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Published August 2, 2007 | public
Journal Article Open

Reversible Intercalation of Fluoride-Anion Receptor Complexes in Graphite

Abstract

We have demonstrated a route to reversibly intercalate fluoride-anion receptor complexes in graphite via a nonaqueous electrochemical process. This approach may find application for a rechargeable lithium–fluoride dual-ion intercalating battery with high specific energy. The cell chemistry presented here uses graphite cathodes with LiF dissolved in a nonaqueous solvent through the aid of anion receptors. Cells have been demonstrated with reversible cathode specific capacity of approximately 80 mAh/g at discharge plateaus of upward of 4.8 V, with graphite staging of the intercalant observed via in situ synchrotron X-ray diffraction during charging. Electrochemical impedance spectroscopy and 11B nuclear magnetic resonance studies suggest that co-intercalation of the anion receptor with the fluoride occurs during charging, which likely limits the cathode specific capacity. The anion receptor type dictates the extent of graphite fluorination, and must be further optimized to realize high theoretical fluorination levels. To find these optimal anion receptors, we have designed an ab initio calculations-based scheme aimed at identifying receptors with favorable fluoride binding and release properties.

Additional Information

©2007 The Electrochemical Society (Submitted: 22 February 2007; revised: 24 May 2007; published online: 2 August 2007) This work was carried out at the Jet Propulsion Laboratory, California Institute of Technology, under contract with the National Aeronautics and Space Administration, funded through the JPL Research and Technology Development fund. The authors thank S. Surampudi for providing guidance throughout the project and Adri van Duin for valuable comments on the theoretical section. Portions of this research were carried out at the Stanford Synchrotron Radiation Laboratory, a national user facility operated by Stanford University on behalf of the U.S. Department of Energy, Office of Basic Energy Sciences. California Institute of Technology assisted in meeting the publication costs of this article.

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August 22, 2023
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