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Probing transport limitations in thick sintered battery electrodes with neutron imaging

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Abstract

Lithium-ion batteries have received significant research interest due to their advantages in energy and power density, which are important to enabling many devices. One route to further increase energy density is to fabricate thicker electrodes in the battery cell; however, careful consideration must be taken when designing electrodes as to how increasing the thickness impacts the multiscale and multiphase molecular transport processes, which can limit the overall battery operating power. Design of these electrodes necessitates probing the molecular processes when the battery cell undergoes electrochemical charge/discharge. One tool for in situ insights into the cell is neutron imaging, because neutron imaging can provide information of where electrochemical processes occur within the electrodes. In this manuscript, neutron imaging is applied to track the lithiation/delithiation processes within electrodes at different current densities for a full cell with a thick sintered Li4Ti5O12 anode and LiCoO2 cathode. The neutron imaging reveals that the molecular distribution of Li+ during discharge within the electrode is sensitive to the current density, or equivalently discharge rate. An electrochemical model provides additional insights into the limiting processes occurring within the electrodes. In particular, the impact of tortuosity and molecular transport in the liquid phase within the interstitial regions in the electrodes are considered, and the influence of tortuosity was shown to be highly sensitive to the current density. Qualitatively, the experimental results suggest that the electrodes behave consistent with the packed hard sphere approximation of Bruggeman tortuosity scaling, which indicates that the electrodes are largely mechanically intact but also that a design that incorporates tunable tortuosity could improve the performance of these types of electrodes.

Graphical abstract: Probing transport limitations in thick sintered battery electrodes with neutron imaging

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Publication details

The article was received on 23 Jul 2019, accepted on 03 Oct 2019 and first published on 16 Oct 2019


Article type: Paper
DOI: 10.1039/C9ME00084D
Mol. Syst. Des. Eng., 2020, Advance Article

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    Probing transport limitations in thick sintered battery electrodes with neutron imaging

    Z. Nie, S. Ong, D. S. Hussey, J. M. LaManna, D. L. Jacobson and G. M. Koenig, Mol. Syst. Des. Eng., 2020, Advance Article , DOI: 10.1039/C9ME00084D

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