Abstract

Graphene and zero-valent-iron based nanohybrid (rGO-nZVI NH) with oxidant H2O2 can remove perfluorooctanoic acid (PFOA) and perfluorooctane sulfonic acid (PFOS) through adsorption-degradation in a controlled aquatic environment. In this study, we evaluated how and to what extent different environmental and operational parameters, such as initial PFAS concentration, H2O2 dose, pH, ionic strength, and natural organic matter (NOM), influenced the removal of PFOS and PFOA by rGO-nZVI. With the increase in initial PFAS concentration (from 0.4 to 50 ppm), pH (3 to 9), ionic strength (0 to 100 mM), and NOM (0 to 10 ppm), PFOS removal reduced by 20%, 30%, 2%, and 6%, respectively, while PFOA removal reduced by 54%, 76%, 11%, and 33% respectively. In contrast, PFOS and PFOA removal increased by 10% and 41%, respectively, with the increase in H2O2 (from 0 to 1 mM). Overall, the effect of changes in environmental and operational parameters was more pronounced for PFOA than PFOS. Mechanistically, •OH radical generation and availability showed a profound effect on PFOA removal. Also, the electrostatic interaction between rGO-nZVI NH and deprotonated PFAS compounds was another key factor for removal. Most importantly, our study confirms that rGO-nZVI in the presence of H2O2 can degrade both PFOS and PFOA to some extent by identifying the important by-products such as acetate, formate, and fluoride.

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