Grain Boundaries Control Lithiation of Solid Solution Substrates in Lithium Metal Batteries
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.
Authors
- Aparna Saksena (ORCID: https://orcid.org/0000-0001-7697-3405)
- Mahander Pratap Singh (ORCID: https://orcid.org/0000-0003-1784-7219)
- Xinren Chen (ORCID: https://orcid.org/0000-0002-9799-4878)
- Dierk Raabe (ORCID: https://orcid.org/0000-0003-0194-6124)
- Chanwon Jung (ORCID: https://orcid.org/0000-0002-9782-0261)
- Ezgi Hatipoğlu
- Ömer K. Büyükuslu (ORCID: https://orcid.org/0000-0002-6807-0270)
- Eric Woods (ORCID: https://orcid.org/0000-0002-1169-893X)
- Baptiste Gault (ORCID: https://orcid.org/0000-0002-4934-0458)
- Christina Scheu (ORCID: https://orcid.org/0000-0001-7916-1533)
- Leonardo Shoji Aota (ORCID: https://orcid.org/0000-0002-1520-2073)
- Se‐Ho Kim (ORCID: https://orcid.org/0000-0003-1227-8897)
- Poonam Yadav
- Siyuan Zhang (ORCID: https://orcid.org/0009-0003-0847-7209)
Institutions
- Korea University (KR)
- Max-Planck-Institut für Nachhaltige Materialien (DE)
- GTT-Technologies (Germany) (DE)
- Imperial College London (GB)
- Pukyong National University (KR)
Publication Details
- Journal
- Advanced Science
- Published
- 2024-12-04
- DOI
- https://doi.org/10.1002/advs.202409275
- Citations
- 6
- Primary Topic
- Advancements in Battery Materials
- Type
- article
- Field-Weighted Citation Impact
- 1.25
Funders
- Alexander von Humboldt-Stiftung
- Pukyong National University
- Ministry of Trade, Industry and Energy
- Korea Institute for Advancement of Technology
- Max-Planck-Institut für Eisenforschung