Three-dimensional porous polyimide anode for high-rate lithium ion batteries

Polymeric electrode materials are widely used in many applications but still suffer from poor electrical conductivity and slow transport kinetics, especially poor performance at high current densities. Herein, a polyimide electrode structure with 3D-ordered interconnected gradient pores was developed to improve the lithium-ion transport efficiency. The homogeneous mixed PMTA-PMMA composite was prepared by a simple one-pot method, followed by removal of PMMA (polymethyl methacrylate) spherical porogenic agent during the synthesis of polyimide material at high temperatures to form a low curvature gradient-pore structure. The large pores in the electrode enhanced the ion transport ability and improved the electrolyte infiltration rate, while the small pores improved the active specific surface area and guided the deposition of lithium ions. As a result, a high specific capacity reaching 907 mAh/g was maintained even after 1000 cycles at 5 A/g, a value about 3-fold that of un-pored electrode materials. The experimental studies and DFT calculations were used to develop a 24Li storage mechanism of PMTA, and the active electrode material was fully electrochemically activated by the constructed three-dimensional porous electrode structure. Overall, the proposed porous material with a high active area and porosity looks potential for use as an ultra-fast charging and discharging electrode of lithium-ion batteries with high specific capacity and excellent cycling performance.