Processing micrometer-sized particles in crumpled graphene network for freestanding membrane enabled by freeze casting

Graphene oxide (GO) is widely used in the construction and application of various 2D membrane-based materials due to its unique colloidal structure. Herein, we demonstrate that micrometer-sized particles can make up freestanding membranes enabled by the extraordinary amphiphilic and polymer-like properties of graphene oxide through freeze casting. The 2D macromolecule, GO could well wrap the particles for better uniformity and stability in either dispersion or membrane. Importantly, freeze casting plays an important role in avoiding the severe aggregation of micrometer-sized particles in the solventremoving process. After reduction, the membrane exhibits good electrical conductivity while maintaining its integral structure, which can be directly used as a freestanding binder-free electrode. This work provides a universal approach to fabricate freestanding membranes with various micrometersized materials for energy storage.