Chemical compatibility at the interface of garnet-type Ga-LLZO solid electrolyte and high-energy Li-rich layered oxide cathode for all-solid-state batteries

Abstract All-solid-state batteries (ASSBs) with a garnet-type solid electrolyte have been considered promising alternatives to traditional batteries with a liquid organic electrolyte, due to their enhanced safety and ability to accommodate high energy density electrodes. In this study, we conducted...

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Main Authors: Natalia B. Timusheva, Alexander A. Golubnichiy, Anatolii V. Morozov, Arseniy S. Burov, Dmitry A. Aksyonov, Aleksandra A. Savina, Roman G. Markopolskii, Artem M. Abakumov
Format: Article
Language:English
Published: Nature Portfolio 2025-01-01
Series:Scientific Reports
Online Access:https://doi.org/10.1038/s41598-024-78927-w
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author Natalia B. Timusheva
Alexander A. Golubnichiy
Anatolii V. Morozov
Arseniy S. Burov
Dmitry A. Aksyonov
Aleksandra A. Savina
Roman G. Markopolskii
Artem M. Abakumov
author_facet Natalia B. Timusheva
Alexander A. Golubnichiy
Anatolii V. Morozov
Arseniy S. Burov
Dmitry A. Aksyonov
Aleksandra A. Savina
Roman G. Markopolskii
Artem M. Abakumov
author_sort Natalia B. Timusheva
collection DOAJ
description Abstract All-solid-state batteries (ASSBs) with a garnet-type solid electrolyte have been considered promising alternatives to traditional batteries with a liquid organic electrolyte, due to their enhanced safety and ability to accommodate high energy density electrodes. In this study, we conducted a comprehensive investigation of the high-temperature chemical compatibility between the garnet-like Li6.4Ga0.2La3Zr2O12 (Ga-LLZO) electrolyte and high-energy-density Li-rich layered Li1.2Ni0.2Mn0.6O2 cathode (LNM). Our findings suggest that a high temperature reaction between the Li-rich cathode and Ga-LLZO occurs at 700-900oC depending on the form of reactants. This reaction results in the formation of La(Ni, Mn)O3 and Li2ZrO3 as the two main products, as confirmed by powder X-ray diffraction and transmission electron microscopy analysis. Li2ZrO3 was discovered for the first time as a reaction product, and its formation in the case of Li-rich layered cathode material was rationalized with DFT + U calculations. The results were also compared with those obtained for a typical layered high-energy-density cathode material LiNi0.8Mn0.1Co0.1O2 (NMC811).
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spelling doaj-art-25086c53280a43f7bae2256bb58cb57a2025-01-05T12:23:10ZengNature PortfolioScientific Reports2045-23222025-01-0115111510.1038/s41598-024-78927-wChemical compatibility at the interface of garnet-type Ga-LLZO solid electrolyte and high-energy Li-rich layered oxide cathode for all-solid-state batteriesNatalia B. Timusheva0Alexander A. Golubnichiy1Anatolii V. Morozov2Arseniy S. Burov3Dmitry A. Aksyonov4Aleksandra A. Savina5Roman G. Markopolskii6Artem M. Abakumov7Center for Energy Science and Technology, Skolkovo Institute of Science and TechnologyCenter for Energy Science and Technology, Skolkovo Institute of Science and TechnologyCenter for Energy Science and Technology, Skolkovo Institute of Science and TechnologyCenter for Energy Science and Technology, Skolkovo Institute of Science and TechnologyCenter for Energy Science and Technology, Skolkovo Institute of Science and TechnologyCenter for Energy Science and Technology, Skolkovo Institute of Science and TechnologyCenter for Energy Science and Technology, Skolkovo Institute of Science and TechnologyCenter for Energy Science and Technology, Skolkovo Institute of Science and TechnologyAbstract All-solid-state batteries (ASSBs) with a garnet-type solid electrolyte have been considered promising alternatives to traditional batteries with a liquid organic electrolyte, due to their enhanced safety and ability to accommodate high energy density electrodes. In this study, we conducted a comprehensive investigation of the high-temperature chemical compatibility between the garnet-like Li6.4Ga0.2La3Zr2O12 (Ga-LLZO) electrolyte and high-energy-density Li-rich layered Li1.2Ni0.2Mn0.6O2 cathode (LNM). Our findings suggest that a high temperature reaction between the Li-rich cathode and Ga-LLZO occurs at 700-900oC depending on the form of reactants. This reaction results in the formation of La(Ni, Mn)O3 and Li2ZrO3 as the two main products, as confirmed by powder X-ray diffraction and transmission electron microscopy analysis. Li2ZrO3 was discovered for the first time as a reaction product, and its formation in the case of Li-rich layered cathode material was rationalized with DFT + U calculations. The results were also compared with those obtained for a typical layered high-energy-density cathode material LiNi0.8Mn0.1Co0.1O2 (NMC811).https://doi.org/10.1038/s41598-024-78927-w
spellingShingle Natalia B. Timusheva
Alexander A. Golubnichiy
Anatolii V. Morozov
Arseniy S. Burov
Dmitry A. Aksyonov
Aleksandra A. Savina
Roman G. Markopolskii
Artem M. Abakumov
Chemical compatibility at the interface of garnet-type Ga-LLZO solid electrolyte and high-energy Li-rich layered oxide cathode for all-solid-state batteries
Scientific Reports
title Chemical compatibility at the interface of garnet-type Ga-LLZO solid electrolyte and high-energy Li-rich layered oxide cathode for all-solid-state batteries
title_full Chemical compatibility at the interface of garnet-type Ga-LLZO solid electrolyte and high-energy Li-rich layered oxide cathode for all-solid-state batteries
title_fullStr Chemical compatibility at the interface of garnet-type Ga-LLZO solid electrolyte and high-energy Li-rich layered oxide cathode for all-solid-state batteries
title_full_unstemmed Chemical compatibility at the interface of garnet-type Ga-LLZO solid electrolyte and high-energy Li-rich layered oxide cathode for all-solid-state batteries
title_short Chemical compatibility at the interface of garnet-type Ga-LLZO solid electrolyte and high-energy Li-rich layered oxide cathode for all-solid-state batteries
title_sort chemical compatibility at the interface of garnet type ga llzo solid electrolyte and high energy li rich layered oxide cathode for all solid state batteries
url https://doi.org/10.1038/s41598-024-78927-w
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