Electrode potential influences the reversibility of lithium-metal anodes

Abstract Lithium-metal batteries are a promising technology to address the emerging demand for high-energy-density storage systems. However, their cycling encounters a low Coulombic efficiency (CE) due to the unceasing electrolyte decomposition. Improving the stability of solid electrolyte interphase (SEI) suppresses the decomposition and increases CE. However, SEI morphology and chemistry alone cannot account for CE, and a full explanation is still lacking. Here we report that in diverse electrolytes, the large shift (>0.6 V) in the Li electrode potential and its association with the Li + coordination structure influence the CE. Machine learning regression analysis and vibrational spectroscopy revealed…