Diffusion-driven
layer-by-layer (dd-LbL) assembly is a simple yet
versatile process that can be used to construct graphene oxide (GO)
into a three-dimensional (3D) porous framework with good mechanical
stability. In particular, the oxygen functional groups on the GO surface
are well retained, providing nucleation sites for further chemical
reactions to be performed upon. Therefore, such a scaffold should
serve as a promising starting material for creating a wide range of
3D graphene-based composites while maintaining a high accessible surface
area. Herein, we demonstrate the use of the porous GO macrostructure
derived from dd-LbL assembly for the preparation of graphene–MnCO3 hybrid structures. MnCO3 is a newly reported pseudocapacitive
material for supercapacitors; however, its electrochemical performance
is hampered by its low electrical conductivity and poor chemical stability.
Through reaction between KMnO4 and GO during a hydrothermal
process, the surface of the porous scaffold was rendered with uniform
MnCO3 nanoparticles. With the reduced graphene oxide (rGO)
sheets serving as the conductive backbone, the resultant MnCO3 nanoparticles exhibited a capacitance of 698 F g–1 at a charge/discharge current of 0.5 mA (320 F g–1 for the combined rGO and MnCO3 composite). Furthermore,
the electrode maintained 77% of its initial capacity even after 5000
cycles of charge/discharge tests at 20 mA.