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Organic nitrate chemistry and its implications for nitrogen budgets in an isoprene- and monoterpene-rich atmosphere: constraints from aircraft (SEAC4RS) and ground-based (SOAS) observations in the Southeast US.
Fisher, J A; Jacob, D J; Travis, K R; Kim, P S; Marais, E A; Miller, C Chan; Yu, K; Zhu, L; Yantosca, R M; Sulprizio, M P; Mao, J; Wennberg, P O; Crounse, J D; Teng, A P; Nguyen, T B; St Clair, J M; Cohen, R C; Romer, P; Nault, B A; Wooldridge, P J; Jimenez, J L; Campuzano-Jost, P; Day, D A; Hu, W; Shepson, P B; Xiong, F; Blake, D R; Goldstein, A H; Misztal, P K; Hanisco, T F; Wolfe, G M; Ryerson, T B; Wisthaler, A; Mikoviny, T.
Afiliación
  • Fisher JA; Centre for Atmospheric Chemistry, School of Chemistry, University of Wollongong, Wollongong, NSW, Australia.
  • Jacob DJ; School of Earth and Environmental Sciences, University of Wollongong, Wollongong, NSW, Australia.
  • Travis KR; Harvard John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA.
  • Kim PS; Department of Earth and Planetary Sciences, Harvard University, Cambridge, MA, USA.
  • Marais EA; Harvard John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA.
  • Miller CC; Department of Earth and Planetary Sciences, Harvard University, Cambridge, MA, USA.
  • Yu K; Harvard John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA.
  • Zhu L; Department of Earth and Planetary Sciences, Harvard University, Cambridge, MA, USA.
  • Yantosca RM; Harvard John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA.
  • Sulprizio MP; Harvard John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA.
  • Mao J; Harvard John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA.
  • Wennberg PO; Harvard John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA.
  • Crounse JD; Program in Atmospheric and Oceanic Sciences, Princeton University, Princeton, NJ, USA.
  • Teng AP; Geophysical Fluid Dynamics Laboratory/National Oceanic and Atmospheric Administration, Princeton, NJ, USA.
  • Nguyen TB; Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA, USA.
  • St Clair JM; Division of Engineering and Applied Science, California Institute of Technology, Pasadena, CA, USA.
  • Cohen RC; Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA, USA.
  • Romer P; Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA, USA.
  • Nault BA; Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA, USA.
  • Wooldridge PJ; Now at Department of Environmental Toxicology, University of California at Davis, Davis, CA, USA.
  • Jimenez JL; Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA, USA.
  • Campuzano-Jost P; Now at Atmospheric Chemistry and Dynamics Laboratory, NASA Goddard Space Flight Center, Greenbelt, MD, USA and Joint Center for Earth Systems Technology, University of Maryland Baltimore County, Baltimore, MD, USA.
  • Day DA; Department of Chemistry, University of California at Berkeley, Berkeley, CA, USA.
  • Hu W; Department of Earth and Planetary Science, University of California at Berkeley, Berkeley, CA, USA.
  • Shepson PB; Department of Chemistry, University of California at Berkeley, Berkeley, CA, USA.
  • Xiong F; Department of Earth and Planetary Science, University of California at Berkeley, Berkeley, CA, USA.
  • Blake DR; Now at Department of Chemistry and Biochemistry and Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA.
  • Goldstein AH; Department of Chemistry, University of California at Berkeley, Berkeley, CA, USA.
  • Misztal PK; Department of Chemistry and Biochemistry, University of Colorado, Boulder, CO, USA.
  • Hanisco TF; Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA.
  • Wolfe GM; Department of Chemistry and Biochemistry, University of Colorado, Boulder, CO, USA.
  • Ryerson TB; Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA.
  • Wisthaler A; Department of Chemistry and Biochemistry, University of Colorado, Boulder, CO, USA.
  • Mikoviny T; Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA.
Atmos Chem Phys ; 16(9): 5969-5991, 2016.
Article en En | MEDLINE | ID: mdl-29681921
Formation of organic nitrates (RONO2) during oxidation of biogenic volatile organic compounds (BVOCs: isoprene, monoterpenes) is a significant loss pathway for atmospheric nitrogen oxide radicals (NOx), but the chemistry of RONO2 formation and degradation remains uncertain. Here we implement a new BVOC oxidation mechanism (including updated isoprene chemistry, new monoterpene chemistry, and particle uptake of RONO2) in the GEOS-Chem global chemical transport model with ∼25 × 25 km2 resolution over North America. We evaluate the model using aircraft (SEAC4RS) and ground-based (SOAS) observations of NOx, BVOCs, and RONO2 from the Southeast US in summer 2013. The updated simulation successfully reproduces the concentrations of individual gas- and particle-phase RONO2 species measured during the campaigns. Gas-phase isoprene nitrates account for 25-50% of observed RONO2 in surface air, and we find that another 10% is contributed by gas-phase monoterpene nitrates. Observations in the free troposphere show an important contribution from long-lived nitrates derived from anthropogenic VOCs. During both campaigns, at least 10% of observed boundary layer RONO2 were in the particle phase. We find that aerosol uptake followed by hydrolysis to HNO3 accounts for 60% of simulated gas-phase RONO2 loss in the boundary layer. Other losses are 20% by photolysis to recycle NOx and 15% by dry deposition. RONO2 production accounts for 20% of the net regional NOx sink in the Southeast US in summer, limited by the spatial segregation between BVOC and NOx emissions. This segregation implies that RONO2 production will remain a minor sink for NOx in the Southeast US in the future even as NOx emissions continue to decline.
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Texto completo: 1 Banco de datos: MEDLINE Tipo de estudio: Health_economic_evaluation Idioma: En Revista: Atmos Chem Phys Año: 2016 Tipo del documento: Article País de afiliación: Australia
Texto completo
Imprimir
XML
PubMed Links
Buscar en Google

Texto completo: 1 Banco de datos: MEDLINE Tipo de estudio: Health_economic_evaluation Idioma: En Revista: Atmos Chem Phys Año: 2016 Tipo del documento: Article País de afiliación: Australia