Metal segregation in hierarchically structured cathode materials for high-energy lithium batteries

Feng Lin, Dennis Nordlund, Yuyi Li, Matthew K. Quan, Lei Cheng, Tsu-Chien Weng, Yijin Liu (), Huolin L. Xin () and Marca M. Doeff ()
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Feng Lin: Lawrence Berkeley National Laboratory
Dennis Nordlund: Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory
Yuyi Li: Lawrence Berkeley National Laboratory
Matthew K. Quan: Lawrence Berkeley National Laboratory
Lei Cheng: Lawrence Berkeley National Laboratory
Tsu-Chien Weng: Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory
Yijin Liu: Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory
Huolin L. Xin: Center for Functional Nanomaterials, Brookhaven National Laboratory
Marca M. Doeff: Lawrence Berkeley National Laboratory

Nature Energy, 2016, vol. 1, issue 1, 1-8

Abstract: Abstract In technologically important LiNi1−x−yMnxCoyO2 cathode materials, surface reconstruction from a layered to a rock-salt structure is commonly observed under a variety of operating conditions, particularly in Ni-rich compositions. This phenomenon contributes to poor high-voltage cycling performance, impeding attempts to improve the energy density by widening the potential window at which these electrodes operate. Here, using advanced nano-tomography and transmission electron microscopy techniques, we show that hierarchically structured LiNi0.4Mn0.4Co0.2O2 spherical particles, made by a simple spray pyrolysis method, exhibit local elemental segregation such that surfaces are Ni-poor and Mn-rich. The tailored surfaces result in superior resistance to surface reconstruction compared with those of conventional LiNi0.4Mn0.4Co0.2O2, as shown by soft X-ray absorption spectroscopy experiments. The improved high-voltage cycling behaviour exhibited by cells containing these cathodes demonstrates the importance of controlling LiNi1−x−yMnxCoyO2 surface chemistry for successful development of high-energy lithium ion batteries.

Date: 2016
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DOI: 10.1038/nenergy.2015.4

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