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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-fu