High oxygen reduction activity of few-walled carbon nanotubes with low nitrogen content

• Few-walled carbon nanotubes (FWCNTs) are synthesized by a CVD method.
• N-FWCNTs are obtained by treatment with polyaniline and pyrolysis at high temperature.
• N-FWCNTs with only ∼0.5 at.% show high activity for oxygen reduction reaction (ORR).
• ORR activity comparable to Pt-C is observed both in electrochemical cell and alkaline fuel cell.

Nitrogen-containing few-walled carbon nanotubes (N-FWCNTs) with very low nitrogen content (0.56 at.%) were obtained by a process involving the coating of acid functionalized FWCNTs with polyaniline (PANI) followed by pyrolysis at high temperatures. The resulting N-FWCNTs exhibited a remarkable electrocatalytic activity for the oxygen reduction reaction (ORR), despite significantly lower nitrogen content than previously reported in literature. The N-FWCNTs performed on par or better than Pt-C in the cathode of an alkaline direct methanol fuel cell, corroborating the ORR activity observed in the electrochemical cell and exhibiting a higher methanol tolerance. Interestingly, N-FWCNTs showed a high activity for the hydrogen evolution reaction and for the hydrogen peroxide decomposition, suggesting that the active sites involved in ORR can simultaneously catalyze other reactions. This unprecedentedly high activity for such a low N-content can be explained by the exceptional accessibility for the catalytic sites located in open and porous N-doped layer surrounding the FWCNT core, along with the minimization of inactive inner volume and mass compared to larger nitrogen doped multiwalled tubes.

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