We describe a water treatment strategy, electrochemically tunable affinity separation (ETAS), which, unlike other previously developed electrochemical processes, targets uncharged organic pollutants in water. Key to achieving ETAS resides in the development of multicomponent polymeric nanostructures that simultaneously exhibit the following characteristics: an oxidation-state dependent affinity towards neutral organics, high porosity for sufficient adsorption capacity, and high conductivity to permit electrical manipulation. A prototype ETAS adsorbent composed of nanostructured binary polymeric surfaces that can undergo an electrically-induced hydrophilic-hydrophobic transition can provide programmable control of capture and release of neutral organics in a cyclic fashion. A quantitative energetic analysis of ETAS offers insights into the tradeoff between energy cost and separation extent through manipulation of electrical swing conditions. We also introduce a generalizable materials design approach to improve the separation degree and energetic efficiency simultaneously, and identify the critical factors responsible for such enhancement via redox electrode simulations and theoretical calculations of electron transfer kinetics. The effect of operation mode and multistage configuration on ETAS performance is examined, highlighting the practicality of ETAS and providing useful guidelines for its operation at large scale. The ETAS approach is energetically efficient, environmentally friendly, broadly applicable to a wide range of organic contaminants of various molecular structures, hydrophobicity and functionality, and opens up new avenues for addressing the urgent, global challenge of water purification and wastewater management.
Broader contextSeparation processes are of paramount importance in the chemical and environmental industries, accounting for 10-25% of the world's energy consumption, and about a third of total capital and operation costs in industrial plants. The development of separation technologies for water treatment with high energy efficiency and low environmental impact has become a primary engineering challenge for the 21st century due to the worldwide occurrence of water contamination and its associated negative impacts on the environment and human health. Electrochemically controlled processes, such as capacitive deionization, have emerged as promising candidates for wastewater management and water desalination. However, since these previously developed electrochemical methods rely primarily on the electrostatic interaction between the electrode and the target pollutant, they only work for charged species (e.g., anions, cations), and are not applicable to uncharged organic pollutants, which constitute the majority of industrial and municipal water contaminants, including many dyes, pesticides, pharmaceuticals and carcinogenic aromatics. This study investigates a conceptually novel separation strategy that enables sensitive, programmable electrochemical control over the release and capture of u...