4.5 Article

Introducing Electrochemically Active Oxygen Species to Boost the Pseudocapacitance of Carbon-based Supercapacitor

Journal

CHEMELECTROCHEM
Volume 8, Issue 16, Pages 3073-3079

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/celc.202100641

Keywords

supercapacitors; carbon-based electrodes; electrochemical oxidation; high energy density; oxygen-containing functional groups

Funding

  1. National Science Fund for the National Natural Science Foundation of China [22075038, 21875028]
  2. Liao Ning Revitalization Talents Program [XLYC1902045]

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By oxidizing carbon electrodes in 1 M H2SO4 electrolyte, this study successfully introduced pseudocapacitance to address the low energy density issue in carbon-based supercapacitors. Manipulating the potential window and sweep rate enhanced oxygen content and specific capacitance, leading to improved rate performance and cycling stability of the oxidized AC electrodes.
Low energy density is the main bottleneck for carbon-based supercapacitors, which can be addressed by introducing extra faradaic pseudocapacitance. Herein, a cyclic voltammetry oxidation method in 1 M H2SO4 electrolyte was employed for carbon electrode to produce electrochemically active oxygen functional groups that are in contact with the conductive substrates, which facilitates the implementation of the pseudocapacitance. Moreover, the influence of potential window and sweep rate on the components and performances of oxidized electrodes in the cyclic voltammetry oxidation process was systematically investigated. The results reveal that a broad potential window of -0.65 similar to 2 V can enhance the oxygen content to 16.4 wt.% (vs. 7.6 wt.% within -0.65 similar to 1.5 V). Additionally, a selective oxygen component dominated with redox active C-OH and C=O groups was achieved by a rapid potentiodynamic sweep at 20 mV s(-1), simultaneously suppressing the -COOH groups with inferior conductivity. The oxidized AC electrodes could substantially improve the specific capacitance (534 vs. 150.3 F g(-1) at 1 A g(-1)) without sacrifice of rate performance (retained 418 F g(-1) at 20 A g(-1)), accompanying excellent cycling stability of 94 % of initial capacitance after 10000 cycles. Such finding would provide some reference for tailoring oxygen species to fabricate advanced carbon-based supercapacitor electrodes.

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