberg, J., Goldstein, A., and Fall, R.: Canopy fluxes of 2-methyl-3-buten-2-ol over a ponderosa pine forest by relaxed eddy accumulation: field data and model comparison, J. Geophys. Res., 104, 26107–26114, 1999.; Bloss, C., Wagner, V., Bonzanini, A., Jenkin, M. E., Wirtz, K., Martin-Reviejo, M., and Pilling, M. J.: Evaluation of detailed aromatic mechanisms (MCMv3 and MCMv3.1) against environmental chamber data, Atmos. Chem. Phys., 5, 623–639, 2005a.; Bloss, C., Wagner, V., Jenkin, M. E., Volkamer, R., Bloss, W. J., Lee, J. D., Heard, D. E., Wirtz, K., Martin-Reviejo, M., Rea, G., Wenger, J. C., and Pilling, M. J.: Development of a detailed chemical mechanism (MCMv3.1) for the atmospheric oxidation of aromatic hydrocarbons, Atmos. Chem. Phys., 5, 641–664, 2005b.; Bytnerowicz, A. and Fenn, M. E.: Nitrogen deposition in California forests: a review, Environ. Pollut., 92, 127–146, 1996.; CARB: California Air Resources Board Air Quality Database, http://www.arb.ca.gov/aqd/aqdcd/aqdcd.htm, 2009.; Carrasco, N., Doussin, J. F., Picquet-Varrault, B., and Carlier, P.: Tropospheric degradation of 2-hydroxy-2-methylpropanal, a photo-oxidation product of 2-methyl-3-buten-2-ol: kinetic and mechanistic study of its photolysis and its reaction with OH radicals, Atmos. Environ., 40, 2011–2019, 2006.; Carroll, J. J. and Dixon, A. J.: Regional scale transport over complex terrain, a case study: tracing the Sacramento plume in the Sierra Nevada of California, Atmos. Environ., 36, 3745–3758, 2002.; Haagen-Smit, A. J.: Chemistry and physiology of Los Angeles smog, Ind. Eng. Chem., 44, 1342–1346, 1952.; Chen, X., Hulbert, D., and Shepson, P.: Measurement of the organic nitrate yield from OH reaction with isoprene, J. Geophys. Res., 103, 25563–25568, 1998.; Chuong, B. and Stevens, P. S.: Measurements of the kinetics of the OH-initiated oxidation of isoprene, J. Geophys. Res., 107, 4162, doi:10.1029/2001JD000865, 2002.; Cleary, P. A., Murphy, J. G., Wooldridge, P. J., Day, D. A., Millet, D. B., McKay, M., Goldstein, A. H., and Cohen, R. C.: Observations of total alkyl nitrates within the Sacramento Urban Plume, Atmos. Chem. Phys. Discuss., 5, 4801–4843, 2005.; Cleary, P. A., Wooldridge, P. J., Millet, D. B., McKay, M., Goldstein, A. H., and Cohen, R. C.: Observations of total peroxy nitrates and aldehydes: measurement interpretation and inference of OH radical concentrations, Atmos. Chem. Phys., 7, 1947–1960, 2007.; Day, D. A., Wooldridge, P. J., Dillon, M. B., Thornton, J. A., and Cohen, R. C.: A thermal dissociation laser-induced fluorescence instrument for in situ detection of NO2, peroxy nitrates, alkyl nitrates, and HNO3, J. Geophys. Res., 107, 4046, doi:10.1029/2001JD000779, 2002.; Day, D. A., Dillon, M. B., Wooldridge, P. J., Thor

 

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