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Resolving complex intralayer transition motifs in high-Ni-content layered cathode materials for lithium-ion batteries



High-Ni-content layered materials are promising cathodes for next-generation lithium-ion batteries. However, investigating the atomic configurations of the delithiation-induced complex phase boundaries and their transitions remains challenging. Here, by using deep-learning-aided super-resolution electron microscopy, we resolve the intralayer transition motifs at complex phase boundaries in high-Ni cathodes. We reveal that an O3 → O1 transformation driven by delithiation leads to the formation of two types of O1–O3 interface, the continuous- and abrupt-transition interfaces. The interfacial misfit is accommodated by a continuous shear-transition zone and an abrupt structural unit, respectively. Atomic-scale simulations show that uneven in-plane Li+ distribution contributes to the formation of both types of interface, and the abrupt transition is energetically more favourable in a delithiated state where O1 is dominant, or when there is an uneven in-plane Li+ distribution in a delithiated O3 lattice. Moreover, a twin-like motif that introduces structural units analogous to the abrupt-type O1–O3 interface is also uncovered. The structural transition motifs resolved in this study provide further understanding of shear-induced phase transformations and phase boundaries in high-Ni layered cathodes.

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Fig. 1: Formation of random O1 domains in delithiated O3 matrix.
Fig. 2: Atomic configurations of two types of O1–O3 interface.
Fig. 3: O1–O3 interface energy as a function of the transition zone length.
Fig. 4: Formation of twin-like structure and its interfacial structures.

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Data availability

The data that support the findings of this study are available from the corresponding author on reasonable request.

Code availability

The code used to perform super-resolution processing can be accessed at


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This work is supported by the Materials Science and Engineering Divisions, Office of Basic Energy Sciences of the US Department of Energy, under award no. DE-SC0021204. R.Z.’s work done for this study was funded by H.L.X.’s startup funding. This research used resources of the Center for Functional Nanomaterials, which is a US DOE Office of Science Facility, and the Scientific Data and Computing Center, a component of the Computational Science Initiative, at Brookhaven National Laboratory under contract no. DE-SC0012704. We acknowledge the use of facilities and instrumentation at the University of California, Irvine Materials Research Institute, which is supported in part by the National Science Foundation through the University of California, Irvine Materials Research Science and Engineering Center (no. DMR-2011967). We would like to acknowledge the generous support from Professor Tim Rupert. We thank Y. Cheng and J. Cheng for illuminating discussions.

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Authors and Affiliations



H.L.X. directed the project. C.W. and H.L.X. conceived the idea. C.W. performed the transmission electron microscopy experiments and data analysis. X.W. performed the DFT simulations and data interpretation. R.Z. performed the materials synthesis and electrochemical tests. C.W. performed the four-dimensional STEM strain mapping and data analysis. C.W. and T.L. performed the scanning nanodiffraction experiments for orientation mapping. K.K. prepared the focused ion beam transmission electron microscopy samples. C.W., X.W. and H.L.X. wrote the paper with help from all authors.

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Correspondence to Huolin L. Xin.

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Wang, C., Wang, X., Zhang, R. et al. Resolving complex intralayer transition motifs in high-Ni-content layered cathode materials for lithium-ion batteries. Nat. Mater. 22, 235–241 (2023).

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