Abstract

Graphene papers have great potential for various applications, such as electrodes in energy storage devices, protective coating, and desalination, because of their free-standing structure, flexibility, and chemical tunability. The inner structures of the graphene papers can affect their physical properties and device performance. Here, we investigated a way to fabricate graphene papers from crumpled reduced graphene oxide (rGO) spheres. We found that ultrasonication was useful for tailoring the morphology of the crumpled graphene spheres, resulting in a successful fabrication of graphene papers with tunable inner pore structures. The fabricated graphene papers showed changes in mechanical and electrical properties depending on their pore structures. In addition, the tailored pore structures had an influence on the electrochemical performance of supercapacitors with the fabricated graphene papers as electrode materials. This work demonstrates a facile method to fabricate graphene papers from crumpled rGO powders, as well as a fundamental understanding of the effect of the inner pore structures in mechanical, electrical, and electrochemical characteristics of graphene papers.

Highlights

  • The mass production of graphene powders has been enabled by the chemical oxidation of graphite, followed by the exfoliation of graphite oxide into individual graphene oxide (GO) and a reduction of GO with chemical and/or thermal treatments [1]

  • A large quantity of reduced graphene oxide with high electrical conductivity, high surface area, and mechanical robustness has shown its potential uses in industrial applications such as energy-related devices, water purification, and nanocomposites among others [2,3,4,5,6,7]

  • The restacking of graphene flakes leads to limited ion-transport paths in electrodes of supercapacitors based on electrical double layer capacitance (EDLC), hindering the development of high-performance supercapacitors using graphene papers [17,18,19]

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Summary

Introduction

The mass production of graphene powders has been enabled by the chemical oxidation of graphite, followed by the exfoliation of graphite oxide into individual graphene oxide (GO) and a reduction of GO with chemical and/or thermal treatments [1]. Among several methods to fabricate macroscopic structures from graphene flakes, a paper-like film presents an attractive form because of its flexibility, mechanical strength, electrical conductivity, and chemical tunability [8,9] These intriguing characteristics of graphene papers have enabled unique applications, including supercapacitor electrodes, filter membranes, actuators, sensors, and protective coating [10,11,12,13,14]. The restacking of graphene flakes leads to limited ion-transport paths in electrodes of supercapacitors based on electrical double layer capacitance (EDLC), hindering the development of high-performance supercapacitors using graphene papers [17,18,19] Nanoparticles, such as SiO2 [20] or polymers [21], have been utilized as templates in order to make porous graphene spheres. Supercapacitors with a two-electrode configuration were assembled with the fabricated graphene papers as electrode materials, and their electrochemical performances were evaluated with respect to the sonication treatment

Materials and Methods
Characterization of rGO Powders and Fabricated Graphene Papers
Tailoring the Morphology of Crumpled Graphene Spheres with Ultrasonication
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