Three-Dimensionally Ordered Mesoporous (3DOm) Carbon Materials as Electrodes for Electrochemical Double-Layer Capacitors with Ionic Liquid Electrolytes

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Abstract

Compared to rechargeable batteries, electrochemical double-layer capacitors (EDLCs) are normally considered to be higher power but lower electrical energy density charge storage devices. To increase the energy density, one can enlarge the interfacial area between electrodes and electrolyte through the introduction of nanopores and employ electrolytes that are stable over wider voltage ranges, such as ionic liquids. However, due to the relatively high viscosity of ionic liquids and large ion sizes, these measures can result in diminished power performance. Here, we describe the synthesis of carbon electrodes that overcome these limitations and simultaneously provide high specific energies and high specific powers in EDLCs using the ionic liquid EMI-TFSI as an electrolyte. A colloidal crystal templating method was optimized to synthesize three-dimensionally ordered mesoporous (3DOm) carbons with well-defined geometry, three-dimensionally interconnected pore structure and tunable pore size in the range from 8 to 40 nm. To achieve precise control over the pore sizes in the carbon products, parameters were established for direct syntheses or seed growth of monodisperse silica nanospheres with specific sizes, using l-lysine-assisted hydrolysis of silicon alkoxide precursors. Porous carbons were then templated from these materials using phenol–formaldehyde (PF) or resorcinol–formaldehyde (RF) precursors. The pore structures of the nanoporous carbon products were characterized in detail, and the materials were tested as electrodes for EDLCs. Optimal pore sizes were identified that provided a large interface between the electrode and the electrolyte while maintaining good ion transport through the relatively viscous electrolyte. 3DOm PF-carbons with pore diameters in the 21–29 nm range exhibited similar high specific capacitance values (146–178 F g–1 at 0.5 A g–1, with respect to the mass of carbon in a single electrode) as typical large-scale activated-carbon-based EDLCs but showed significantly better high-rate performance (80–123 F g–1 at 25 A g–1), a result of the more accessible pore space in which ion diffusion was less restricted.

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