Temperature-Dependent Chemical and Physical Microstructure of Li Metal Anodes Revealed through Synchrotron-Based Imaging Techniques

Abstract

The Li metal anode has been long sought-after for application in Li metal batteries due to its high specific capacity (3860 mAh g^-1 ) and low electrochemical potential (-3.04 V vs the standard hydrogen electrode). Nevertheless, the behavior of Li metal in different environments has been scarcely reported. Herein, the temperature-dependent behavior of Li metal anodes in carbonate electrolyte from the micro- to macroscales are explored with advanced synchrotron-based characterization techniques such as X-ray computed tomography and energy-dependent X-ray fluorescence mapping. The importance of testing methodology is exemplified, and the electrochemical behavior and failure modes of Li anodes cycled at different temperatures are discussed. Moreover, the origin of cycling performance at different temperatures is identified through analysis of Coulombic efficiencies, surface morphology, and the chemical composition of the solid electrolyte interphase in quasi-3D space with energy-dependent X-ray fluorescence mappings coupled with micro-X-ray absorption near edge structure. This work provides new characterization methods for Li metal anodes and serves as an important basis toward the understanding of their electrochemical behavior in carbonate electrolytes at different temperatures.

Keywords: Li dendrites; Li metal anodes; carbonate electrolytes; electrochemical behavior; failure modes.