Journal
JOURNAL OF THE AMERICAN CERAMIC SOCIETY
Volume 100, Issue 1, Pages 276-285Publisher
WILEY
DOI: 10.1111/jace.14572
Keywords
conductivity; garnets; glass-ceramics; sinter/sintering
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Funding
- Japan Society for the Promotion of Science (JSPS) [P13371]
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Lithium ion conductors with garnet-type structure are promising candidates for applications in all solid-state lithium ion batteries, because these materials present a high chemical stability against Li metal and a rather high Li+ conductivity (10(-3)-10(-4)S/cm). Producing densified Li-ion conductors by lowering sintering temperature is an important issue, which can achieve high Li conductivity in garnet oxide by preventing the evaporation of lithium and a good Li-ion conduction in grain boundary between garnet oxides. In this study, we concentrate on the use of sintering additives to enhance densification and microstructure of Li7La3ZrNbO12 at sintering temperature of 900 degrees C. Glasses in the LiO2-B2O3-SiO2-CaO-Al2O3 (LBSCA) and BaO-B2O3-SiO2-CaO-Al2O3 (BBSCA) system with low softening temperature (<700 degrees C) were used to modify the grain-boundary resistance during sintering process. Lithium compounds with low melting point (<850 degrees C) such as LiF, Li2CO3, and LiOH were also studied to improve the rearrangement of grains during the initial and middle stages of sintering. Among these sintering additives, LBSCA and BBSCA were proved to be better sintering additives at reducing the porosity of the pellets and improving connectivity between the grains. Glass additives produced relative densities of 85-92%, whereas those of lithium compounds were 62-77%. Li7La3ZrNbO12 sintered with 4 wt% of LBSCA at 900 degrees C for 10h achieved a rather high relative density of 85% and total Li-ion conductivity of 0.8x10(-4)S/cm at room temperature (30 degrees C).
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