Abstract
Anthropogenic emissions are recognized as significant contributors to atmospheric soluble iron (Fe) in recent years, which may affect marine primary productivity, especially in Fe-limited areas. However, the contribution of different emission sources to Fe in marine aerosol has been primarily estimated by modeling approaches. Quantifying anthropogenic Fe based on field measurements remains a great challenge. In this study, online multi-element measurements and Positive Matrix Factorization (PMF) were combined for the first time to quantify sources of atmospheric Fe and soluble Fe in the Northwest Pacific during a cruise in spring 2015. Fe concentration in 624 atmospheric PM2.5 samples measured online was 74.58 ± 90.87 ng/m3. The PMF results showed anthropogenic activities, including industrial coal combustion, biomass burning, and maritime transport, were important in this region, contributing 31.4 % of atmospheric Fe on average. In addition, anthropogenic Fe concentration resolved by PMF was comparable to the simulation results of the CMAQ (Community Multiscale Air Quality) and GEOS-Chem (Goddard Earth Observing System-Chemical transport) models, with better correlation to CMAQ (r = 0.76) than GEOS-Chem (r = 0.26). This study developed a new method to estimate atmospheric soluble Fe, which integrates Fe source apportionment results and Fe solubility from different sources. Soluble Fe concentration was estimated as 3.93 ± 5.14 ng/m3, of which 87.0 % was attributed to anthropogenic emissions. Notably, ship emission alone contributed 27.5 % of soluble Fe, though its contribution to total Fe was only 2.2 %. Finally, the total deposition fluxes of atmospheric Fe (37.11 ± 38.43 μg/m2/day) and soluble Fe (1.85 ± 2.13 μg/m2/day) were estimated. This study developed a new methodology for quantifying contribution of anthropogenic emissions to Fe in marine aerosol, which could greatly help the assessment of impacts of human activities on marine environment.
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