Preparation of Tough, Binder‐Free, and Self‐Supporting LiFePO4 Cathode by Using Mono‐Dispersed Ultra‐Long Single‐Walled Carbon Nanotubes for High‐Rate Performance Li‐Ion Battery

Abstract Low‐contents/absence of non‐electrochemical activity binders, conductive additives, and current collectors are a concern for improving lithium‐ion batteries' fast charging/discharging performance and developing free‐standing electrodes in the aspects of flexible/wearable electronic devices. Herein, a simple yet powerful fabricating method for the massive production of mono‐dispersed ultra‐long single‐walled carbon nanotubes (SWCNTs) in N ‐methyl‐2‐pyrrolidone solution, benefiting from the electrostatic dipole interaction and steric hindrance of dispersant molecules, is reported. These SWCNTs form a highly efficient conductive network to firmly fix LiFePO 4 (LFP) particles in the electrode at low contents of 0.5 wt% as conductive additives. The binder‐free LFP/SWCNT cathode delivers a superior rate capacity of 161.5 mAh g −1 at 0.5 C and 130.2 mAh g −1 at 5 C, with a high‐rate capacity retention of 87.4% after 200 cycles at 2 C. The self‐supporting LFP/SWCNT cathode shows excellent mechanical properties, which can withstand at least 7.2 MPa stress and 5% strain, allowing the fabrication of high mass loading electrodes with thicknesses up to 39.1 mg cm −2 . Such self‐supporting electrodes display conductivities up to 1197 S m −1 and low charge‐transfer resistance of 40.53 Ω, allowing fast charge delivery and enabling near‐theoretical specific capacities.