Abstract
Abstract Solid-state batteries (SSBs) are a promising next step in electrochemical energy storage but are plagued by a number of problems. In this study, we demonstrate the recurring issue of mechanical degradation because of volume changes in layered Ni-rich oxide cathode materials in thiophosphate-based SSBs. Specifically, we explore superionic solid electrolytes (SEs) of different crystallinity, namely glassy 1.5Li2S-0.5P2S5-LiI and argyrodite Li6PS5Cl, with emphasis on how they affect the cyclability of slurry-cast cathodes with NCM622 (60% Ni) or NCM851005 (85% Ni). The application of a combination of ex situ and in situ analytical techniques helped to reveal the benefits of using a SE with a low Young’s modulus. Through a synergistic interplay of (electro)chemical and (chemo)mechanical effects, the glassy SE employed in this work was able to achieve robust and stable interfaces, enabling intimate contact with the cathode material while at the same time mitigating volume changes. Our results emphasize the importance of considering chemical, electrochemical, and mechanical properties to realize long-term cycling performance in high-loading SSBs.
Highlights
With the advance in technology ranging from mobile devices to electric vehicles and a global push toward renewable resources, research in electrochemical energy storage has been catapulted to a position front and center
We focus on industrially relevant materials, with the cathode active material (CAM) being a layered Ni-rich oxide, Li1+x(Ni0.6Co0.2Mn0.2)1–xO2 (NCM622) or Li1+x(Ni0.85Co0.10Mn0.05)1–xO2 (NCM851005), and the solid electrolytes (SEs) being lithium thiophosphates
The solid-state batteries (SSBs) cells were cycled with a similar protocol as the pelletized cells in the voltage range of 1.35–2.85 V vs Li4Ti5O12/Li7Ti5O12 at a C/5 rate and 45 ◦C for 200 cycles
Summary
With the advance in technology ranging from mobile devices to electric vehicles and a global push toward renewable resources (away from fossil fuels), research in electrochemical energy storage has been catapulted to a position front and center. LIBs have limitations, such as the inherent safety problems caused by flammable components in the system and the limited temperature window for operation [2, 4, 5] They are approaching their theoretical energy densities. These limitations could be theoretically overcome with the inception of solid-state batteries (SSBs), i.e. replacing the liquid electrolyte by a solid electrolyte (SE) With their promise of increased gravimetric and volumetric energy densities by allowing the use of lithium-metal anodes as well as offering improved safety conditions and larger operating temperature windows, SSBs could be applied in a wider range of applications [6]. The net effect of either process on the capacity retention depends primarily on the choice of materials and their mutual interactions
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