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Atmospheric deposition of anthropogenic soluble iron (Fe) to the ocean hasbeen suggested to modulate primary ocean productivity and thus indirectlyaffect the climate. A key process contributing to anthropogenic sources ofsoluble Fe is associated with air pollution, which acidifies Fe-containingmineral aerosols during their transport and leads to Fe transformation frominsoluble to soluble forms. However, there is large uncertainty in ourestimate of this anthropogenic soluble Fe. In this study, for the first time,we interactively combined laboratory kinetic experiments with global aerosolmodeling to more accurately quantify anthropogenic soluble Fe due to airpollution. Firstly, we determined Fe dissolution kinetics of African dustsamples at acidic pH values with and without ionic species commonly found inaerosol water (i.e., sulfate and oxalate). Then, by using acidity as a mastervariable, we constructed a new empirical scheme for Fe release from mineraldust due to inorganic and organic anions in aerosol water. We implementedthis new scheme and applied an updated mineralogical emission database in aglobal atmospheric chemistry transport model to estimate the atmosphericconcentration and deposition flux of soluble Fe under preindustrial andmodern conditions. Our improved model successfully captured the inverserelationship of Fe solubility and total Fe loading measured over the NorthAtlantic Ocean (i.e., 1–2 orders of magnitude lower Fe solubility innorthern-African- than combustion-influenced aerosols). The model resultsshow a positive relationship between Fe solubility and water-soluble organiccarbon (WSOC)/Fe molar ratio, which is consistent with previous fieldmeasurements. We estimated that deposition of soluble Fe to the oceanincreased from 0.05–0.07 Tg Fe yr<sup>−1</sup> in the preindustrial era to0.11–0.12 Tg Fe yr<sup>−1</sup> in the present day, due to air pollution. Overthe high-nitrate, low-chlorophyll (HNLC) regions of the ocean, the modeled Fesolubility remains low for mineral dust (< 1 %) in a base simulationbut is substantially enhanced in a sensitivity simulation, which permits theFe dissolution for mineral aerosols in the presence of excess oxalate underlow acidity during daytime. Our model results suggest that human activitiescontribute to about half of the soluble Fe supply to a significant portion ofthe oceans in the Northern Hemisphere, while their contribution to oceans inhigh latitudes remains uncertain due to limited understanding of Fe sourceand its dissolution under pristine conditions

Delivery of anthropogenic bioavailable iron from mineral dust and combustion aerosols to the ocean