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Organic-based electrode materials for lithium-ion batteries (LIBs) are promising due to their high theoretical capacity, structure versatility and environmental benignity. However, the poor intrinsic electric conductivity of most polymers results in slow reaction kinetics and hinders their application as electrode materials for LIBs. A binder-free self-supporting organic electrode with excellent redox kinetics is herein demonstrated via in situ polymerization of a uniform thin polyimide (PI) layer on a porous and highly conductive carbonized nanofiber (CNF) framework. The PI active material in the porous PI@CNF film has large physical contact area with both the CNF and the electrolyte thus obtains superior electronic and ionic conduction. As a result, the PI@CNF cathode exhibits a discharge capacity of 170 mAh·g-1 at 1 C (175 mA·g-1), remarkable rate-performance (70.5% of 0.5 C capacity can be obtained at a 100 C discharge rate), and superior cycling stability with 81.3% capacity retention after 1, 000 cycles at 1 C. Last but not least, a four-electron transfer redox process of the PI polymer was realized for the first time thanks to the excellent redox kinetics of the PI@CNF electrode, showing a discharge capacity exceeding 300 mAh·g-1 at a current of 175 mA·g-1.
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