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Molecular Tuning of Redox-Copolymers for Selective Electrochemical Remediation

机译：用于选择性电化学修复的氧化还原共聚物的分子调谐

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Molecular design of redox-materials provides a promising technique for tuning physicochemical properties which are critical for selective separations and environmental remediation. Here, the structural tuning of redox-copolymers, 4-methacryloyloxy-2,2,6,6-tetramethylpiperidin-1-oxyl (TMA) and 4-methacryloyloxy-2,2,6,6-tetramethylpiperidine (TMPMA), denoted as P(TMA(x)-co-TMPMA(1-)(x)), is investigated for the selective separation of anion contaminants ranging from perfluorinated substances to halogenated aromatic compounds. The amine functional groups provide high affinity toward anionic functionalities, while the redox-active nitroxyl radical groups promote electrochemically-controlled capture and release. Controlling the ratio of amines to nitroxyl radicals provides a pathway for tuning the redox-activity, hydrophobicity, and binding affinity of the copolymer, to synergistically enhance adsorption and regeneration. P(TMA(x)-co-TMPMA(1-)(x)) removes a model perfluorinated compound (perfluorooctanoic acid (PFOA)) with a high uptake capacity (1000 mg g(-1)) and separation factors (500 vs chloride), and demonstrates exceptional removal efficiencies in diverse per- and polyfluoroalkyl substances (PFAS) and halogenated aromatic compounds, in various water matrices. Integration with a boron-doped diamond electrode allows for tandem separation and destruction of pollutants within the same electrochemical cell, enabling the energy integration of the separation step with the catalytic degradation step. The study demonstrates for the first time the tuning of redox-copolymers for selective remediation of organic anions, and integration with an advanced electrochemical oxidation process for energy-efficient water purification.
机译：氧化还原材料的分子设计提供了一种用于调整物理化学性质的有希望的技术，这对于选择性分离和环境修复至关重要。这里，氧化还原共聚物，4-甲基丙烯酰氧基-2,2,6,6-四甲基哌啶-1-氧基（TMA）和4-甲基丙烯酰氧基-2,2,6,6-四甲基哌啶（TMPMA）的结构调整，表示为P（TMA（X）-CO-TMPMA（1 - ）（X））研究，用于选择性分离来自全氟化物质对卤代芳族化合物的阴离子污染物。胺官能团对阴离子官能团提供高亲和力，而氧化还原活性硝基根基自由基促进电化学控制的捕获和释放。控制胺与硝基氧基的比例提供了用于调节共聚物的氧化还原活性，疏水性和结合亲和力的途径，以协同增强吸附和再生。 P（TMA（x）-co-tmpma（1 - ）（x））除去具有高吸收能力（> 1000mg g（-1））和分离因子的模型全氟化化合物（全氟辛酸（PFOA））（500 vs氯化物），并在各种水基质中展示了各种（PFAS）和卤代芳族化合物中不同的去除效率。与掺杂金刚石电极的整合允许串联分离和破坏相同电化学电池内的污染物，使得分离步骤能够与催化降解步骤的能量集成。该研究表明，首次调整氧化还原共聚物以选择性地修复有机阴离子，以及与先进的电化学氧化过程集成，以节能水净化。

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