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Modeling the Electrical Double Layer at Solid-State Electrochemical Interfaces

13 Pages Posted: 16 Jul 2020 Publication Status: Review Complete

See all articles by Michael W. Swift

Michael W. Swift

Michigan State University - Department of Chemical and Materials Engineering

James W. Swift

Northern Arizona University - Department of Mathematics and Statistics

Yue Qi

Michigan State University - Department of Chemical and Materials Engineering

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Abstract

Models of the electrical double-layer (EDL) at electrode/liquid-electrolyte interfaces no longer hold for all-solid-state electrochemistry.  In this work, a new model for the EDL at a solid-state electrochemical interface based on the ``Poisson-Fermi-Dirac equation'' is formulated.  By combining this model with density functional theory predictions, the interconnected electronic and ionic degrees of freedom in all-solid-state batteries, including the electronic band bending and defect concentration variation in the space-charge layer, are captured self-consistently.  Along with a general mathematical solution, the EDL structure is presented in various materials that are thermodynamically stable in contact with a lithium metal anode: the solid electrolyte LLZO and the solid interlayer materials LiF, Li2O, and Li2CO3.  The model further predicts the optimum interlayer thicknesses to minimize the electrostatic barrier for lithium transport at relevant solid-state battery interfaces.

Keywords: energy storage, solid state batteries, electrical double layer, space-charge layer, interfacial impedance, interlayers, band bending, LLZO, LiPON, Lithium metal anode

Suggested Citation

Swift, Michael W. and Swift, James W. and Qi, Yue, Modeling the Electrical Double Layer at Solid-State Electrochemical Interfaces. Available at SSRN: https://ssrn.com/abstract=3636570 or http://dx.doi.org/10.2139/ssrn.3636570
This version of the paper has not been formally peer reviewed.

Michael W. Swift

Michigan State University - Department of Chemical and Materials Engineering

East Lansing, MI 48824-1122
United States

James W. Swift

Northern Arizona University - Department of Mathematics and Statistics

PO Box 15066
Flagstaff, AZ 86011
United States

Yue Qi (Contact Author)

Michigan State University - Department of Chemical and Materials Engineering

East Lansing, MI 48824-1122
United States

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