New solid lithium-conducting electrolytes of nominal composition Li8La3Zr2–0.75x Al x O12.5 and Li9La3Zr2–0.75x Al x O13 (x = 0.05–0.30) were obtained. It is shown that the superionic cubic phase can be stabilized for compositions with x > 0.5 by annealing at 1150°C. The electrical conductivity of the electrolytes under study grows with increasing content of Al3+ and reaches the maximum value of 5.9 × 10–5 S cm–1 (at (25°C) at the point x = 0.20 for the Li8La3Zr2–0.75x Al x O12 system and 2.2 × 10–5 S cm–1 at the point x = 0.15 for the Li9La3Zr2–0.75x Al x O13 system. No further rise in the conductivity is observed with increasing x because of the formation of the LaAlO3 and La2Li0.5Al0.5O4 phases. The activation energy of conductivity is approximately constant for all compositions with stabilized cubic structure and is close to 35.8 ± 0.7 kJ mol–1 (Li8La3Zr1.85Al0.20O12.5 composition). The smaller values of the conductivity, compared with the Li7La3Zr2–0.75x Al x O12, are due to the filling of vacant lithium sites in the structure of the cubic LLZ and, accordingly, to the blocking of conduction paths.
Russian Journal of Applied Chemistry – Springer Journals
Published: Aug 15, 2015
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