Grain boundaries control lithiation of solid solution substrates in lithium metal batteries

Fuente: arXiv
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Autori principali: Aota, Leonardo Shoji, Jung, Chanwon, Zhang, Siyuan, Büyükuslu, Ömer K., Yadav, Poonam, Singh, Mahander Pratap, Chen, Xinren, Woods, Eric, Scheu, Christina, Kim, Se-Ho, Raabe, Dierk, Gault, Baptiste
Natura: Preprint
Pubblicazione: 2024
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author Aota, Leonardo Shoji
Jung, Chanwon
Zhang, Siyuan
Büyükuslu, Ömer K.
Yadav, Poonam
Singh, Mahander Pratap
Chen, Xinren
Woods, Eric
Scheu, Christina
Kim, Se-Ho
Raabe, Dierk
Gault, Baptiste
author_facet Aota, Leonardo Shoji
Jung, Chanwon
Zhang, Siyuan
Büyükuslu, Ömer K.
Yadav, Poonam
Singh, Mahander Pratap
Chen, Xinren
Woods, Eric
Scheu, Christina
Kim, Se-Ho
Raabe, Dierk
Gault, Baptiste
contents 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, we deploy a correlative, near-atomic scale probing approach through combined ion- and electron-microscopy to examine the distribution of Li in Li-Ag diffusion couples as model system. We reveal that Li regions with over 93.8% at.% nucleate within Ag at random high angle grain boundaries, whereas grain interiors are not lithiated. We evidence the role of kinetics and mechanical constraint from the microstructure over equilibrium thermodynamics in dictating the lithiation process. 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 Preprint
id arxiv_https___arxiv_org_abs_2407_09374
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Grain boundaries control lithiation of solid solution substrates in lithium metal batteries
Aota, Leonardo Shoji
Jung, Chanwon
Zhang, Siyuan
Büyükuslu, Ömer K.
Yadav, Poonam
Singh, Mahander Pratap
Chen, Xinren
Woods, Eric
Scheu, Christina
Kim, Se-Ho
Raabe, Dierk
Gault, Baptiste
Materials Science
Chemical Physics
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, we deploy a correlative, near-atomic scale probing approach through combined ion- and electron-microscopy to examine the distribution of Li in Li-Ag diffusion couples as model system. We reveal that Li regions with over 93.8% at.% nucleate within Ag at random high angle grain boundaries, whereas grain interiors are not lithiated. We evidence the role of kinetics and mechanical constraint from the microstructure over equilibrium thermodynamics in dictating the lithiation process. 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.
title Grain boundaries control lithiation of solid solution substrates in lithium metal batteries
topic Materials Science
Chemical Physics
url https://arxiv.org/abs/2407.09374