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Analysis of Interfacial Effects in All-Solid-State Batteries with Thiophosphate Solid Electrolytes

Neumann, Anton and Randau, Simon and Becker-Steinberger, Katharina and Danner, Timo and Hein, Simon and Ning, Ziyang and Marrow, James and Richter, Felix H. and Janek, Jürgen and Latz, Arnulf (2020) Analysis of Interfacial Effects in All-Solid-State Batteries with Thiophosphate Solid Electrolytes. ACS Applied Materials and Interfaces, 12 (8), pp. 9277-9291. American Chemical society (ACS). doi: 10.1021/acsami.9b21404. ISSN 1944-8244.

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Official URL: https://pubs.acs.org/doi/10.1021/acsami.9b21404


All-solid-state batteries (ASSBs) present a promising route toward safe and high-power battery systems in order to meet the future demands in the consumer and automotive market. Composite cathodes are one way to boost the energy density of ASSBs compared to thin-film configurations. In this manuscript, we investigate composites consisting of Li3PS4 (LPS) solid electrolyte and high-energy Li(Ni0.6Mn0.2Co0.2)O2 (NMC622). The fabricated cells show a good cycle life with a satisfactory capacity retention. Still, the cathode utilization is below the values reported in the literature for systems with liquid electrolytes. The common understanding is that interface processes between the active material and solid electrolyte are responsible for the reduced performance. In order to throw some light on this topic, we perform 3D microstructure-resolved simulations on virtual samples obtained via X-ray tomography. Through this approach, we are able to correlate the composite microstructure with electrode performance and impedance. We identify the low electronic conductivity in the fully lithiated NMC622 as material inherent restriction preventing high cathode utilization. Moreover, we find that geometrical properties and morphological changes of the microstructure interact with the internal and external interfaces, significantly affecting the capacity retention at higher currents.

Item URL in elib:https://elib.dlr.de/139587/
Document Type:Article
Title:Analysis of Interfacial Effects in All-Solid-State Batteries with Thiophosphate Solid Electrolytes
AuthorsInstitution or Email of AuthorsAuthor's ORCID iD
Neumann, AntonAnton.Neumann (at) dlr.dehttps://orcid.org/0000-0002-4575-8697
Randau, SimonJustus-Liebig-Universität GießenUNSPECIFIED
Becker-Steinberger, KatharinaKatharina.Becker-Steinberger (at) dlr.deUNSPECIFIED
Danner, TimoTimo.Danner (at) dlr.dehttps://orcid.org/0000-0003-2336-6059
Hein, SimonSimon.Hein (at) dlr.dehttps://orcid.org/0000-0002-6728-9983
Ning, ZiyangUniversity of OxfordUNSPECIFIED
Marrow, JamesUniversity of OxfordUNSPECIFIED
Richter, Felix H.Justus-Liebig-Universität GießenUNSPECIFIED
Janek, JürgenJustus-Liebig-Universität GießenUNSPECIFIED
Latz, ArnulfArnulf.Latz (at) dlr.dehttps://orcid.org/0000-0003-1449-8172
Date:10 February 2020
Journal or Publication Title:ACS Applied Materials and Interfaces
Refereed publication:Yes
Open Access:Yes
Gold Open Access:No
In ISI Web of Science:Yes
DOI :10.1021/acsami.9b21404
Page Range:pp. 9277-9291
Publisher:American Chemical society (ACS)
Keywords:all-solid-state batteries thiophosphate solid electrolyte 3D microstructure-resolved simulations nickel-rich layered oxides impedance analysis
HGF - Research field:Energy
HGF - Program:Storage and Cross-linked Infrastructures
HGF - Program Themes:Electrochemical Energy Storage
DLR - Research area:Energy
DLR - Program:E SP - Energy Storage
DLR - Research theme (Project):E - Electrochemical Prcesses (Batteries) (old)
Location: Ulm
Institutes and Institutions:Institute of Engineering Thermodynamics > Computational Electrochemistry
Deposited By: Danner, Timo
Deposited On:16 Dec 2020 21:03
Last Modified:01 May 2021 03:00

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