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Interplay of Dynamic Constriction and Interface Morphology between Reversible Metal Anode and Solid Electrolyte in Solid State Batteries

[Image: see text] In an all-solid-state battery, the electrical contact between its individual components is of key relevance in addition to the electrochemical stability of its interfaces. Impedance spectroscopy is particularly suited for the non-destructive investigation of interfaces and of their...

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Autores principales: Eckhardt, Janis K., Klar, Peter J., Janek, Jürgen, Heiliger, Christian
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2022
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9376931/
https://www.ncbi.nlm.nih.gov/pubmed/35878322
http://dx.doi.org/10.1021/acsami.2c07077
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author Eckhardt, Janis K.
Klar, Peter J.
Janek, Jürgen
Heiliger, Christian
author_facet Eckhardt, Janis K.
Klar, Peter J.
Janek, Jürgen
Heiliger, Christian
author_sort Eckhardt, Janis K.
collection PubMed
description [Image: see text] In an all-solid-state battery, the electrical contact between its individual components is of key relevance in addition to the electrochemical stability of its interfaces. Impedance spectroscopy is particularly suited for the non-destructive investigation of interfaces and of their stability under load. Establishing a valid correlation between microscopic processes and the macroscopic impedance signal, however, is challenging and prone to errors. Here, we use a 3D electric network model to systematically investigate the effect of various electrode/sample interface morphologies on the impedance spectrum. It is demonstrated that the interface impedance generally results from a charge transfer step and a geometric constriction contribution. The weights of both signals depend strongly on the material parameters as well as on the interface morphology. Dynamic constriction results from a non-ideal local contact, e.g., from pores or voids, which reduce the electrochemical active surface area only in a certain frequency range. Constriction effects dominate the interface behavior for systems with small charge transfer resistance like garnet-type solid electrolytes in contact with a lithium metal electrode. An in-depth analysis of the origin and the characteristics of the constriction phenomenon and their dependence on the interface morphology is conducted. The discussion of the constriction effect provides further insight into the processes at the microscopic level, which are, e.g., relevant in the case of reversible metal anodes.
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spelling pubmed-93769312022-08-16 Interplay of Dynamic Constriction and Interface Morphology between Reversible Metal Anode and Solid Electrolyte in Solid State Batteries Eckhardt, Janis K. Klar, Peter J. Janek, Jürgen Heiliger, Christian ACS Appl Mater Interfaces [Image: see text] In an all-solid-state battery, the electrical contact between its individual components is of key relevance in addition to the electrochemical stability of its interfaces. Impedance spectroscopy is particularly suited for the non-destructive investigation of interfaces and of their stability under load. Establishing a valid correlation between microscopic processes and the macroscopic impedance signal, however, is challenging and prone to errors. Here, we use a 3D electric network model to systematically investigate the effect of various electrode/sample interface morphologies on the impedance spectrum. It is demonstrated that the interface impedance generally results from a charge transfer step and a geometric constriction contribution. The weights of both signals depend strongly on the material parameters as well as on the interface morphology. Dynamic constriction results from a non-ideal local contact, e.g., from pores or voids, which reduce the electrochemical active surface area only in a certain frequency range. Constriction effects dominate the interface behavior for systems with small charge transfer resistance like garnet-type solid electrolytes in contact with a lithium metal electrode. An in-depth analysis of the origin and the characteristics of the constriction phenomenon and their dependence on the interface morphology is conducted. The discussion of the constriction effect provides further insight into the processes at the microscopic level, which are, e.g., relevant in the case of reversible metal anodes. American Chemical Society 2022-07-25 2022-08-10 /pmc/articles/PMC9376931/ /pubmed/35878322 http://dx.doi.org/10.1021/acsami.2c07077 Text en © 2022 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by-nc-nd/4.0/Permits non-commercial access and re-use, provided that author attribution and integrity are maintained; but does not permit creation of adaptations or other derivative works (https://creativecommons.org/licenses/by-nc-nd/4.0/).
spellingShingle Eckhardt, Janis K.
Klar, Peter J.
Janek, Jürgen
Heiliger, Christian
Interplay of Dynamic Constriction and Interface Morphology between Reversible Metal Anode and Solid Electrolyte in Solid State Batteries
title Interplay of Dynamic Constriction and Interface Morphology between Reversible Metal Anode and Solid Electrolyte in Solid State Batteries
title_full Interplay of Dynamic Constriction and Interface Morphology between Reversible Metal Anode and Solid Electrolyte in Solid State Batteries
title_fullStr Interplay of Dynamic Constriction and Interface Morphology between Reversible Metal Anode and Solid Electrolyte in Solid State Batteries
title_full_unstemmed Interplay of Dynamic Constriction and Interface Morphology between Reversible Metal Anode and Solid Electrolyte in Solid State Batteries
title_short Interplay of Dynamic Constriction and Interface Morphology between Reversible Metal Anode and Solid Electrolyte in Solid State Batteries
title_sort interplay of dynamic constriction and interface morphology between reversible metal anode and solid electrolyte in solid state batteries
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9376931/
https://www.ncbi.nlm.nih.gov/pubmed/35878322
http://dx.doi.org/10.1021/acsami.2c07077
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