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Lithium Battery Electrolyte Stability and Performance from Molecular Modeling and Simulations

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Batteries for Sustainability

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Abstract

Lithium batteries are complex devices whose performance optimization necessitates that they be well understood on multiple timescales and length scales, ranging from systems level to molecular. Optimization of the electrolyte, in particular, requires detailed, fundamental, molecular-level understanding of the chemical features that lead to stable electrolytes with large electrochemical windows – what electrolyte solvents and additives facilitate the formation of stable solid electrolyte interface layers and which features of the electrolyte result in good bulk and interfacial lithium transport properties as well as thermal stability, low-temperature transport, and low volatility/high safety [1, 2].

This chapter was originally published as part of the Encyclopedia of Sustainability Science and Technology edited by Robert A. Meyers. DOI:10.1007/978-1-4419-0851-3

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Abbreviations

Interfacial impedance:

The resistance to lithium motion at the interface between the electrolyte and an electrode due to structure imposed on the electrolyte by the electrode, barriers to intercalation into the electrode, lithium desolvation energy, and/or the SEI layer.

Ionic liquid electrolyte:

An electrolyte comprised of a lithium salt dissolved in a room-temperature ionic liquid.

One-electron reduction:

The reduction of an electrolyte molecule by a single electron resulting in formation of species believed to be important contributors to the outer part of the SEI.

Organic liquid electrolyte:

An electrolyte comprised of a lithium salt dissolved in liquid carbonates, esters, ethers, or a mixture thereof.

Oxidative stability:

The ability of an electrolyte to remain electrochemically stable against oxidation at the surface of the cathode.

SEI layer:

The layer of electrolyte decomposition products that forms at the interface between an electrode (primarily the anode) and the electrolyte, called the solid electrolyte interphase or solid electrolyte interface. The SEI is believed to be comprised of an inner SEI layer and an outer SEI layer.

Solid polymer electrolyte:

An electrolyte comprised of a lithium salt dissolved in a polymer matrix.

Two-electron reduction:

The reduction of an electrolyte molecule by two electrons resulting in formation of species believed to be important contributors to the inner part of the SEI.

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Acknowledgments

The authors are grateful to the Department of Energy under Contract grant DE-SC0001912 to University of Utah and Air Force Office of Scientific Research contract number FA9550-09-C-0110 for the financial support of this work. We would also like to thank T. Richard Jow and Phil Ross for their comments and suggestions. This work was partially supported by an Interagency Agreement between the U.S. Department of Energy and the U.S. Army Research Laboratory under DE-IAOI-11EE003413 for the office of vehicle technologies programs including Batteries for Advanced Transporation Technologies (BATT) program.

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Authors and Affiliations

  1. Department of Materials Science and Engineering, University of Utah, Salt Lake City, UT, 84112, USA

    Grant D. Smith & Oleg Borodin

  2. Electrochemistry Branch, SEDD, AMSRD–ARL–RDRL–SED–C, 2800 Powder Mill Rd, Adelphi, MD, 20783, USA

    Oleg Borodin

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    Ralph J. Brodd

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Smith, G.D., Borodin, O. (2013). Lithium Battery Electrolyte Stability and Performance from Molecular Modeling and Simulations. In: Brodd, R. (eds) Batteries for Sustainability. Springer, New York, NY. https://doi.org/10.1007/978-1-4614-5791-6_7

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