Transitions of lithium occupation in graphite: A physically informed model in the dilute lithium occupation limit supported by electrochemical and thermodynamic measurements

A. SIGAL

ELECTROCHIMICA ACTA

PERGAMON-ELSEVIER SCIENCE LTD

Lugar: Amsterdam; Año: 2019

0013-4686

nderstanding the role of the phase transitions during lithiation and delithiation of graphite remains a problem of fundamental importance, but also practical relevance owing to its widespread use as the anode material in most commercial lithium-ion cells. Previously performed density functional theory (DFT) calculations show a rapid change in the lithium-carbon interaction at low occupation, due to partial charge transfer from Li to C. We integrate this effect in our previously developed two level mean field model, which describes the Stage I ? Stage II transition in graphite. The modified model additionally describes the most predominant transition that occurs at low Li content in graphite, which results in a previously unexplained feature in voltage and dQ/dV profiles, and thermodynamic measurements of partial molar enthalpy. In contrast with the Stage I-Stage II transition, this extra feature is not associated with observable features in the partial molar entropy and our model demo