Ultrafast Sintering of Dense Li7La3Zr2O12 Membranes for Li Metal All‐Solid‐State Batteries
Abstract Ultrafast sintering (UFS) is a compelling approach for fabricating Li7La3Zr2O12 (LLZO) solid‐state electrolytes (SSEs), paving the way for advancing and commercializing Li‐garnet solid‐state batteries. Although this method is commonly applied to the sintering of LLZO ceramics, its use for p...
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Wiley
2025-01-01
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| Series: | Advanced Science |
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| Online Access: | https://doi.org/10.1002/advs.202412370 |
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| author | Faruk Okur Huanyu Zhang Julian F. Baumgärtner Jaka Sivavec Matthias Klimpel Gregor Paul Wasser Romain Dubey Lars P.H. Jeurgens Dmitry Chernyshov Wouter vanBeek Kostiantyn V. Kravchyk Maksym V. Kovalenko |
| author_facet | Faruk Okur Huanyu Zhang Julian F. Baumgärtner Jaka Sivavec Matthias Klimpel Gregor Paul Wasser Romain Dubey Lars P.H. Jeurgens Dmitry Chernyshov Wouter vanBeek Kostiantyn V. Kravchyk Maksym V. Kovalenko |
| author_sort | Faruk Okur |
| collection | DOAJ |
| description | Abstract Ultrafast sintering (UFS) is a compelling approach for fabricating Li7La3Zr2O12 (LLZO) solid‐state electrolytes (SSEs), paving the way for advancing and commercializing Li‐garnet solid‐state batteries. Although this method is commonly applied to the sintering of LLZO ceramics, its use for producing dense, phase‐pure LLZO SSEs has thus far been primarily limited to millimeter‐thick pellets, which are unsuitable for commercial solid‐state batteries. This study presents ultrafast sintering as a highly effective approach for fabricating self‐standing, dense, 45 µm‐thick LLZO membranes. The chemical and structural evolution of LLZO membranes during the UFS process is characterized through in situ synchrotron X‐ray diffraction and thermogravimetric analysis‐mass spectrometry, complemented by an in‐depth investigation of surface chemistry using X‐ray photoelectron spectroscopy. The membranes in Li/LLZO/Li symmetrical cell configuration exhibit a high critical current density of up to 12.5 mA cm−2 and maintain superior cycling stability for 250 cycles at a current density of 1 mA cm−2, with an areal capacity limit of 1 mAh cm−2. The electrochemical performance of LLZO membranes is also assessed in full cell configuration using a pyrochlore‐type iron (III) hydroxy fluoride cathode. |
| format | Article |
| id | doaj-art-bf13cfff2e8f40fcb9d34f6f02a3879f |
| institution | Kabale University |
| issn | 2198-3844 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Wiley |
| record_format | Article |
| series | Advanced Science |
| spelling | doaj-art-bf13cfff2e8f40fcb9d34f6f02a3879f2025-01-13T15:29:43ZengWileyAdvanced Science2198-38442025-01-01122n/an/a10.1002/advs.202412370Ultrafast Sintering of Dense Li7La3Zr2O12 Membranes for Li Metal All‐Solid‐State BatteriesFaruk Okur0Huanyu Zhang1Julian F. Baumgärtner2Jaka Sivavec3Matthias Klimpel4Gregor Paul Wasser5Romain Dubey6Lars P.H. Jeurgens7Dmitry Chernyshov8Wouter vanBeek9Kostiantyn V. Kravchyk10Maksym V. Kovalenko11Laboratory of Inorganic Chemistry Department of Chemistry and Applied Biosciences ETH Zürich Zürich CH‐8093 SwitzerlandLaboratory of Inorganic Chemistry Department of Chemistry and Applied Biosciences ETH Zürich Zürich CH‐8093 SwitzerlandLaboratory of Inorganic Chemistry Department of Chemistry and Applied Biosciences ETH Zürich Zürich CH‐8093 SwitzerlandLaboratory of Inorganic Chemistry Department of Chemistry and Applied Biosciences ETH Zürich Zürich CH‐8093 SwitzerlandLaboratory of Inorganic Chemistry Department of Chemistry and Applied Biosciences ETH Zürich Zürich CH‐8093 SwitzerlandLaboratory of Inorganic Chemistry Department of Chemistry and Applied Biosciences ETH Zürich Zürich CH‐8093 SwitzerlandLaboratory of Inorganic Chemistry Department of Chemistry and Applied Biosciences ETH Zürich Zürich CH‐8093 SwitzerlandLaboratory for Joining Technologies & Corrosion Empa – Swiss Federal Laboratories for Materials Science & Technology Dübendorf CH‐8600 SwitzerlandSwiss‐Norwegian Beamlines European Synchrotron Radiation Facility Grenoble 38000 FranceSwiss‐Norwegian Beamlines European Synchrotron Radiation Facility Grenoble 38000 FranceLaboratory of Inorganic Chemistry Department of Chemistry and Applied Biosciences ETH Zürich Zürich CH‐8093 SwitzerlandLaboratory of Inorganic Chemistry Department of Chemistry and Applied Biosciences ETH Zürich Zürich CH‐8093 SwitzerlandAbstract Ultrafast sintering (UFS) is a compelling approach for fabricating Li7La3Zr2O12 (LLZO) solid‐state electrolytes (SSEs), paving the way for advancing and commercializing Li‐garnet solid‐state batteries. Although this method is commonly applied to the sintering of LLZO ceramics, its use for producing dense, phase‐pure LLZO SSEs has thus far been primarily limited to millimeter‐thick pellets, which are unsuitable for commercial solid‐state batteries. This study presents ultrafast sintering as a highly effective approach for fabricating self‐standing, dense, 45 µm‐thick LLZO membranes. The chemical and structural evolution of LLZO membranes during the UFS process is characterized through in situ synchrotron X‐ray diffraction and thermogravimetric analysis‐mass spectrometry, complemented by an in‐depth investigation of surface chemistry using X‐ray photoelectron spectroscopy. The membranes in Li/LLZO/Li symmetrical cell configuration exhibit a high critical current density of up to 12.5 mA cm−2 and maintain superior cycling stability for 250 cycles at a current density of 1 mA cm−2, with an areal capacity limit of 1 mAh cm−2. The electrochemical performance of LLZO membranes is also assessed in full cell configuration using a pyrochlore‐type iron (III) hydroxy fluoride cathode.https://doi.org/10.1002/advs.202412370Li metal all‐solid‐state batterieslithiumLLZOmembranessolid‐state electrolyte |
| spellingShingle | Faruk Okur Huanyu Zhang Julian F. Baumgärtner Jaka Sivavec Matthias Klimpel Gregor Paul Wasser Romain Dubey Lars P.H. Jeurgens Dmitry Chernyshov Wouter vanBeek Kostiantyn V. Kravchyk Maksym V. Kovalenko Ultrafast Sintering of Dense Li7La3Zr2O12 Membranes for Li Metal All‐Solid‐State Batteries Advanced Science Li metal all‐solid‐state batteries lithium LLZO membranes solid‐state electrolyte |
| title | Ultrafast Sintering of Dense Li7La3Zr2O12 Membranes for Li Metal All‐Solid‐State Batteries |
| title_full | Ultrafast Sintering of Dense Li7La3Zr2O12 Membranes for Li Metal All‐Solid‐State Batteries |
| title_fullStr | Ultrafast Sintering of Dense Li7La3Zr2O12 Membranes for Li Metal All‐Solid‐State Batteries |
| title_full_unstemmed | Ultrafast Sintering of Dense Li7La3Zr2O12 Membranes for Li Metal All‐Solid‐State Batteries |
| title_short | Ultrafast Sintering of Dense Li7La3Zr2O12 Membranes for Li Metal All‐Solid‐State Batteries |
| title_sort | ultrafast sintering of dense li7la3zr2o12 membranes for li metal all solid state batteries |
| topic | Li metal all‐solid‐state batteries lithium LLZO membranes solid‐state electrolyte |
| url | https://doi.org/10.1002/advs.202412370 |
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