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Research Papers

Phase Field Modeling of Coupled Phase Separation and Diffusion-Induced Stress in Lithium Iron Phosphate Particles Reconstructed From Synchrotron Nano X-ray Tomography

[+] Author and Article Information
Linmin Wu

Department of Mechanical and Energy Engineering,
Indiana University-Purdue University Indianapolis,
Indianapolis, IN 46202
e-mail: lw54@umail.iu.edu

Vincent De Andrade

Advanced Photon Source,
Argonne National Laboratory,
9700 Cass Avenue,
Lemont, IL 60439
e-mail: vdeandrade@anl.gov

Xianghui Xiao

Advanced Photon Source,
Argonne National Laboratory,
9700 Cass Avenue,
Lemont, IL 60439;
National Synchrotron Light Source II (NSLS-II),
Brookhaven National Laboratory,
98 Rochester Street,
Upton, NY 11973
e-mail: xiao@bnl.gov

Jing Zhang

Department of Mechanical and Energy Engineering,
Indiana University-Purdue University Indianapolis,
Indianapolis, IN 46202
e-mail: jz29@iupui.edu

1Corresponding author.

Manuscript received December 22, 2018; final manuscript received February 25, 2019; published online April 12, 2019. Assoc. Editor: Partha P. Mukherjee. The United States Government retains, and by accepting the article for publication, the publisher acknowledges that the United States Government retains, a non-exclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this work, or allow others to do so, for United States Government purposes.

J. Electrochem. En. Conv. Stor. 16(4), 041006 (Apr 12, 2019) (7 pages) Paper No: JEECS-18-1132; doi: 10.1115/1.4043155 History: Received December 22, 2018; Accepted February 26, 2019

In this study, the phase separation phenomenon and diffusion-induced stresses in lithium iron phosphate (LiFePO4) particles under a potentiostatic discharging process have been simulated using the phase field method. The realistic particles reconstructed from synchrotron nano X-ray tomography along with idealized spherical and ellipsoid shaped particles were studied. The results show that stress and diffusion process in particles are strongly influenced by particle shapes, especially at the initial lithiation stage. Stresses in the realistic particles are higher than that in the idealized spherical ones by at least 30%. The diffusion-induced hydrostatic stress has a strong relationship with lithium ion concentration. The hydrostatic stresses and first principal stresses tend to shift from lower values to higher values as the particle takes in more lithium ions. Additionally, the diffusion-induced stresses are related to the maximum concentration difference in the particle. High concentration difference will cause high stresses. In ellipsoid particles, the stress levels increase with the aspect ratios. The model provides a design tool to optimize the performance of cathode materials with phase separation phenomena.

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Figures

Grahic Jump Location
Fig. 1

LiFePO4 particles reconstructed from nano X-ray tomography: (a) 0.402 µm equivalent radius and (b) 0.548 µm equivalent radius

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Fig. 2

Lithium ion concentration and hydrostatic stresses for different SOC: (a) and (d) are concentration distribution and hydrostatic stresses for the spherical particle with 1 µm radius, (b) and (e) are those for the ellipsoid particle with 1 µm equivalent radius and 1.414 aspect ratio, (c) and (f) are those for the realistic particle with 0.548 µm equivalent radius

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Fig. 3

Concentration and stresses along the radial axis for the spherical LiFePO4 particle with 1 µm radius: (a) concentration distributions, (b) hydrostatic stresses, and (c) first principal stresses

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Fig. 4

(a) Maximum concentration difference and (b) maximum first principal stress for ellipsoid particles with different aspect ratios during the discharging process. The equavalent radius of all three cases is 1 µm.

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Fig. 5

Maximum first principal stress in ellipsoid particles with different aspect ratios

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Fig. 6

Maximum concentration difference and first principal stress for spherical and realistic particles during the discharging process. The equivalent radius for both cases are 0.402 µm: (a) maximum concentration difference and (b) maximum first principal stress.

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Fig. 7

Lithium ion concentration and hydrostatic stresses for different SOC for the realistic LiFePO4 particle with 0.402 µm equivalent radius: (a) concentration distributions and (b) first principal stresses

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Fig. 8

Maximum first principal stresses of spherical and realistic particles

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