Title |
Photo-tautomerization of acetaldehyde as a photochemical source of formic acid in the troposphere
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Published in |
Nature Communications, July 2018
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DOI | 10.1038/s41467-018-04824-2 |
Pubmed ID | |
Authors |
Miranda F. Shaw, Bálint Sztáray, Lisa K. Whalley, Dwayne E. Heard, Dylan B. Millet, Meredith J. T. Jordan, David L. Osborn, Scott H. Kable |
Abstract |
Organic acids play a key role in the troposphere, contributing to atmospheric aqueous-phase chemistry, aerosol formation, and precipitation acidity. Atmospheric models currently account for less than half the observed, globally averaged formic acid loading. Here we report that acetaldehyde photo-tautomerizes to vinyl alcohol under atmospherically relevant pressures of nitrogen, in the actinic wavelength range, λ = 300-330 nm, with measured quantum yields of 2-25%. Recent theoretical kinetics studies show hydroxyl-initiated oxidation of vinyl alcohol produces formic acid. Adding these pathways to an atmospheric chemistry box model (Master Chemical Mechanism) demonstrates increased formic acid concentrations by a factor of ~1.7 in the polluted troposphere and a factor of ~3 under pristine conditions. Incorporating this mechanism into the GEOS-Chem 3D global chemical transport model reveals an estimated 7% contribution to worldwide formic acid production, with up to 60% of the total modeled formic acid production over oceans arising from photo-tautomerization. |
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