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Active and widespread halogen chemistry in the tropical and subtropical free troposphere.
Wang, Siyuan; Schmidt, Johan A; Baidar, Sunil; Coburn, Sean; Dix, Barbara; Koenig, Theodore K; Apel, Eric; Bowdalo, Dene; Campos, Teresa L; Eloranta, Ed; Evans, Mathew J; DiGangi, Joshua P; Zondlo, Mark A; Gao, Ru-Shan; Haggerty, Julie A; Hall, Samuel R; Hornbrook, Rebecca S; Jacob, Daniel; Morley, Bruce; Pierce, Bradley; Reeves, Mike; Romashkin, Pavel; Ter Schure, Arnout; Volkamer, Rainer.
Afiliación
  • Wang S; Department of Chemistry & Biochemistry, University of Colorado, Boulder, CO 80309-0215; Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO 80309-0216;
  • Schmidt JA; School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138; Department of Chemistry, University of Copenhagen, 2100 Copenhagen, Denmark;
  • Baidar S; Department of Chemistry & Biochemistry, University of Colorado, Boulder, CO 80309-0215; Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO 80309-0216;
  • Coburn S; Department of Chemistry & Biochemistry, University of Colorado, Boulder, CO 80309-0215; Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO 80309-0216;
  • Dix B; Department of Chemistry & Biochemistry, University of Colorado, Boulder, CO 80309-0215;
  • Koenig TK; Department of Chemistry & Biochemistry, University of Colorado, Boulder, CO 80309-0215; Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO 80309-0216;
  • Apel E; Earth System Laboratory, Atmospheric Chemistry Division, National Center for Atmospheric Research, Boulder, CO 80307;
  • Bowdalo D; Department of Chemistry, University of York, York YO10 5DD, United Kingdom;
  • Campos TL; Earth System Laboratory, Atmospheric Chemistry Division, National Center for Atmospheric Research, Boulder, CO 80307;
  • Eloranta E; Space Science and Engineering Center, University of Wisconsin, Madison, WI 02138;
  • Evans MJ; Department of Chemistry, University of York, York YO10 5DD, United Kingdom;
  • DiGangi JP; Department of Civil and Environmental Engineering, Princeton University, Princeton, NJ 08544;
  • Zondlo MA; Department of Civil and Environmental Engineering, Princeton University, Princeton, NJ 08544;
  • Gao RS; Earth System Research Laboratory, Chemical Science Division, National Oceanic and Atmospheric Administration, Boulder, CO 80305;
  • Haggerty JA; Earth Observing Laboratory, Research Aviation Facility, National Center for Atmospheric Research, Boulder, CO 80307;
  • Hall SR; Earth System Laboratory, Atmospheric Chemistry Division, National Center for Atmospheric Research, Boulder, CO 80307;
  • Hornbrook RS; Earth System Laboratory, Atmospheric Chemistry Division, National Center for Atmospheric Research, Boulder, CO 80307;
  • Jacob D; School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138;
  • Morley B; Earth Observing Laboratory, Research Aviation Facility, National Center for Atmospheric Research, Boulder, CO 80307;
  • Pierce B; The National Environmental Satellite, Data, and Information Service, National Oceanic and Atmospheric Administration, Madison, WI 53706;
  • Reeves M; Earth Observing Laboratory, Research Aviation Facility, National Center for Atmospheric Research, Boulder, CO 80307;
  • Romashkin P; Earth Observing Laboratory, Research Aviation Facility, National Center for Atmospheric Research, Boulder, CO 80307;
  • Ter Schure A; Electric Power Research Institute, Palo Alto, CA 94304.
  • Volkamer R; Department of Chemistry & Biochemistry, University of Colorado, Boulder, CO 80309-0215; Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO 80309-0216; rainer.volkamer@colorado.edu.
Proc Natl Acad Sci U S A ; 112(30): 9281-6, 2015 Jul 28.
Article en En | MEDLINE | ID: mdl-26124148
Halogens in the troposphere are increasingly recognized as playing an important role for atmospheric chemistry, and possibly climate. Bromine and iodine react catalytically to destroy ozone (O3), oxidize mercury, and modify oxidative capacity that is relevant for the lifetime of greenhouse gases. Most of the tropospheric O3 and methane (CH4) loss occurs at tropical latitudes. Here we report simultaneous measurements of vertical profiles of bromine oxide (BrO) and iodine oxide (IO) in the tropical and subtropical free troposphere (10 °N to 40 °S), and show that these halogens are responsible for 34% of the column-integrated loss of tropospheric O3. The observed BrO concentrations increase strongly with altitude (∼ 3.4 pptv at 13.5 km), and are 2-4 times higher than predicted in the tropical free troposphere. BrO resembles model predictions more closely in stratospheric air. The largest model low bias is observed in the lower tropical transition layer (TTL) over the tropical eastern Pacific Ocean, and may reflect a missing inorganic bromine source supplying an additional 2.5-6.4 pptv total inorganic bromine (Bry), or model overestimated Bry wet scavenging. Our results highlight the importance of heterogeneous chemistry on ice clouds, and imply an additional Bry source from the debromination of sea salt residue in the lower TTL. The observed levels of bromine oxidize mercury up to 3.5 times faster than models predict, possibly increasing mercury deposition to the ocean. The halogen-catalyzed loss of tropospheric O3 needs to be considered when estimating past and future ozone radiative effects.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Tipo de estudio: Prognostic_studies Idioma: En Revista: Proc Natl Acad Sci U S A Año: 2015 Tipo del documento: Article Pais de publicación: Estados Unidos
Texto completo
Añadir a Mi BVS
Imprimir
XML
PubMed Links
Buscar en Google

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Tipo de estudio: Prognostic_studies Idioma: En Revista: Proc Natl Acad Sci U S A Año: 2015 Tipo del documento: Article Pais de publicación: Estados Unidos