Improvement of Short-Circuit Tolerance of Garnet Type Solid Electrolyte Li6.4La3Zr1.4Ta0.6O12 by Li2WO4 and Al2O3 Sintering Aids and La Deficiency
Garnet-type Li6.4La3Zr1.4Ta0.6O12 (LLZT) is one of the most promising solid electrolytes for all solid-state batteries due to its relatively high Li-ion conductivity and electrochemical stability against Li metal anode. However, the presence of pores and voids in the electrolyte causes short circuit...
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The Electrochemical Society of Japan
2025-06-01
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| Series: | Electrochemistry |
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| Online Access: | https://www.jstage.jst.go.jp/article/electrochemistry/93/6/93_25-71040/_html/-char/en |
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| author | Yuya KONO Yuta MASUO Kento OBINATA Takayuki DOI Masakazu HARUTA Hitoshi ONODERA Shuhei YOSHIDA Minoru INABA |
| author_facet | Yuya KONO Yuta MASUO Kento OBINATA Takayuki DOI Masakazu HARUTA Hitoshi ONODERA Shuhei YOSHIDA Minoru INABA |
| author_sort | Yuya KONO |
| collection | DOAJ |
| description | Garnet-type Li6.4La3Zr1.4Ta0.6O12 (LLZT) is one of the most promising solid electrolytes for all solid-state batteries due to its relatively high Li-ion conductivity and electrochemical stability against Li metal anode. However, the presence of pores and voids in the electrolyte causes short circuit due to lithium dendrites growth. In the present study, the effects of Li2WO4 (LWO) and Al2O3 sintering aids on the densification of LLZT were investigated to decrease the pores and voids and thereby to improve the tolerance for Li dendrite growth. Both sintering aids were effective for improving the densification; however, their effects were totally different. While 2 wt% Al2O3 significantly enhanced the grain growth, 4 wt% LWO gave smaller grains of uniform size distribution (3–5 µm). Simultaneous addition of 4 wt% LWO and 2 wt% Al2O3 gave relatively larger grains (5–20 µm) with very few voids, and a very high relative density of 99.3 % was obtained. The critical current density (CCD) was improved from 0.2 to 0.4 mA cm−2. Reducing the amount of lanthanum in LLZT led to the formation of lithium zirconate as a self-forming sintering aid and achieved a higher relative density (99.7 %) for La-deficient (6 %) LLZT with 4 wt% LWO and 2 wt% Al2O3. The CCD was further improved to 0.6 mA cm−2. |
| format | Article |
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| institution | OA Journals |
| issn | 2186-2451 |
| language | English |
| publishDate | 2025-06-01 |
| publisher | The Electrochemical Society of Japan |
| record_format | Article |
| series | Electrochemistry |
| spelling | doaj-art-e8a59b08013042ab8a6c6314e2f150832025-08-20T02:10:25ZengThe Electrochemical Society of JapanElectrochemistry2186-24512025-06-0193606302206302210.5796/electrochemistry.25-71040electrochemistryImprovement of Short-Circuit Tolerance of Garnet Type Solid Electrolyte Li6.4La3Zr1.4Ta0.6O12 by Li2WO4 and Al2O3 Sintering Aids and La DeficiencyYuya KONO0Yuta MASUO1Kento OBINATA2Takayuki DOI3https://orcid.org/0000-0003-1081-9223Masakazu HARUTA4https://orcid.org/0000-0001-9107-8425Hitoshi ONODERA5https://orcid.org/0009-0000-3387-5055Shuhei YOSHIDA6https://orcid.org/0009-0001-8430-0013Minoru INABA7https://orcid.org/0000-0002-2480-0585Department of Molecular Chemistry and Biochemistry, Doshisha UniversityDENSO CORPORATIONDepartment of Molecular Chemistry and Biochemistry, Doshisha UniversityDepartment of Molecular Chemistry and Biochemistry, Doshisha UniversityFaculty of Humanity-Oriented Science and Engineering, Kindai UniversityDENSO CORPORATIONDENSO CORPORATIONDepartment of Molecular Chemistry and Biochemistry, Doshisha UniversityGarnet-type Li6.4La3Zr1.4Ta0.6O12 (LLZT) is one of the most promising solid electrolytes for all solid-state batteries due to its relatively high Li-ion conductivity and electrochemical stability against Li metal anode. However, the presence of pores and voids in the electrolyte causes short circuit due to lithium dendrites growth. In the present study, the effects of Li2WO4 (LWO) and Al2O3 sintering aids on the densification of LLZT were investigated to decrease the pores and voids and thereby to improve the tolerance for Li dendrite growth. Both sintering aids were effective for improving the densification; however, their effects were totally different. While 2 wt% Al2O3 significantly enhanced the grain growth, 4 wt% LWO gave smaller grains of uniform size distribution (3–5 µm). Simultaneous addition of 4 wt% LWO and 2 wt% Al2O3 gave relatively larger grains (5–20 µm) with very few voids, and a very high relative density of 99.3 % was obtained. The critical current density (CCD) was improved from 0.2 to 0.4 mA cm−2. Reducing the amount of lanthanum in LLZT led to the formation of lithium zirconate as a self-forming sintering aid and achieved a higher relative density (99.7 %) for La-deficient (6 %) LLZT with 4 wt% LWO and 2 wt% Al2O3. The CCD was further improved to 0.6 mA cm−2.https://www.jstage.jst.go.jp/article/electrochemistry/93/6/93_25-71040/_html/-char/ensolid electrolytelithium dendriterelative densitysintering aid |
| spellingShingle | Yuya KONO Yuta MASUO Kento OBINATA Takayuki DOI Masakazu HARUTA Hitoshi ONODERA Shuhei YOSHIDA Minoru INABA Improvement of Short-Circuit Tolerance of Garnet Type Solid Electrolyte Li6.4La3Zr1.4Ta0.6O12 by Li2WO4 and Al2O3 Sintering Aids and La Deficiency Electrochemistry solid electrolyte lithium dendrite relative density sintering aid |
| title | Improvement of Short-Circuit Tolerance of Garnet Type Solid Electrolyte Li6.4La3Zr1.4Ta0.6O12 by Li2WO4 and Al2O3 Sintering Aids and La Deficiency |
| title_full | Improvement of Short-Circuit Tolerance of Garnet Type Solid Electrolyte Li6.4La3Zr1.4Ta0.6O12 by Li2WO4 and Al2O3 Sintering Aids and La Deficiency |
| title_fullStr | Improvement of Short-Circuit Tolerance of Garnet Type Solid Electrolyte Li6.4La3Zr1.4Ta0.6O12 by Li2WO4 and Al2O3 Sintering Aids and La Deficiency |
| title_full_unstemmed | Improvement of Short-Circuit Tolerance of Garnet Type Solid Electrolyte Li6.4La3Zr1.4Ta0.6O12 by Li2WO4 and Al2O3 Sintering Aids and La Deficiency |
| title_short | Improvement of Short-Circuit Tolerance of Garnet Type Solid Electrolyte Li6.4La3Zr1.4Ta0.6O12 by Li2WO4 and Al2O3 Sintering Aids and La Deficiency |
| title_sort | improvement of short circuit tolerance of garnet type solid electrolyte li6 4la3zr1 4ta0 6o12 by li2wo4 and al2o3 sintering aids and la deficiency |
| topic | solid electrolyte lithium dendrite relative density sintering aid |
| url | https://www.jstage.jst.go.jp/article/electrochemistry/93/6/93_25-71040/_html/-char/en |
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