Probing the Structure-Performance Relationship of Lithium-Ion Battery Cathodes Using Pore-Networks Extracted from Three-Phase Tomograms Articles uri icon

authors

  • KHAN, ZOHAIB ATIQ
  • GARCIA SALABERRI, PABLO ANGEL
  • HEENAN, THOMAS M. M.
  • JERVIS, RHODRI
  • SHEARING, PAUL R.
  • BRETT, DAN
  • ELKAMEL, ALI
  • GOSTICK, JEFF T.

publication date

  • March 2020

start page

  • 1

end page

  • 13

issue

  • 4, 040528

volume

  • 167

International Standard Serial Number (ISSN)

  • 0013-4651

Electronic International Standard Serial Number (EISSN)

  • 1945-7111

abstract

  • Pore-scale simulations of Li-ion battery electrodes were conducted using both pore-network modeling and direct numerical simulation. Ternary tomographic images of NMC811 cathodes were obtained and used to create the pore-scale computational domains. A novel network extraction method was developed to manage the extraction of N-phase networks which was used to extract all three phases of NMC-811 electrode along with their interconnections Pore network results compared favorably with direct numerical simulations (DNS) in terms of effective transport properties of each phase but were obtained in significantly less time. Simulations were then conducted with combined diffusion-reaction to simulate the limiting current behavior. It was found that when considering only ion and electron transport, the electrode structure could support current densities about 300 times higher than experimentally observed values. Additional case studies were conducted to illustrate the necessity of ternary images which allow separate consideration of carbon binder domain and active material. The results showed a 24.4% decrease in current density when the carbon binder was treated as a separate phase compared to lumping the CBD and active material into a single phase. The impact of nanoporosity in the carbon binder phase was also explored and found to enhance the reaction rate by 16.8% compared to solid binder. In addition, the developed technique used 58 times larger domain volume than DNS which opens up the possibility of modelling much larger tomographic data sets, enabling representative areas of typically inhomogeneous battery electrodes to be modelled accurately, and proposes a solution to the conflicting needs of high-resolution imaging and large volumes for image-based modelling. For the first time, three-phase pore network modelling of battery electrodes has been demonstrated and evaluated, opening the path towards a new modelling framework for lithium ion batteries.

subjects

  • Chemistry
  • Industrial Engineering
  • Mechanical Engineering