4.8 Article

Sulfur Doping: Unique Strategy To Improve the Supercapacitive Performance of Carbon Nano-onions

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 11, Issue 8, Pages 8040-8050

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.8b21534

Keywords

carbon nano-onion; in situ sulfur doping; supercapacitor; exohedral; graphitization; mesoporous; thiophene

Funding

  1. National Research Foundation (NRF) of the Republic of Korea - Ministry of Education of Korea [NRF-2014R1A6A1031189, NRF-2015R1D1A1A09060292]
  2. International Cooperation Program of the NRF of Korea [NRF-2015K2A2A7053101]

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Recently, enhancement of the energy density of a supercapacitor is restricted by the inferior capacitance of negative electrodes, which impedes the commercial development of high-performance symmetric and asymmetric super-capacitors. This article introduces the in situ bulk-quantity synthesis of hydrophilic, porous, graphitic sulfur-doped carbon nano-onions (S-CNO) using a facile flame-pyrolysis technique and evaluated its potential applications as a high-performance supercapacitor electrode in a symmetric device configuration. The high-surface wettability in the as-prepared state enables the formation of highly suspended active conducting material S-CNO ink, which eliminates the routine use of binders for the electrode preparation. The as-prepared S-CNO displayed encouraging features for electrochemical energy storage applications with a high specific surface area (950 m(2) g(-1)), ordered mesoporous structure (similar to 3.9 nm), high S-content (similar to 3.6 at. %), and substantial electronic conductivity, as indicated by the similar to 80% sp(2) graphitic carbon content. The in situ sulfur incorporation into the carbon framework of the CNO resulted in a high-polarized surface with well-distributed reversible pseudosites, increasing the electrode-electrolyte interaction and improving the overall conductivity. The S-CNOs showed a specific capacitance of 305 F g(-1), an energy density of 10.6 W h kg(-1), and a power density of 1004 W kg(-1) at an applied current density of 2 A g(-1) in a symmetrical two-electrode cell configuration, which is approximately three times higher than that of the pristine CNO-based device in a similar electrochemical testing environment. Even at 11 A g(-1), the S-CNOIIS-CNO device rendered an energy density (6.1 W h kg(-1)) at a deliverable power density of 5.5 kW kg(-1), indicating a very good rate capability and power management during peak power delivery applications. Furthermore, it showed a high degree of electrochemical reversibility with excellent cycling stability, retaining similar to 95% of its initial capacitance after more than 10 000 repetitive charge-discharge cycles at an applied current density of 5 A g(-1).

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