Two-dimensional lithium diffusion behavior and probable hybrid phase transformation kinetics in olivine lithium iron phosphate

Liang Hong, Linsen Li (), Yuchen-Karen Chen-Wiegart, Jiajun Wang, Kai Xiang, Liyang Gan, Wenjie Li, Fei Meng, Fan Wang, Jun Wang, Yet-Ming Chiang, Song Jin () and Ming Tang ()
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Liang Hong: Rice University
Linsen Li: University of Wisconsin-Madison
Yuchen-Karen Chen-Wiegart: Brookhaven National Laboratory
Jiajun Wang: Brookhaven National Laboratory
Kai Xiang: Massachusetts Institute of Technology
Liyang Gan: University of Wisconsin-Madison
Wenjie Li: University of Wisconsin-Madison
Fei Meng: University of Wisconsin-Madison
Fan Wang: Rice University
Jun Wang: Brookhaven National Laboratory
Yet-Ming Chiang: Massachusetts Institute of Technology
Song Jin: University of Wisconsin-Madison
Ming Tang: Rice University

Nature Communications, 2017, vol. 8, issue 1, 1-13

Abstract: Abstract Olivine lithium iron phosphate is a technologically important electrode material for lithium-ion batteries and a model system for studying electrochemically driven phase transformations. Despite extensive studies, many aspects of the phase transformation and lithium transport in this material are still not well understood. Here we combine operando hard X-ray spectroscopic imaging and phase-field modeling to elucidate the delithiation dynamics of single-crystal lithium iron phosphate microrods with long-axis along the [010] direction. Lithium diffusivity is found to be two-dimensional in microsized particles containing ~3% lithium-iron anti-site defects. Our study provides direct evidence for the previously predicted surface reaction-limited phase-boundary migration mechanism and the potential operation of a hybrid mode of phase growth, in which phase-boundary movement is controlled by surface reaction or lithium diffusion in different crystallographic directions. These findings uncover the rich phase-transformation behaviors in lithium iron phosphate and intercalation compounds in general and can help guide the design of better electrodes.

Date: 2017
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DOI: 10.1038/s41467-017-01315-8

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