Controlling the Thickness of Thermally Expanded Films of Graphene Oxide

"Paper-like" film material made from stacked and overlapping graphene oxide sheets can be exfoliated (expanded) through rapid heating, and this has until now been done with no control of the final geometry of the expanded graphene oxide material, i.e., the expansion has been physically unconstrained. (As a consequence of the heating and exfoliation, the graphene oxide is "reduced", i.e., the graphene oxide platelets are deoxygenated to a degree.) We have used a confined space to constrain the expanding films to a controllable and uniform thickness. By changing the gap above the film, the final thickness of expanded films prepared from, e.g., a 10 μm-thick graphene oxide film, could be controlled to values such as 20, 30, 50, or 100 μm. When the expansion of the films was unconstrained, the final film was broken into pieces or had many cracks. In contrast, when the expansion was constrained, it never cracked or broke. Hot pressing the expanded reduced graphene oxide films at 1000 °C yielded a highly compact structure and promoted graphitization. Such thickness-controlled expansion of graphene oxide films up to tens or hundreds of times the original film thickness was used to emboss patterns on the films to produce areas with different thicknesses that remain connected "in plane". In another set of experiments, we treated the original graphene oxide film with NaOH before its controlled expansion resulted in a different structure featuring uniformly distributed pores and interconnected layers as well as simultaneous activation of the carbon.