Issue 12, 2021

Emerging investigator series: electrochemically-mediated remediation of GenX using redox-copolymers

Abstract

Per- and polyfluorinated alkyl substances (PFAS) are persistent contaminants that have been continuously detected in groundwater and drinking water around the globe. Hexafluoropropylene oxide dimer acid (tradename GenX) has been used to substitute traditional PFAS, such as PFOA, but its intense use has caused widespread occurrence in water streams and often in high levels. Here, we evaluate a redox-copolymer, poly(4-methacryloyloxy-2,2,6,6-tetramethylpiperidin-1-oxyl-co-4-methacryloyloxy-2,2,6,6-tetramethylpiperidine) (PTMA-co-PTMPMA), for the selective electrochemical removal of GenX. The amine functional groups promote affinity towards the anionic PFAS, and the redox-active nitroxide radicals provide electrochemical control for adsorption and desorption. Faster kinetics and higher uptake (>475 mg g−1 adsorbent) were obtained with the redox-copolymer when applying 0.8 V vs. Ag/AgCl potential compared to open circuit. The copolymer electrosorbents were evaluated over a wide pH range and diverse water matrices, with electrostatic-based mechanisms dependent on the state of protonation of the PFAS. Moreover, we translated the redox-electrodes from a batch to flow-by cell configuration, showing successful adsorption and release of GenX under flow and electrochemical control. Finally, prolonged exposure of GenX at reduction potentials generated smaller PFAS fragments at the redox-electrodes. To fully defluorinate GenX, the copolymer-functionalized electrodes were coupled with a boron-doped diamond (BDD) counter electrode for integrating separation and defluorination within the same device. The combined system demonstrated close to 100% defluorination efficiency. Thus, we highlight the potential of electroactive redox platforms for the reactive separation of fluorotelomers, and point to future directions for their practical implementation for water treatment.

Graphical abstract: Emerging investigator series: electrochemically-mediated remediation of GenX using redox-copolymers

Supplementary files

Article information

Article type
Paper
Submitted
21 ذو الحجة 1442
Accepted
23 صفر 1443
First published
23 صفر 1443

Environ. Sci.: Water Res. Technol., 2021,7, 2231-2240

Author version available

Emerging investigator series: electrochemically-mediated remediation of GenX using redox-copolymers

P. Baldaguez Medina, S. Cotty, K. Kim, J. Elbert and X. Su, Environ. Sci.: Water Res. Technol., 2021, 7, 2231 DOI: 10.1039/D1EW00544H

To request permission to reproduce material from this article, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements