<p>High-Entropy Argyrodite Glass-Ceramic Electrolytes for All-Solid-State Batteries</p>

Jing Lin; Mareen Schaller; Ruizhuo Zhang; Volodymyr Baran; Hao Liu; Ziming Ding; Sylvio Indris; Aleksandr Kondrakov; Torsten Brezesinski; and Florian Strauss

doi:10.1088/2752-5724/adde76

High-Entropy Argyrodite Glass-Ceramic Electrolytes for All-Solid-State Batteries

1 Battery and Electrochemistry Laboratory (BELLA), Institute of Nanotechnology, Karlsruhe Institute of Technology (KIT), Kaiserstr. 12, 76131 Karlsruhe, Germany;
2 Institute for Applied Materials-Energy Storage Systems, Karlsruhe Institute of Technology (KIT), Kaiserstr. 12, 76131 Karlsruhe, Germany;
3 Deutsches Elektronen-Synchrotron DESY, Notkestr. 85, 22607 Hamburg, Germany;
4 Institute of Nanotechnology, Karlsruhe Institute of Technology (KIT), Kaiserstr. 12, 76131 Karlsruhe, Germany;
5 Applied Chemistry and Engineering Research Centre of Excellence (ACER CoE), Université Mohammed VI Polytechnique (UM6P), Lot 660, Hay Moulay Rachid, Ben Guerir, 43150, Morocco;
6 BASF SE, Carl-Bosch-Str. 38, 67056 Ludwigshafen, Germany

基金项目:

F.S. is grateful to the Federal Ministry of Education and Research (BMBF) for funding within the project MELLi (03XP0447).

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- 收稿日期: 2025-05-01
- 网络出版日期: 2025-05-29

High-Entropy Argyrodite Glass-Ceramic Electrolytes for All-Solid-State Batteries

1 Battery and Electrochemistry Laboratory (BELLA), Institute of Nanotechnology, Karlsruhe Institute of Technology (KIT), Kaiserstr. 12, 76131 Karlsruhe, Germany;
2 Institute for Applied Materials-Energy Storage Systems, Karlsruhe Institute of Technology (KIT), Kaiserstr. 12, 76131 Karlsruhe, Germany;
3 Deutsches Elektronen-Synchrotron DESY, Notkestr. 85, 22607 Hamburg, Germany;
4 Institute of Nanotechnology, Karlsruhe Institute of Technology (KIT), Kaiserstr. 12, 76131 Karlsruhe, Germany;
5 Applied Chemistry and Engineering Research Centre of Excellence (ACER CoE), Université Mohammed VI Polytechnique (UM6P), Lot 660, Hay Moulay Rachid, Ben Guerir, 43150, Morocco;
6 BASF SE, Carl-Bosch-Str. 38, 67056 Ludwigshafen, Germany

Funds:

F.S. is grateful to the Federal Ministry of Education and Research (BMBF) for funding within the project MELLi (03XP0447).

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Corresponding author:
Torsten Brezesinski,E-mail:torsten.brezesinski@kit.edu

摘要

摘要: Only Lithium argyrodite superionic conductors with the general formula Li₆PS₅X (X = Cl, Br, I) have been intensively investigated in recent years and further successfully adopted in the field of solid-state batteries (SSBs). The transport properties of argyrodite solid electrolytes usually strongly depend on the degree of occupational disorder. Increasing disorder through complex doping or substitution has been shown to directly affect ionic conductivity. Herein, we explore a high-entropy lithium argyrodite of nominal composition Li_6.6[P_0.2Si_0.2Sn_0.2Ge_0.2Sb_0.2]S₅I. This material can be readily prepared by mechanochemistry. Using complementary diffraction techniques, nuclear magnetic resonance spectroscopy, and charge-transport measurements, we show that upon tailoring crystallinity and defect concentration by post-annealing at temperatures up to 220 °C, a high room-temperature ionic conductivity of about 0.9 mS/cm (~4.4 mS/cm bulk conductivity) can be achieved. Both as-prepared and annealed (at 220 °C) samples were also tested in pellet-stack SSB cells. The mechanochemically prepared glass-ceramic solid electrolyte was found to exhibit superior performance, even outperforming commercially available Li₆PS₅Cl. Collectively, the results highlight the importance of considering structural aspects on different length scales when optimizing the properties of lithium argyrodites for SSB applications.
- high-entropy materials /
- solid electrolytes /
- solid-state batteries
Abstract: Only Lithium argyrodite superionic conductors with the general formula Li₆PS₅X (X = Cl, Br, I) have been intensively investigated in recent years and further successfully adopted in the field of solid-state batteries (SSBs). The transport properties of argyrodite solid electrolytes usually strongly depend on the degree of occupational disorder. Increasing disorder through complex doping or substitution has been shown to directly affect ionic conductivity. Herein, we explore a high-entropy lithium argyrodite of nominal composition Li_6.6[P_0.2Si_0.2Sn_0.2Ge_0.2Sb_0.2]S₅I. This material can be readily prepared by mechanochemistry. Using complementary diffraction techniques, nuclear magnetic resonance spectroscopy, and charge-transport measurements, we show that upon tailoring crystallinity and defect concentration by post-annealing at temperatures up to 220 °C, a high room-temperature ionic conductivity of about 0.9 mS/cm (~4.4 mS/cm bulk conductivity) can be achieved. Both as-prepared and annealed (at 220 °C) samples were also tested in pellet-stack SSB cells. The mechanochemically prepared glass-ceramic solid electrolyte was found to exhibit superior performance, even outperforming commercially available Li₆PS₅Cl. Collectively, the results highlight the importance of considering structural aspects on different length scales when optimizing the properties of lithium argyrodites for SSB applications.
- high-entropy materials /
- solid electrolytes /
- solid-state batteries

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High-Entropy Argyrodite Glass-Ceramic Electrolytes for All-Solid-State Batteries

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High-Entropy Argyrodite Glass-Ceramic Electrolytes for All-Solid-State Batteries

Corresponding author: Torsten Brezesinski,E-mail:torsten.brezesinski@kit.edu

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Corresponding author:
Torsten Brezesinski,E-mail:torsten.brezesinski@kit.edu