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ETAS relies on the use of a stimulus-responsive adsorbent system that has surface hydrophobicity programmable by an electrical signal. Such an adsorbent displays an electrically-controlled affinity toward neutral organic molecules, enabling the use of exquisite electrical swing to release and capture organics cyclically. The key to achieving ETAS resides in the development of multicomponent polymeric nanostructures that simultaneously exhibit an oxidation-state dependent affinity towards neutral organics, high porosity for sufficient adsorption capacity, and high conductivity to permit electrical manipulation. The ETAS absorbent system consists of a carbon cloth (CC) that serves as a flexible and robust conductive substrate, with a conformal coating of a polyvinylferrocene/polypyrrole (PVF/PPY) composite. The binary polymer film is fabricated via simultaneous electro-polymerization of pyrrole and electrodeposition of PVF. The ferrocene moieties in PVF render redox-tunable hydrophobicity while the conjugated PPY chains establish electron transport pathways to permit electrical control. Furthermore, through redox electrode simulations and theoretical calculations of electron transfer kinetics, a generalizable material design strategy is developed to simultaneously improve the separation degree and energetic efficiency during ETAS operation.