Structure optimization of solvent-free Li4Ti5O12 electrodes by electrostatic spraying for lithium-ion capacitors

The manufacturing processes of electrodes have a prominent influence on the cost and performance of lithium-ion capacitors (LICs), which are limited by the conventional wet-coated method due to the usage of solvent. Herein, the solvent-free Li4Ti5O12 (LTO) electrodes are prepared with electrostatic spraying deposition using for LICs. Owing to the solvent being avoided during the manufacturing, the dry-sprayed electrode exhibits a higher porosity (∼40%) than that of the wet-coated electrode (∼30%), together with a larger electrochemically active surface area. The optimized microstructure improves electrolyte infiltration and offers effective Li-ion transport paths, which reduces the electrochemical polarization and boosts the specific capacity of the dry-sprayed electrode. When the current density increases from 0.5 C to 10 C, the reversible capacity retention of the dry-sprayed electrode is 74%, which is higher than that of the wet-coated electrode (56%). In addition, the powder resistivity of the dry-sprayed electrode decreases sharply by introducing two-dimension (2D) graphene nanoplate (GN) as the conductive agent, thus side effects have been effectively suppressed during the spraying process. As a result, the assembled LICs using the dry-sprayed LTO electrodes show superior energy density and excellent cycling performance, demonstrating this novel fabrication method has practical application prospects. [Display omitted] •Solvent-free Li4Ti5O12 electrodes are prepared by electrostatic spraying.•The differences between dry-sprayed and wet-coated electrodes are explored.•The optimization of electrode microstructure helps properties improve.•Adopting graphene nanoplates as conductive agents perfects spraying results.•Li-ion capacitors with solvent-free electrodes exhibit better performance.