First-Principles Prediction of Vacancy Order-Disorder and Intercalation Battery Voltages in
- 20 July 1998
- journal article
- research article
- Published by American Physical Society (APS) in Physical Review Letters
- Vol. 81 (3), 606-609
- https://doi.org/10.1103/physrevlett.81.606
Abstract
We present a first-principles technique for predicting the ordered vacancy ground states, intercalation voltage profiles, and voltage-temperature phase diagrams of Li intercalation battery electrodes. Application to the system yields correctly the observed ordered vacancy phases. We further predict the existence of additional ordered phases, their thermodynamic stability ranges, and their intercalation voltages in battery cells. Our calculations provide insight into the remarkable electronic stability of this system with respect to Li removal: A rehybridization of the Co-O orbitals acts to restore charge to the Co site (“self-regulating response”), thereby minimizing the effect of the perturbation.
Keywords
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