Budgets for nocturnal VOC oxidation by nitrate radicals aloft during the 2006 Texas Air Quality Study

Steven S. Brown, William P. Dubé, Jeff Peischl, Thomas B. Ryerson, Elliot L Atlas, Carsten Warneke, Joost A. De Gouw, Sacco Te Lintel Hekkert, Charles A. Brock, Frank Flocke, Michael Trainer, David D. Parrish, Frederick C. Feshenfeld, A. R. Ravishankara

Research output: Contribution to journalArticle

38 Citations (Scopus)

Abstract

Industrial emissions in Houston, Texas, and along the U.S. Gulf Coast are a large source of highly reactive anthropogenic volatile organic compounds (VOCs), principally alkenes, that affect air quality in that region. Nighttime oxidation by either O3 or NO3 removes these VOCs. This paper presents a regional analysis of nighttime P-3 flights during the 2006 Texas Air Quality Study (TexAQS) to quantify the loss rates and budgets for both NO3 and highly reactive VOC. Mixing ratios and production rates of NO3 were large, up to 400 parts per trillion by volume (pptv) and 1-2 parts per billion by volume (ppbv) per hour, respectively. Budgets for NO 3 show that it was lost primarily to reaction with VOCs, with the sum of anthropogenic VOCs (30-54%) and isoprene (10-50%) being the largest contributors. Indirect loss of NO3 to N2O5 hydrolysis was of lesser importance (14-28%) but was the least certain due to uncertainty in the aerosol uptake coefficient for N2O5. Reaction of NO3 with peroxy radicals was a small but nonzero contribution to NO3 loss but was also uncertain because there were no direct measurements of peroxy radicals. Net VOC oxidation rates were rapid (up to 2 ppbv VOC h-1 in industrial plumes) and were dominated by NO 3, which was 3-5 times more important as an oxidant than O 3. Plumes of high NO3 reactivity (i.e., short steady state lifetimes, on the order of 1 min) identified the presence of concentrated emissions of highly reactive VOCs from the Houston Ship Channel (HSC), which, depending on the particular VOC, may be efficiently oxidized during overnight transport.

Original languageEnglish (US)
Article numberD24305
JournalJournal of Geophysical Research C: Oceans
Volume116
Issue number24
DOIs
StatePublished - 2011

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Volatile Organic Compounds
air quality
volatile organic compounds
Air quality
budgets
Nitrates
volatile organic compound
nitrates
nitrate
oxidation
Oxidation
Houston (TX)
peroxy radical
plumes
plume
Industrial emissions
budget
industrial emission
gulfs
alkene

ASJC Scopus subject areas

  • Atmospheric Science
  • Geophysics
  • Earth and Planetary Sciences (miscellaneous)
  • Space and Planetary Science

Cite this

Budgets for nocturnal VOC oxidation by nitrate radicals aloft during the 2006 Texas Air Quality Study. / Brown, Steven S.; Dubé, William P.; Peischl, Jeff; Ryerson, Thomas B.; Atlas, Elliot L; Warneke, Carsten; De Gouw, Joost A.; Te Lintel Hekkert, Sacco; Brock, Charles A.; Flocke, Frank; Trainer, Michael; Parrish, David D.; Feshenfeld, Frederick C.; Ravishankara, A. R.

In: Journal of Geophysical Research C: Oceans, Vol. 116, No. 24, D24305, 2011.

Research output: Contribution to journalArticle

Brown, SS, Dubé, WP, Peischl, J, Ryerson, TB, Atlas, EL, Warneke, C, De Gouw, JA, Te Lintel Hekkert, S, Brock, CA, Flocke, F, Trainer, M, Parrish, DD, Feshenfeld, FC & Ravishankara, AR 2011, 'Budgets for nocturnal VOC oxidation by nitrate radicals aloft during the 2006 Texas Air Quality Study', Journal of Geophysical Research C: Oceans, vol. 116, no. 24, D24305. https://doi.org/10.1029/2011JD016544
Brown, Steven S. ; Dubé, William P. ; Peischl, Jeff ; Ryerson, Thomas B. ; Atlas, Elliot L ; Warneke, Carsten ; De Gouw, Joost A. ; Te Lintel Hekkert, Sacco ; Brock, Charles A. ; Flocke, Frank ; Trainer, Michael ; Parrish, David D. ; Feshenfeld, Frederick C. ; Ravishankara, A. R. / Budgets for nocturnal VOC oxidation by nitrate radicals aloft during the 2006 Texas Air Quality Study. In: Journal of Geophysical Research C: Oceans. 2011 ; Vol. 116, No. 24.
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abstract = "Industrial emissions in Houston, Texas, and along the U.S. Gulf Coast are a large source of highly reactive anthropogenic volatile organic compounds (VOCs), principally alkenes, that affect air quality in that region. Nighttime oxidation by either O3 or NO3 removes these VOCs. This paper presents a regional analysis of nighttime P-3 flights during the 2006 Texas Air Quality Study (TexAQS) to quantify the loss rates and budgets for both NO3 and highly reactive VOC. Mixing ratios and production rates of NO3 were large, up to 400 parts per trillion by volume (pptv) and 1-2 parts per billion by volume (ppbv) per hour, respectively. Budgets for NO 3 show that it was lost primarily to reaction with VOCs, with the sum of anthropogenic VOCs (30-54{\%}) and isoprene (10-50{\%}) being the largest contributors. Indirect loss of NO3 to N2O5 hydrolysis was of lesser importance (14-28{\%}) but was the least certain due to uncertainty in the aerosol uptake coefficient for N2O5. Reaction of NO3 with peroxy radicals was a small but nonzero contribution to NO3 loss but was also uncertain because there were no direct measurements of peroxy radicals. Net VOC oxidation rates were rapid (up to 2 ppbv VOC h-1 in industrial plumes) and were dominated by NO 3, which was 3-5 times more important as an oxidant than O 3. Plumes of high NO3 reactivity (i.e., short steady state lifetimes, on the order of 1 min) identified the presence of concentrated emissions of highly reactive VOCs from the Houston Ship Channel (HSC), which, depending on the particular VOC, may be efficiently oxidized during overnight transport.",
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AU - Atlas, Elliot L

AU - Warneke, Carsten

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AU - Te Lintel Hekkert, Sacco

AU - Brock, Charles A.

AU - Flocke, Frank

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