Wet Chemical Method ZnF2 Interlayer for High Critical Current Density Lithium Metal Batteries Utilizing Ba and Ta–Doped Li7La3Zr2O12 Garnet Solid Electrolyte
Abstract Li metal batteries with garnet‐type solid electrolytes have the potential to increase specific energy and power densities of current Li‐ion batteries. Li metal batteries have been hampered by the poor wettability of solid electrolyte with elemental lithium. Here, to resolve the solid garnet...
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Wiley-VCH
2025-01-01
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Online Access: | https://doi.org/10.1002/admi.202400570 |
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author | Subhajit Sarkar Vishnu Surendran Venkataraman Thangadurai |
author_facet | Subhajit Sarkar Vishnu Surendran Venkataraman Thangadurai |
author_sort | Subhajit Sarkar |
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description | Abstract Li metal batteries with garnet‐type solid electrolytes have the potential to increase specific energy and power densities of current Li‐ion batteries. Li metal batteries have been hampered by the poor wettability of solid electrolyte with elemental lithium. Here, to resolve the solid garnet electrolyte/Li interface issue, a scalable, cost‐effective, and efficient surfactant‐assisted wet‐chemical strategy is developed. A ZnF2 interlayer coating is applied on Ba and Ta ‐co‐doped Li7La2.75Ba0.25Zr1.75Ta0.25O12 that formed LiF and Li‐Zn alloy upon contact with molten Li. Conformal contact applying a homogenous surfactant‐assisted ZnF2 coating reduced the interfacial resistance from 87 to 15.5 Ω cm2 which enhanced critical current density to a record high value of 5 mA cm−2 at room temperature. Dense and Li2CO3 free garnet solid electrolyte assisted in achieving long‐term stability for 1000 cycles at 1 mA cm−2. Interface stabilized Li/ZnF2‐ solid electrolyte/liquid electrolyte/LiFePO4 cell displayed a 90% capacity retention over 800 cycles at 0.2 C, with Coulombic efficiency of 99% as well as excellent cycle stability at 1 C, with ≈91% of capacity retention for 500 cycles. Using a new design principle for Li anode interfaces, next‐generation power‐intensive and stable solid‐state Li metal batteries can be developed. |
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institution | Kabale University |
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language | English |
publishDate | 2025-01-01 |
publisher | Wiley-VCH |
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series | Advanced Materials Interfaces |
spelling | doaj-art-2c434b50de69479cabf03e637db447672025-01-03T08:39:29ZengWiley-VCHAdvanced Materials Interfaces2196-73502025-01-01121n/an/a10.1002/admi.202400570Wet Chemical Method ZnF2 Interlayer for High Critical Current Density Lithium Metal Batteries Utilizing Ba and Ta–Doped Li7La3Zr2O12 Garnet Solid ElectrolyteSubhajit Sarkar0Vishnu Surendran1Venkataraman Thangadurai2Department of ChemistryUniversity of Calgary2500 University DriveCalgaryABT2N 1N4CanadaDepartment of ChemistryUniversity of Calgary2500 University DriveCalgaryABT2N 1N4CanadaDepartment of ChemistryUniversity of Calgary2500 University DriveCalgaryABT2N 1N4CanadaAbstract Li metal batteries with garnet‐type solid electrolytes have the potential to increase specific energy and power densities of current Li‐ion batteries. Li metal batteries have been hampered by the poor wettability of solid electrolyte with elemental lithium. Here, to resolve the solid garnet electrolyte/Li interface issue, a scalable, cost‐effective, and efficient surfactant‐assisted wet‐chemical strategy is developed. A ZnF2 interlayer coating is applied on Ba and Ta ‐co‐doped Li7La2.75Ba0.25Zr1.75Ta0.25O12 that formed LiF and Li‐Zn alloy upon contact with molten Li. Conformal contact applying a homogenous surfactant‐assisted ZnF2 coating reduced the interfacial resistance from 87 to 15.5 Ω cm2 which enhanced critical current density to a record high value of 5 mA cm−2 at room temperature. Dense and Li2CO3 free garnet solid electrolyte assisted in achieving long‐term stability for 1000 cycles at 1 mA cm−2. Interface stabilized Li/ZnF2‐ solid electrolyte/liquid electrolyte/LiFePO4 cell displayed a 90% capacity retention over 800 cycles at 0.2 C, with Coulombic efficiency of 99% as well as excellent cycle stability at 1 C, with ≈91% of capacity retention for 500 cycles. Using a new design principle for Li anode interfaces, next‐generation power‐intensive and stable solid‐state Li metal batteries can be developed.https://doi.org/10.1002/admi.202400570critical current densitygarnet‐type solid electrolytehybrid solid‐state cellsmultifunctional alloysurfactant‐assisted interlayer |
spellingShingle | Subhajit Sarkar Vishnu Surendran Venkataraman Thangadurai Wet Chemical Method ZnF2 Interlayer for High Critical Current Density Lithium Metal Batteries Utilizing Ba and Ta–Doped Li7La3Zr2O12 Garnet Solid Electrolyte Advanced Materials Interfaces critical current density garnet‐type solid electrolyte hybrid solid‐state cells multifunctional alloy surfactant‐assisted interlayer |
title | Wet Chemical Method ZnF2 Interlayer for High Critical Current Density Lithium Metal Batteries Utilizing Ba and Ta–Doped Li7La3Zr2O12 Garnet Solid Electrolyte |
title_full | Wet Chemical Method ZnF2 Interlayer for High Critical Current Density Lithium Metal Batteries Utilizing Ba and Ta–Doped Li7La3Zr2O12 Garnet Solid Electrolyte |
title_fullStr | Wet Chemical Method ZnF2 Interlayer for High Critical Current Density Lithium Metal Batteries Utilizing Ba and Ta–Doped Li7La3Zr2O12 Garnet Solid Electrolyte |
title_full_unstemmed | Wet Chemical Method ZnF2 Interlayer for High Critical Current Density Lithium Metal Batteries Utilizing Ba and Ta–Doped Li7La3Zr2O12 Garnet Solid Electrolyte |
title_short | Wet Chemical Method ZnF2 Interlayer for High Critical Current Density Lithium Metal Batteries Utilizing Ba and Ta–Doped Li7La3Zr2O12 Garnet Solid Electrolyte |
title_sort | wet chemical method znf2 interlayer for high critical current density lithium metal batteries utilizing ba and ta doped li7la3zr2o12 garnet solid electrolyte |
topic | critical current density garnet‐type solid electrolyte hybrid solid‐state cells multifunctional alloy surfactant‐assisted interlayer |
url | https://doi.org/10.1002/admi.202400570 |
work_keys_str_mv | AT subhajitsarkar wetchemicalmethodznf2interlayerforhighcriticalcurrentdensitylithiummetalbatteriesutilizingbaandtadopedli7la3zr2o12garnetsolidelectrolyte AT vishnusurendran wetchemicalmethodznf2interlayerforhighcriticalcurrentdensitylithiummetalbatteriesutilizingbaandtadopedli7la3zr2o12garnetsolidelectrolyte AT venkataramanthangadurai wetchemicalmethodznf2interlayerforhighcriticalcurrentdensitylithiummetalbatteriesutilizingbaandtadopedli7la3zr2o12garnetsolidelectrolyte |