Journal
CHEMISTRY OF MATERIALS
Volume 27, Issue 8, Pages 2903-2910Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.5b00149
Keywords
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Funding
- National Research Foundation, Prime Minister's Office, Singapore under its Competitive Research Programme (CRP) [NRF-CRP 10-2012-6, NRF-CRP 8-2011-4]
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The favorable combination of fast-ionic conductivity and high electrochemical stability of Li-stuffed garnet type Li7La3Zr2O12 (LLZ) makes this material a promising candidate for applications as a solid-state electrolyte in high-energy-density batteries. However, a widespread technical use of LLZ is impeded by difficulty in reliable formation and densification of the pure fast-ion conducting phase. The present study of the phase-formation process enables rational fabrication procedures to be devised based on a thorough understanding of the complex phase formation of LLZ. In situ neutron powder diffraction monitoring of the phase formation revealed an influence of the partial melting of precursors on the formation of the fast-ion conducting phase, indicating that in the typical synthesis route LLZ is not formed in a solid-state reaction but from a partial carbonate melt that decomposes on further heating. The cooling rate critically influences lithium ordering and ionic conductivity.
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