Removal and Reoccurrence of LLZTO Surface Contaminants under Glovebox Conditions
The reactivity of Li6.4La3Zr1.4Ta0.6O12 (LLZTO) solid electrolytes to form lithio-phobic species such as Li2CO3 on their surface when exposed to trace amounts of H2O and CO2 limits the progress of LLZTO-based solid-state batteries. Various treatments, such as annealing LLZTO within a glovebox or aci...
| Үндсэн зохиолчид: | , , , , , , , , , , , |
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| Формат: | Journal article |
| Хэл сонгох: | English |
| Хэвлэсэн: |
American Chemical Society
2024
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| _version_ | 1826313054324785152 |
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| author | Siniscalchi, M Gibson, JS Tufnail, J Swallow, JEN Lewis, J Matthews, G Karagoz, B van Spronsen, MA Held, G Weatherup, RS Grovenor, CRM Speller, SC |
| author_facet | Siniscalchi, M Gibson, JS Tufnail, J Swallow, JEN Lewis, J Matthews, G Karagoz, B van Spronsen, MA Held, G Weatherup, RS Grovenor, CRM Speller, SC |
| author_sort | Siniscalchi, M |
| collection | OXFORD |
| description | The reactivity of Li6.4La3Zr1.4Ta0.6O12 (LLZTO) solid electrolytes to form lithio-phobic species such as Li2CO3 on their surface when exposed to trace amounts of H2O and CO2 limits the progress of LLZTO-based solid-state batteries. Various treatments, such as annealing LLZTO within a glovebox or acid etching, aim at removing the surface contaminants, but a comprehensive understanding of the evolving LLZTO surface chemistry during and after these treatments is lacking. Here, glovebox-like H2O and CO2 conditions were recreated in a near ambient pressure X-ray photoelectron spectroscopy chamber to analyze the LLZTO surface under realistic conditions. We find that annealing LLZTO at 600 °C in this atmosphere effectively removes the surface contaminants, but a significant level of contamination reappears upon cooling down. In contrast, HCl(aq) acid etching demonstrates superior Li2CO3 removal and stable surface chemistry post treatment. To avoid air exposure during the acid treatment, an anhydrous HCl solution in diethyl ether was used directly within the glovebox. This novel acid etching strategy delivers the lowest lithium/LLZTO interfacial resistance and the highest critical current density. |
| first_indexed | 2024-09-25T04:06:48Z |
| format | Journal article |
| id | oxford-uuid:453b0395-9262-46be-9a44-c88843f4a50a |
| institution | University of Oxford |
| language | English |
| last_indexed | 2024-09-25T04:06:48Z |
| publishDate | 2024 |
| publisher | American Chemical Society |
| record_format | dspace |
| spelling | oxford-uuid:453b0395-9262-46be-9a44-c88843f4a50a2024-05-30T20:05:59ZRemoval and Reoccurrence of LLZTO Surface Contaminants under Glovebox ConditionsJournal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:453b0395-9262-46be-9a44-c88843f4a50aEnglishJisc Publications RouterAmerican Chemical Society2024Siniscalchi, MGibson, JSTufnail, JSwallow, JENLewis, JMatthews, GKaragoz, Bvan Spronsen, MAHeld, GWeatherup, RSGrovenor, CRMSpeller, SCThe reactivity of Li6.4La3Zr1.4Ta0.6O12 (LLZTO) solid electrolytes to form lithio-phobic species such as Li2CO3 on their surface when exposed to trace amounts of H2O and CO2 limits the progress of LLZTO-based solid-state batteries. Various treatments, such as annealing LLZTO within a glovebox or acid etching, aim at removing the surface contaminants, but a comprehensive understanding of the evolving LLZTO surface chemistry during and after these treatments is lacking. Here, glovebox-like H2O and CO2 conditions were recreated in a near ambient pressure X-ray photoelectron spectroscopy chamber to analyze the LLZTO surface under realistic conditions. We find that annealing LLZTO at 600 °C in this atmosphere effectively removes the surface contaminants, but a significant level of contamination reappears upon cooling down. In contrast, HCl(aq) acid etching demonstrates superior Li2CO3 removal and stable surface chemistry post treatment. To avoid air exposure during the acid treatment, an anhydrous HCl solution in diethyl ether was used directly within the glovebox. This novel acid etching strategy delivers the lowest lithium/LLZTO interfacial resistance and the highest critical current density. |
| spellingShingle | Siniscalchi, M Gibson, JS Tufnail, J Swallow, JEN Lewis, J Matthews, G Karagoz, B van Spronsen, MA Held, G Weatherup, RS Grovenor, CRM Speller, SC Removal and Reoccurrence of LLZTO Surface Contaminants under Glovebox Conditions |
| title | Removal and Reoccurrence of LLZTO Surface Contaminants under Glovebox Conditions |
| title_full | Removal and Reoccurrence of LLZTO Surface Contaminants under Glovebox Conditions |
| title_fullStr | Removal and Reoccurrence of LLZTO Surface Contaminants under Glovebox Conditions |
| title_full_unstemmed | Removal and Reoccurrence of LLZTO Surface Contaminants under Glovebox Conditions |
| title_short | Removal and Reoccurrence of LLZTO Surface Contaminants under Glovebox Conditions |
| title_sort | removal and reoccurrence of llzto surface contaminants under glovebox conditions |
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