Fabrication and Characterization of Lithium-ion Battery Electrode Filaments Used for Fused Deposition Modeling 3D Printing

Abstract

Lithium-Ion Batteries (Li-ion batteries or LIBs) have been extensively used in a wide variety of industrial applications and consumer electronics. Additive Manufacturing (AM) or 3D printing (3DP) techniques have evolved to allow the fabrication of complex structures of various compositions in a wide range of applications. The objective of the thesis is to investigate the application of 3DP to fabricate a LIB, using a modified process from the literature [1]. The ultimate goal is to improve the electrochemical performances of LIBs while maintaining design flexibility with a 3D printed 3D architecture. In this research, both the cathode and anode in the form of specifically formulated slurry were extruded into filaments using a high-temperature pellet-based extruder. Specifically, filament composites made of graphite and Polylactic Acid (PLA) were fabricated and tested to produce anodes. Investigations on two other types of PLA-based filament composites respectively made of Lithium Manganese Oxide (LMO) and Lithium Nickel Manganese Cobalt Oxide (NMC) were also conducted to produce cathodes. Several filaments with various materials ratios were formulated in order to optimize printability and battery capacities. Finally, flat battery electrode disks similar to conventional electrodes were fabricated using the fused deposition modeling (FDM) process and assembled in half-cells and full cells. Finally, the electrochemical properties of half cells and full cells were characterized. Additionally, in parallel to the experiment, a 1-D finite element (FE) model was developed to understand the electrochemical performance of the anode half-cells made of graphite. Moreover, a simplified machine learning (ML) model through the Gaussian Process Regression was used to predict the voltage of a certain half-cell based on input parameters such as charge and discharge capacity. The results of this research showed that 3D printing technology is capable to fabricate LIBs. For the 3D printed LIB, cells have improved electrochemical properties by increasing the material content of active materials (i.e., graphite, LMO, and NMC) within the PLA matrix, along with incorporating a plasticizer material. The FE model of graphite anode showed a similar trend of discharge curve as the experiment. Finally, the ML model demonstrated a reasonably good prediction of charge and discharge voltages.