Change of iron species and iron solubility in Asian dust during the long-range transport from western China to Japan

In the North Pacific, transport and deposition of mineral dust from Asia appear to be one of major sources of iron which can regulate growth of phytoplankton in the ocean. In this process, it is essential to identify chemical species of iron contained in Asian dust, because bioavailability of iron in the ocean is strongly influenced by the solubility of iron, which in turn is dependent on iron species in the dust. Here, we report that clay minerals (illite and chlorite) in the dusts near the source collected at Aksu (western China) can be transformed into ferrihydrite by atmospheric chemical processes during their long-range transport to eastern China (Qingdao) and Japan (Tsukuba) based on the speciation by X-ray absorption fine structure (XAFS) and other methods such as X-ray diffraction and chemical extraction. As a result, Fe molar ratio in Aksu (illite : chlorite : ferrihydrite = 70 : 25 : 5) was changed to that in Tsukuba (illite : chlorite : ferrihydrite = 65 : 10 : 25). Moreover, leaching experiments were conducted to study the change of iron solubility. It was found that the iron solubility for the dust in Tsukuba (soluble iron fraction: 11.8% and 1.10% for synthetic rain water and seawater, respectively) was larger than that in Aksu (4.1% and 0.28%, respectively), showing that iron in the dust after the transport becomes more soluble possibly due to the formation of ferrihydrite in the atmosphere. Our findings suggested that secondary formation of ferrihydrite during the transport should be considered as one of important processes in evaluating the supply of soluble iron to seawater.