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Issue 7, 2012
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Exploration of the active center structure of nitrogen-doped graphene-based catalysts for oxygen reduction reaction

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Abstract

We present two different ways to fabricate nitrogen-doped graphene (N-graphene) and demonstrate its use as a metal-free catalyst to study the catalytic active center for the oxygen reduction reaction (ORR). N-graphene was produced by annealing of graphene oxide (G-O) under ammonia or by annealing of a N-containing polymer/reduced graphene oxide (RG-O) composite (polyaniline/RG-O or polypyrrole/RG-O). The effects of the N precursors and annealing temperature on the performance of the catalyst were investigated. The bonding state of the N atom was found to have a significant effect on the selectivity and catalytic activity for ORR. Annealing of G-O with ammonia preferentially formed graphitic N and pyridinic N centers, while annealing of polyaniline/RG-O and polypyrrole/RG-O tended to generate pyridinic and pyrrolic N moieties, respectively. Most importantly, the electrocatalytic activity of the catalyst was found to be dependent on the graphitic N content which determined the limiting current density, while the pyridinic N content improved the onset potential for ORR. However, the total N content in the graphene-based non-precious metal catalyst does not play an important role in the ORR process.

Graphical abstract: Exploration of the active center structure of nitrogen-doped graphene-based catalysts for oxygen reduction reaction

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Supplementary files

Article information


Submitted
30 Mar 2012
Accepted
25 Apr 2012
First published
26 Apr 2012

Energy Environ. Sci., 2012,5, 7936-7942
Article type
Paper

Exploration of the active center structure of nitrogen-doped graphene-based catalysts for oxygen reduction reaction

L. Lai, J. R. Potts, D. Zhan, L. Wang, C. K. Poh, C. Tang, H. Gong, Z. Shen, J. Lin and R. S. Ruoff, Energy Environ. Sci., 2012, 5, 7936
DOI: 10.1039/C2EE21802J

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