Achieving enhanced densification and superior ionic conductivity of garnet electrolytes via a co-doping strategy coupled with pressureless sintering |
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| Affiliation: | 1. Department of Chemical and Materials Engineering, The University of Auckland, Private Bag 92019, Auckland 1142, New Zealand;2. School of Materials Science and Engineering, Jiangsu University of Science and Technology, Zhenjiang 212003, China;3. School of Chemical Sciences, The University of Auckland, Private Bag 92019, Auckland 1142, New Zealand;4. School of Materials Science and Technology, Beijing Key Laboratory of Materials Utilization of Nonmetallic Minerals and Solid Wastes, National Laboratory of Mineral Materials, China University of Geosciences, Beijing 100083, China;5. Nanoyang Group, State Key Laboratory of Chemical Engineering, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300350, China;6. MacDiarmid Institute for Advanced Materials and Nanotechnology, Victoria University of Wellington, Wellington, New Zealand;1. Temasek Laboratories, Nanyang Technological University, 637553, Singapore;2. School of Materials Science and Engineering, Nanyang Technological University, 639798, Singapore;1. College of Materials Science and Engineering, Nanjing Tech University, No. 5 Xinmofan Road, Nanjing, Jiangsu 210009, PR China;2. Lejin Chemical (Nanjing) Information Material Co., Ltd, No. 17 Hengyi Road, Nanjing, Jiangsu 210038, PR China;1. State Key Laboratory of Advanced Welding and Joining, Harbin Institute of Technology, Harbin 150001, China;2. Key Laboratory of Advanced Structural-Functional Integration Materials & Green Manufacturing Technology, Harbin Institute of Technology, Harbin 150001, China;1. State Key Laboratory of Advanced Welding and Joining, Harbin Institute of Technology, Harbin, 150001, China;2. Key Laboratory of Advanced Structural-Functional Integration Materials & Green Manufacturing Technology, Harbin Institute of Technology, Harbin, 150001, China |
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| Abstract: | ![]()
Lithium garnet oxides with 6.5 mol Li, such as Li6.5La3Zr1.5(Ta/Nb)0.5O12, typically crystallise in cubic structure and exhibit excellent room-temperature ionic conductivity close to 1 mS cm?1. However, it is challenging to densify garnet oxides. In this work, we investigated how the co-doping of tantalum (Ta) and niobium (Nb) affects the densification of pressureless sintered garnet electrolytes with compositions of Li6.5La3Zr1.5Ta(0.5?x)NbxO12, where x = 0–0.5. The highest densification (94.5% of relative density) was achieved in Li6.5La3Zr1.5Ta0.1Nb0.4O12 (TN-LLZO) when it was sintered at 1150 °C for 6 h. This TN-LLZO garnet electrolyte delivers an ionic conductivity of 1.04 × 10?3 S cm?1 (at 22 °C) with a low activation energy of 0.41 eV. Our findings demonstrate that the content of dopants (Ta and Nb) plays a critical role in enhancing the sintering performance of garnet ceramics at ambient pressure. |
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| Keywords: | Solid-state electrolytes Garnet-type oxide Ionic conductivity Pressureless sintering Densification |
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