Abstract

Summary Pseudocapacitors with a fast faradic redox reaction during the electrochemical charge/discharge process hold great promise for delivering high power and high energy. Here, we used emerging oxygenated carbon nitride (OCN) as a model for nitrogen- and oxygen-enriched carbons and found an anion-selective charging behavior in aqueous electrolytes. The N- and O-mediated hydroxyl anion-selective charging originates from inbuilt surface-positive electrostatic potential localized at heptazine and quaternary N atom structural units. The carbon atoms in heptazine adjacent to pyridinic N act as the electron transfer active sites for faradic pseudocapacitance. The OCN free-standing films (FSFs) were developed as current collector-free electrodes, and stacking OCN FSFs can confer a cell with loading weight over a commercial level. For demonstration, a symmetrical cell with 17.7 mg cm−2 delivers an energy of 140.9 mW h at a high power of 2,499.9 mW, and almost 100% capacitance retention after 20,000 charge/discharge cycles at 50 mA.

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