Strain-induced self-adhesion morphs graphene toward 3D

Abstract

Crumpled graphene, a three-dimensional (3D) form of graphene with a high surface area, has garnered significant interest for applications in energy storage, catalysis, and encapsulation. However, conventional crumpled graphene structures remain relatively open, limiting their potential for nanoscale confinement. Here, we demonstrate a method to systematically tune the fractal dimension (D) of crumpled graphene via controlled perforation. By introducing in-plane pores to graphene oxide (GO) sheets before crumpling, we achieve denser, more compact morphologies that approach a near-spherical configuration with D increasing from 2.38 to 2.87. The mechanism is governed by the interplay between mechanical softening and self-adhesion, facilitating a higher packing density. We further investigate the implications of this structural transformation on ion diffusion kinetics and demonstrate that increasing D effectively modulates molecular transport within crumpled graphene particles. Finally, we demonstrate the encapsulation capabilities of these graphene structures by stabilizing platinum nanoparticles against sintering. Our findings provide a scalable strategy for designing crumpled graphene with tunable dimensionality, unlocking new possibilities in nanoscale packaging, storage, and functional nanomaterials.