Mesoscale Effects of Composition and Calendering in Lithium-Ion Battery Composite Electrodes

Trembacki, Bradley L.; Noble, David R.; Ferraro, Mark E.; Roberts, Scott A.

doi:10.1115/1.4045973

Title: Mesoscale Effects of Composition and Calendering in Lithium-Ion Battery Composite Electrodes

Journal Article · Tue Mar 10 00:00:00 EDT 2020 · Journal of Electrochemical Energy Conversion and Storage

DOI:https://doi.org/10.1115/1.4045973· OSTI ID:1605730

Trembacki, Bradley L. ^[1]; Noble, David R. ^[1]; Ferraro, Mark E. ^[1]; Roberts, Scott A. ^[1]

Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Macrohomogeneous battery models are widely used to predict battery performance, necessarily relying on effective electrode properties, such as specific surface area, tortuosity, and electrical conductivity. While these properties are typically estimated using ideal effective medium theories, in practice they exhibit highly non-ideal behaviors arising from their complex mesostructures. In this paper, we computationally reconstruct electrodes from X-ray computed tomography of 16 nickel–manganese–cobalt-oxide electrodes, manufactured using various material recipes and calendering pressures. Due to imaging limitations, a synthetic conductive binder domain (CBD) consisting of binder and conductive carbon is added to the reconstructions using a binder bridge algorithm. Reconstructed particle surface areas are significantly smaller than standard approximations predicted, as the majority of the particle surface area is covered by CBD, affecting electrochemical reaction availability. Finite element effective property simulations are performed on 320 large electrode subdomains to analyze trends and heterogeneity across the electrodes. Significant anisotropy of up to 27% in tortuosity and 47% in effective conductivity is observed. Electrical conductivity increases up to 7.5× with particle lithiation. We compare the results to traditional Bruggeman approximations and offer improved alternatives for use in cell-scale modeling, with Bruggeman exponents ranging from 1.62 to 1.72 rather than the theoretical value of 1.5. We also conclude that the CBD phase alone, rather than the entire solid phase, should be used to estimate effective electronic conductivity. This study provides insight into mesoscale transport phenomena and results in improved effective property approximations founded on realistic, image-based morphologies.

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Research Organization:: Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Sustainable Transportation Office. Vehicle Technologies Office

Grant/Contract Number:: AC04-94AL85000

OSTI ID:: 1605730

Report Number(s):: SAND-2020-2279J; 684142

Journal Information:: Journal of Electrochemical Energy Conversion and Storage, Vol. 17, Issue 4; ISSN 2381-6872

Publisher:: ASMECopyright Statement

Country of Publication:: United States

Language:: English

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