Investigating the Coating Effect on Charge Transfer Mechanisms in Composite Electrodes for Lithium-Ion Batteries.

The performance of lithium-ion batteries (LIBs) relies on the characteristics of the cathode material, including both intentionally applied coatings and naturally formed surface layers or binder adhesion. This study investigated the influence of the ion-permeable surface fraction, distribution, and characteristics of the coating on the performance of a lithium iron phosphate (LFP) electrode material. We developed an extended Newman-type half-cell model and examined the impact of coating parameters on the galvanostatic discharge curves of the LFP electrode material. The study found that the ion-permeable surface fraction has a significant influence on the diffusion and charge transfer characteristics of the electrode material. A decrease in the ion-permeable surface fraction leads to a decrease in the measured diffusion coefficients and to an increase in the overall coating resistance of the electrode material. Interestingly, the distribution of the ion-permeable surface also plays a role in the diffusion characteristics, with a coarsely dispersed coating resulting in lower diffusion coefficients. Additionally, the coating characteristics significantly affect the polarization and capacity of the electrode material at different C-rates. The model was used to approximate the experimental discharge curves of the LFP-based composite electrodes with two different compositions, and the simulated data showed satisfactory agreement with the experiment. Thus, we believe that the developed model and its further extension will be useful in numerical simulations that aim to facilitate the search for optimal compositions.