Grain Boundaries Control Lithiation of Solid Solution Substrates in Lithium Metal Batteries
Abstract The development of sustainable transportation and communication systems requires an increase in both energy density and capacity retention of Li‐batteries. Using substrates forming a solid solution with body‐centered cubic Li enhances the cycle stability of anode‐less batteries. However, it...
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| Format: | Article |
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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.202409275 |
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| author | Leonardo Shoji Aota Chanwon Jung Siyuan Zhang Ömer K. Büyükuslu Aparna Saksena Ezgi Hatipoglu Poonam Yadav Mahander Pratap Singh Xinren Chen Eric Woods Christina Scheu Se‐Ho Kim Dierk Raabe Baptiste Gault |
| author_facet | Leonardo Shoji Aota Chanwon Jung Siyuan Zhang Ömer K. Büyükuslu Aparna Saksena Ezgi Hatipoglu Poonam Yadav Mahander Pratap Singh Xinren Chen Eric Woods Christina Scheu Se‐Ho Kim Dierk Raabe Baptiste Gault |
| author_sort | Leonardo Shoji Aota |
| collection | DOAJ |
| description | Abstract The development of sustainable transportation and communication systems requires an increase in both energy density and capacity retention of Li‐batteries. Using substrates forming a solid solution with body‐centered cubic Li enhances the cycle stability of anode‐less batteries. However, it remains unclear how the substrate microstructure affects the lithiation behavior. Here, a correlative, near‐atomic scale probing approach is deployed through combined ion‐ and electron‐microscopy to examine the distribution of Li in Li‐Ag diffusion couples as model system mimicking high current densities. It is revealed that Li regions with over 93.8% at.% nucleate within Ag at random high‐angle grain boundaries, whereas grain interiors are not lithiated. The role of kinetics and mechanical constraint from the microstructure over equilibrium thermodynamics in dictating the lithiation process is evidenced. The findings suggest that grain size and grain boundary character are critical to enhance the electrochemical performance of interlayers/electrodes, particularly for improving lithiation kinetics and hence reducing dendrite formation. |
| format | Article |
| id | doaj-art-452976792f5741c98a4dba883a52ee7a |
| institution | Kabale University |
| issn | 2198-3844 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Wiley |
| record_format | Article |
| series | Advanced Science |
| spelling | doaj-art-452976792f5741c98a4dba883a52ee7a2025-01-29T09:50:19ZengWileyAdvanced Science2198-38442025-01-01124n/an/a10.1002/advs.202409275Grain Boundaries Control Lithiation of Solid Solution Substrates in Lithium Metal BatteriesLeonardo Shoji Aota0Chanwon Jung1Siyuan Zhang2Ömer K. Büyükuslu3Aparna Saksena4Ezgi Hatipoglu5Poonam Yadav6Mahander Pratap Singh7Xinren Chen8Eric Woods9Christina Scheu10Se‐Ho Kim11Dierk Raabe12Baptiste Gault13Max Planck Institute for Sustainable Materials 40237 Düsseldorf GermanyMax Planck Institute for Sustainable Materials 40237 Düsseldorf GermanyMax Planck Institute for Sustainable Materials 40237 Düsseldorf GermanyGTT‐Technologies 52134 Herzogenrath GermanyMax Planck Institute for Sustainable Materials 40237 Düsseldorf GermanyMax Planck Institute for Sustainable Materials 40237 Düsseldorf GermanyMax Planck Institute for Sustainable Materials 40237 Düsseldorf GermanyMax Planck Institute for Sustainable Materials 40237 Düsseldorf GermanyMax Planck Institute for Sustainable Materials 40237 Düsseldorf GermanyMax Planck Institute for Sustainable Materials 40237 Düsseldorf GermanyMax Planck Institute for Sustainable Materials 40237 Düsseldorf GermanyMax Planck Institute for Sustainable Materials 40237 Düsseldorf GermanyMax Planck Institute for Sustainable Materials 40237 Düsseldorf GermanyMax Planck Institute for Sustainable Materials 40237 Düsseldorf GermanyAbstract The development of sustainable transportation and communication systems requires an increase in both energy density and capacity retention of Li‐batteries. Using substrates forming a solid solution with body‐centered cubic Li enhances the cycle stability of anode‐less batteries. However, it remains unclear how the substrate microstructure affects the lithiation behavior. Here, a correlative, near‐atomic scale probing approach is deployed through combined ion‐ and electron‐microscopy to examine the distribution of Li in Li‐Ag diffusion couples as model system mimicking high current densities. It is revealed that Li regions with over 93.8% at.% nucleate within Ag at random high‐angle grain boundaries, whereas grain interiors are not lithiated. The role of kinetics and mechanical constraint from the microstructure over equilibrium thermodynamics in dictating the lithiation process is evidenced. The findings suggest that grain size and grain boundary character are critical to enhance the electrochemical performance of interlayers/electrodes, particularly for improving lithiation kinetics and hence reducing dendrite formation.https://doi.org/10.1002/advs.202409275atom probe tomographychemomechanicalgrain boundarylithiationsolid solution |
| spellingShingle | Leonardo Shoji Aota Chanwon Jung Siyuan Zhang Ömer K. Büyükuslu Aparna Saksena Ezgi Hatipoglu Poonam Yadav Mahander Pratap Singh Xinren Chen Eric Woods Christina Scheu Se‐Ho Kim Dierk Raabe Baptiste Gault Grain Boundaries Control Lithiation of Solid Solution Substrates in Lithium Metal Batteries Advanced Science atom probe tomography chemomechanical grain boundary lithiation solid solution |
| title | Grain Boundaries Control Lithiation of Solid Solution Substrates in Lithium Metal Batteries |
| title_full | Grain Boundaries Control Lithiation of Solid Solution Substrates in Lithium Metal Batteries |
| title_fullStr | Grain Boundaries Control Lithiation of Solid Solution Substrates in Lithium Metal Batteries |
| title_full_unstemmed | Grain Boundaries Control Lithiation of Solid Solution Substrates in Lithium Metal Batteries |
| title_short | Grain Boundaries Control Lithiation of Solid Solution Substrates in Lithium Metal Batteries |
| title_sort | grain boundaries control lithiation of solid solution substrates in lithium metal batteries |
| topic | atom probe tomography chemomechanical grain boundary lithiation solid solution |
| url | https://doi.org/10.1002/advs.202409275 |
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