Surface reconstruction and chemical evolution of stoichiometric layered cathode materials for lithium-ion batteries

Feng Lin (), Isaac M. Markus, Dennis Nordlund, Tsu-Chien Weng, Mark D. Asta, Huolin L. Xin () and Marca M. Doeff
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Feng Lin: Lawrence Berkeley National Laboratory
Isaac M. Markus: Lawrence Berkeley National Laboratory
Dennis Nordlund: Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory
Tsu-Chien Weng: Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory
Mark D. Asta: University of California
Huolin L. Xin: Center for Functional Nanomaterials, Brookhaven National Laboratory
Marca M. Doeff: Lawrence Berkeley National Laboratory

Nature Communications, 2014, vol. 5, issue 1, 1-9

Abstract: Abstract The present study sheds light on the long-standing challenges associated with high-voltage operation of LiNixMnxCo1−2xO2 cathode materials for lithium-ion batteries. Using correlated ensemble-averaged high-throughput X-ray absorption spectroscopy and spatially resolved electron microscopy and spectroscopy, here we report structural reconstruction (formation of a surface reduced layer, to transition) and chemical evolution (formation of a surface reaction layer) at the surface of LiNixMnxCo1−2xO2 particles. These are primarily responsible for the prevailing capacity fading and impedance buildup under high-voltage cycling conditions, as well as the first-cycle coulombic inefficiency. It was found that the surface reconstruction exhibits a strong anisotropic characteristic, which predominantly occurs along lithium diffusion channels. Furthermore, the surface reaction layer is composed of lithium fluoride embedded in a complex organic matrix. This work sets a refined example for the study of surface reconstruction and chemical evolution in battery materials using combined diagnostic tools at complementary length scales.

Date: 2014
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DOI: 10.1038/ncomms4529

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