Grain Boundary Transport in the Argyrodite‐Type Li6PS5Br Solid Electrolyte: Influence of Misorientation and Anion Disorder on Li Ion Mobility
Abstract To realize efficient solid‐state batteries, many efforts are directed toward maximizing the bulk Li+ conductivity of sulfide superionic conductors, as demonstrated for the argyrodite‐type materials Li6PS5Cl and Li6PS5Br. Notably, in these archetype materials, the fast Li+ transport benefits...
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Wiley-VCH
2024-11-01
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| Series: | Advanced Materials Interfaces |
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| Online Access: | https://doi.org/10.1002/admi.202400423 |
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| author | Marcel Sadowski Karsten Albe |
| author_facet | Marcel Sadowski Karsten Albe |
| author_sort | Marcel Sadowski |
| collection | DOAJ |
| description | Abstract To realize efficient solid‐state batteries, many efforts are directed toward maximizing the bulk Li+ conductivity of sulfide superionic conductors, as demonstrated for the argyrodite‐type materials Li6PS5Cl and Li6PS5Br. Notably, in these archetype materials, the fast Li+ transport benefits from considerable anion disorder on the halide and sulfur sublattices. To further improve the Li+ conductivity, however, one must consider not only the bulk properties of the solid electrolyte (SE) but also microstructural aspects. It is, however, controversially discussed whether grain boundary (GB) transport is generally detrimental for the overall ion conductivity in agyrodite‐type SEs. Thus, by means of atomistic computer simulations, the Li+ ion transport is studied in twist and tilt GBs of Li6PS5Br, revealing that the Br/S site exchange determines whether the presence of GBs deteriorates the ionic conductivity: Whereas the material with 0% Br/S site exchange only shows locally limited bulk diffusion but enhanced GB conductivity, at higher degrees of site exchange, GBs deteriorate Li+ diffusion. These results show that the interplay of GB transport directly depends on the degree of site exchange in argyrodite‐type materials. |
| format | Article |
| id | doaj-art-e62553187e5743aa80eb6d7c294be43b |
| institution | OA Journals |
| issn | 2196-7350 |
| language | English |
| publishDate | 2024-11-01 |
| publisher | Wiley-VCH |
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| series | Advanced Materials Interfaces |
| spelling | doaj-art-e62553187e5743aa80eb6d7c294be43b2025-08-20T02:23:44ZengWiley-VCHAdvanced Materials Interfaces2196-73502024-11-011133n/an/a10.1002/admi.202400423Grain Boundary Transport in the Argyrodite‐Type Li6PS5Br Solid Electrolyte: Influence of Misorientation and Anion Disorder on Li Ion MobilityMarcel Sadowski0Karsten Albe1Institute of Materials Science Technical University of Darmstadt Otto‐Bernd‐Straße 3 64287 Darmstadt GermanyInstitute of Materials Science Technical University of Darmstadt Otto‐Bernd‐Straße 3 64287 Darmstadt GermanyAbstract To realize efficient solid‐state batteries, many efforts are directed toward maximizing the bulk Li+ conductivity of sulfide superionic conductors, as demonstrated for the argyrodite‐type materials Li6PS5Cl and Li6PS5Br. Notably, in these archetype materials, the fast Li+ transport benefits from considerable anion disorder on the halide and sulfur sublattices. To further improve the Li+ conductivity, however, one must consider not only the bulk properties of the solid electrolyte (SE) but also microstructural aspects. It is, however, controversially discussed whether grain boundary (GB) transport is generally detrimental for the overall ion conductivity in agyrodite‐type SEs. Thus, by means of atomistic computer simulations, the Li+ ion transport is studied in twist and tilt GBs of Li6PS5Br, revealing that the Br/S site exchange determines whether the presence of GBs deteriorates the ionic conductivity: Whereas the material with 0% Br/S site exchange only shows locally limited bulk diffusion but enhanced GB conductivity, at higher degrees of site exchange, GBs deteriorate Li+ diffusion. These results show that the interplay of GB transport directly depends on the degree of site exchange in argyrodite‐type materials.https://doi.org/10.1002/admi.202400423batteriesdiffusiongrain boundariesion disorderlithiumsulfide solid electrolytes |
| spellingShingle | Marcel Sadowski Karsten Albe Grain Boundary Transport in the Argyrodite‐Type Li6PS5Br Solid Electrolyte: Influence of Misorientation and Anion Disorder on Li Ion Mobility Advanced Materials Interfaces batteries diffusion grain boundaries ion disorder lithium sulfide solid electrolytes |
| title | Grain Boundary Transport in the Argyrodite‐Type Li6PS5Br Solid Electrolyte: Influence of Misorientation and Anion Disorder on Li Ion Mobility |
| title_full | Grain Boundary Transport in the Argyrodite‐Type Li6PS5Br Solid Electrolyte: Influence of Misorientation and Anion Disorder on Li Ion Mobility |
| title_fullStr | Grain Boundary Transport in the Argyrodite‐Type Li6PS5Br Solid Electrolyte: Influence of Misorientation and Anion Disorder on Li Ion Mobility |
| title_full_unstemmed | Grain Boundary Transport in the Argyrodite‐Type Li6PS5Br Solid Electrolyte: Influence of Misorientation and Anion Disorder on Li Ion Mobility |
| title_short | Grain Boundary Transport in the Argyrodite‐Type Li6PS5Br Solid Electrolyte: Influence of Misorientation and Anion Disorder on Li Ion Mobility |
| title_sort | grain boundary transport in the argyrodite type li6ps5br solid electrolyte influence of misorientation and anion disorder on li ion mobility |
| topic | batteries diffusion grain boundaries ion disorder lithium sulfide solid electrolytes |
| url | https://doi.org/10.1002/admi.202400423 |
| work_keys_str_mv | AT marcelsadowski grainboundarytransportintheargyroditetypeli6ps5brsolidelectrolyteinfluenceofmisorientationandaniondisorderonliionmobility AT karstenalbe grainboundarytransportintheargyroditetypeli6ps5brsolidelectrolyteinfluenceofmisorientationandaniondisorderonliionmobility |