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- W3036444432 abstract "Abstract. Cloudwater acidity affects the atmospheric chemistry of sulfate and organic aerosol formation, halogen radical cycling, and trace metal speciation. Rainwater acidity including post-depositional inputs adversely affects soil and freshwater ecosystems. Here we use the GEOS-Chem model of atmospheric chemistry to simulate the global distributions of cloud- and rainwater acidity, and the total acid inputs to ecosystems from wet deposition. The model accounts for strong acids (H2SO4, HNO3, HCl), weak acids (HCOOH, CH3COOH, CO2, SO2), and weak bases (NH3, dust and sea salt aerosol alkalinity). We compile a global dataset of cloudwater pH measurements for comparison with the model. The global mean observed cloudwater pH is 5.2 ± 0.9, compared to 5.0 ± 0.8 in the model, with a range of 3 to 8 depending on region. The lowest values are over East Asia and the highest values are over deserts. Cloudwater pH over East Asia is low because of large acid inputs (H2SO4, HNO3), despite NH3 and dust neutralizing 70 % of these inputs. Cloudwater pH is typically 4–5 over the US and Europe. Carboxylic acids account for less than 25 % of cloudwater H+ in the northern hemisphere on an annual basis, but 25–50 % in the southern hemisphere and over 50 % in the southern tropical continents where they push the cloudwater pH below 4.5. Anthropogenic emissions of SO2 and NOx (precursors of H2SO4 and HNO3) are decreasing at northern mid-latitudes, but the effect on cloudwater pH is strongly buffered by NH4+ and carboxylic acids. The global mean rainwater pH is 5.5 in GEOS-Chem, higher than the cloudwater pH because of dilution and below-cloud scavenging of NH3 and dust. GEOS-Chem successfully reproduces the rainwater pH observations in North America, Europe, and eastern Asia. Carboxylic acids, which are undetected in routine observations due to biodegradation, lower the annual mean rainwater pH in these areas by 0.2 units. The acid wet deposition flux to terrestrial ecosystems taking into account the acidifying potential of NO3− and NH4+ in N-saturated ecosystems exceeds 50 meq m−2 a−1 in East Asia and the Americas, which would affect sensitive ecosystems. NH4+ is the dominant acidifying species in wet deposition, contributing 41 % of the global acid flux to continents under N-saturated conditions." @default.
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- W3036444432 date "2020-06-22" @default.
- W3036444432 modified "2023-09-29" @default.
- W3036444432 title "Global modeling of cloudwater acidity, rainwater acidity, and acid inputs to ecosystems" @default.
- W3036444432 doi "https://doi.org/10.5194/acp-2020-485" @default.
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