Per-and polyfluoroalkyl substances (PFAS), a large class of synthesized chemicals, are persistent in nature and generally recalcitrant to conventional chemical and biological treatment. Adsorption is considered an economical and practical method for PFAS treatment. Layered double hydroxides (LDHs) represent a promising class of mineral-based adsorbents for PFAS removal because of the highly positive charge of their structural layers. In this research, the performance of two representative LDHs with varied cation compositions, namely Zn-Al and Mg-Al LDHs, were investigated and compared for the removal of perfluorinated carboxylic acids (PFCAs) with an emphasis on perfluorooctanoic acid (PFOA). Zn-Al LDH showed high efficiency for the removal of medium- and long-chain PFCAs (i.e., C ≥ 7), and performed consistently better than Mg-Al LDH. Based on detailed adsorption kinetics and isotherm studies toward PFOA, Zn-Al LDH showed higher adsorption capacity, stronger adsorption affinity, and faster kinetics than Mg-Al LDH. Presence of natural organic matter had minimal impact on PFOA removal by Zn-Al LDH, but sulfate severely inhibited PFOA adsorption. Combined results of aqueous adsorption experiments and sorbent characterization suggested that electrostatic interactions may be the primary mechanism for PFOA adsorption onto LDHs. Our results suggested that cation composition of LDHs can have significant effect on the performance for PFCA removal.
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