Fluorous-Core Nanoparticle-Embedded Hydrogel Synthesized via Tandem Photo-Controlled Radical Polymerization: Facilitating the Separation of Perfluorinated Alkyl Substances from Water

Per- and polyfluorinated alkyl substances (PFASs) are broadly used as surfactants and water/oil repellents for many decades. However, they are toxic, environmental persistence, and widely detected in water sources. In this work, we developed a fluorous-core nanoparticle-embedded hydrogel (FCH) synthesized by the metal-free tandem photocontrolled radical polymerization under visible-light irradiation. With the FCH material, the scope of absorbable PFASs has been expanded to neutral, anionic, cationic and zwitterionic PFASs with the same adsorbent for the first time. The fluorous nanoparticles exhibited strong and selective affinity toward PFASs without being dramatically influenced by pH levels and background ions, enabling efficient removing of PFASs at high to environmentally relevant concentrations (10 mg/L to 1 μg/L). Furthermore, the FCH network has shown good mechanical performance, facilitating the separation, regeneration, and recycling of adsorbent for multiple runs. These results demonstrate the promise of the FCH material for PFASs separation and adsorbent recycling toward sustainable environment.