Efficiency and long-term durability of a nitrogen-doped single-walled carbon nanotube electrocatalyst synthesized by defluorination-assisted nanotube-substitution for oxygen reduction reaction

Koji Yokoyama, Shun Yokoyama, Kazutaka Hirano, Shinji Hashiguchi, Kenichi Motomiya, Hiromichi Ohta, Hideyuki Takahashi, Kazuyuki Tohji, Yoshinori Sato

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15 Citations (Scopus)

Abstract

Nitrogen-doped carbon nanomaterials are known to be excellent electrocatalysts for the oxygen reduction reaction (ORR) in polymer electrolyte fuel cells. In this study, we used a new and simple post-doping synthesis method to prepare nitrogen-doped single-walled carbon nanotubes (SWCNTs) by reacting fluorinated SWCNTs with ammonia gas at 300-600 °C. The structure and morphology of the Nx°C-doped SWCNTs (x: reaction temperature) synthesized by the defluorination-assisted nanotube-substitution reaction were characterized. Their levels of nitrogen doping (1.38-3.04 at%) are fairly high, with enriched pyridinic- and pyrrolic-nitrogen species. Their electrochemical catalytic activity for ORR in 0.5 M H2SO4 was evaluated by cyclic voltammetry and linear sweep voltammetry, and their catalytic durability was assessed in load-potential cycle tests. For the Nx°C-doped SWCNTs, the peak and the onset potential (Epeak and Eonset, respectively) shifted towards the positive and the current density (j@E1/2) at the half-wave potential (E1/2) increased with increasing reaction temperature. The Eonset values of N500°C- and N600°C-doped SWCNTs were +0.51 V while that of the non-fluorinated hc-SWCNTs was +0.16 V. The number of electrons transferred per oxygen molecule (n) in ORR was determined to be 2.32-3.64 at the potential of -0.3 V. The ORR catalytic activity was evaluated comprehensively through the measured parameters Epeak, Eonset, n, and j@E1/2. The N500°C-doped SWCNTs possessed the highest ORR catalytic activity. After 11000 cycles in the load-potential test, its current density remained at 93% of the initial value, indicating better durability than platinum nanoparticles supported on carbon black (Pt-C).

Original languageEnglish
Pages (from-to)9184-9195
Number of pages12
JournalJournal of Materials Chemistry A
Volume4
Issue number23
DOIs
Publication statusPublished - 2016 Jan 1

ASJC Scopus subject areas

  • Chemistry(all)
  • Renewable Energy, Sustainability and the Environment
  • Materials Science(all)

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