Phase evolution for conversion reaction electrodes in lithium-ion batteries

Feng Lin (), Dennis Nordlund, Tsu-Chien Weng, Ye Zhu, Chunmei Ban, Ryan M. Richards and Huolin L. Xin ()
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Feng Lin: 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
Ye Zhu: Monash Centre for Electron Microscopy, Monash University
Chunmei Ban: Chemical and Materials Science Center, National Renewable Energy Laboratory
Ryan M. Richards: Materials Science Program, Colorado School of Mines
Huolin L. Xin: Center for Functional Nanomaterials, Brookhaven National Laboratory

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

Abstract: Abstract The performance of battery materials is largely governed by structural and chemical evolutions during electrochemical reactions. Therefore, resolving spatially dependent reaction pathways could enlighten mechanistic understanding, and enable rational design for rechargeable battery materials. Here, we present a phase evolution panorama via spectroscopic and three-dimensional imaging at multiple states of charge for an anode material (that is, nickel oxide nanosheets) in lithium-ion batteries. We reconstruct the three-dimensional lithiation/delithiation fronts and find that, in a fully electrolyte immersion environment, phase conversion can nucleate from spatially distant locations on the same slab of material. In addition, the architecture of a lithiated nickel oxide is a bent porous metallic framework. Furthermore, anode–electrolyte interphase is found to be dynamically evolving upon charging and discharging. The present study has implications for resolving the inhomogeneity of the general electrochemically driven phase transition (for example, intercalation reactions) and for the origin of inhomogeneous charge distribution in large-format battery electrodes.

Date: 2014
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DOI: 10.1038/ncomms4358

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