Jeffrey Lopez1 Yang Shao-Horn1

1, Massachusetts Institute of Technology, Cambridge, Massachusetts, United States

Lithium ion batteries have become the dominant form of energy storage used in consumer electronics and, recently, electric vehicles. However, high costs have prevented widespread deployment of lithium ion batteries for applications other than portable electronics, and the safety issues associated with liquid organic electrolytes remain to be addressed. In order to enable the greater utilization of electric vehicles, allow for grid scale energy storage, and meet the demands of new electronic applications, new materials for high energy density batteries must be developed. High capacity electrode materials like lithium metal have the potential to facilitate these technologies, but lithium metal electrodes are presently limited by significant side reactions, poor quality deposition, and the potential to form hazardous dendrites. Therefore, it is important to develop a clear understanding of the surface reactivity and growth behavior of the lithium metal at the interface with the electrolyte in order to enable stable long-term cycling.

The products that form as a result of electrolyte decomposition reactions at the electrode interface are known to be extremely important in determining the final cell performance. Specifically, fluorinated salts and solvent additives have been shown to enable stable cycling of Li metal anodes. This improvement is ascribed to the formation of LiF in the solid electrolyte interphase (SEI), yet the understanding of how LiF and other SEI compounds are formed and how they affect battery cycling is not complete. In this presentation, in situ spectroelectrochemical techniques including infrared spectroscopy (FTIR), differential electrochemical mass spectrometry (DEMS), and electrochemical quartz crystal microbalance (EQCM), are used to clearly identify components of the Li metal SEI. An understanding of SEI formation with respect to electrochemical potential and time will be discussed. With this understanding we provide new insights into the formation and chemical nature of SEI components that promote stable cycling of lithium metal electrodes.