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Switchable electrolyte properties and redox chemistry in aqueous media based on temperature-responsive polymers

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Abstract

Macromolecular ionomer solutions exhibiting macroscopic properties that change in response to temperature are referred to as thermally responsive polymer electrolytes (RPEs). Such materials provide a means to control electrochemical systems using an external stimulus that affects the polymer phase behavior and electrolyte properties. RPEs were synthesized with N-isopropylacrylamide, which governs the thermal properties, and varying fractions of acrylic acid, which provides ionic properties. These polymers undergo a thermally activated phase separation in aqueous solutions at a given temperature, thereby altering the ionic strength, pH, and conductivity of the electrolyte solution. In this article, we demonstrate how the molecular properties of RPEs, specifically the ionic composition, influence the temperature-dependent electrolyte properties and the extent to which these electrolytes can control the activity of redox electrodes. Materials with high ionic content provide the highest room temperature ion conductivity and redox activity; however, RPEs with low ionic content provide the highest “on–off” ratio in electrochemical activity at elevated temperatures.

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Acknowledgments

M.E.R. acknowledges partial support from the 3 M Non-Tenured Faculty Grant. A portion of this work was performed at the Center for Integrated Nanotechnologies, a U.S. Department of Energy, Office of Basic Energy Sciences user facility. Sandia National Laboratories is a multi-program laboratory operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy’s National Nuclear Security Administration under contract DE-AC04-94AL85000. The authors declare no competing financial interest.

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Authors and Affiliations

  1. Department of Chemical & Biomolecular Engineering, Clemson University, 127 Earle Hall, Clemson, SC, 29634, USA

    Jesse C. Kelly & Mark E. Roberts

  2. Center for Integrated Nanotechnologies, Sandia National Laboratories, Albuquerque, NM, 87123, USA

    Dale L. Huber & Andrew D. Price

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  1. Jesse C. Kelly
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  2. Dale L. Huber
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  3. Andrew D. Price
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  4. Mark E. Roberts
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Correspondence to Mark E. Roberts.

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Kelly, J.C., Huber, D.L., Price, A.D. et al. Switchable electrolyte properties and redox chemistry in aqueous media based on temperature-responsive polymers. J Appl Electrochem 45, 921–930 (2015). https://doi.org/10.1007/s10800-015-0839-7

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  • DOI: https://doi.org/10.1007/s10800-015-0839-7

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