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.
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