Projects per year
The Li-stuffed garnets Li xM 2M3′O 12 are promising Li-ion solid electrolytes with potential use in solid-state batteries. One strategy for optimizing ionic conductivities in these materials is to tune lithium stoichiometries through aliovalent doping, which is often assumed to produce proportionate numbers of charge-compensating Li vacancies. The native defect chemistry of the Li-stuffed garnets and their response to doping, however, are not well understood, and it is unknown to what degree a simple vacancy-compensation model is valid. Here, we report hybrid density functional theory calculations of a broad range of native defects in the prototypical Li garnet Li 7La 3Zr 2O 12. We calculate equilibrium defect concentrations as a function of synthesis conditions and model the response of these defect populations to extrinsic doping. We predict a rich defect chemistry that includes Li and O vacancies and interstitials, and significant numbers of cation-antisite defects. Under reducing conditions, O vacancies act as color centers by trapping electrons. We find that supervalent (donor) doping does not produce charge compensating Li vacancies under all synthesis conditions; under Li-rich/Zr-poor conditions the dominant compensating defects are Li Zr antisites, and Li stoichiometries strongly deviate from those predicted by simple "vacancy compensation" models.
ASJC Scopus subject areas
- Chemical Engineering(all)
- Materials Chemistry
FingerprintDive into the research topics of 'Native Defects and their Doping Response in the Lithium Solid Electrolyte Li7La3Zr2O12'. Together they form a unique fingerprint.
- 1 Finished
1/10/14 → 30/09/19
Project: Research council
Dataset for "Native Defects and their Doping Response in the Lithium Solid Electrolyte Li7La3Zr2O12"
Squires, A. G. (Creator), Scanlon, D. O. (Creator) & Morgan, B. (Creator), University of Bath, 23 Dec 2019