Key Takeaways & Executive Findings
- •• A novel 'glitter-cake' AM@SE composite design enables high volumetric energy density (1258 Wh L−1) at 85 wt% active material content in all-solid-state batteries. • The core–shell structure with a thin, conformal SE shell from mechanofusion ensures efficient ionic and electronic transport pathways. • Small SE particles act as fillers to reduce porosity, enhancing electrode density and interfacial contact. • The optimized electrode design outperforms reported ASSB cells, providing guidance for high-energy-density electrode engineering.
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.
1. Introduction
Lithium-ion batteries (LIBs) are currently the dominant power source for portable electronics and electric vehicles (EVs), whose importance is ever-increasing for a sustainable future [1, 2]. Unfortunately, conventional LIBs that make use of organic liquid electrolytes (LEs) and graphite anode are reaching the limitation in terms of energy density [1–6], and the flammability of organic LEs is also a concern [7, 8]. All-solid-state batteries (ASSBs) that use lithium metal anode and SEs are considered as a promising alternative for replacing the conventional LIBs and are now at the forefront of next-generation rechargeable battery research [9–13]. The ASSBs research should not only provide solution to the safety issues but also focus on surpassing the energy density of the conventional LIBs [14–17].
Among various types of SEs, sulfide-based SEs, such as Li10GP2S12 [18] and Li7P3S12 [10], have been widely applied as electrolytes for ASSBs due to their high ionic conductivity at room temperature and high ductility [19–22]. However, contrary to conventional LIBs where electrode–electrolyte contact is secured due to the fluidic nature of LEs, SEs cannot penetrate well into the electrode, resulting in insufficient contact area between cathode active materials (CAMs) and SEs [23]. The loss in physical contact hinders the lithium-ion transport due to high interfacial resistance, which may induce low initial Coulombic efficiency and poor cycle performance due to the gradual degradation of lithium-ion percolation network [24, 25]. This phenomenon becomes more obvious as the AM content increases, thereby resulting in lower lithium-ion percolation and CAM utilization, which is detrimental in terms of energy density [26–28].
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Min Ji Kim, Jin-Sung Park, Jin Woong Lee, Sung Eun Wang, Dowoong Yoon, Jong Deok Lee, Jung Hyun Kim, Taeseup Song, Ju Li, Yun Chan Kang, 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. https://doi.org/10.1007/s40820-024-01644-6
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Frequently Asked Questions
What is the 'glitter-cake' AM@SE composite design?
It is a novel cathode design where active material (AM) particles are partially coated with a thin solid electrolyte (SE) shell, resembling a glitter cake. This structure optimizes both ionic and electronic conduction pathways, enabling high energy density in all-solid-state batteries.
How does the proposed design achieve high energy density?
By combining core-shell AM@SE particles with small SE particles as fillers, the design reduces porosity and enhances contact between AM and SE, achieving a volumetric energy density of 1258 Wh L−1 at 85 wt% active material content.
What is the role of small SE particles in the electrode?
Small SE particles act as fillers that reduce packing porosity in the cathode composite and between the cathode and SE separator, improving ionic transport and overall electrode density.
What method was used to prepare the core-shell composite?
The core-shell AM@SE composite was prepared using a mechanofusion process, which creates a conformal and thin SE shell on the AM particles.
How does this design compare to conventional ASSB cathodes?
The optimized electrode design outperforms reported ASSB cells in terms of volumetric energy density, demonstrating a promising strategy for high-energy-density all-solid-state batteries.
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