Molecularly Selective Polymer Interfaces for Electrochemical Separations

The molecular design of polymer interfaces has been key for advancing electrochemical separation processes. Precise control of molecular interactions at electrochemical interfaces has enabled the removal or recovery of charged species with enhanced selectivity, capacity, and stability. In this Perspective, we provide an overview of recent developments in polymer interfaces applied to liquid-phase electrochemical separations, with a focus on their role as electrosorbents as well as membranes in electrodialysis systems. In particular, we delve into both the single-site and macromolecular design of redox polymers and their use in heterogeneous electrochemical separation platforms. We highlight the significance of incorporating both redox-active and non-redox-active moieties to tune binding toward ever more challenging separations, including structurally similar species and even isomers. Furthermore, we discuss recent advances in the development of selective ion-exchange membranes for electrodialysis and the critical need to control the physicochemical properties of the polymer. Finally, we share perspectives on the challenges and opportunities in electrochemical separations, ranging from the need for a comprehensive understanding of binding mechanisms to the continued innovation of electrochemical architectures for polymer electrodes.