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BCN Graphene as Efficient Metal-Free Electrocatalyst for the Oxygen Reduction Reaction

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      Preparation of Graphitic Oxide

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        Nitrogen-doped carbon nanotube arrays with high electrocatalytic activity for oxygen reduction.

        The large-scale practical application of fuel cells will be difficult to realize if the expensive platinum-based electrocatalysts for oxygen reduction reactions (ORRs) cannot be replaced by other efficient, low-cost, and stable electrodes. Here, we report that vertically aligned nitrogen-containing carbon nanotubes (VA-NCNTs) can act as a metal-free electrode with a much better electrocatalytic activity, long-term operation stability, and tolerance to crossover effect than platinum for oxygen reduction in alkaline fuel cells. In air-saturated 0.1 molar potassium hydroxide, we observed a steady-state output potential of -80 millivolts and a current density of 4.1 milliamps per square centimeter at -0.22 volts, compared with -85 millivolts and 1.1 milliamps per square centimeter at -0.20 volts for a platinum-carbon electrode. The incorporation of electron-accepting nitrogen atoms in the conjugated nanotube carbon plane appears to impart a relatively high positive charge density on adjacent carbon atoms. This effect, coupled with aligning the NCNTs, provides a four-electron pathway for the ORR on VA-NCNTs with a superb performance.
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          Nitrogen-doped graphene as efficient metal-free electrocatalyst for oxygen reduction in fuel cells.

          Nitrogen-doped graphene (N-graphene) was synthesized by chemical vapor deposition of methane in the presence of ammonia. The resultant N-graphene was demonstrated to act as a metal-free electrode with a much better electrocatalytic activity, long-term operation stability, and tolerance to crossover effect than platinum for oxygen reduction via a four-electron pathway in alkaline fuel cells. To the best of our knowledge, this is the first report on the use of graphene and its derivatives as metal-free catalysts for oxygen reduction. The important role of N-doping to oxygen reduction reaction (ORR) can be applied to various carbon materials for the development of other metal-free efficient ORR catalysts for fuel cell applications, even new catalytic materials for applications beyond fuel cells.
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            Author and article information

            Journal
            Angewandte Chemie International Edition
            Angew. Chem. Int. Ed.
            Wiley-Blackwell
            14337851
            April 23 2012
            April 23 2012
            : 51
            : 17
            : 4209-4212
            10.1002/anie.201109257
            © 2012

            http://doi.wiley.com/10.1002/tdm_license_1.1

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