Abstract
Understanding the interfacial dynamics of batteries is crucial to control degradation and
increase electrochemical performance and cycling life. If the chemical potential of a negative
electrode material lies outside of the stability window of an electrolyte (either solid or liquid),
a decomposition layer (interphase) will form at the interface. To better understand and control
degradation at interfaces in batteries, theoretical models describing the rate of formation of
these interphases are required. This study focuses on the growth kinetics of the interphase
forming between solid electrolytes and metallic negative electrodes in solid-state batteries. More
specifically, we demonstrate that the rate of interphase formation and metal plating during
charge can be accurately described by adapting the theory of coupled ion-electron transfer
(CIET). The model is validated by fitting experimental data presented in the first part of this
study. The data was collected operando as a Na metal layer was plated on top of a NaSICON
solid electrolyte (Na3.4Zr2Si2.4P0.6O12 or NZSP) inside a XPS chamber. This study highlights
the depth of information which can be extracted from this single operando experiment, and is
widely applicable to other solid-state electrolyte systems.
Supplementary materials
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Supplementary information
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The file contains additional sets of equations and simulation data.
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