Microporous activated carbon originating from coconut shell, as received or oxidized with nitric acid, is treated with melamine and urea and heated to 950 °C in an inert atmosphere to modify the carbon surface with nitrogen‐ and oxygen‐containing groups for a systematic investigation of their combined effect on electrochemical performance in 1 M H2SO4 supercapacitors. The chemistry of the samples is characterized using elemental analysis, Boehm titration, potentiometric titration, and X‐ray photoelectron spectroscopy. Sorption of nitrogen and carbon dioxide is used to determine the textural properties. The results show that the surface chemistry is affected by the type of nitrogen precursor and the specific groups present on the surface before the treatment leading to the incorporation of nitrogen. Analysis of the electrochemical behavior of urea‐ and melamine‐treated samples reveal pseudocapacitance from both the oxygen and the nitrogen containing functional groups located in the pores larger than 10 Å. On the other hand, pores between 5 Å and 6 Å are most effective in a double‐layer formation, which correlates well with the size of hydrated ions. Although the quaternary and pyridinic‐N‐oxides nitrogen groups have enhancing effects on capacitance due to the positive charge, and thus an improved electron transfer at high current loads, the most important functional groups affecting energy storage performance are pyrrolic and pyridinic nitrogen along with quinone oxygen.
Nitrogen‐enriched nonporous carbon materials derived from melamine–mica composites are subjected to ammonia treatment to further increase the nitrogen content. For samples preoxidized prior to the ammonia treatment, the nitrogen content is doubled and is mainly incorporated in pyrrol‐like groups. The materials are tested as electrodes for supercapacitors, and in acidic or basic electrolytes, the gravimetric capacitance of treated samples is three times higher than that of untreated samples. This represents a tenfold increase of the capacitance per surface area (3300 µF cm−2) in basic electrolyte. Due to the small volume of the carbon materials, high volumetric capacitances are achieved in various electrolytic systems: 280 F cm−3 in KOH, 152 F cm−3 in H2SO4, and 92 F cm−3 in tetraethylammonium tetrafluoroborate/propylene carbonate.
Honeycomb catalysis: a facile oxygen reduction reaction has been observed on a graphitic C(3)N(4)/carbon catalyst with three-dimensional interconnected macropores (see picture with SiO(2) template). This material not only shows catalytic activity that is comparable to that of commercial Pt/C, but also has much higher organic-fuel tolerance and long-term stability.
Phosphorus-rich microporous carbons (P-carbons) prepared by a simple H(3)PO(4) activation of three different carbon precursors exhibit enhanced supercapacitive performance in 1 M H(2)SO(4) when highly stable performance can be achieved at potentials larger than the theoretical decomposition potential of water. This ability of P-carbons greatly enhances the energy density of supercapacitors that are capable of delivering 16 Wh/kg compared to 5 Wh/kg for the commercial carbon. An intercept-free multiple linear regression model confirms the strongest influence of phosphorus on capacitance together with micropores 0.65-0.83 nm in width that are the most effective in forming the electric double layer.
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