Self-assembled high polypyrrole loading flexible paper-based electrodes for high-performance supercapacitors

Despite the intriguing features of freestanding flexible electronic devices, such as their binder-free nature and cost-effectiveness, the limited loading capacity of active material poses a challenge to achieving practical high-performance flexible electrodes. We propose a novel approach that integrates multiple self-assembly and in-situ polymerization techniques to fabricate a high-loading paper-based flexible electrode (MXene/Polypyrrole/Paper) with exceptional areal capacitance. The approach enables polypyrrole to form a porous conductive network structure on the surface of paper fiber through MXene grafting via hydrogen bonding and electrostatic interaction, resulting in an exceptionally high polypyrrole loading of 10.0 mg/cm2 and a conductivity of 2.03 S/cm. Moreover, MXene-modified polypyrrole paper exhibits a more homogeneous pore size distribution ranging from 5 to 50 μm and an increased specific surface area of 3.11 m2/g. Additionally, we have optimized in-situ polymerization cycles for paper-based supercapacitors, resulting in a remarkable areal capacitance of 2316 mF/cm2 (at 2 mA/cm2). The capacitance retention rate and conductivity rate maintain over 90% after undergoing 100 bends.The maximum energy density and cycling stability are characterized to be 83.6 μWh/cm2 and up to 96% retention after 10000 cycles. These results significantly outperform those previously reported for paper-based counterparts. Overall, our work presents a facile and versatile strategy for assembling high-loading, paper-based flexible supercapacitors network architecture that can be employed in developing large-scale energy storage devices.