4.7 Article

Facile construction of highly redox active carbons with regular micropores and rod-like morphology towards high-energy supercapacitors

期刊

MATERIALS CHEMISTRY FRONTIERS
卷 5, 期 7, 页码 3061-3072

出版社

ROYAL SOC CHEMISTRY
DOI: 10.1039/d0qm01101k

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资金

  1. National Natural Science Foundation of China [21875165, 51772216, 21905207]
  2. Science and Technology Commission of Shanghai Municipality, China [20ZR1460300, 14DZ2261100]
  3. Zhejiang Provincial Natural Science Foundation of China [LY19B010003]
  4. Fundamental Research Funds for the Central Universities
  5. Large Equipment Test Foundation of Tongji University

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A facile route to construct highly redox active carbons is designed based on potassium bicarbonate-involved calcination, resulting in carbon materials with large specific surface area, high-level heteroatom activity, and regular micropore diameters. The carbon electrode shows outstanding capacitive performance and energy output in a hybrid aqueous electrolyte, with boosted energy density in an ionic liquid cell. The satisfactory supercapacitive performance can be attributed to the high-level superiority retention in the preset precursor, inspiring structure optimization for other functionalized carbons.
Redox active carbonaceous materials have recently absorbed a wide range of interest in energy-related fields owing to their trade-off superiorities between carbon stability and heteroatom activity. Feasible alkali-calcination of heteroatom-rich precursors is considered as an effective route to obtain large-surface-area carbons in supercapacitors, but preset structure/heteroatomic functionalities generally suffer from a great loss of efficacy due to severe corrosion. In this work, a facile route to construct highly redox active carbons is designed based on one-step potassium bicarbonate-involved calcination of an electroactive benzoquinone/p-phenylenediamine precursor. The resulting high-yield (74.9%) carbon not only presents large specific surface area (1840 m(2) g(-1)) with regular micropore diameters predominantly at 0.55 and 0.85 nm, but also retains the high-level heteroatom activity (e.g. N: 11.46 wt%) and rod-like morphology of the synthetic precursor. When applied as a supercapacitor electrode, the representative material delivers a prominent capacitance of 365 F g(-1) at 1 A g(-1) and energy output of 18.25 W h kg(-1) in a hybrid aqueous electrolyte (H2SO4 + KBr) at 600 W kg(-1) by magnificent support of an extra redox mechanism. Additionally, on account of efficient electrolyte-ion electrosorption by optimized microporous spaces, the as-assembled EMIMBF4-based ionic liquid cell offers boosted energy density up to 89.5 W h kg(-1) under the broadened potential of 3.8 V. Such satisfactory supercapacitive performance of the carbon electrode can be fundamentally assigned to the high-level superiority retention in the preset precursor, which may inspire structure optimization for other functionalized carbons.

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