3D-printing of easily recyclable all-ceramic thick LiCoO2 electrodes with enhanced areal capacity for Li-ion batteries using a highly filled thermoplastic filament

J Colloid Interface Sci. 2023 Jul 15:642:351-363. doi: 10.1016/j.jcis.2023.03.117. Epub 2023 Mar 21.

Abstract

In this work, the production of thick ceramic LiCoO2 (LCO) electrodes using a conventional desktop 3D-printing was developed as an alternative to conventional electrode manufacturing for Li-ion batteries. Firstly, the filament formulation, based on LCO powders and a sacrificial polymers blend, is optimized to achieve suitable features (viscosity, flexibility and mechanical consistency) to be used in the 3-D printing. Printing parameters were optimized to produce defect-free bodies with coin geometry (12 mm diameter and 230-850 µm thickness). Thermal debinding and sintering were studied in order to obtain all ceramic LCO electrodes with adequate porosity. The additive-free sintered electrodes (850 µm thickness) have enhanced areal and volumetric capacities (up to 28 mA·h·cm-2 and 354 mA·h·cm-3) due to their extremely high mass loading (up to 285 mg·cm-2). Thus, the Li//LCO half-cell delivered an energy density of 1310 W·h·L-1. The ceramic nature of the electrode permits the use of a thin film of paint gold as current collector, reducing considerably the polarization of thick electrodes. Thus, the whole manufacturing process developed in this work is a complete solvent-free method to produce tuneable shape electrodes with enhanced energy density, opening the door for the manufacturing of high-density batteries with complex geometries and good recyclable.

Keywords: Additive manufacturing; Additive-free electrodes; Fused filament fabrication; Recyclable electrodes; Thick LiCoO(2) electrodes.