Development of full ceramic electrodes for lithium-ion batteries via desktop-fused filament fabrication and further sintering

The fabrication of energy storage devices and their components via 3D printing involves unquestionable benefits in this field compared to traditional manufacturing processes such as doctor blading or die pressing, providing wide versatility for the development of electrodes with high surface area or the production of devices with geometries that fit specific product designs and maximize the amount of active material within the systems. Among these technologies, fused filament fabrication (FFF) represents a promising and low-cost method to fabricate lithium-ion batteries with tailored geometries. However, the high amount of polymer often included in the electrodes produced via FFF involves important capacity limitations for their use as functional electrodes. In this work, we report for the first time the fabrication of full ceramic LTO anode and LCO cathode electrodes via FFF 3D printing of composite filaments and further sintering, including a thorough study of the micro and macrostructure, phase stability, electrical conductivity, and electrochemical performance of the printed electrodes. With this strategy, 3D printed LTO and LCO electrodes were produced exhibiting similar electrical conductivity values to those of uniaxially pressed ceramic pellets and displayed 168 and 129 mAh g-1, i.e., 96% and 94% of their theoretical capacities, respectively (considering the conventional insertion/deinsertion of 3 Li+ for LTO and 0.5 Li+ for LCO).