We designed high-volumetric-energy-density supercapacitors from monolithic composites composed of self-standing carbon foam (CF) as the conducting matrix and embedded hierarchically organized porous carbon (PICK) as the active material. Using multiprobe scanning tunneling microscopy at selected areas, we were able to disentangle morphology-dependent contributions of the heterogeneous composite to the overall conductivity. Adding PICK is found to enhance the conductivity of the monoliths by providing additional links for the CF network, enabling high and stable performance. The resulting all-carbon CF-PICK composites were used as self-standing electrodes for symmetric supercapacitors without the need for a binder, additional conducting additive, metals as a current collector, or casting/drying steps. Supercapacitors achieved a capacitance of 181 F g-1 based on the entire mass of the monolithic electrode as well as an outstanding rate capability. Our symmetrical supercapacitors also delivered a record volumetric energy density of 19.4 mW h cm-3 when using aqueous electrolytes. Excellent cycling stability with almost quantitative retention of capacitance was found after 10,000 cycles in 6.0 M KOH as the electrolyte. Furthermore, charge-discharge testing at different currents demonstrated the fast charge-discharge capability of this material system that meets the requirements for practical applications.
Keywords: areal energy density; birnessite; high mass loading; micro-supercapacitors; porous carbons.