Comparative study on the electrochemical performance of LiFePO4 cathodes fabricated by low temperature 3D printing, direct ink writing and conventional roller coating process

Abstract

Electrodes for lithium-ion batteries can be fabricated in many ways including conventional roller coating and 3D printing. Roller coating is a standardized process in current lithium-ion battery industry, while 3D printing has been used to fabricate three-dimensional (3D) unconventional electrodes with tailored geometries. Our previous study proposed a low temperature 3D printing process to fabricate highly-porous LiFePO4 (LFP) electrodes. However, there still lack a study on the comparison of electrochemical performance of LFP electrodes fabricated via the three different fabrication processes including low temperature direct writing-based 3D printing (LTDW), room temperature direct ink writing (DIW) and roller coating process. In this study, we fabricated LFP cathodes using these three fabrication processes from LFP inks with different solid contents. By varying the solid content, LFP electrodes with different geometries (including width and thickness), morphologies and porous microstructures were obtained via LTDW and DIW. Mercury porosimetry was performed to examine the differences of the three types of LFP electrodes in porous microstructures. Electrochemical performance including charge/discharge, rate performance, cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) of the three types of electrodes were measured and compared. Results showed that electrode fabrication processes have important effects on the electrochemical performance of LFP electrodes depending on the ink solid content. LTDW-fabricated electrodes had the best performance at high solid content (≥0.467 g/mL) and conventional roller coated electrodes performed better at low solid content (≤0.356 g/mL). Relationships between ink solid content, fabrication process, resulting porous microstructures and electrochemical performance were discussed. Finally, an optimal specific capacity of ∼82 mAh.g-1 @ 10C was achieved at a solid content of 0.467 g/mL by LTDW process.