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. 2022 Jan 4;56(1):228-238.
doi: 10.1021/acs.est.1c04277. Epub 2021 Dec 15.

Sea Spray Aerosol (SSA) as a Source of Perfluoroalkyl Acids (PFAAs) to the Atmosphere: Field Evidence from Long-Term Air Monitoring

Affiliations

Affiliations

  • 1 Department of Environmental Science, Stockholm University, SE-106 91 Stockholm, Sweden.
  • 2 Bolin Centre for Climate Research, SE-106 91 Stockholm, Sweden.
  • 3 NILU - Norwegian Institute for Air Research, P.O. Box 100, 2027 Kjeller, Norway.

Sea Spray Aerosol (SSA) as a Source of Perfluoroalkyl Acids (PFAAs) to the Atmosphere: Field Evidence from Long-Term Air Monitoring

Bo Sha et al. Environ Sci Technol. .
. 2022 Jan 4;56(1):228-238.
doi: 10.1021/acs.est.1c04277. Epub 2021 Dec 15.

Affiliations

  • 1 Department of Environmental Science, Stockholm University, SE-106 91 Stockholm, Sweden.
  • 2 Bolin Centre for Climate Research, SE-106 91 Stockholm, Sweden.
  • 3 NILU - Norwegian Institute for Air Research, P.O. Box 100, 2027 Kjeller, Norway.

Abstract

The effective enrichment of perfluoroalkyl acids (PFAAs) in sea spray aerosols (SSA) demonstrated in previous laboratory studies suggests that SSA is a potential source of PFAAs to the atmosphere. In order to investigate the influence of SSA on atmospheric PFAAs in the field, 48 h aerosol samples were collected regularly between 2018 and 2020 at two Norwegian coastal locations, Andøya and Birkenes. Significant correlations (p < 0.05) between the SSA tracer ion, Na+, and PFAA concentrations were observed in the samples from both locations, with Pearson's correlation coefficients (r) between 0.4-0.8. Such significant correlations indicate SSA to be an important source of atmospheric PFAAs to coastal areas. The correlations in the samples from Andøya were observed for more PFAA species and were generally stronger than in the samples from Birkenes, which is located further away from the coast and closer to urban areas than Andøya. Factors such as the origin of the SSA, the distance of the sampling site to open water, and the presence of other PFAA sources (e.g., volatile precursor compounds) can have influence on the contribution of SSA to PFAA in air at the sampling sites and therefore affect the observed correlations between PFAAs and Na+.

Keywords: Arctic; Norway; air monitoring; coastal areas; long-range atmospheric transport; per- and polyfluoroalkyl substances (PFAS); perfluoroalkyl acids (PFAAs); sea spray aerosols (SSA).

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Conflict of interest statement

The authors declare no competing financial interest.

Figures

Figure 1

Figure 1

Box-whisker plot of concentrations of…

Figure 1

Box-whisker plot of concentrations of PFAAs, Na + , and Mg 2+ in…

Figure 1
Box-whisker plot of concentrations of PFAAs, Na+, and Mg2+ in the air samples from Andøya and Birkenes. The lower and upper hinges correspond to the first and third quartiles (the 25th and 75th percentiles). The black lines and dots inside the boxes indicate the medians and means, respectively. Values below the MDLs were replaced by 1/2MDLs. The whiskers extend to no further than 1.5*IQR (interquartile range) from the hinges. The circles indicate values outside of 1.5*IQR. The gray dashed lines indicate MDLs (lower) and MQLs (upper). The numbers below the compound names are detection frequencies at each of the two sampling locations.
Figure 2

Figure 2

Correlations between PFAAs and Na

Figure 2

Correlations between PFAAs and Na + in (a) air samples with PFAA/Na +

Figure 2
Correlations between PFAAs and Na+ in (a) air samples with PFAA/Na+ ratios between the 5th and 95th percentiles and (b) in summer and winter samples. The strength of the log–log linear correlation is indicated by the r value (Pearson’s correlation coefficient). The significance of the correlation is indicated by the number of asterisks (*p < 0.05, **p < 0.01, ***p < 0.001). Data not included in the correlation analysis are marked as “×”. In Figure 1a, the solid lines are fitted by orthogonal linear regression in the form of log10[PFAA] = k × log10[Na+] + b and the dashed lines in parallel represent ± σ. The gray horizontal dashed lines in panel (a) indicate MDLs (lower) and MQLs (upper) of individual PFAAs. In Figure 1b, the solid lines are fitted in the form of log10[PFAA] = log10(kSSA × [Na+] + [PFAA]other).
Figure 3

Figure 3

First row: air mass transport…

Figure 3

First row: air mass transport probability function (P[A i,j ]) for the summer…

Figure 3
First row: air mass transport probability function (P[Ai,j]) for the summer and winter samples at Andøya (a, b) and Birkenes (c, d). Second row: source attribution function (i,j) for PFOA in summer and winter samples at Andøya (e, f) and Birkenes (g, h). Third row: source attribution function for PFOS in summer and winter samples at Andøya (i, j) and Birkenes (k, l). Fourth row: P[Ai,j] × i,j normalized to 1 for PFOA and PFOS in all samples from Andøya (m, n) and Birkenes (o, p). Fifth row: correlations (ri,j) between PFOA and Na+ and between PFOS and Na+ in all samples from Andøya (q, r) and Birkenes (s, t).
Figure 4

Figure 4

Comparison between the k SSA

Figure 4

Comparison between the k SSA determined by the linear fit (log10[PFAA] = log10(

Figure 4
Comparison between the kSSA determined by the linear fit (log10[PFAA] = log10(kSSA × [Na+] + [PFAA]other) and the estimation, kSSA_est, based on previous laboratory results and median PFAA seawater concentrations from the literature. The error bar represents the standard deviation of kSSA_est, [PFAA]seawater × (EFMean ± SD).

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