Non-equilibrium thermodynamics of mixed ionic-electronic conductive electrodes and their interfaces: a Ni/CGO study

Williams, Nicholas J.; Seymour, Ieuan D.; Leah, Robert; Banerjee, Aayan; Mukerjee, Subhasish; Skinner, Stephen

doi:10.1039/d1ta07351f

Cited by 9 publications

(5 citation statements)

References 42 publications

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“…The (electro)chemical potential, μ i (eV), of a mobile species in an electrochemical system is expressed as − μ i = μ i normalΘ + k normalB T nobreak0em0.25em⁢ ln nobreak0em.25em⁡ a i + z i e ϕ i = k normalB T nobreak0em0.25em⁢ ln nobreak0em.25em⁡ c i + μ i ex where μ i o , a i , and ϕ i represent the standard chemical potential, activity, and electrostatic potential of species i . The activity ( a i = γ i c i ) is the product of the concentration and activity coefficient, which is a measure of the nonideality of the (electro)chemical potential using the excess chemical potential (μ i ex ) which collects all nonidealities of species i . , Here, we use the definition of (electro)chemical potential, meaning that if the species of interest is charged, we find the electrochemical potential, and if the species of interest is neutral, we find the chemical potential.…”

Section: Theorymentioning

confidence: 99%

Operando Characterization and Theoretical Modeling of Metal|Electrolyte Interphase Growth Kinetics in Solid-State Batteries. Part II: Modeling

et al. 2023

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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 an 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.

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Section: Theorymentioning

confidence: 99%

Operando Characterization and Theoretical Modeling of Metal|Electrolyte Interphase Growth Kinetics in Solid-State Batteries. Part II: Modeling

et al. 2023

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“…The (electro)chemical potential, µ i (eV), of a mobile species in an electrochemical system is expressed as: [12][13][14][15][16]…”

Section: Theorymentioning

confidence: 99%

Operando characterization and theoretical modelling of metal|electrolyte interphase growth kinetics in solid-state-batteries - Part II: Modelling

Quérel

Seymour

Skinner

et al. 2022

Preprint

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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.

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“…natural gas) and future fuel (i.e. renewably sourced hydrogen) infrastructures [1][2][3][4]. Electrochemical devices, such as solid-oxide fuel cells (SOFCs), allow for reversible chemical to electrical energy conversion, with efficiency surpassing that of the combustion engine [5].…”

Section: Introductionmentioning

confidence: 99%

Application of Finite Gaussian Process Distribution of Relaxation Times on Sofc Electrodes

Williams

Osborne²,

Seymour

et al. 2023

Preprint

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Non-equilibrium thermodynamics of mixed ionic-electronic conductive electrodes and their interfaces: a Ni/CGO study

Abstract: Non-equilibrium thermodynamics describe the current-voltage characteristics of electrochemical devices. For conventional electrode-electrolyte interfaces, the local activation overpotential is used to describe the electrostatic potential step between the two materials as...

Cited by 9 publications

References 42 publications

Operando Characterization and Theoretical Modeling of Metal|Electrolyte Interphase Growth Kinetics in Solid-State Batteries. Part II: Modeling

Operando Characterization and Theoretical Modeling of Metal|Electrolyte Interphase Growth Kinetics in Solid-State Batteries. Part II: Modeling

Operando characterization and theoretical modelling of metal|electrolyte interphase growth kinetics in solid-state-batteries - Part II: Modelling

Application of Finite Gaussian Process Distribution of Relaxation Times on Sofc Electrodes

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