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On the electrocatalytic activity of nitrogen-doped reduced graphene Oxide: Does the nature of nitrogen really control the activity towards oxygen reduction?

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Abstract

Synthesis of metal-free electrocatalyst for the cathodic reduction of oxygen is of great interest for fuel cell and metal-air battery applications. The heteroatom-doped graphene/reduced graphene oxide (rGO) is very promising and the nitrogen-doped rGO (N-rGO) is emerging as a new inexpensive electrocatalyst for oxygen reduction reaction (ORR). Herein, we describe the effect of the chemical nature and amount of nitrogen in N-rGO towards ORR in acidic solution. Four different samples of N-rGO with different nitrogen content were synthesized by simple chemical route. The chemical nature and nitrogen content were analyzed with X-ray photoelectron spectroscopic measurements. The electrocatalytic performance of the catalyst was examined by cyclic and hydrodynamic voltammetric studies. All the N-rGO samples favor 4-electron pathway for the reduction of oxygen in acidic solution. The onset potential and kinetic current density depends on the nature of the doped nitrogen. It is demonstrated that the chemical nature and the amount of nitrogen actually control the ORR activity. The N-rGO which contains a large amount of pyridinic nitrogen with N/C ratio of 0.074 has high catalytic activity. The carbon bonded to pyridinic nitrogen could be a possible catalytic site in ORR. Our studies suggest that the graphitic nitrogen does not significantly influence the electrocatalytic activity of N-rGO.

It is demonstrated that the chemical nature and the amount of nitrogen atom substitutionally doped onto the carbon framework of the N-doped reduced graphene oxide controls the electrocatalytic performance towards oxygen reduction reaction.

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Acknowledgements

This work was financially supported by Department of Science and Technology, New Delhi. We thank Department of Physics, Indian Institute of Technology Kharagpur for XPS measurements.

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Authors and Affiliations

  1. Functional Materials and Electrochemistry Laboratory, Department of Chemistry, Indian Institute of Technology Kharagpur, Kharagpur, 721 302, India

    SOURAV BAG & C RETNA RAJ

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  1. SOURAV BAG
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Correspondence to C RETNA RAJ.

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Supplementary Information (SI)

Experimental details, elemental mapping, XPS survey scan, deconvoluted C1s spectra, and cyclic voltammogram are given as supplementary information. For details see www.ias.ac.in/chemsci.

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BAG, S., RAJ, C.R. On the electrocatalytic activity of nitrogen-doped reduced graphene Oxide: Does the nature of nitrogen really control the activity towards oxygen reduction?. J Chem Sci 128, 339–347 (2016). https://doi.org/10.1007/s12039-016-1034-z

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  • DOI: https://doi.org/10.1007/s12039-016-1034-z

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