Graphene oxide with 1-nm-thick adlayer for efficient and near-instant removal of per- and polyfluoroalkyl substances

The environmental occurrence of anthropogenic chemicals-especially persistent micropollutants of per- and polyfluoroalkyl substances (PFAS)-raises pressing concerns for global drinking-water safety. Adsorption is an effective technology for removing PFAS but is limited by unsatisfactory adsorption capacity and efficiency. We report a strategy to attach polyamine adlayers to graphene oxide (GO) nanosheets that produces highly charged and monodispersed 2D adsorbents of a GO nanosheet sandwiched between two 1-nm-thick polyamine adlayers. This adsorbent has a high adsorption capacity for PFAS of ∼3070 mg/g-tens of times greater than that of GO and commercial activated carbon. It also provides almost instant adsorption of a variety of PFAS and reaches 57%-95% of its equilibrium capacity in a minute and removes ∼100% of PFAS from contaminated water sources within a few minutes, transforming real-life PFAS-contaminated water into safe drinking water. Experiment and theory show that the planar nature of the 2D adsorbent combined with its abundant surface adsorption sites that electrostatically attract the polar groups of the PFAS, and hydrogen bonding and hydrophobic-hydrophobic interactions with their non-polar groups, account for its ultra-high adsorption capacity and rapid removal efficiency. We also show that regeneration of the adsorbents removes the adsorbed PFAS and allows subsequent destruction, demonstrating a closed-loop treatment solution for micropollutant contamination.