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The global prevalence and environmental risks of per- and polyfluoroalkyl substances (PFASs) have caused increasing concern regarding their strategic elimination from aqueous environments. It has recently been recognized that advanced oxidation–reduction technologies (AO/RTs) exhibit superior removal performance for these ubiquitous pollutants. However, the detailed mechanisms and product risks have not been well summarized and systematically deciphered. In this mini-review article, the basic operating principles of two typical AO/RTs (electron beam and plasma irradiation) and their reported applications in the abatement of PFASs are described in detail. It is noteworthy that these reductive treatments induced remarkable defluorination efficiency of PFOA and PFOS with the generation of short-chain congeners in water. The reaction mechanisms mainly included desulfonization, decarboxylation, H/F exchange, radical cyclization, and stepwise losses of CF2 groups. Unexpectedly, partial degradation products manifested high potential in triggering acute and chronic aquatic toxicity, genotoxicity, and developmental toxicity. Additionally, high or even increased resistance to biodegradability was observed for multiple products relative to the parent chemicals. Taken together, both electron beam and plasma irradiation hold great promise in remediating PFAS-contaminated water and wastewater, while the secondary ecological risks should be taken into account during practical applications.

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