| About this Abstract |
| Meeting |
2020 TMS Annual Meeting & Exhibition
|
| Symposium
|
Computational Thermodynamics and Kinetics
|
| Presentation Title |
Probing Solid-solid Interfacial Reactions in All-solid-state Batteries |
| Author(s) |
Hanmei Tang, Zhi Deng, Abhik Banerjee, Erik A. Wu, Han Nguyen, Zhuoying Zhu, Shirley Meng, Shyue Ping Ong |
| On-Site Speaker (Planned) |
Zhuoying Zhu |
| Abstract Scope |
We have developed a hierarchy of DFT-based approaches to understand and design electrode/buffer/SE interfaces in all-solid-state batteries. With relatively efficient thermodynamics approximations, we reveal that S-O exchange reactions between oxides and thiophosphates resulting in the formation of phosphates are responsible for large reaction driving force between common NaMO2 cathodes and Na3PS4 electrolyte. Such reactions, with their associated large volume changes, can be mitigated by careful selection of the cathode/SE combination, or by applying coatings.
We further demonstrate that explicit modelling of the electrode/SE interface via AIMD simulations yield different and more realistic predictions of interfacial reactions. For example, AIMD predicts that formation of SO42– and is kinetically favored over the formation of PO43– at the NaCoO2/Na3PS4 interface. These observations have been validated experimentally. We have also extended such studies to the LiNi0.85Co0.1Al0.05O2/Li6PS5Cl interface, with and without buffer layers, and the predicted interfacial reactions are in good agreement with experimental characterizations. |
| Proceedings Inclusion? |
Planned: Supplemental Proceedings volume |