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If the levels in the spray are much higher than in the water itself, I'm guessing most of the ocean PFAS is floating on the surface like a layer of scum? If freshwater lakes/rivers/reservoirs are similar maybe it would be possible to use some kind of surface-skimming filtration method to capture?
Yup.

> ...the results showed how the chemicals are powerful surfactants that concentrate on the surface of water, which helps explain why they move from the ocean to the air and atmosphere.

And skimming the surface sounds great, except for the fact that the oceans are awfully large. Maybe create PFAS-eating bacteria? What could go wrong? ;-)

As long as we have something to eat the birds that eat the snakes that eat the mice
Where did the PFAS contained in the ocean water spray originate?

I'm pretty sure industrial polluters are responsible for the bulk of it.