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 the subsequent deposition to the oceans have been accounted for in only few ocean 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 5.3 Tg yr⁻¹ (90% confidence of 2.3 to 12.1). Of these emissions, 1, 27 and 72% were emitted in particles < 1 μm (PM₁), 1–10 μm (PM_1-10), and > 10 μm (PM_{> 10}), respectively, compared to a total Fe emission from mineral dust of 41.0 Tg yr⁻¹ in a log-normal distribution with a mass median diameter of 2.5 μm and a geometric standard deviation of 2. For combustion sources, different temporal trends were found in fine and medium-to-coarse particles, with a notable increase in Fe emissions in PM₁ since 2000 due to an increase in Fe emission from motor vehicles (from 0.008 to 0.0103 Tg yr⁻¹ in 2000 and 2007, respectively). These emissions have been introduced in a global 3-D transport model run at a spatial resolution of 0.94° latitude by 1.28° longitude to evaluate our estimation of Fe emissions. The modelled Fe concentrations as monthly means were compared with the monthly (57 sites) or daily (768 sites) measured concentrations at a total of 825 sampling stations. The deviation between modelled and observed Fe concentrations attached to aerosols at the surface was within a factor of 2 at most sampling stations, and the deviation was within a factor of 1.5 at sampling stations dominated by combustion sources. We analysed 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, 7% of which originated from the combustion sources. Our central estimates of Fe emissions from fossil fuel combustion (mainly from coal) are generally higher than those in previous studies, although they are within the uncertainty range of our estimates. In particular, the higher than previously estimated Fe emission from coal combustion implies a larger atmospheric anthropogenic input of soluble Fe to the northern Atlantic and northern Pacific Oceans, which is expected to enhance the biological carbon pump in those regions.