Abstract
Perfluoroalkyl acids (PFAAs) are persistent organic substances that have been widely detected in the global oceans. Previous laboratory experiments have demonstrated effective enrichment of PFAAs in nascent sea spray aerosols (SSA), suggesting that SSA are an important source of PFAAs to the atmosphere. In the present study, the effects of the water concentration of PFAAs on their size-resolved enrichment in SSA were examined using a sea spray simulation chamber. Aerosolization of the target compounds in almost all sizes of SSA revealed a strong linear relationship with their water concentrations (p < 0.05, r2 > 0.9). The enrichment factors (EF) of the target compounds showed no correlation with their concentrations in the chamber water, despite the concentrations varying by a factor of 500 (∼0.3 to ∼150 ng L–1). The particle surface-area-to-volume ratio appeared to be a key predictor of the enrichment of perfluoroalkyl carboxylic acids (PFCAs) with ≥7 perfluorinated carbons and perfluoroalkanesulfonic acids (PFSAs) with ≥6 perfluorinated carbons in supermicron particles (p < 0.05, r2 > 0.8), but not in submicron particles. The different enrichment behaviors of PFAAs in submicron and supermicron particles might be a result of the different production mechanisms of film droplets and jet droplets. The results suggest that the variability in seawater concentrations of PFAAs has little influence on EFs and that modeling studies designed to quantify the source of PFAAs via SSA emissions do not need to consider this factor.
Highlights
Perfluoroalkyl acids (PFAAs) are a subgroup of per- and polyfluoroalkyl substances (PFAS) that have been widely used in numerous industrial and commercial applications since the 1950s.1−4 Their productions and emissions has been reviewed by Wang et al.[2,4] PFAAs are the terminal degradation products of a wide range of polyfluoroalkyl substances.[1,2] They have been detected in environmental media, biota, and humans worldwide,[5−10] even in remote areas such as the Arctic[11,12] and Antarctic.[13]
The results suggest that the variability in seawater concentrations of PFAAs has little influence on enrichment factors (EF) and that modeling studies designed to quantify the source of PFAAs via sea spray aerosols (SSA) emissions do not need to consider this factor
The EFSSA of the target compounds was dependent on the number of perfluorinated carbons (NPC) and revealed a curvilinear relationship with NPC (Figures 1 and S9)
Summary
Perfluoroalkyl acids (PFAAs) are a subgroup of per- and polyfluoroalkyl substances (PFAS) that have been widely used in numerous industrial and commercial applications since the 1950s.1−4 Their productions and emissions has been reviewed by Wang et al.[2,4] PFAAs are the terminal degradation products of a wide range of polyfluoroalkyl substances (socalled precursor substances).[1,2] They have been detected in environmental media, biota, and humans worldwide,[5−10] even in remote areas such as the Arctic[11,12] and Antarctic.[13]. Johansson et al.[17] observed that PFAA concentrations in laboratory-generated SSA < 1.6 μm can be up to
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