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  1. Capacitive deionization (CDI) technologies have gained intense attention for water purification and desalination in recent years. Inexpensive and widely available porous carbon materials have enabled the fast growth of electrosorption research, highlighting the promise of CDI as a potentially cost-effective technology to remove ions. Whereas the main focus of CDI has been on bulk desalination, there has been a recent shift towards electrosorption for selective ion separations. Heavy metals are pollutants that can have severe health impacts and are present in both industrial wastewater and groundwater leachates. Heavy metal ions, such as chromium, cadmium, or arsenic, are of great concern to traditional treatment technologies, due to their low concentration and the presence of competing species. The modification/functionalization of porous carbon and recent developments of faradaic and redox-active materials have offered a new avenue for selective ion-binding of heavy metal contaminants. Here, we review the progress in electrosorptive technologies for heavy metal separations. We provide an overview of the wide applicability of carbon-based electrodes for heavy metal removal. In parallel, we highlight the trend toward modification of carbon materials, new developments in faradaic interfaces, and the underlying physico-chemical mechanisms that promote selective heavy metal separations. 
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  2. Abstract

    Electro‐responsive functional materials can play a critical role in selective metal recovery and recycling due to the need for molecular differentiation between transition metals in complex mixtures. Redox‐active metallopolymers are a promising platform for electrochemical separations, offering versatile structural tuning and fast electron transfer. First, through a judicious selection of polymer structure between a main‐chain metallopolymer (polyferrocenylsilane) and a pendant‐group metallopolymer (polyvinylferrocene), charge‐transfer interactions and binding strength toward competing metal ions are tuned, which as a result, dictate selectivity. For example, almost an order of magnitude increase in separation factor between chromate and meta‐vanadate can be achieved, depending on polymer structure. Second, these metallopolymer electrodes exhibit potential‐dependent selectivity that can even flip ion preference, based solely on electrical means—indicating a control parameter that is orthogonal to structural modifications. Finally, this work presents a framework for evaluating electrochemical separations in multicomponent ion mixtures and elucidates the underlying charge‐transfer mechanisms resulting in molecular selectivity through a combination of spectroscopy and electronic structure calculations. The findings demonstrate the applicability of redox‐metallopolymers in tailored electrochemical separations for environmental remediation, value‐added metal recovery, waste recycling, and even mining processing.

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  3. Abstract

    Advanced redox‐polymer materials offer a powerful platform for integrating electroseparations and electrocatalysis, especially for water purification and environmental remediation applications. The selective capture and remediation of trivalent arsenic (As(III)) is a central challenge for water purification due to its high toxicity and difficulty to remove at ultra‐dilute concentrations. Current methods present low ion selectivity, and require multistep processes to transform arsenic to the less harmful As(V) state. The tandem selective capture and conversion of As(III) to As(V) is achieved using an asymmetric design of two redox‐active polymers, poly(vinyl)ferrocene (PVF) and poly‐TEMPO‐methacrylate (PTMA). During capture, PVF selectively removes As(III) with exceptional uptake (>100 mg As/g adsorbent), and during release, synergistic electrocatalytic oxidation of As(III) to As(V) with >90% efficiency can be achieved by PTMA, a radical‐based redox polymer. The system demonstrates >90% removal efficiencies with real wastewater and concentrations of arsenic as low as 10 ppb. By integrating electron‐transfer through the judicious design of asymmetric redox‐materials, an order‐of‐magnitude energy efficiency increase can be achieved compared to non‐faradaic, carbon‐based materials. The study demonstrates for the first time the effectiveness of asymmetric redox‐active polymers for integrated reactive separations and electrochemically mediated process intensification for environmental remediation.

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