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Electrochemical and oxygen reduction properties of pristine and nitrogen-doped few layered graphene nanoflakes (FLGs)

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Abstract

Vertically aligned few layered graphene (FLGs) nanoflakes were synthesized by microwave plasma deposition for various time durations ranging from 30 to 600 s to yield graphene films of varying morphology, microstructure and areal/edge density. Their intrinsic electrochemical properties were explored using Fe(CN)6 3−/4− and Ru(NH3)6 3+/2+ redox species. All the FLG electrodes demonstrate fast electron transfer kinetics with near ideal ΔEp values of 60–65 mV. Using a relationship between electron transfer rate and edge plane density, an estimation of the edge plane density was carried out which revealed a moderation of edge plane density with increase in growth time. The pristine FLGs also possess excellent electrocatalytic activity towards oxygen reduction reaction (ORR) in alkaline solutions. This ORR activity can be further enhanced by exposing the pristine FLGs to nitrogen electron cyclotron resonance plasma. The metal free N-doped FLGs exhibit much higher electrocatalytic activity towards ORR than pristine FLGs with higher durability and selectivity than Pt-based catalysts. The excellent electrochemical performance of N-doped FLGs is explained in terms of enhanced edge plane exposure, high content of pyridinic nitrogen and an increase in the electronic density of states.

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Notes

  1. There is a lot of discrepancy and disparity in the literature regarding the nomenclature used for carbon nanostructures like these such as few-layered graphene nanoflakes, multi-layered graphene petals and carbon nanowalls. Strictly speaking, graphene is a single sheet of sp2 hybridised carbon atoms; hence, the use of term few-layered graphene can be considered as slightly controversial. In the past, we have reported on the synthesis, growth mechanism and applications of these structures wherein they have been addressed as few-layered graphene nanoflakes. So, in order to maintain parity, we continue to call it as few-layered graphene nanoflakes.

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Author information

Author notes

  1. Navneet Soin

    Present address: Institute of Renewable Energy and Environmental Technologies (IREET), Knowledge Centre for Materials Chemistry (KCMC), University of Bolton, Bolton, BL3 5AB, UK

Authors and Affiliations

  1. Nanotechnology and Integrated Bioengineering Centre (NIBEC), University of Ulster at Jordanstown, Shore Road, Newtownabbey, BT37 0QB, UK

    Navneet Soin & James A. McLaughlin

  2. Department of Physics, School of Natural Sciences, Shiv Nadar University, Gautam Budh Nagar, 203207, Uttar Pradesh, India

    Susanta Sinha Roy

  3. School of Chemical Engineering, University of Birmingham, Edgbaston, Birmingham, B15 2TT, UK

    Surbhi Sharma

  4. Chemical and Materials Engineering Department, University of Alberta, Edmonton, AB, T6G 2V4, Canada

    Thomas Thundat

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  1. Navneet Soin
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  2. Susanta Sinha Roy
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  5. James A. McLaughlin
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Correspondence to Navneet Soin.

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Soin, N., Roy, S.S., Sharma, S. et al. Electrochemical and oxygen reduction properties of pristine and nitrogen-doped few layered graphene nanoflakes (FLGs). J Solid State Electrochem 17, 2139–2149 (2013). https://doi.org/10.1007/s10008-013-2073-8

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  • DOI: https://doi.org/10.1007/s10008-013-2073-8

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