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Formation and Stability of Bulk Carbonic Acid (H2CO3) by Protonation of Tropospheric Calcite

Authors
Journal
ChemPhysChem
1439-4235
Publisher
Wiley Blackwell (John Wiley & Sons)
Publication Date
Volume
13
Issue
13
Identifiers
DOI: 10.1002/cphc.201200422
Keywords
  • Communications
Disciplines
  • Chemistry

Abstract

Formation and Stability of Bulk Carbonic Acid (H2CO3) by Protonation of Tropospheric Calcite DOI: 10.1002/cphc.201200422 Formation and Stability of Bulk Carbonic Acid (H2CO3) by Protonation of Tropospheric Calcite Juergen Bernard,[a] Markus Seidl,[a] Erwin Mayer,[b] and Thomas Loerting*[a] Organic acids play an important role in the acidification of our atmosphere. These weak acids can contribute up to 60% of the free airborne acidity. By far the most abundant organic acids are the C1 and C2 monocarboxylic acids, formic acid (HCOOH) and acetic acid (CH3COOH), which show mixing ratios in the gas phase ranging up to 20 ppb over land[1,2] and down to 0.2 ppb in the remote oceanic boundary layer or tropo- sphere.[3,4] These acids are partitioned between the gas phase and the particulate phase, where roughly one half to two thirds can be found in particulate matter (PM2.5).[2] The most important removal mechanism is dry deposition, which ac- counts for more than 90% of the total organic acid deposition budget. The remaining fraction is removed by rain as particu- late-phase acids, whereas removal by chemical reactions is negligible.[1, 5] In addition to the two most important organic acids, C3–C10 aliphatic monocarboxylic acids[1] and C2–C11 ali- phatic dicarboxylic acids[1,2,6–11] as well as aromatic carboxylic acids[1] have also been observed in air. The water-soluble frac- tion of organic carbon can on average consist of 35% mono- and dicarboxylic acids.[12] While the C2-dicarboxylic acid, oxalic acid (COOH)2, is commonly observed in all field studies, the C1-dicarboxylic acid, carbonic acid (H2CO3), has barely received any attention, mainly because it is thought that it immediately decomposes to water and carbon dioxide. However, it has pre- viously been shown that gaseous, water-free carbonic acid is surprisingly stable,[13] that amorphous and crystalline solids of pure carbonic acid can be produced and stored without de- composition at temperatures up to 230 K even in the presence of

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