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Vol. 17 (2025)

Half-Covered ‘Glitter-Cake’ AM@SE Composite: A Novel Electrode Design for High Energy Density All-Solid-State Batteries

https://doi.org/10.1007/s40820-024-01644-6
Min Ji Kim
Energy and Environmental Division, Korea Institute of Ceramic Engineering and Technology, Jinju, Gyeongnam 52851, Republic of Korea
Jin‑Sung Park
Department of Nuclear Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA 20139, USA
Jin Woong Lee
Energy and Environmental Division, Korea Institute of Ceramic Engineering and Technology, Jinju, Gyeongnam 52851, Republic of Korea
Sung Eun Wang
Energy and Environmental Division, Korea Institute of Ceramic Engineering and Technology, Jinju, Gyeongnam 52851, Republic of Korea
Dowoong Yoon
Energy and Environmental Division, Korea Institute of Ceramic Engineering and Technology, Jinju, Gyeongnam 52851, Republic of Korea
Jong Deok Lee
Energy and Environmental Division, Korea Institute of Ceramic Engineering and Technology, Jinju, Gyeongnam 52851, Republic of Korea
Jung Hyun Kim
Energy and Environmental Division, Korea Institute of Ceramic Engineering and Technology, Jinju, Gyeongnam 52851, Republic of Korea
Taeseup Song
Department of Energy Engineering, Hanyang University, Seoul 04763, Republic of Korea
Ju Li
Department of Nuclear Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA 20139, USA
Yun Chan Kang
Department of Materials Science and Engineering, Korea University, Anam‑Dong, Seongbuk‑Gu, Seoul 136‑713, Republic of Korea
Dae Soo Jung
Energy and Environmental Division, Korea Institute of Ceramic Engineering and Technology, Jinju, Gyeongnam 52851, Republic of Korea

Corresponding Author: Dae Soo Jung

dsjung@kicet.re.kr

Nano-Micro Letters, Vol. 17 (2025), Article Number: 119

Abstract

All-solid-state batteries (ASSBs) are pursued due to their potential for better safety and high energy density. However, the energy density of the cathode for ASSBs does not seem to be satisfactory due to the low utilization of active materials (AMs) at high loading. With small amount of solid electrolyte (SE) powder in the cathode, poor electrochemical performance is often observed due to contact loss and non-homogeneous distribution of AMs and SEs, leading to high tortuosity and limitation of lithium and electron transport pathways. Here, we propose a novel cathode design that can achieve high volumetric energy density of 1258 Wh L−1 at high AM content of 85 wt% by synergizing the merits of AM@SE core–shell composite particles with conformally coated thin SE shell prepared from mechanofusion process and small SE particles. The core–shell structure with an intimate and thin SE shell guarantees high ionic conduction pathway while unharming the electronic conduction. In addition, small SE particles play the role of a filler that reduces the packing porosity in the cathode composite electrode as well as between the cathode and the SE separator layer. The systematic demonstration of the optimization process may provide understanding and guidance on the design of electrodes for ASSBs with high electrode density, capacity, and ultimately energy density.


Highlights:
1 A novel electrode design for high energy density all-solid-state batteries (ASSBs) is realized through the control of nano- and microstructures.
2 An active materials@solid electrolyte composite with a half-covered “glitter-cake” morphology is adopted to optimize the transport of electrons and ions in the electrode.
3 The optimized electrode design exhibited a volumetric energy density of 1258 Wh L−1 at an active material content of 85 wt%, exceeding the performance of the reported ASSB cells.

Keywords

All-solid-state batteries Cathodes Sulfide-based solid electrolytes Interfaces Mechanofusion
Kim, Min Ji, Jin‑Sung Park, Jin Woong Lee, Sung Eun Wang, Dowoong Yoon, Jong Deok Lee, Jung Hyun Kim, Taeseup Song, Ju Li, Yun Chan Kang, and Dae Soo Jung. 2025. “Half-Covered ‘Glitter-Cake’ AM@SE Composite: A Novel Electrode Design for High Energy Density All-Solid-State Batteries”. Nano-Micro Letters 17 (January):119. https://doi.org/10.1007/s40820-024-01644-6.
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