Influence of measurement uncertainties on fractional solubility of iron in mineral aerosols over the oceans

The atmospheric supply of mineral dust iron (Fe) plays a crucial role in the Earth’s biogeochemical cycle and is of specific importance as a micronutrient in the marine environment. Observations show several orders of magnitude variability in the fractional solubility of Fe in mineral dust aerosols, making it hard to assess the role of mineral dust in the global ocean biogeochemical Fe cycle. In this study we compare the operational solubility of mineral dust aerosol Fe associated with the flow-through leaching protocol to the results of the global 3-D chemical transport model GEOS-Chem. According to the protocol, aerosol Fe is defined as soluble by first deionized water leaching of mineral dust through a 0.45 lm pore size membrane followed by acidification and storage of the leachate over a long period of time prior to analysis. To estimate the uncertainty in soluble Fe results introduced by the flow-through leaching protocol, we prescribe an average 50% (range of 30–70%) fractional solubility to sub-0.45 lm sized mineral dust particles that may inadvertently pass the filter and end up in the acidified (at pH ~1.7) leachate for a couple of month period. In the model, the fractional solubility of Fe is either explicitly calculated using a complex mineral aerosol Fe dissolution equations, or prescribed to be 1% and 4% often used by global ocean biogeochemical Fe cycle models to reproduce the broad characteristics of the presently observed ocean dissolved iron distribution. Calculations show that the fractional solubility of Fe derived through the flow-through leaching is higher compared to the model results. The largest differences (~40%) are predicted to occur farther away from the dust source regions, over the areas where sub-0.45 lm sized mineral dust particles contribute a larger fraction of the total mineral dust mass. This study suggests that different methods used in soluble Fe measurements and inconsistences in the operational definition of filterable Fe in marine environment and soluble Fe in atmospheric aerosols are likely to contribute to the wide range of fractional solubility of aerosol Fe reported in the literature.