Carbon Adsorbent Properties Impact Hydrated Electron Activity and Perfluorocarboxylic Acid (PFCA) Destruction

Abstract

Carbon-based adsorbents used to remove recalcitrant water contaminants, including perfluoroalkyl substances (PFAS), are often regenerated using energy-intensive treatments that can form harmful byproducts. We explore mechanisms for sorbent regeneration using hydrated electrons (e(aq) -) from sulfite ultraviolet photolysis (UV/sulfite) in water. We studied the UV/sulfite treatment on three carbon-based sorbents with varying material properties: granular activated carbon (GAC), carbon nanotubes (CNTs), and polyethylenimine-modified lignin (lignin). Reaction rates and defluorination of dissolved and adsorbed model perfluorocarboxylic acids (PFCAs), perfluorooctanoic acid (PFOA) and perfluorobutanoic acid (PFBA), were measured. Monochloroacetic acid (MCAA) was employed to empirically quantify e(aq) - formation rates in heterogeneous suspensions. Results show that dissolved PFCAs react rapidly compared to adsorbed ones. Carbon particles in solution decreased aqueous reaction rates by inducing light attenuation, e(aq) - scavenging, and sulfite consumption. The magnitude of these effects depended on adsorbent properties and surface chemistry. GAC lowered PFOA destruction due to strong adsorption. CNT and lignin suspensions decreased e(aq )- formation rates by attenuating light. Lignin showed high e(aq) - quenching, likely due to its oxygenated functional groups. These results indicate that desorbing PFAS and separating the adsorbent before initiating PFAS degradation reactions will be the best engineering approach for adsorbent regeneration using UV/sulfite.

Publisher

ACS Publications

Publication Date

8-1-2024

Publication Title

ACS ES&T Engineering

Department

Chemistry and Biochemistry

Document Type

Article

DOI

https://dx.doi.org/10.1021/acsestengg.4c00211

Keywords

PFAS, Hydrated electron, Carbon adsorbents, Regeneration, Advanced reduction process

Language

English

Format

text

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