Here a new global emission inventory of C4-C10 perfluoroalkanesulfonic acids (PFSAs) from the life cycle of perfluorooctanesulfonyl fluoride (POSF)-based products in 1958-2030 is presented. In particular, we substantially improve and expand the previous frameworks by incorporating missing pieces (e.g., emissions to soil through land treatment, overlooked precursors) and updating parameters (e.g., emission factors, degradation half-lives). In 1958-2015, total direct and indirect emissions of perfluorooctanesulfonic acid (PFOS) are estimated as 1228-4930 tonnes, and emissions of PFOS precursors are estimated as 1230-8738 tonnes and approximately 670 tonnes for x-perfluorooctanesulfonamides/sulfonamido ethanols (xFOSA/Es) and POSF, respectively. Most of these emissions occurred between 1958 and 2002, followed by a substantial decrease. This confirms the positive effect of the ongoing transition to phase out POSF-based products, although this transition may still require substantial time and cause substantial additional releases of PFOS (8-153 tonnes) and xFOSA/Es (4-698 tonnes) in 2016 to 2030. The modeled environmental concentrations obtained by coupling the emission inventory and a global multimedia mass-balance model generally agree well with reported field measurements, suggesting that the inventory captures the actual emissions of PFOS and xFOSA/Es for the time being despite remaining uncertainties. Our analysis of the key uncertainties and open questions of and beyond the inventory shows that, among others, degradation of side-chain fluorinated polymers in the environment and landfills can be a long-term, (potentially) substantial source of PFOS.

Department of Environmental Science and Analytical Chemistry Stockholm University 10691 Stockholm Sweden

Institute for Chemical and Bioengineering ETH Zurich Vladimir Prelog Weg 1 8093 Zürich Switzerland

RECETOX Masaryk University Kamenice 753 5 62500 Brno Czech Republic

Citace poskytuje Crossref.org

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