Abstract

Nanoporous polymers are becoming increasingly interesting materials for electrochemical applications, as their large surface areas with redox-active sites allow efficient adsorption and diffusion of ions. However, their limited electrical conductivity remains a major obstacle in practical applications. The conventional approach that alleviates this problem is the hybridisation of the polymer with carbon-based additives, but this directly prevents the utilisation of the maximum capacity of the polymers. Here, we report a layer-by-layer fabrication technique where we separated the active (porous polymer, top) layer and the conductive (carbon, bottom) layer and used these “layered” electrodes in a supercapacitor (SC). Through this approach, direct contact with the electrolyte and polymer material is greatly enhanced. With extensive electrochemical characterisation techniques, we show that the layered electrodes allowed a significant contribution of fast faradic surface reactions to the overall capacitance. The electrochemical performance of the layered-electrode SC outperformed other reported porous polymer-based devices with a specific gravimetric capacitance of 388 F·g−1 and an outstanding energy density of 65 Wh·kg−1 at a current density of 0.4 A·g−1. The device also showed outstanding cyclability with 90% of capacitance retention after 5000 cycles at 1.6 A·g−1, comparable to the reported porous polymer-based SCs. Thus, the introduction of a layered electrode structure would pave the way for more effective utilisation of porous organic polymers in future energy storage/harvesting and sensing devices by exploiting their nanoporous architecture and limiting the negative effects of the carbon/binder matrix.

Highlights

  • Introduction published maps and institutional affilThe development of low cost, eco-friendly and high-performance energy storage devices is becoming crucial to meeting modern energy storage demand in various applications, including electric vehicles, portable electronics, and power grids

  • A temperature of 546 ◦ C was observed at 5% weight loss for

  • Per-TAPB-PPI, which is on par with the current state-of-the-art porous polyimides [24,34], and it emphasises the advantage of using imide-linkages in porous polymers

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Summary

Introduction

The development of low cost, eco-friendly and high-performance energy storage devices is becoming crucial to meeting modern energy storage demand in various applications, including electric vehicles, portable electronics, and power grids. There are two types of supercapacitor electrodes; one that uses the electric double layer phenomenon and one based on fast faradic surface reactions (pseudocapacitive SCs). High-performance electrode materials should have properties such as an electrical conductivity, a large specific surface area, and good wettability by the electrolyte in both cases. Several materials have been used to fabricate electrodes for supercapacitors, including carbon nanotubes [1,3], graphene [4,5], metal oxides nanoparticles [6,7,8], transition metal dichalcogenides [9], and carbon-based composites [10,11]. Several materials have been used to fabricate electrodes for supercapacitors, including carbon nanotubes [1,3], graphene [4,5], metal oxides nanoparticles [6,7,8], transition metal dichalcogenides [9], and carbon-based composites [10,11]. iations.

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