Native lattice strain induced structural earthquake in sodium layered oxide cathodes

Gui-Liang Xu (), Xiang Liu, Xinwei Zhou, Chen Zhao, Inhui Hwang, Amine Daali, Zhenzhen Yang, Yang Ren, Cheng-Jun Sun, Zonghai Chen, Yuzi Liu () and Khalil Amine ()
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Gui-Liang Xu: Argonne National Laboratory
Xiang Liu: Argonne National Laboratory
Xinwei Zhou: Argonne National Laboratory
Chen Zhao: Argonne National Laboratory
Inhui Hwang: Argonne National Laboratory
Amine Daali: Argonne National Laboratory
Zhenzhen Yang: Argonne National Laboratory
Yang Ren: Argonne National Laboratory
Cheng-Jun Sun: Argonne National Laboratory
Zonghai Chen: Argonne National Laboratory
Yuzi Liu: Argonne National Laboratory
Khalil Amine: Argonne National Laboratory

Nature Communications, 2022, vol. 13, issue 1, 1-12

Abstract: Abstract High-voltage operation is essential for the energy and power densities of battery cathode materials, but its stabilization remains a universal challenge. To date, the degradation origin has been mostly attributed to cycling-initiated structural deformation while the effect of native crystallographic defects induced during the sophisticated synthesis process has been significantly overlooked. Here, using in situ synchrotron X-ray probes and advanced transmission electron microscopy to probe the solid-state synthesis and charge/discharge process of sodium layered oxide cathodes, we reveal that quenching-induced native lattice strain plays an overwhelming role in the catastrophic capacity degradation of sodium layered cathodes, which runs counter to conventional perception—phase transition and cathode interfacial reactions. We observe that the spontaneous relaxation of native lattice strain is responsible for the structural earthquake (e.g., dislocation, stacking faults and fragmentation) of sodium layered cathodes during cycling, which is unexpectedly not regulated by the voltage window but is strongly coupled with charge/discharge temperature and rate. Our findings resolve the controversial understanding on the degradation origin of cathode materials and highlight the importance of eliminating intrinsic crystallographic defects to guarantee superior cycling stability at high voltages.

Date: 2022
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DOI: 10.1038/s41467-022-28052-x

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