Cargando…
Ubiquitous atmospheric production of organic acids mediated by cloud droplets
Atmospheric acidity is increasingly determined by carbon dioxide and organic acids(1–3). Among the latter, formic acid facilitates the nucleation of cloud droplets(4) and contributes to the acidity of clouds and rainwater(1,5). At present, chemistry–climate models greatly underestimate the atmospher...
Autores principales: | , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , |
---|---|
Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2021
|
Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8116209/ https://www.ncbi.nlm.nih.gov/pubmed/33981052 http://dx.doi.org/10.1038/s41586-021-03462-x |
_version_ | 1783691344734060544 |
---|---|
author | Franco, B. Blumenstock, T. Cho, C. Clarisse, L. Clerbaux, C. Coheur, P.-F. De Mazière, M. De Smedt, I. Dorn, H.-P. Emmerichs, T. Fuchs, H. Gkatzelis, G. Griffith, D. W. T. Gromov, S. Hannigan, J. W. Hase, F. Hohaus, T. Jones, N. Kerkweg, A. Kiendler-Scharr, A. Lutsch, E. Mahieu, E. Novelli, A. Ortega, I. Paton-Walsh, C. Pommier, M. Pozzer, A. Reimer, D. Rosanka, S. Sander, R. Schneider, M. Strong, K. Tillmann, R. Van Roozendael, M. Vereecken, L. Vigouroux, C. Wahner, A. Taraborrelli, D. |
author_facet | Franco, B. Blumenstock, T. Cho, C. Clarisse, L. Clerbaux, C. Coheur, P.-F. De Mazière, M. De Smedt, I. Dorn, H.-P. Emmerichs, T. Fuchs, H. Gkatzelis, G. Griffith, D. W. T. Gromov, S. Hannigan, J. W. Hase, F. Hohaus, T. Jones, N. Kerkweg, A. Kiendler-Scharr, A. Lutsch, E. Mahieu, E. Novelli, A. Ortega, I. Paton-Walsh, C. Pommier, M. Pozzer, A. Reimer, D. Rosanka, S. Sander, R. Schneider, M. Strong, K. Tillmann, R. Van Roozendael, M. Vereecken, L. Vigouroux, C. Wahner, A. Taraborrelli, D. |
author_sort | Franco, B. |
collection | PubMed |
description | Atmospheric acidity is increasingly determined by carbon dioxide and organic acids(1–3). Among the latter, formic acid facilitates the nucleation of cloud droplets(4) and contributes to the acidity of clouds and rainwater(1,5). At present, chemistry–climate models greatly underestimate the atmospheric burden of formic acid, because key processes related to its sources and sinks remain poorly understood(2,6–9). Here we present atmospheric chamber experiments that show that formaldehyde is efficiently converted to gaseous formic acid via a multiphase pathway that involves its hydrated form, methanediol. In warm cloud droplets, methanediol undergoes fast outgassing but slow dehydration. Using a chemistry–climate model, we estimate that the gas-phase oxidation of methanediol produces up to four times more formic acid than all other known chemical sources combined. Our findings reconcile model predictions and measurements of formic acid abundance. The additional formic acid burden increases atmospheric acidity by reducing the pH of clouds and rainwater by up to 0.3. The diol mechanism presented here probably applies to other aldehydes and may help to explain the high atmospheric levels of other organic acids that affect aerosol growth and cloud evolution. |
format | Online Article Text |
id | pubmed-8116209 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2021 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
spelling | pubmed-81162092021-05-26 Ubiquitous atmospheric production of organic acids mediated by cloud droplets Franco, B. Blumenstock, T. Cho, C. Clarisse, L. Clerbaux, C. Coheur, P.-F. De Mazière, M. De Smedt, I. Dorn, H.-P. Emmerichs, T. Fuchs, H. Gkatzelis, G. Griffith, D. W. T. Gromov, S. Hannigan, J. W. Hase, F. Hohaus, T. Jones, N. Kerkweg, A. Kiendler-Scharr, A. Lutsch, E. Mahieu, E. Novelli, A. Ortega, I. Paton-Walsh, C. Pommier, M. Pozzer, A. Reimer, D. Rosanka, S. Sander, R. Schneider, M. Strong, K. Tillmann, R. Van Roozendael, M. Vereecken, L. Vigouroux, C. Wahner, A. Taraborrelli, D. Nature Article Atmospheric acidity is increasingly determined by carbon dioxide and organic acids(1–3). Among the latter, formic acid facilitates the nucleation of cloud droplets(4) and contributes to the acidity of clouds and rainwater(1,5). At present, chemistry–climate models greatly underestimate the atmospheric burden of formic acid, because key processes related to its sources and sinks remain poorly understood(2,6–9). Here we present atmospheric chamber experiments that show that formaldehyde is efficiently converted to gaseous formic acid via a multiphase pathway that involves its hydrated form, methanediol. In warm cloud droplets, methanediol undergoes fast outgassing but slow dehydration. Using a chemistry–climate model, we estimate that the gas-phase oxidation of methanediol produces up to four times more formic acid than all other known chemical sources combined. Our findings reconcile model predictions and measurements of formic acid abundance. The additional formic acid burden increases atmospheric acidity by reducing the pH of clouds and rainwater by up to 0.3. The diol mechanism presented here probably applies to other aldehydes and may help to explain the high atmospheric levels of other organic acids that affect aerosol growth and cloud evolution. Nature Publishing Group UK 2021-05-12 2021 /pmc/articles/PMC8116209/ /pubmed/33981052 http://dx.doi.org/10.1038/s41586-021-03462-x Text en © The Author(s) 2021 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) . |
spellingShingle | Article Franco, B. Blumenstock, T. Cho, C. Clarisse, L. Clerbaux, C. Coheur, P.-F. De Mazière, M. De Smedt, I. Dorn, H.-P. Emmerichs, T. Fuchs, H. Gkatzelis, G. Griffith, D. W. T. Gromov, S. Hannigan, J. W. Hase, F. Hohaus, T. Jones, N. Kerkweg, A. Kiendler-Scharr, A. Lutsch, E. Mahieu, E. Novelli, A. Ortega, I. Paton-Walsh, C. Pommier, M. Pozzer, A. Reimer, D. Rosanka, S. Sander, R. Schneider, M. Strong, K. Tillmann, R. Van Roozendael, M. Vereecken, L. Vigouroux, C. Wahner, A. Taraborrelli, D. Ubiquitous atmospheric production of organic acids mediated by cloud droplets |
title | Ubiquitous atmospheric production of organic acids mediated by cloud droplets |
title_full | Ubiquitous atmospheric production of organic acids mediated by cloud droplets |
title_fullStr | Ubiquitous atmospheric production of organic acids mediated by cloud droplets |
title_full_unstemmed | Ubiquitous atmospheric production of organic acids mediated by cloud droplets |
title_short | Ubiquitous atmospheric production of organic acids mediated by cloud droplets |
title_sort | ubiquitous atmospheric production of organic acids mediated by cloud droplets |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8116209/ https://www.ncbi.nlm.nih.gov/pubmed/33981052 http://dx.doi.org/10.1038/s41586-021-03462-x |
work_keys_str_mv | AT francob ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT blumenstockt ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT choc ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT clarissel ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT clerbauxc ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT coheurpf ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT demazierem ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT desmedti ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT dornhp ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT emmerichst ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT fuchsh ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT gkatzelisg ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT griffithdwt ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT gromovs ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT hanniganjw ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT hasef ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT hohaust ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT jonesn ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT kerkwega ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT kiendlerscharra ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT lutsche ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT mahieue ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT novellia ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT ortegai ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT patonwalshc ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT pommierm ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT pozzera ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT reimerd ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT rosankas ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT sanderr ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT schneiderm ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT strongk ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT tillmannr ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT vanroozendaelm ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT vereeckenl ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT vigourouxc ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT wahnera ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets AT taraborrellid ubiquitousatmosphericproductionoforganicacidsmediatedbyclouddroplets |