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Issue 42, 2016
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In situ formation of nitrogen-doped carbon nanoparticles on hollow carbon spheres as efficient oxygen reduction electrocatalysts

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Abstract

In situ formation of nitrogen-doped carbon nanoparticles on hollow carbon spheres (NHCSs) were successfully realised via a simple, scalable emulsion polymerization route using melamine as the nitrogen precursor, followed by thermal treatment at 1000 °C in N2. All NHCSs show large BET specific surface areas (648.2–837.7 cm2 g−1) and pore volumes (0.91–1.16 cm3 g−1), evidently superior to N-free hollow carbon spheres (HCSs) (524.3 cm2 g−1 and 0.48 cm3 g−1, respectively). This unique nanocomposite has hierarchical micro-/mesoporosity (1.9 nm and 16.2–19.0 nm). The X-ray photoelectron spectroscopy (XPS) measurements indicate the successful introduction of N atoms into the carbon framework and that the N-doping level can be controlled by changing the amount of melamine. The N-doping by adding melamine during the hydrothermal process not only affects the morphologies and porosities of the final samples, but also improves the electrocatalytic activity compared to N-free HCSs. NHCS-2, prepared with the molar melamine/hexamethylentetramine ratio of 1, showed the best electrocatalytic activity for the oxygen reduction reaction (ORR) in terms of onset potential, half-wave potential and limit current density. The NHCS-2 exhibited not only excellent activity with a mainly four-electron reaction pathway, but also superior long-term durability and methanol tolerance to that of commercial Pt/C in alkaline solution. The excellent electrocatalytic activity of the NHCS-2 is mainly due to its high relative content of pyridinic- and graphitic-N groups as well as unique hierarchical micro-/mesoporosity and a large specific surface area, advantageous for mass transfer and thus improving the electrocatalytic activity.

Graphical abstract: In situ formation of nitrogen-doped carbon nanoparticles on hollow carbon spheres as efficient oxygen reduction electrocatalysts

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Publication details

The article was received on 24 Aug 2016, accepted on 29 Sep 2016 and first published on 30 Sep 2016


Article type: Paper
DOI: 10.1039/C6NR06716F
Citation: Nanoscale, 2016,8, 18134-18142
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    In situ formation of nitrogen-doped carbon nanoparticles on hollow carbon spheres as efficient oxygen reduction electrocatalysts

    T. Zhou, Y. Zhou, R. Ma, Z. Zhou, G. Liu, Q. Liu, Y. Zhu and J. Wang, Nanoscale, 2016, 8, 18134
    DOI: 10.1039/C6NR06716F

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