Establishing Li-acetylide (Li2C2) as functional element in solid-electrolyte interphases in lithium-ion batteries

Previously, lithium-acetylide (Li 2 C 2 ) had been identified as electrolyte degradation product on lithium -metal based electrodes using Raman spectroscopy. This raised the question, if Li 2 C 2 is also be formed on graphitic electrodes in lithium -ion batteries without lithium metal present. In order to shed light on this research question, we performed a series of in situ Raman experiments with graphitic electrodes in half- and full -cell configuration. The recorded cell potential dependent spectra clearly prove the presence of Li 2 C 2 in the lithiated state of the electrodes, but the according peak vanishes when delithiating. This observation indicates a somewhat reversible process involving Li 2 C 2 . Several chemical/electrochemical reactions are in question to contribute to this effect. With respect to its properties and potential role in the solid -electrolyte interphase (SEI) DFT calculations of Li 2 C 2 - nanoclusters were performed, which revealed an exceptionally low energy band gap, hence a remarkable electric conductivity. In conjunction with a relatively high ionic conductivity, Li 2 C 2 appears to play a key role in the degradation of lithium -ion batteries, which had not yet been revealed nor taken into account in simulations of the interphase.