1Environmental Chemical Processes Laboratory, Department of Chemistry, University of Crete, P.O. Box 2208, 70013 Heraklion, Greece
2Institute of Chemical Engineering Sciences (ICE-HT), FORTH, Patras, Greece
3Institute for Environmental Research and Sustainable Development, National Observatory of Athens, Athens, Greece
4School of Environmental Sciences, University of East Anglia, Norwich, NR4 7TJ, UK
5School of Earth and Atmospheric Sciences, Georgia Institute of Technology, 311 Ferst Drive, Atlanta, GA 30332-0100, USA
6School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, 311 Ferst Drive, Atlanta, GA 30332-0100, USA
Received: 31 Dec 2014 – Discussion started: 02 Mar 2015
Abstract. The global atmospheric iron (Fe) cycle is parameterized in the global 3-D chemical transport model TM4-ECPL to simulate the proton- and the organic ligand-promoted mineral-Fe dissolution as well as the aqueous-phase photochemical reactions between the oxidative states of Fe (III/II). Primary emissions of total (TFe) and dissolved (DFe) Fe associated with dust and combustion processes are also taken into account, with TFe mineral emissions calculated to amount to ~ 35 Tg-Fe yr−1 and TFe emissions from combustion sources of ~ 2 Tg-Fe yr−1. The model reasonably simulates the available Fe observations, supporting the reliability of the results of this study. Proton- and organic ligand-promoted Fe dissolution in present-day TM4-ECPL simulations is calculated to be ~ 0.175 Tg-Fe yr−1, approximately half of the calculated total primary DFe emissions from mineral and combustion sources in the model (~ 0.322 Tg-Fe yr−1). The atmospheric burden of DFe is calculated to be ~ 0.024 Tg-Fe. DFe deposition presents strong spatial and temporal variability with an annual flux of ~ 0.496 Tg-Fe yr−1, from which about 40 % (~ 0.191 Tg-Fe yr−1) is deposited over the ocean. The impact of air quality on Fe deposition is studied by performing sensitivity simulations using preindustrial (year 1850), present (year 2008) and future (year 2100) emission scenarios. These simulations indicate that about a 3 times increase in Fe dissolution may have occurred in the past 150 years due to increasing anthropogenic emissions and thus atmospheric acidity. Air-quality regulations of anthropogenic emissions are projected to decrease atmospheric acidity in the near future, reducing to about half the dust-Fe dissolution relative to the present day. The organic ligand contribution to Fe dissolution shows an inverse relationship to the atmospheric acidity, thus its importance has decreased since the preindustrial period but is projected to increase in the future. The calculated changes also show that the atmospheric DFe supply to the globe has more than doubled since the preindustrial period due to 8-fold increases in the primary non-dust emissions and about a 3-fold increase in the dust-Fe dissolution flux. However, in the future the DFe deposition flux is expected to decrease (by about 25 %) due to reductions in the primary non-dust emissions (about 15 %) and in the dust-Fe dissolution flux (about 55 %). The present level of atmospheric deposition of DFe over the global ocean is calculated to be about 3 times higher than for 1850 emissions, and about a 30 % decrease is projected for 2100 emissions. These changes are expected to impact most on the high-nutrient–low-chlorophyll oceanic regions.
Revised: 31 May 2015 – Accepted: 09 Jun 2015 – Published: 02 Jul 2015
Myriokefalitakis, S., Daskalakis, N., Mihalopoulos, N., Baker, A. R., Nenes, A., and Kanakidou, M.: Changes in dissolved iron deposition to the oceans driven by human activity: a 3-D global modelling study, Biogeosciences, 12, 3973-3992, doi:10.5194/bg-12-3973-2015, 2015.