The
concerns about the fate of per- and polyfluoroalkyl substances
(PFAS) in the atmosphere are continuously growing. In this study,
size-fractionated particles, gas, and rainwater samples were simultaneously
collected in Shijiazhuang, China, to investigate the multiphase distribution
of PFAS in the atmosphere. Perfluoroalkyl carboxylic acids (PFCAs)
dominated the total concentration of PFAS in atmospheric media. A
strong positive relationship (0.79 < R
2 < 0.99) was observed between the concentration of PFCAs and organic
matter fraction (f
OM) in different particle
size fractions, while no such relationship for perfluoroalkyl sulfonic
acids (PFSAs) and f
OM, suggesting f
OM may be an important factor influencing the
size-dependent distribution of PFCAs. Temperature played a key role
in the gas-particle partitioning of PFAS, while it did not significantly
affect their particle-size-dependent distribution. The associative
concentration fluctuation of particle and particle-bound PFAS during
precipitation suggested that precipitation scavenging was an important
mechanism for the removal of PFAS from the atmosphere. Furthermore,
temporary increases in atmospheric PFAS concentrations were observed
during the precipitation. Fugacity ratios of PFAS in rainwater and
gas phase (log f
R/f
G ranged between 2.0 and 6.6) indicated a strong trend for
PFAS to diffuse from the rainwater to the gas phase during the precipitation,
which may explain that the concentration of PFAS in the gas phase
continued to increase even at the end of the precipitation.