Tracking inhomogeneity in high-capacity lithium iron phosphate batteries

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Energy-dispersive x-ray diffraction (EDXRD) is one of the few techniques that can internally probe a sealed battery under operating conditions. In this paper, we use EDXRD with ultrahigh energy synchrotron radiation to track inhomogeneity in a cycled high-capacity lithium iron phosphate cell under in-situ and operando conditions. A sequence of depth-profile x-ray diffraction spectra are collected with 40 μm resolution as the cell is discharged. Additionally, nine different locations of the cell are tracked independently throughout a second discharge process. In each case, a two-peak reference intensity ratio analysis (RIR) was used on the LiFePO4 311 and the FePO4 020 reflections to estimate the relative phase abundance of the lithiated and non-lithiated phases. The data provide a first-time look at the dynamics of electrochemical inhomogeneity in a real-world battery. We observe a strong correlation between inhomogeneity and overpotential in the galvanic response of the cell. Additionally, the data closely follow the behavior that is predicted by the resistive-reactant model originally proposed by Thomas-Alyea. Despite a non-linear response in the independently measured locations, the behavior of the ensemble is strikingly linear. This suggests that effects of inhomogeneity can be elusive and highlights the power of the EDXRD technique.




Paxton, W. A., Zhong, Z., & Tsakalakos, T. (2015). Tracking inhomogeneity in high-capacity lithium iron phosphate batteries. Journal of Power Sources, 275, 429–434.

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