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An Asymmetric Iron-Based Redox-Active System for Electrochemical Separation of Ions in Aqueous Media

机译：一种非对称铁基氧化还原活性体系，用于水介质中离子的电化学分离

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Electrochemically mediated redox-active processes are gaining momentum as a promising liquid-phase separation technology. Compared to conventional systems, they offer potential benefits, such as smaller energy footprints, nondestructive operation, reversibility, and tunability for specific analyte removal, with clear applications to societal and industrial challenges like water treatment and chemical synthesis. An asymmetric Faradaic cell heterogeneously functionalized with a metallopolymer at the anode and a hexacyanoferrate material at the cathode is presented for the first time. The redox-active species' iron centers enhance the electrosorption of heavy metal oxyanions with up to 98% removal in the ppb range, and offer tunable operating windows as low as approximate to 0.1 V at approximate to 1 A m(-2). By avoiding water splitting, the hexacyanoferrate cathode imparts additional advantages, namely a four-fold reduction in adsorption energy requirements, full suppression of solution pH increase, and the ability to capture redox-active catalytic anions such as polyoxometalates without altering their bulk oxidation state. This hybrid framework of a polymeric ferrocene anode and crystalline hexacyanoferrate cathode allows for simultaneous and synergistic uptake of anions and cations, respectively, creating a new asymmetric scheme for water-based separations, with foreseeable future extension to fields such as ion-sensing, energy storage, and electrocatalysis.
机译：作为一种有前途的液相分离技术，电化学介导的氧化还原活性过程正获得发展势头。与传统系统相比，它们具有潜在的优势，例如较小的能源足迹，无损运行，可逆性和可去除特定分析物的可调性，可明确应用于社会和工业挑战，例如水处理和化学合成。首次提出了一种不对称的法拉第电池，该电池在阳极被金属聚合物异构化，在阴极被六氰合铁酸盐材料异构化。氧化还原活性物质的铁中心可提高重金属氧阴离子的电吸附能力，在ppb范围内去除率高达98％，并提供可调的工作窗口，在大约1 A m（-2）时可低至大约0.1V。通过避免水分解，六氰合铁酸盐阴极具有其他优点，即吸附能量需求降低了四倍，溶液pH值升高得到了完全抑制，并且能够捕获氧化还原活性催化阴离子（如多金属氧酸盐）而不会改变其整体氧化态。聚合二茂铁阳极和结晶六氰合铁酸盐阴极的混合框架分别允许同时和协同吸收阴离子和阳离子，为水基分离创造了新的不对称方案，可预见的将来将扩展到离子传感，储能等领域和电催化。

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