Ultra-Thick Cathodes for High-Energy Lithium-Ion Batteries Based on Aluminium Foams—Microstructural Evolution during Densification and Its Impact on the Electrochemical Properties

Abstract

Using three-dimensional (3D) metal foams as current collectors is considered to be a promising approach to improve the areal specific capacity and meet the demand for increased energy density of lithium-ion batteries. Electrodes with an open-porous metal foam as current collector exhibit a 3D connected electronic network within the active mass, shortening the electron transport pathways and lowering the electrodes’ intrinsic electronic resistance. In this study, NMC622 cathodes using an aluminium foam as current collector with a measured areal capacity of up to 7.6 mAh cm−2 were investigated. To this end, the infiltrated foams were densified to various thicknesses between 200 µm and 400 µm corresponding to an electrode porosity between 65% and 30%. The microstructural analysis reveals (i) the elimination of shrinking cavities and a decrease in the porosity of the infiltrated active mass, (ii) an improved contact of active mass to the current collector structure and (iii) a pronounced clogging of the surface pores. The electrochemical properties such as capacity and rate capability are correlated to the electrode’s microstructure, demonstrating that densification is necessary to improve active material utilization and volumetric capacity. However, strong densification impairs the rate capability caused by increased pore resistance and hindered electrolyte accessibility.