TY - JOUR
T1 - First-principles prediction of vacancy order-disorder and intercalation battery voltages in LixCoO2
AU - Wolverton, C.
AU - Zunger, Alex
PY - 1998
Y1 - 1998
N2 - 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 LixCoO2 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 LixCoO2/Li 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.
AB - 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 LixCoO2 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 LixCoO2/Li 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.
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U2 - 10.1103/PhysRevLett.81.606
DO - 10.1103/PhysRevLett.81.606
M3 - Article
AN - SCOPUS:0000272732
VL - 81
SP - 606
EP - 609
JO - Physical Review Letters
JF - Physical Review Letters
SN - 0031-9007
IS - 3
ER -