Dominant Contribution of Non-dust Primary Emissions and Secondary Processes to Dissolved Aerosol Iron

Solubility largely determines the impacts of aerosol Fe on marine ecosystems and human health. Currently, modeling studies have large uncertainties in aerosol Fe solubility due to inadequate understanding of the sources of dissolved Fe. This work investigated seasonal variations of Fe solubility in coarse and fine aerosols in Qingdao, a coastal city in the Northwest Pacific, and utilized a receptor model for source apportionment of total and dissolved aerosol Fe. Desert dust was found to be the main source of total Fe, contributing 65 and 81% annually to total Fe in coarse and fine particles, respectively; in contrast, dissolved aerosol Fe originated primarily from combustion, industrial, and secondary sources. The annual average contributions to dissolved Fe in coarse and fine particles were 68 and 47% for the secondary source and 32 and 33% for the combustion source, respectively. Aerosol Fe solubility was found to be highest in summer and lowest in spring, showing seasonal patterns similar to those of aerosol acidity. Increase in Fe solubility in atmospheric particles, when compared to desert dust, was mainly caused by secondary processing and combustion emission, and the effect of secondary processes was dictated by aerosol acidity and liquid water content.