A Universal Electrolyte Formulation for the Electrodeposition of Pristine Carbon and Polypyrrole Composites for Supercapacitors.

Electrodeposition of conducting polymer-carbon composites from an electrolyte precursor solution is a facile one-step approach to fabricate device-ready electrodes for energy storage. A key challenge in this approach is the dispersion of the carbon nanomaterials with the aqueous precursor solution with previous approaches either heavily oxidizing the carbon nanomaterials or using high concentrations of anionic surfactants as dopants. However, the former reduces the electrical conductivity of carbon, while the latter reduces the ionic mobility of the conducting polymer due to the large anion size. Herein, for the first time we present a quaternary electrolyte formulation for the fabrication of pristine carbon and polypyrrole (PPy) composites that does not sacrifice either electron or ion mobility. The electrolyte uses lithium perchlorate (20 mM) as a supporting electrolyte and dopant, sodium dodecylbenzenesulfonate at a very low concentration (1.43 mM) as a surfactant, together with pristine carbon nanomaterials and pyrrole monomers. The order of magnitude difference between the concentration of the dopant and surfactant ion allows the as-deposited PPy to be doped predominantly by small-sized and mobile perchlorate anions. Composites of PPy with carbon black, carbon nanotubes, and electrochemical exfoliated graphene (EEG) have been successfully prepared using this new quaternary electrolyte. The as-fabricated PPy/EEG composite electrodes showed a specific capacitance of 348.8 F g-1 with a high rate capability (190.7 F g-1 at 71 A g-1). Supercapacitor devices based on the PPy/EEG composite electrodes exhibit a high rate behavior up to 500 mV s-1 and a long cycle life of 5000 cycles.

Two-Step Electrochemical Intercalation and Oxidation of Graphite for the Mass Production of Graphene Oxide.

Conventional chemical oxidation routes for the production of graphene oxide (GO), such as the Hummers' method, suffer from environmental and safety issues due to their use of hazardous and explosive chemicals. These issues are addressed by electrochemical oxidation methods, but such approaches typically have a low yield due to inhomogeneous oxidation. Herein we report a two-step electrochemical intercalation and oxidation approach to produce GO on the large laboratory scale (tens of grams) comprising (1) forming a stage 1 graphite intercalation compound (GIC) in concentrated sulfuric acid and (2) oxidizing and exfoliating the stage 1 GIC in an aqueous solution of 0.1 M ammonium sulfate. This two-step approach leads to GO with a high yield (>70 wt %), good quality (>90%, monolayer), and reasonable oxygen content (17.7 at. %). Moreover, the as-produced GO can be subsequently deeply reduced (3.2 at. % oxygen; C/O ratio 30.2) to yield highly conductive (54 600 S m-1) reduced GO. Electrochemical capacitors based on the reduced GO showed an ultrahigh rate capability of up to 10 V s-1 due to this high conductivity.