Sources, transport and deposition of iron in the global atmosphere

Abstract. Atmospheric deposition of iron (Fe) plays an important role in controlling oceanic primary productivity. However, the sources of Fe in the atmosphere are not well understood. In particular, the combustion sources of Fe and their deposition over oceans are not accounted for in current biogeochemical models of the carbon cycle. Here we used a mass-balance method to estimate the emissions of Fe from the combustion of fossil fuels and biomass by accounting for the Fe contents in fuel and the partitioning of Fe during combustion. The emissions of Fe attached to aerosols from combustion sources were estimated by particle size, and their uncertainties were quantified by a Monte Carlo simulation. The emissions of Fe from mineral sources were estimated using the latest soil mineralogical database to date. As a result, the total Fe emissions from combustion averaged for 1960–2007 were estimated to be 5.1 Tg yr−1 (90% confidence of 2.2 to 11.5). Of these emissions, 2, 33 and 65% were emitted in particles <1 μm (PM1), 1–10 μm (PM1−10), and >10 μm (PM>10), respectively, compared to total Fe emissions from mineral sources of 41.0 Tg yr−1. For combustion sources, different temporal trends were found in fine and medium-to-coarse particles, with a notable increase in Fe emissions in PM1 and PM1−10 since 2000 due to a rapid increase from motor vehicles. These emissions have been introduced in a global 3-D transport model run at a spatial resolution of of 0.94° latitude by 1.28° longitude to evaluate our estimation of Fe emissions. The modelled Fe concentrations were compared to measurements at 825 sampling stations. The deviation between modelled and observed Fe concentrations attached to aerosols at the surface was within a factor of two at most sampling stations, and the deviation was within a factor of 1.5 at sampling stations dominated by combustion sources. We analyzed the relative contribution of combustion sources to total Fe concentrations over different regions of the world. The new mineralogical database led to a modest improvement in the simulation relative to station data even in dust dominated regions, but could provide useful information on the chemical forms of Fe in dust for coupling with ocean biota models. We estimated a total Fe deposition sink of 8.4 Tg yr−1 over global oceans, 6.6% of which originated from the combustion sources. The higher than previously estimated combustion-related Fe emissions implies a larger atmospheric input of soluble Fe over the northern Atlantic and northern Pacific Oceans, which is expected to enhance the biological carbon pump in those regions.