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Coupling structural evolution and oxygen-redox electrochemistry in layered transition metal oxides
Donggun Eum1,2, Byunghoon Kim1,2, Jun-Hyuk Song1
1Department of Materials Science and Engineering, Research Institute of Advanced Materials (RIAM), Seoul National University, Seoul, Republic of Korea.
Nature Materials
|March 18, 2022
Summary
Lattice oxygen redox in transition metal oxides (TMOs) offers battery potential but faces degradation. This study reveals how cation migration mechanisms influence oxygen redox reversibility and structural stability in layered TMOs.
Area of Science:
- Materials Science
- Electrochemistry
- Battery Technology
Background:
- Lattice oxygen redox in transition metal oxides (TMOs) presents a promising avenue for enhanced electrochemical properties in rechargeable batteries.
- However, practical application is hindered by unfavorable structural transformations and electrochemical degradation associated with this reaction.
Purpose of the Study:
- To investigate the intricate relationship between local structural changes and oxygen electrochemistry in layered TMOs during battery operation.
- To elucidate the role of cation migration mechanisms in governing oxygen redox activity and reversibility.
Main Methods:
- In-situ/operando characterization techniques to monitor local structural evolution during electrochemical cycling.
- Electrochemical performance testing of layered TMOs under various conditions.
- Computational modeling to understand cation migration pathways and their impact on oxygen interactions.
Main Results:
- Distinct evolution patterns of oxygen-redox activity and reversibility were observed, directly linked to different cation-migration mechanisms during de/intercalation.
- Initial oxygen oxidation stabilization via π interactions, prevalent without cation migration, transitions to σ interactions, leading to O-O dimer formation and structural destabilization.
- Cation migration pathways in layered TMOs critically control the kinetics of π to σ interaction conversion.
Conclusions:
- A deeper understanding of the correlation between local structural dynamics and the reversibility of oxygen electrochemistry has been achieved.
- The findings provide crucial insights for designing and developing advanced layered electrode materials that leverage oxygen redox for improved battery performance.
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