4.8 Article

Advanced Carbon-Nickel Sulfide Hybrid Nanostructures: Extending the Limits of Battery-Type Electrodes for Redox-Based Supercapacitor Applications

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 17, Pages 20559-20572

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c03053

Keywords

nickel sulfide; heazlewoodite Ni3S2; vertical carbon nanostructure; redox-based supercapacitor; binder-free; plasma synthesis

Funding

  1. European Union [766894]
  2. Slovenian Research Agency [N2-0107]
  3. AD FUTURA, Public Scholarship, Development, Disability, and Maintenance Fund of the Republic of Slovenia
  4. FCT [UIDB/QUI/00100/2020]

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The study demonstrates the successful fabrication of metal sulfide-carbon nanostructure electrode materials with ultra-high capacity and outstanding rate capability. By combining vertically aligned carbon nanotubes with single-crystal metallic nickel grains, the hybrid binder-free electrodes exhibit remarkable electrochemical performance compared to other reported Ni3S2-based electrodes, showing high specific capacity, retention rate at high current densities, and cycling stability.
Transition-metal sulfides combined with conductive carbon nano-structures are consid ered promising electrode materials for redox-based super-capacitors due to their high specific capacity. However, the low rate capability of these electrodes, still considered battery-type electrodes, presents an obstacle for general use. In this work, we demonstrate a successful and fast fabrication process of metal sulfide-carbon nanostructures ideal for charge-storage electrodes with ultra-high capacity and outstanding rate capability. The novel hybrid binder-free electrode material consists of a vertically aligned carbon nanotube (VCN), terminated by a nanosized single-crystal metallic Ni grain; Ni is covered by a nickel nitride (Ni3N) interlayer and topped by trinickel disulfide (Ni3S2, heazlewoodite). Thus, the electrode is formed by a Ni3S2/Ni3N/Ni@NVCN architecture with a unique broccoli-like morphology. Electrochemical measurements show that these hybrid binder-free electrodes exhibit one of the best electrochemical performances compared to the other reported Ni3S2-based electrodes, evidencing an ultra-high specific capacity (856.3 C g(-1) at 3 A g(-1)), outstanding rate capability (77.2% retention at 13 A g(-1)), and excellent cycling stability (83% retention after 4000 cycles at 13 A g(-1)). The remarkable electrochemical performance of the binder-free Ni3S2/Ni3N/Ni@ NVCN electrodes is a significant step forward, improving rate capability and capacity for redox-based supercapacitor applications.

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