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Abstract

Emerging perfluoroalkyl and polyfluoroalkyl substances contaminate waters at trace concentrations, thus rapid and selective adsorbents are pivotal to mitigate the consequent energy-intensive and time-consuming issues in remediation. In this study, coal combustion residuals-fly ash was modified (FA-SCA) to overcome the universal trade-off between high adsorption capacity and fast kinetics. FA-SCA presented rapid adsorption (teq = 2 min) of PFOX (perfluorooctanoic acid and perfluorooctanesulfonic acid, collectively), where the dynamic adsorption capacity (qdyn = qm/teq) was 2–3 orders of magnitude higher than that of benchmark activated carbons and anion-exchange resins. Investigated by advanced characterization and kinetic models, the fast kinetics and superior qdyn are attributed to (1) elevated external diffusion driven by the submicron particle size; (2) enhanced intraparticle diffusion caused by the developed mesoporous structure (Vmeso/Vmicro = 8.1); (3) numerous quaternary ammonium anion-exchange sites (840 μmol/g), and (4) appropriate adsorption affinity (0.031 L/μmol for PFOS, and 0.023 L/μmol for PFOA). Since the adsorption was proven to be a synergistic process of electrostatic and hydrophobic interactions, effective adsorption ([PFOX]ini = 1.21 μM, concentration levels of highly-contaminant-sites) was obtained at conventional natural water chemistries. High selectivity (>85.4% removal) was also achieved with organic/inorganic competitors, especially compounds with partly similar molecular structures to PFOX. In addition, >90% PFOX was removed consistently during five cycles in mild regeneration conditions (pH 12 and 50 ◦C). Overall, FA-SCA showed no leaching issues of toxic metals and exhibits great potential in both single-adsorption processes and treatment train systems.

Document Type

Article

Publication Date

4-2022

Notes/Citation Information

1385-8947/© 2021 Elsevier B.V. All rights reserved.

Digital Object Identifier (DOI)

https://doi.org/10.1016/j.cej.2021.133271

Funding Information

This work was supported by China Postdoctoral Science Foundation [2020M681204]; the National Natural Science Foundation of China [21908054 & 22075076]; and NIEHS-SRP grant [P42ES007380]. We highly appreciate the collaborations with the UK superfund center and the UK CAER

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