Efficient Concentration and Complete Destruction of Short‐Chain and Emerging PFAS in Contaminated Water via Integrated Interface Engineering‐Enhanced Carbon Felt Sorption and Photochemical Processes

ABSTRACT Short‐chain and emerging per‐ and polyfluoroalkyl substances (PFAS) pose a significant threat to water security due to their high mobility and environmental persistence. Current strategies relying solely on adsorption or degradation remain inefficient and incomplete solutions. Herein, a closed‐loop “Concentrate‐&‐Destroy” strategy integrating an interface engineering‐enhanced sorbent of the polypyrrole (PPy) nanostructured coating carbon felt (PPy@P‐CF) with Cu ²⁺ ‐mediated photochemical destruction is presented. This designed PPy@P‐CF enabled rapid and efficient adsorption of short‐chain PFAS (C2‐C4) and emerging GenX, with equilibrium achieved within 300 s and maximum sorption capacities reaching 283.2–572.1 mg g ⁻¹ , surpassing those of granular activated carbon (GAC) and CF by over 21 and 5 times, respectively, under identical conditions. Dynamic column tests demonstrated a 5‐fold improvement in breakthrough volume (exceeding 4000 bed volumes) compared to GAC and CF columns. Furthermore, the spent PPy@P‐CF can be regenerated by solvent washing for reusability, and Cu ²⁺ ‐mediated photochemical degradation achieved complete defluorination of concentrated PFAS in eluate within 5 h by a ligand‐to‐metal charge transfer process. In practical applications, a bulk PPy@P‐CF module achieved > 96% removal of 27 diverse PFAS from real contaminated water, followed by complete photochemical defluorination. This integrated approach provides an adoptable solution for eliminating persistent short‐chain and emerging PFAS.