{"title":"La2Zr1.4Ta0.6O7/Li6.4La3Zr1.4Ta0.6O12纳米复合材料在石榴石型固态电解质中的助烧结效果","authors":"Teruaki Fuchigami, Hayato Yamamoto, Tanibata Naoto, Sawao Honda, Masanobu Nakayama, Ken-ichi Kakimoto","doi":"10.1111/jace.20484","DOIUrl":null,"url":null,"abstract":"<p>Garnet-type lithium lanthanum zirconium oxide is a promising solid electrolyte for lithium–oxygen batteries owing to its high ionic conductivity and stability against Li metal anodes. The development of novel sintering aids is crucial for achieving densification, grain growth, and the formation of Li conducting and mechanically strong grain interfaces, enabling ionic conductivity >10<sup>−3</sup> S/cm and long-term stability. In this study, 120 nm composite nanoparticles of La<sub>2</sub>Zr<sub>1.4</sub>Ta<sub>0.6</sub>O<sub>7</sub>/Li<sub>6.4</sub>La<sub>3</sub>Zr<sub>1.4</sub>Ta<sub>0.6</sub>O<sub>12</sub> were synthesized via planetary ball milling of Li<sub>6.4</sub>La<sub>3</sub>Zr<sub>1.4</sub>Ta<sub>0.6</sub>O<sub>12</sub> (LLZTO) microparticles followed by annealing under Ar atmosphere at 900°C. The presence of the La<sub>2</sub>Zr<sub>1.4</sub>Ta<sub>0.6</sub>O<sub>7</sub> layer and size effect in the composite nanoparticles facilitated the sintering of cubic LLZTO microparticles at 1160°C, resulting in improvement of ionic conductivity (3.9 × 10<sup>−4</sup> S/cm) and Vickers hardness (6.3 GPa) without significant particle growth. The mixing ratio of the composite nanoparticles was optimized at 20 wt%. Simulation of the nanoparticle arrangement on the microparticles with various mixing ratios revealed that adding 10‒20 wt% nanoparticles is essential to cover microparticles with a single layer, suppressing highly resistive grain boundary formation.</p>","PeriodicalId":200,"journal":{"name":"Journal of the American Ceramic Society","volume":"108 7","pages":""},"PeriodicalIF":3.5000,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1111/jace.20484","citationCount":"0","resultStr":"{\"title\":\"Sintering aid effect of La2Zr1.4Ta0.6O7/Li6.4La3Zr1.4Ta0.6O12 nanocomposite in garnet-type solid-state electrolyte\",\"authors\":\"Teruaki Fuchigami, Hayato Yamamoto, Tanibata Naoto, Sawao Honda, Masanobu Nakayama, Ken-ichi Kakimoto\",\"doi\":\"10.1111/jace.20484\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Garnet-type lithium lanthanum zirconium oxide is a promising solid electrolyte for lithium–oxygen batteries owing to its high ionic conductivity and stability against Li metal anodes. The development of novel sintering aids is crucial for achieving densification, grain growth, and the formation of Li conducting and mechanically strong grain interfaces, enabling ionic conductivity >10<sup>−3</sup> S/cm and long-term stability. In this study, 120 nm composite nanoparticles of La<sub>2</sub>Zr<sub>1.4</sub>Ta<sub>0.6</sub>O<sub>7</sub>/Li<sub>6.4</sub>La<sub>3</sub>Zr<sub>1.4</sub>Ta<sub>0.6</sub>O<sub>12</sub> were synthesized via planetary ball milling of Li<sub>6.4</sub>La<sub>3</sub>Zr<sub>1.4</sub>Ta<sub>0.6</sub>O<sub>12</sub> (LLZTO) microparticles followed by annealing under Ar atmosphere at 900°C. The presence of the La<sub>2</sub>Zr<sub>1.4</sub>Ta<sub>0.6</sub>O<sub>7</sub> layer and size effect in the composite nanoparticles facilitated the sintering of cubic LLZTO microparticles at 1160°C, resulting in improvement of ionic conductivity (3.9 × 10<sup>−4</sup> S/cm) and Vickers hardness (6.3 GPa) without significant particle growth. The mixing ratio of the composite nanoparticles was optimized at 20 wt%. Simulation of the nanoparticle arrangement on the microparticles with various mixing ratios revealed that adding 10‒20 wt% nanoparticles is essential to cover microparticles with a single layer, suppressing highly resistive grain boundary formation.</p>\",\"PeriodicalId\":200,\"journal\":{\"name\":\"Journal of the American Ceramic Society\",\"volume\":\"108 7\",\"pages\":\"\"},\"PeriodicalIF\":3.5000,\"publicationDate\":\"2025-03-20\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://onlinelibrary.wiley.com/doi/epdf/10.1111/jace.20484\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of the American Ceramic Society\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://onlinelibrary.wiley.com/doi/10.1111/jace.20484\",\"RegionNum\":3,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"MATERIALS SCIENCE, CERAMICS\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of the American Ceramic Society","FirstCategoryId":"88","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1111/jace.20484","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, CERAMICS","Score":null,"Total":0}
Sintering aid effect of La2Zr1.4Ta0.6O7/Li6.4La3Zr1.4Ta0.6O12 nanocomposite in garnet-type solid-state electrolyte
Garnet-type lithium lanthanum zirconium oxide is a promising solid electrolyte for lithium–oxygen batteries owing to its high ionic conductivity and stability against Li metal anodes. The development of novel sintering aids is crucial for achieving densification, grain growth, and the formation of Li conducting and mechanically strong grain interfaces, enabling ionic conductivity >10−3 S/cm and long-term stability. In this study, 120 nm composite nanoparticles of La2Zr1.4Ta0.6O7/Li6.4La3Zr1.4Ta0.6O12 were synthesized via planetary ball milling of Li6.4La3Zr1.4Ta0.6O12 (LLZTO) microparticles followed by annealing under Ar atmosphere at 900°C. The presence of the La2Zr1.4Ta0.6O7 layer and size effect in the composite nanoparticles facilitated the sintering of cubic LLZTO microparticles at 1160°C, resulting in improvement of ionic conductivity (3.9 × 10−4 S/cm) and Vickers hardness (6.3 GPa) without significant particle growth. The mixing ratio of the composite nanoparticles was optimized at 20 wt%. Simulation of the nanoparticle arrangement on the microparticles with various mixing ratios revealed that adding 10‒20 wt% nanoparticles is essential to cover microparticles with a single layer, suppressing highly resistive grain boundary formation.
期刊介绍：
The Journal of the American Ceramic Society contains records of original research that provide insight into or describe the science of ceramic and glass materials and composites based on ceramics and glasses. These papers include reports on discovery, characterization, and analysis of new inorganic, non-metallic materials; synthesis methods; phase relationships; processing approaches; microstructure-property relationships; and functionalities. Of great interest are works that support understanding founded on fundamental principles using experimental, theoretical, or computational methods or combinations of those approaches. All the published papers must be of enduring value and relevant to the science of ceramics and glasses or composites based on those materials.
Papers on fundamental ceramic and glass science are welcome including those in the following areas:
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Materials design, selection, synthesis and processing methods[...]
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