LAUSR

Since the introduction of the first commercial rechargeable lithium batteries in the early 1990s such battery types have become vital power sources for manifold technical applications. Currently, the operation of, for example, mobile electronic devices, electrical vehicles and many stationary energy storage facilities is inconceivable without using advanced lithium ion batteries. Positive electrodes of lithium batteries are originally based on layered oxide LiCoO2 and their negative electrodes are typically composed of carbon-based materials. However, there is an increasing demand for both higher energy and power densities as well as improved safety, extended operation lifetime (cyclability) and reduced costs. This boosts research and development activities on innovative active materials and electrolytes for appropriately improved lithium ion batteries. The electrochemical behavior and performance of a huge amount of different candidate electrode and electrolyte materials were, and presently are, under major investigation and thousands of papers are published each year. Also, analytical methods of materials science and engineering are frequently used to study fundamental properties of the active materials and their behavior in operating electrochemical cells. Crystal chemistries, phase stabilities and transformations are investigated by post-mortem, in-situ and in-operando studies, respectively. This experimental–analytical work is largely supported by modeling and computer simulations. However, a while ago our literature research showed that there was surprisingly little work published on the thermodynamics, kinetics and phase diagrams (materials constitution) of battery materials, as well as on the overall thermodynamics of cells and batteries. There was an obvious lack of data and scientific knowledge regarding active materials’ heterogeneous equilibria, heat capacities, enthalpies, entropies and chemical potentials. Therefore, no fundamental basis was available for analyzing specific relationships between: