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Redox-active porous organic polymers (POPs) demonstrate significant potential in supercapacitors. However, their intrinsic low electrical conductivity and stacking tendencies often lead to low utilization rates of redox-active sites within their structural units. Herein, polyimide POPs (donated as PMTA) are synthesized in situ on multi-walled carbon nanotubes (MWCNTs) from tetramino-benzoquinone (TABQ) and 1,4,5,8-naphthalene tetracarboxylic dianhydride (PMDA) monomers. The strong π–π stacking interactions drive the PMTA POPs and the MWCNTs together to form a PMTA/MWCNT composite. With the assistance of MWCNTs, the stacking issue and low conductivity of PMTA POPs are well addressed, leading to the obvious activation and enhanced utilization of the redox-active groups in the PMTA POPs. PMTA/MWCNT then achieves a high capacitance of 375.2 F g⁻¹ at 1 A g⁻¹ as compared to the pristine PMTA POPs (5.7 F g⁻¹) and excellent cycling stability of 89.7% after 8000 cycles at 5 A g⁻¹. Cyclic voltammetry (CV) and in situ Fourier-Transform Infrared (FT-IR) results reveal that the electrode reactions involve the reversible structural evolution of carbonyl groups, which are activated to provide rich pseudocapacitance. Asymmetric supercapacitors (ASCs) assembled with PMTA/MWCNTs and activated carbon (AC) offer a high energy density of 15.4 Wh kg⁻¹ at 980.4 W kg⁻¹ and maintain a capacitance retention of 125% after 10,000 cycles at 5 A g⁻¹, indicating their good potential for practical applications.