Three-dimensional (3D) graphene-based structures combine the unique physical properties of graphene with the opportunity to get high electrochemically available surface area per unit of geometric surface area. Several preparation techniques have been reported to fabricate 3D graphene-based macroscopic structures for energy storage applications such as supercapacitors. Although reaserch has been focused so far on achieving either high specific capacitance or high volumetric capacitance, much less attention has been dedicated to obtain high specific and high volumetric capacitance simultaneously. Here, we present a facile technique to fabricate graphene foams (GF) of high crystal quality with tunable pore size grown by chemical vapor deposition. We exploited porous sacrificial templates prepared by sintering nickel and copper metal powders. Tuning the particle size of the metal powders and the growth temperature allow fine control of the resulting pore size of the 3D graphene-based structures smaller than 1 µm. The as-produced 3D graphene structures provide a high volumetric electric double layer capacitance (165 mF cm −3). High specific capacitance (100 F g −1) is obtained by lowering the number of layers down to single layer graphene. Furthermore, the small pore size increases the stability of these GFs in contrast to the ones that have been grown so far on commercial metal foams. Electrodes based on the as-prepared GFs can be a boost for the development of supercapacitors, where both low volume and mass are required.
Supercapacitors are called to play a prominent role in the newly emerging markets of electric vehicles, flexible displays and sensors, and wearable electronics. In order to compete with current battery technology, supercapacitors have to be designed with highly conductive current collectors exhibiting high surface area per unit volume and uniformly coated with pseudocapacitive materials, which is crucial to boost the energy density while maintaining a high power density. Here, we present a versatile technique to prepare thickness-controlled thin-film micro graphene foams (μGFs) with pores in the lower micrometer range grown by chemical vapor deposition which can be used as highly conductive current collectors in flexible supercapacitors. To fabricate the μGF, we use porous metallic catalytic substrates consisting of nickel/copper alloy synthesized on nickel foil by electrodeposition in an electrolytic solution. Changing the duration of the electrodeposition allows the control of the thickness of the metal foam, and thus of the μGF, ranging from a few micrometers to the millimeter scale. The resulting μGF with a thickness and pores in the micrometer regime exhibits high structural quality which leads to a very low intrinsic resistance of the devices. Transferred onto flexible substrates, we demonstrate a uniform coating of the μGFs with manganese oxide, a pseudocapacitively active material. Considering the porous structure and the thickness of the μGFs, square wave potential pulses are used to ensure uniform coverage by the oxide material boosting the volumetric and areal capacitance to 14 F cm and 0.16 F cm. The μGF with a thickness and pores in the micrometer regime in combination with a coating technique tuned to the porosity of the μGF is of great relevance for the development of supercapacitors based on state-of-the-art graphene foams.
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