Synthesis and characterization of LLZTO solid electrolyte via the solid-state ball-milling method
DOI:
https://doi.org/10.18321/cpc23(2)163-171Keywords:
solid electrolyte, LLZTO, ionic conductivity, garnet-type, X-ray diffraction, SEMAbstract
The rapid advancement of electronic devices and energy storage systems demands the development of safe, durable, and high-performance battery components. One of the key challenges in this field is replacing flammable liquid electrolytes with more stable and reliable inorganic solid electrolytes. Among various candidates, garnet-type lithium lanthanum zirconium tantalum oxide Li₆.₄La₃Zr₁.₄Ta₀.₆O₁₂ (LLZTO) has emerged as a promising material due to its excellent chemical stability and high ionic conductivity. In this study, we present the synthesis and characterization of LLZTO solid electrolyte prepared using the solid-state ball-milling method. The as-prepared LLZTO exhibited a well-defined grain structure with particle sizes ranging from 3 to 5 micrometers. Electrochemical analysis revealed an ionic conductivity on the order of 10⁻⁵ S·cm⁻¹ at room temperature, demonstrating its potential for application in solid-state lithium-ion batteries. These findings contribute to the ongoing efforts to develop safer and more efficient energy storage solutions, paving the way for next-generation battery technologies.References
(1) X. Sun, et al., Technology development of electric vehicles: A review, Energies 13 (2019) 0090. Crossref
(2) A. Prabhakaran, et al., Design and development of an intelligent zone based master electronic control unit for power optimization in electric vehicles, Sci. Rep. 14 (2024) 70580. Crossref
(3) Y. Horowitz, et al., Between Liquid and All Solid: A Prospect on Electrolyte Future in Lithium-Ion Batteries for Electric Vehicles, Energy Technol. 8 (2020) 2000580. Crossref
(4) F. Zheng, et al., Review on solid electrolytes for all-solid-state lithium-ion batteries, J. Power Sources 389 (2018) 198–213. Crossref
(5) S. Kundu, et al., Recent development in the field of ceramics solid-state electrolytes: I–oxide ceramic solid-state electrolytes, J. Solid State Electrochem. 26 (2022) 1809–1838.
(6) N. Tolganbek, et al., Enhancing purity and ionic conductivity of NASICON-typed Li₁.₃Al₀.₃Ti₁.₇(PO₄)₃ solid electrolyte, Ceram. Int. 47 (2021) 18188–18195. Crossref
(7) S. Chen, et al., Sulfide solid electrolytes for all-solid-state lithium batteries: Structure, conductivity, stability and application, Energy Storage Mater. 14 (2018) 58–74. Crossref
(8) S. Wang, et al., Interfacial challenges for all-solid-state batteries based on sulfide solid electrolytes, J. Materiomics 7 (2021) 209–218. Crossref
(9) C. Wang, et al., Garnet-Type Solid-State Electrolytes: Materials, Interfaces and Batteries, Chem. Rev. 120 (2020) 4257–4300. Crossref
(10) J.S. Lv, et al., Modification strategies of Li₇La₃Zr₂O₁₂ ceramic electrolyte for high-performance solid-state batteries, Tungsten 3 (2021) 260–278. Crossref
(11) M. Jia, et al., Comprehensive investigation into garnet electrolytes toward application-oriented solid lithium batteries, Electrochem. Energy Rev. 3 (2020) 656–689. Crossref
(12) Y. Li, et al., Garnet electrolyte with an ultralow interfacial resistance for Li-metal batteries, J. Am. Chem. Soc. 140 (2018) 6448–6455. Crossref
(13) J.M. Weller, et al., Observation of elemental inhomogeneity and its impact on ionic conductivity in Li-conducting garnets prepared with different synthesis methods, Adv. Energy Sustain. Res. 2 (2021) 2000109. Crossref
(14) F. Shen, et al., A simple and highly efficient method toward high-density garnet-type LLZTO solid-state electrolyte, ACS Appl. Mater. Interfaces 12 (2020) 30313–30319. Crossref
(15) W. Guo, et al., Preparation of transparent LLZTO electrolyte and its application in the observation of Li dendrite, Ceram. Int. 48 (2022) 18949–18955. Crossref
(16) H. Zheng, et al., Influence of dry- and wet-milled LLZTO particles on the sintered pellets, J. Am. Ceram. Soc. 106 (2023) 274–284. Crossref
(17) Y. Li, et al., Effect of Al-Mo codoping on the structure and ionic conductivity of sol-gel derived Li₇La₃Zr₂O₁₂ ceramics, Ionics 24 (2018) 3305–3315. Crossref
(18) J.M. Weller, et al., Nonaqueous polymer combustion synthesis of cubic Li₇La₃Zr₂O₁₂ nanopowders, ACS Appl. Mater. Interfaces 12 (2020) 953–962. Crossref
(19) S. Ramakumar, et al., Lithium garnets: Synthesis, structure, Li⁺ conductivity, Li⁺ dynamics and applications, Prog. Mater. Sci. 88 (2017) 325–411. Crossref
(20) X. Huang, et al., Preparation of dense Ta-LLZO/MgO composite Li-ion solid electrolyte: Sintering, microstructure, performance and the role of MgO. J. Energy Chem. 39 (2019) 8–16. Crossref
(21) E. Il’ina. et al., Recent Strategies for Lithium-Ion Conductivity Improvement in Li₇La₃Zr₂O₁₂ Solid Electrolytes. Int. J. Mol. Sci. 24 (2023) 12905. Crossref
(22) Z. Wang, et al., Synthesis of lithium garnet oxides of the compositions series Li₇₋ₓLa₃Zr₂₋ₓTaₓO₁₂. J. Wuhan Univ. Technol. Mater. Sci. Ed. 32 (2017) 1261–1264. Crossref
(23) R. Inada, et al., Synthesis and properties of Al-free Li₇₋ₓLa₃Zr₂₋ₓTaₓO₁₂ garnet related oxides. Solid State Ion. 262 (2014) 568–572. Crossref
(24) H. Yang, et al., Ionic conductivity and ion transport mechanisms of solid-state lithium-ion battery electrolytes: A review. Energy Sci. Eng. 10 (2022) 1643–1671. Crossref
(25) T. Alam, et al., Review on Impurity and Conductivity Issues of Garnet Type Li₇La₃Zr₂O₁₂: Mechanisms, Solutions, and Perspectives. Energy Fuels 37 (2023) 15267–15282. Crossref
(26) Z. Zhang, et al., An all-solid-state lithium battery using the Li₇La₃Zr₂O₁₂ and Li₆.₇La₃Zr₁.₇Ta₀.₃O₁₂ ceramic enhanced polyethylene oxide electrolytes with superior electrochemical performance. Ceram. Int. 46 (2020) 11397–11405. Crossref
(27) S. Wang, et al., Optimized Lithium Ion Coordination via Chlorine Substitution to Enhance Ionic Conductivity of Garnet-Based Solid Electrolytes. Small 20 (2024) 2309874. Crossref
(28) Y. Gong, et al., Effect of sintering process on the microstructure and ionic conductivity of Li₇₋ₓLa₃Zr₂₋ₓTaₓO₁₂ ceramics. Ceram. Int. 45 (2019) 18439–18444. Crossref
(29) A.Y. Sang, et al., Preparation and Characterization of Ta-substituted Li₇La₃Zr₂₋ₓO₁₂ Garnet Solid Electrolyte by Sol-Gel Processing. J. Korean Ceram. Soc. 54 (2017) 332–339. Crossref