Rapid cycling of reactive nitrogen in the marine boundary layer
Nitrogen oxides are essential for the formation of secondary atmospheric aerosols and of atmospheric oxidants such as ozone and the hydroxyl radical, which controls the self-cleansing capacity of the atmosphere. Nitric acid, a major oxidation product of nitrogen oxides, has traditionally been consid...
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Online Access: | http://nldr.library.ucar.edu/repository/collections/OSGC-000-000-022-819 https://doi.org/10.1038/nature17195 |
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ftncar:oai:drupal-site.org:articles_18385 2023-09-05T13:21:39+02:00 Rapid cycling of reactive nitrogen in the marine boundary layer Ye, Chunxiang (author) Zhou, Xianliang (author) Pu, Dennis (author) Stutz, Jochen (author) Festa, James (author) Spolaor, Max (author) Tsai, Catalina (author) Cantrell, Christopher (author) Mauldin, Roy (author) Campos, Teresa (author) Weinheimer, Andrew (author) Hornbrook, Rebecca (author) Apel, Eric (author) Guenther, Alex (author) Kaser, Lisa (author) Yuan, Bin (author) Karl, Thomas (author) Haggerty, Julie (author) Hall, Samuel (author) Ullmann, Kirk (author) Smith, James (author) Ortega, John (author) Knote, Christoph (author) 2016-04-28 http://nldr.library.ucar.edu/repository/collections/OSGC-000-000-022-819 https://doi.org/10.1038/nature17195 en eng Nature Publishing Group Nature articles:18385 ark:/85065/d7s46tkg http://nldr.library.ucar.edu/repository/collections/OSGC-000-000-022-819 doi:10.1038/nature17195 Copyright 2016 Authors. Text article 2016 ftncar https://doi.org/10.1038/nature17195 2023-08-14T18:47:01Z Nitrogen oxides are essential for the formation of secondary atmospheric aerosols and of atmospheric oxidants such as ozone and the hydroxyl radical, which controls the self-cleansing capacity of the atmosphere. Nitric acid, a major oxidation product of nitrogen oxides, has traditionally been considered to be a permanent sink of nitrogen oxides1. However, model studies predict higher ratios of nitric acid to nitrogen oxides in the troposphere than are observed, 'renoxification' process that recycles nitric acid into nitrogen oxides has been proposed to reconcile observations with model studies, but the mechanisms responsible for this process remain uncertain. Here we present data from an aircraft measurement campaign over the North Atlantic Ocean and find evidence for rapid recycling of nitric acid to nitrous acid and nitrogen oxides in the clean marine boundary layer via particulate nitrate photolysis. Laboratory experiments further demonstrate the photolysis of particulate nitrate collected on filters at a rate more than two orders of magnitude greater than that of gaseous nitric acid, with nitrous acid as the main product. Box model calculations based on the Master Chemical Mechanism suggest that particulate nitrate photolysis mainly sustains the observed levels of nitrous acid and nitrogen oxides at midday under typical marine boundary layer conditions. Given that oceans account for more than 70 per cent of Earth's surface, we propose that particulate nitrate photolysis could be a substantial tropospheric nitrogen oxide source. Recycling of nitrogen oxides in remote oceanic regions with minimal direct nitrogen oxide emissions could increase the formation of tropospheric oxidants and secondary atmospheric aerosols on a global scale. Article in Journal/Newspaper North Atlantic OpenSky (NCAR/UCAR - National Center for Atmospheric Research/University Corporation for Atmospheric Research) Nature 532 7600 489 491 |
institution |
Open Polar |
collection |
OpenSky (NCAR/UCAR - National Center for Atmospheric Research/University Corporation for Atmospheric Research) |
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ftncar |
language |
English |
description |
Nitrogen oxides are essential for the formation of secondary atmospheric aerosols and of atmospheric oxidants such as ozone and the hydroxyl radical, which controls the self-cleansing capacity of the atmosphere. Nitric acid, a major oxidation product of nitrogen oxides, has traditionally been considered to be a permanent sink of nitrogen oxides1. However, model studies predict higher ratios of nitric acid to nitrogen oxides in the troposphere than are observed, 'renoxification' process that recycles nitric acid into nitrogen oxides has been proposed to reconcile observations with model studies, but the mechanisms responsible for this process remain uncertain. Here we present data from an aircraft measurement campaign over the North Atlantic Ocean and find evidence for rapid recycling of nitric acid to nitrous acid and nitrogen oxides in the clean marine boundary layer via particulate nitrate photolysis. Laboratory experiments further demonstrate the photolysis of particulate nitrate collected on filters at a rate more than two orders of magnitude greater than that of gaseous nitric acid, with nitrous acid as the main product. Box model calculations based on the Master Chemical Mechanism suggest that particulate nitrate photolysis mainly sustains the observed levels of nitrous acid and nitrogen oxides at midday under typical marine boundary layer conditions. Given that oceans account for more than 70 per cent of Earth's surface, we propose that particulate nitrate photolysis could be a substantial tropospheric nitrogen oxide source. Recycling of nitrogen oxides in remote oceanic regions with minimal direct nitrogen oxide emissions could increase the formation of tropospheric oxidants and secondary atmospheric aerosols on a global scale. |
author2 |
Ye, Chunxiang (author) Zhou, Xianliang (author) Pu, Dennis (author) Stutz, Jochen (author) Festa, James (author) Spolaor, Max (author) Tsai, Catalina (author) Cantrell, Christopher (author) Mauldin, Roy (author) Campos, Teresa (author) Weinheimer, Andrew (author) Hornbrook, Rebecca (author) Apel, Eric (author) Guenther, Alex (author) Kaser, Lisa (author) Yuan, Bin (author) Karl, Thomas (author) Haggerty, Julie (author) Hall, Samuel (author) Ullmann, Kirk (author) Smith, James (author) Ortega, John (author) Knote, Christoph (author) |
format |
Article in Journal/Newspaper |
title |
Rapid cycling of reactive nitrogen in the marine boundary layer |
spellingShingle |
Rapid cycling of reactive nitrogen in the marine boundary layer |
title_short |
Rapid cycling of reactive nitrogen in the marine boundary layer |
title_full |
Rapid cycling of reactive nitrogen in the marine boundary layer |
title_fullStr |
Rapid cycling of reactive nitrogen in the marine boundary layer |
title_full_unstemmed |
Rapid cycling of reactive nitrogen in the marine boundary layer |
title_sort |
rapid cycling of reactive nitrogen in the marine boundary layer |
publisher |
Nature Publishing Group |
publishDate |
2016 |
url |
http://nldr.library.ucar.edu/repository/collections/OSGC-000-000-022-819 https://doi.org/10.1038/nature17195 |
genre |
North Atlantic |
genre_facet |
North Atlantic |
op_relation |
Nature articles:18385 ark:/85065/d7s46tkg http://nldr.library.ucar.edu/repository/collections/OSGC-000-000-022-819 doi:10.1038/nature17195 |
op_rights |
Copyright 2016 Authors. |
op_doi |
https://doi.org/10.1038/nature17195 |
container_title |
Nature |
container_volume |
532 |
container_issue |
7600 |
container_start_page |
489 |
op_container_end_page |
491 |
_version_ |
1776202242255224832 |