Enabling Fast-Charging of Lithium-Ion Batteries through Printed Electrodes

It has been well recognized that introducing secondary porous networks (SPNs) into the electrodes can effectively improve the electrochemical performance of lithium-ion batteries (LIBs), especially under fast-charging operations. However, the process complexity and high cost limit the commercial success of advanced electrodes with SPNs. To address this issue, we developed a facile screen-printing process to produce structured graphite electrodes with SPNs. The experimental results demonstrated that, by tuning the diameter and center-to-center (C2C) distance of emulsion dots on the stencil screen, the pore diameters and C2C pore distances of SPNs in screen-printed electrodes can be precisely controlled in the range of 100 μm to 1mm and 100 μm to 3mm respectively. In addition, the SPNs with hexagonal and square-shape pore alignments have also been imprinted onto the electrode coatings through adjusting the patterns of screen stencils. Used as anodes, the printed graphite electrodes demonstrated significantly reduced overpotential and voltage fluctuation under fast-charging operations from 2C to 6C. Coupled with LiNi_0.6Mn_0.2Co_0.2O₂ (NMC622) cathodes, the full cells with printed graphite anodes exhibited an unprecedently stable performance with almost no capacity decay up to 170 cycles when charged to 80% SOC at 2C. Observations from electron microscopy showed plated lithium undetectable at the surface of printed graphite electrodes after numerous cycles. The electrochemical analysis on the voltage evolution during the cell rest period indicated the significantly delayed onset of lithium plating in the presence of printed graphite electrodes. All these results suggest that the significantly improved cell performance is associated with the shortened Li-ion diffusion distance, reduced polarization and suppressed Li plating in the printed electrodes with patterned SPNs.