Journal
JOURNAL OF PHYSICAL CHEMISTRY C
Volume 124, Issue 31, Pages 16796-16805Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.0c03558
Keywords
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Funding
- Austrian Federal Ministry of Science, Research and Economy (BMWFW)
- National Foundation for Research, Technology, and Development (CD-Laboratory of Lithium Batteries: Ageing Effects, Technology, and New Materials)
- Austrian Science Fund (FWF) [P 31437]
- FFG (Austrian Research promotion Agency)
- European Union [769929]
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Cubic Li7La3Zr2O12(LLZO), stabilized by supervalent cations, is one of the most promising oxide electrolyte to realize inherently safe all-solid-state batteries. It is of great interest to evaluate the strategy of supervalent stabilization in similar compounds and to describe its effect on ionic bulk conductivity sigma'(bulk). Here, we synthesized solid solutions of Li7-xLa3M2-xTaxO12 with M = Hf, Sn over the full compositional range (x = 0, 0.25...2). It turned out that Ta contents at x of 0.25 (M = Hf, LLHTO) and 0.5 (M = Sn, LLSTO) are necessary to yield phase pure cubic Li7-xLa3M2-xTaxO12. The maximum in total conductivity for LLHTO (2 x 10(-4) S cm(-1)) is achieved for x = 1.0; the associated activation energy is 0.46 eV. At x = 0.5 and x = 1.0, we observe two conductivity anomalies that are qualitatively in agreement with the rule of Meyer and Neldel. For LLSTO, at x = 0.75 the conductivity sigma'(bulk) turned out to be 7.94 x 10(-5) S cm(-1) (0.46 eV); the almost monotonic decrease of ion bulk conductivity from x = 0.75 to x = 2 in this series is in line with Meyer-Neldel's compensation behavior showing that a decrease in Ea is accompanied by a decrease of the Arrhenius prefactor. Altogether, the system might serve as an attractive alternative to Al-stabilized (or Ga-stabilized) Li7La3Zr2O12 as LLHTO is also anticipated to be highly stable against Li metal.
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