Publication date: 10th April 2024
Solid state lithium metal batteries are promising as the next-generation energy storage system due to their high energy density, thermal stability, and volumetric miniaturization.[1] However, the use of Li metal anode is detrimental in terms of dendrite formation and Li deposition in the solid electrolyte (SE) layer that causes short-circuit, thereby limits the battery cyclability. Besides, the mechanochemical instability of the Li-SE interface, and the low earth abundance of Li establish the need for alternative high-capacity anode development. In this regard, silicon is a potential alternative due to its high theoretical capacity of 4200 mAh/g and low lithiation potential. The realization of electrochemically stable and high-performance Si based anode is limited by low electronic and ionic conductivity of Si. [2, 3] Despite appreciable advances in achieving stable Si based anode, the influence of the transport properties on the rate capability and long-term stability remain unclear.
In this study, we investigated the role of effective ionic and electronic conductivity in modulating the electrochemical performance of Si based anodes. First, we have developed Si-based composites with SE (Argyrodite) and carbon additive, which significantly improved the ionic and electronic conductivity of the electrode composite, respectively. By optimizing the ion/electron conducting phase ratio in the composite and relating corresponding cell performance with effective transport coefficients we have estimated the limiting conductivity values. The particle size of Si is also found to significantly influence the effective transport properties, which in turn modulate the rate performance as well as the long-term stability.[4] This study provides a comprehensive understanding on the role of charge carrier transport in achieving high-performance silicon based anode for solid-state batteries.
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