Ubiquitous atmospheric production of organic acids mediated by cloud droplets

B. Franco (1, 2) , T. Blumenstock (3) , C. Cho (1) , Lieven Clarisse (2) , Cathy Clerbaux (2, 4) , Pierre-François Coheur (2) , M. de Mazière (5) , I. de Smedt (5) , H.-P. Dorn (1) , T. Emmerichs (1) , H. Fuchs (1) , G. Gkatzelis (1) , D. W. T. Griffith (6) , S. Gromov (7, 8) , J. W. Hannigan (9) , F. Hase (3) , T. Hohaus (1) , N. Jones (6) , A. Kerkweg (1) , A. Kiendler-Scharr (1) , E. Lutsch (10) , E. Mahieu (11) , A. Novelli (1) , I. Ortega (9) , C. Paton-Walsh (6) , Matthieu Pommier (4, 12) , A. Pozzer (7) , D. Reimer (1) , S. Rosanka (1) , R. Sander (7) , M. Schneider (3) , K. Strong (10) , R. Tillmann (1) , M. van Roozendaël (5) , L. Vereecken (1) , C. Vigouroux (5) , A. Wahner (1) , D. Taraborrelli (1)

1 IEK-8 - Institut für Energie- und Klimaforschung - Troposphäre
2 SQUARES - Spectroscopy, Quantum Chemistry and Atmospheric Remote Sensing
3 Institute of Meteorology and Climate Research
4 TROPO - LATMOS
5 BIRA-IASB - Belgian Institute for Space Aeronomy / Institut d'Aéronomie Spatiale de Belgique
6 CAC - Centre for Atmospheric Chemistry [Wollongong]
7 MPIC - Max-Planck-Institut für Chemie
8 IGCE - Yu. A. Izrael Institute of Global Climate and Ecology
9 NCAR - National Center for Atmospheric Research [Boulder]
10 Department of Physics [Toronto]
11 Institut d'Astrophysique et de Géophysique [Liège]
12 Ricardo Energy and Environment

Atmospheric acidity is increasingly determined by carbon dioxide and organic acids1–3. Among the latter, formic acid facilitates the nucleation of cloud droplets4 and contributes to the acidity of clouds and rainwater1,5. At present, chemistry–climate models greatly underestimate the atmospheric burden of formic acid, because key processes related to its sources and sinks remain poorly understood2,6–9. Here we present atmospheric chamber experiments that show that formaldehyde is e ciently 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 ndings 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 a ect aerosol growth and cloud evolution.

Domains: Atmospheric and Oceanic Physics [physics.ao-ph]

B. Franco, T. Blumenstock, C. Cho, Lieven Clarisse, Cathy Clerbaux, et al.. Ubiquitous atmospheric production of organic acids mediated by cloud droplets. Nature, 2021, 593, pp.233 - 237. ⟨10.1038/s41586-021-03462-x⟩. ⟨insu-03354820⟩