Electrifying separation processes can be an important avenue for integrating renewable energy into traditionally energy processes, and promoting sustainability by minimizing chemical waste. Separation processes play a critical role in water purification and chemical and biomolecular manufacturing, and can often be the most energy-intensive step in an industrial process. Here, we will discuss the engineering of redox-interfaces for achieving molecular selectivity in electrosorption processes, with a focus on wastewater treatment and environmnetal remediation. The design of electrochemically-driven binding interactions is presented, by leveraging redox-active polymers as flexible platforms for controlling charge-transfer and hydrophilic/hydrophobic properties. First, we discuss the molecular design of copolymers for the selective binding of per- and polyfluoroalkyl substances (PFAS), including the co-operative interactions required for enhancing binding and regeneration towards these persistent pollutants. We explore the electrochemical capture of long-chain, short-chain as well as fluorotelomer PFAS. Next, we discuss opportunities for the integration of contaminant removal and destruction by electrochemical approaches, such as the tandem capture and defluorination of PFAS, or the electrooxidation of transition metals. Leveraging these same reactive separation concepts, we also discuss opportunities for the valorization of waste streams, especially nitrogenous compounds. From a fundamental perspective, these concepts point towards an emerging direction in electrochemical interface design – by superimposing specific molecular interactions, we can reach beyond double-layer effects to achieve precision separations. In parallel, through judicious electrochemical engineering, we demonstrated that reaction and separation steps can be coupled for energy-efficient environmental remediation and resource recovery contexts.

Electrochemically-driven reactive separations for environmental remediation and resource recovery

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ACS Spring 2023

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