Photoactive Polyethylenimine-Coated Graphene Oxide Composites for Enhanced Cr(VI) Reduction and Recovery

The application of positively charged polymers is a common treatment strategy for the sorption and separation of dissolved hexavalent chromium Cr(VI). In particular, polyethylenimine (PEI) has been demonstrated as an effective polymer for Cr treatment due to abundant amine groups and cost-effectiveness. However, PEI as a photoactive polymer has not been previously explored for Cr treatment. Toward this, we demonstrate the significant photoactive potential of PEI for Cr sorption and reduction [to Cr (III)], delineating amine structure-function relationships. Overall, Cr(VI) photoreduction is enhanced dramatically as a function of amine group density. Additionally, among the types of amine groups evaluated, tertiary amines are observed to be the most reactive followed by secondary and primary amines. When PEI is incorporated onto graphene oxide (GO) as a stabilizing scaffold, mass loading of PEI is a key variable for Cr(VI) treatment performance, which is observed to be a function of PEI molecular weight and oxidation extent of GO. Finally, when combined with magnetic nanomaterials, low energy, high efficiency separation, and reuse are demonstrated. For these, sorption-based separation processes maintained excellent performance over five cycles. Taken together, this work demonstrates that PEI can serve as highly effective, multifunctional material coating(s) not only for chromium treatment but potentially for other oxidized aqueous species as well.