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Understanding the Performance Gap between Polycrystalline and Single-Crystal Nickel-Rich Layered Oxide Cathodes.

Jing Wang^1,2, Jinghao Huang³, Weiyuan Huang²

¹Pritzker School of Molecular Engineering, University of Chicago, Chicago, Illinois 60637, United States.

Journal of the American Chemical Society

|February 27, 2026

Summary

Single-crystal (SC) cathodes show better energy density but degrade faster than polycrystalline (PC) ones. Heterogeneous nickel redox in SC cathodes causes irreversible oxygen activity and bulk degradation, leading to capacity decay.

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Area of Science:

Materials Science
Electrochemistry
Battery Technology

Background:

Single-crystal (SC) nickel-rich layered oxide cathodes offer superior volumetric energy density and mechanical strength.
SC cathodes with high nickel content (≥80%) exhibit faster performance degradation than polycrystalline (PC) counterparts.
The reasons for this performance gap between SC and PC Ni-rich cathodes are not well understood.

Purpose of the Study:

To investigate the distinct Ni redox behaviors in SC and PC Ni-rich cathodes.
To elucidate the underlying causes of performance degradation in SC Ni-rich cathodes.
To provide insights for designing improved Ni-rich cathode architectures.

Main Methods:

Multiscale characterization techniques.
Operando characterization methods.
Electrochemical performance analysis.

Main Results:

Heterogeneous Ni oxidation in SC cathodes leads to irreversible oxygen redox activity.
Irreversible oxygen activity deteriorates the mechanical and chemical structures of SC cathodes.
PC cathodes exhibit greater chemomechanical stability due to homogeneous redox reactions, despite surface reconstruction.
Bulk degradation, not surface reactions, is the primary cause of capacity decay in SC cathodes.

Conclusions:

Distinct Ni redox behaviors significantly impact the electrochemical performance and stability of SC and PC Ni-rich cathodes.
Heterogeneous Ni redox in SC cathodes drives bulk degradation and capacity fade.
Understanding Ni redox evolution is crucial for enhancing the chemomechanical stability and cycle life of Ni-rich layered oxide cathodes.