Investigation of Cellulose-Based Separators for Secondary Lithium Metal Batteries

Abstract

Lithium-ion batteries (LIBs) have been the predominant energy storage technology for a variety of applications such as portable electronic devices and wireless power tools. However, the rising demand for emerging technologies such as long-range electric vehicles and grid-level energy storage and delivery has drastically increased the necessity for low-cost LIBs with enhanced performance and safety.Improvements in the modern LIB technology can be achieved through improvements in different, individual components of the battery. Among the key components of the battery, the separator plays a vital role. To date, polypropylene (PP)/polyethylene (PE) membranes have been used as separators in LIBs due to their desired electrochemical stability. However, these separator materials suffer from low thermal stability, which results in their deformation or decomposition at elevated temperatures upon high charging rates1. A dangerous consequence of this material degradation is an electrical short, leading to an aggressive discharge of the battery and subsequent fire. Moreover, PP/PE separators possess relatively low electrolyte wettability and an expensive and eco-unfriendly fabrication process. Hence, alternative separator materials for future LIB technology are indispensable.Among alternative separator materials, cellulose is a promising candidate2. Cellulose is derived from biomass which is one of the most abundant and renewable resources on Earth. It also is non-toxic and has high mechanical and chemical stability. Additionally, with an initial decomposition temperature of 270°C, cellulose offers a major advantage in thermal stability compared to its polymeric competitors3. The thermal and electrochemical stability, electrolyte wettability, and performance of cellulose-based separators in LIBs have been studied3,4. However, those reports mostly consider the conventional LIB electrode materials– Li transition metal oxide and graphite; and focus on the separator/electrolyte compatibility. Therefore, to be considered for future generations of high-performance Li-based batteries, cellulose-based separators must be investigated in batteries with new electrode chemistries.This work presents new insights on the interaction of cellulose-based separator and metallic Li – the leading candidate for future anodes. Coin cells were prepared using various cathode materials, Li metal anode, and a commercial cellulose-based separator. The cycling performance of the cells was tested at different C rates. Results were compared with the cycling performance of the coin cells with similar electrodes but a commercial PP/PE separator. Comparable discharge profiles were observed in the two groups of cells, but the cellulose separator hampered the charging process. Additional electrochemical analysis suggested an undesired interaction between the cellulose-based separator and metallic Li. To further understand this interaction, various protective coatings on the separator were investigated, the results of which suggest a mechanical degradation in the cellulose separator during cycling and consequently a soft short. These results are expected to provide a new understanding regarding the stability of cellulose-based separators in Li metal-containing batteries, which can help with their implementation in the next generation of Li-based batteries with enhanced performance and safety.