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Elucidating Interfacial Stability between Lithium Metal Anode and Li Phosphorus Oxynitride via In Situ Electron
Zachary D Hood1, Xi Chen2, Robert L Sacci3
1School of Chemistry and Biochemistry, Georgia Institute of Technology Atlanta, Georgia 30332-0400, United States.
Nano Letters
|December 18, 2020
Summary
Lithium phosphorus oxynitride (LiPON) forms a stable interface layer with lithium metal, explaining its excellent performance in solid-state batteries. This passivation layer enables high Coulombic efficiency and extended cyclability for next-generation energy storage.
Area of Science:
- Materials Science
- Electrochemistry
- Battery Technology
Background:
- Lithium phosphorus oxynitride (LiPON) is a promising solid electrolyte for all-solid-state batteries (ASSBs).
- Theoretical studies suggest LiPON reacts with lithium metal, raising concerns about interface stability.
- Experimental evidence on the LiPON-Li interface stability remains debated.
Purpose of the Study:
- To investigate the dynamic interfacial evolution between LiPON and lithium metal.
- To understand the mechanisms behind LiPON's stability and cyclability in ASSBs.
- To reconcile conflicting theoretical and experimental findings regarding the LiPON-Li interface.
Main Methods:
- Utilized in situ electron microscopy to observe the LiPON-Li interface in real-time.
- Analyzed the composition and spatial distribution of the interface layer.
- Studied interfacial behavior under electrochemical biasing.
Main Results:
- A stable ~60 nm interface layer forms upon contact between LiPON and Li metal.
- This layer comprises conductive binary compounds with a unique spatial distribution.
- The interface layer acts as an effective passivation layer, ensuring electrochemical stability.
- Observed dynamic evolutions at the LiPON-Li interface under biasing.
Conclusions:
- The formed interface layer explains the excellent cyclability and Coulombic efficiency of LiPON in ASSBs.
- Glassy solid electrolytes like LiPON can achieve electrochemical stability with Li metal despite initial reactivity.
- Findings reconcile debates on LiPON-Li interface stability and highlight its potential for ASSB applications.

