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High concentrations and photochemical fate of oxygenated hydrocarbons in the global troposphere

Abstract

Oxygenated species in the atmosphere are important sources of free radicals and are intricately linked with the fate of nitrogen oxides (NO{sub x}), which are themselves necessary for tropospheric ozone formation. With the exception of formaldehyde, oxygenated hydrocarbons have rarely been measured in the free troposphere. Here we report airborne measurements indicating the presence of high concentrations (compared to those routinely measured C{sub 2}-C{sub 6} tropospheric hydrocarbons) of acetone and methanol. We use a three-dimensional model to show that acetone photochemistry provides a quantitatively significant (up to 50%) pathway for sequestering NO{sub x} in the form of peroxyacetylnitrate, a relatively unreactive temporary reservoir of NO{sub x}. Furthermore, in the dry regions of the upper troposphere, acetone can provide a large primary source of HO{sub x} (OH + HO{sub 2}) radicals, resulting in increased ozone production. This surprisingly significant contribution of such oxygenated hydrocarbons to tropospheric NO{sub x}, HO{sub x} and ozone cycling is likely to be affected by their changing natural and anthropogenic emissions due to land-use change, biomass burning and alcohol-based biofuel use. (author)
Authors:
Singh, H B; [1]  Kanakidou, M; [2]  Crutzen, P J; [3]  Jacob, D J [4] 
  1. National Aeronautics and Space Administration, Moffett Field, CA (United States). Ames Research Center
  2. Centre National de la Recherche Scientifique (CNRS), 91 - Gif-sur-Yvette (France). Centre des Faibles Radioactivites
  3. Max-Planck-Institut fuer Chemie (Otto-Hahn-Institut), Mainz (Germany)
  4. Harvard Univ., Cambridge, MA (United States)
Publication Date:
Nov 02, 1995
Product Type:
Journal Article
Reference Number:
SCA: 540110; PA: GB-95:052423; EDB-96:020151; SN: 95001501115
Resource Relation:
Journal Name: Nature (London); Journal Volume: 378; Journal Issue: 6552; Other Information: PBD: 2 Nov 1995
Subject:
54 ENVIRONMENTAL SCIENCES; PHOTOCHEMICAL REACTIONS; TROPOSPHERE; NITROGEN OXIDES; MATHEMATICAL MODELS; HYDROCARBONS; ATMOSPHERIC CHEMISTRY
OSTI ID:
154952
Country of Origin:
United Kingdom
Language:
English
Other Identifying Numbers:
Journal ID: NATUAS; ISSN 0028-0836; TRN: GB9552423
Submitting Site:
GB
Size:
pp. 50-54
Announcement Date:
Jan 16, 1996

Citation Formats

Singh, H B, Kanakidou, M, Crutzen, P J, and Jacob, D J. High concentrations and photochemical fate of oxygenated hydrocarbons in the global troposphere. United Kingdom: N. p., 1995. Web. doi:10.1038/378050a0.
Singh, H B, Kanakidou, M, Crutzen, P J, & Jacob, D J. High concentrations and photochemical fate of oxygenated hydrocarbons in the global troposphere. United Kingdom. https://doi.org/10.1038/378050a0
Singh, H B, Kanakidou, M, Crutzen, P J, and Jacob, D J. 1995. "High concentrations and photochemical fate of oxygenated hydrocarbons in the global troposphere." United Kingdom. https://doi.org/10.1038/378050a0.
@misc{etde_154952,
title = {High concentrations and photochemical fate of oxygenated hydrocarbons in the global troposphere}
author = {Singh, H B, Kanakidou, M, Crutzen, P J, and Jacob, D J}
abstractNote = {Oxygenated species in the atmosphere are important sources of free radicals and are intricately linked with the fate of nitrogen oxides (NO{sub x}), which are themselves necessary for tropospheric ozone formation. With the exception of formaldehyde, oxygenated hydrocarbons have rarely been measured in the free troposphere. Here we report airborne measurements indicating the presence of high concentrations (compared to those routinely measured C{sub 2}-C{sub 6} tropospheric hydrocarbons) of acetone and methanol. We use a three-dimensional model to show that acetone photochemistry provides a quantitatively significant (up to 50%) pathway for sequestering NO{sub x} in the form of peroxyacetylnitrate, a relatively unreactive temporary reservoir of NO{sub x}. Furthermore, in the dry regions of the upper troposphere, acetone can provide a large primary source of HO{sub x} (OH + HO{sub 2}) radicals, resulting in increased ozone production. This surprisingly significant contribution of such oxygenated hydrocarbons to tropospheric NO{sub x}, HO{sub x} and ozone cycling is likely to be affected by their changing natural and anthropogenic emissions due to land-use change, biomass burning and alcohol-based biofuel use. (author)}
doi = {10.1038/378050a0}
journal = []
issue = {6552}
volume = {378}
journal type = {AC}
place = {United Kingdom}
year = {1995}
month = {Nov}
}