Chain engineering-tailored microstructures and lithium storage performance of hydrothermally-synthesized linear polyimides

Abstract Polyimides with high capacity, fast kinetics, abundant resource, and structural diversity offer an exhilarating opportunity for developing sustainable rechargeable batteries. Herein, a series of 1,4,5,8-naphthalenetetracarboxylic dianhydride (NTCDA)-based polyimides were successfully crafted through a facile and eco-friendly hydrothermal synthesis route. The microstructure and lithium storage performance of polyimides were tailored by regulating diamine linkers between NTCDA units. Interestingly, the moderate increased length of flexible diamine units with ethylenediamine and diaminobutane can stabilize the polymer skeleton. This leads to the formation of honeycomb-like porous structures with a sufficient exposure of active carbonyl groups, thereby achieving a large capacity and high rate capability. Therefore, polyimides derived from ethylenediamine and diaminobutane show larger reversible capacities (123 and 113.5 mA h/g at 50 mA/g, respectively) and better rate capabilities with capacity retentions of up to 50% when the current increased from 50 to 2000 mA/g. This work would provide new insights into macromolecular engineering of polymers for advanced electrode materials.