The principal challenge for water remediation, across the U.S. and worldwide, are toxic contaminants in dilute concentrations. We focus on complex organic molecules including pharmaceuticals, endocrine inhibitors and pesticides, which are pollutants of emerging concern in many parts of the world.[1] These are often present in remote locations, such as agricultural sites in developing countries that are inaccessible to large-scale water treatment. Electrochemical methods are an attractive solution to address these problems due to their modularity, fast kinetics and possible integration with renewable energy.[2] We have developed a redox-mediated separation method based on organometallic-functionalized electrodes (e.g. ferrocene or cobaltocene) for the separation of target species under oxidizing and reducing conditions (Figure 1).[3] Many organic contaminants are anionic (e.g. carboxylates or sulfonates), thus selectivity based on chemical interactions is crucial. Rather than rely solely on charge or size, our redox-centers targets these compounds through specific chemical interactions. Moreover, electrochemical charge can be accumulated during the ion-selective adsorption, thus storing energy and decreasing costs. Here, we present the many levels of design, starting from the fundamental chemistry of binding between ions and organometallic receptor, to creating the heterogeneous electrode, and finally, integrating all these components into a flow device. We aim at applications in (1) water remediation, through targeting dilute organic contaminants in the aqueous phase, (2) tandem energy recovery by pseudocapacitive energy storage and (3) increasing sustainability in chemical processes, through the recovery of expensive synthesis products from catalysis by electrochemical adsorption, thus reducing organic waste and water usage. [1] a) Gilliom R.; Hamilton P. U.S. Geological Survey. 2014. (USGS fact sheet: http://pubs.usgs.gov/fs/2006/3028/). b) Doughton, C.G. and Thomas, A. T. (1999). EHP 107 (6), 907-938. [2] Suss, M. E.; et al. Energy & Environmental Science 2015. Zhao, R.; et al A. Water Res 2013, 47, 1941. [3] Su, X.; Kulik, H; Jamison, T.F.; Hatton, T. A. Submitted 2015. Under Review.

Redox-mediated electrochemical separations as a novel technology for water remediation and removal of trace contaminants

251st National Meeting (2016)

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