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Highly Reversible Conversion-Type FeOF Composite Electrode with Extended Lithium Insertion by Atomic Layer Deposition LiPON Protection

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Department of Materials Science and Engineering, University of Maryland, College Park, Maryland 20742, United States
Institute for Systems Research, University of Maryland, College Park, Maryland 20740, United States
§ Department of Chemical and Biomolecular Engineering, University of Maryland, College Park, Maryland 20740, United States
Department of Chemistry, Bar-Ilan University, Ramat Gan 52900, Israel
Department of Materials and Interfaces, Weizmann Institute of Science, Rehovot 76100, Israel
# AIM Laboratory, Nano Center, University of Maryland, College Park, Maryland 20742, United States
@ Department of Chemistry and Biochemistry, University of Maryland, College Park, Maryland 20742, United States
Cite this: Chem. Mater. 2017, 29, 20, 8780–8791
Publication Date (Web):September 28, 2017
https://doi.org/10.1021/acs.chemmater.7b03058
Copyright © 2017 American Chemical Society

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    Abstract

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    High-energy conversion electrodes undergo successive Li insertion and conversion during lithiation. A primary scientific obstacle to harnessing the potentially high lithium storage capabilities of conversion electrode materials has been the formation of insulating new phases throughout the conversion reactions. These new phases are chemically stable, and electrochemically irreversible if formed in large amounts with coarsening. Herein, we synthesized FeOF conversion material as a model system and mechanistically demonstrate that a thin solid electrolyte [lithium phosphorus oxynitride (LiPON)] atomic layer deposition-deposited on the composite electrode extends the Li insertion process to higher concentrations, delaying the onset of a parasitic chemical conversion reaction and rendering the redox reaction of the protected conversion electrode electrochemically reversible. Reversibility is demonstrated to at least 100 cycles, with the LiPON protective coating increasing capacity retention from 29 to 89% at 100 cycles. Pursuing the chemical mechanism behind the boosted electrochemical reversibility, we conducted electron energy-loss spectroscopy, X-ray photoelectron spectroscopy, solid-state nuclear magnetic resonance, and electrochemical measurements that unrevealed the suppression of undesired phase formation and extended lithium insertion of the coated electrode. Support for the delayed consequences of the conversion reaction is also obtained by high-resolution transmission electron microscopy. Our findings strongly suggest that undesired new phase formation upon lithiation of electrode materials can be suppressed in the presence of a thin protection layer not only on the surface of the coated electrode but also in the bulk of the material through mechanical confinement that modulates the electrochemical reaction.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.chemmater.7b03058.

    • Additional experimental methods and details, XRD data, XPS spectrum, TEM micrographs, solid-state NMR description, and cyclic voltammograms (PDF)

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