High micropore‐utilization carbon aerogel with controlled nanostructures via adjusting aggregation state of polyacrylonitrile for energy storage systems

Abstract Designing and optimizing the pore structure of porous carbon electrodes is essential for diverse energy storage systems. In this study, an innovative approach spray phase‐inversion strategy was developed for the rapid and efficient fabrication of controlled porous carbon aerogel. Moreover, the aggregation structure of polyacrylonitrile is controlled by adjusting the Hansen's solubility parameter, thereby regulating the electrode material structure. Furthermore, the theoretical analysis of the spray phase‐inversion process revealed that this regulation process is jointly regulated by solvent hydrodynamic diameter and phase‐inversion kinetics. Through optimization, a novel porous carbon material was obtained that exhibited excellent performance as an electrode material. When utilized in supercapacitors for energy storage, it demonstrated a high specific capacitance of 373.1 F g −1 in a 6 M KOH electrolyte solution. Simultaneously, it has been observed that the preparation strategy for porous electrodes offers notable advantages in terms of excellent designability, broad universality, simplicity, and high efficiency, thereby holding promise for large‐scale fabrication of diverse porous electrode materials and various types of electrodes for diverse energy storage applications.