Physicochemical and electrochemical properties of the carbon materials containing nitrogen and cobalt derived from acetonitrile and Co–Al layered double hydroxides
Two sets of the carbon materials containing nitrogen and cobalt were prepared by simultaneous carbonization of CH3CN and decomposition of Co–Al layered double hydroxides (LDHs) (of Co/Al atomic ratios equal to 2 or 3) at 600, 700 and 800 °C followed by treatment with HCl. The physicochemical features of the samples were characterized by means of XRD, TG, EA, XPS, XRF, FT-IR, SEM, Raman spectroscopy and nitrogen sorption. All of the composites were active in oxygen reduction reaction (ORR) in alkaline medium. Their ORR behaviour was determined by the contribution of structural defects and N-doping in graphitic lattice. The beneficial effect of metallic cobalt encapsulated inside the N-CNTs on the ORR performance was also taken into consideration. The studies showed that the likelihood of the existence of Co–N–C species and their participation in ORR seemed to be suppressed by the formation of CoAl2O4. The samples prepared at 600 and 700 °C appeared to be more active in ORR than that obtained at 800 °C. The number of electrons involved in ORR (2.89, 2.82 and 2.77) decreased with increasing synthesis temperature for the samples prepared with LDHs of Co/Al = 2 as a consequence of lowering concentration of nitrogen (3.2, 2.4 and 1.5 wt%), in particular diminishing contribution of pyridinic nitrogen, and decreasing exposure of graphitic edges (ID1/IG ~ 2.6, 2.0 and 1.0). The ORR performance of the samples prepared with LDHs of Co/Al = 3 is comparable to that of the corresponding samples prepared with LDHs of Co/Al = 2.
This research received funding from National Science Centre in Poland within decision number DEC-2013/11/B/ST5/01417. This work was also financially supported by National Science Centre in Poland within the research project 2699/B/T02/2009/36 for the years 2009–2012. Raman spectra were recorded by means of the equipment purchased thanks to the financial support of the European Regional Development Fund in the framework of the Polish Innovation Economy Operational Program (Contract No. POIG.02.01.00-12-023/08). Prof. Alicja Drelinkiewicz and Prof. Paweł Nowak both from Jerzy Haber Institute of Catalysis and Surface Chemistry Polish Academy of Sciences are gratefully acknowledged for fruitful discussions.
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Conflicts of interest
The authors declare that they have no conflict of interest.
- 15.Faubert G, Lalande G, Côté R, Guay D, Dodelet JP, Weng LT, Bertrand P, Dénès G (1996) Heat-treated iron and cobalt tetraphenylporphyrins adsorbed on carbon black: physical characterization and catalytic properties of these materials for the reduction of oxygen in polymer electrolyte fuel cells. Electrochim Acta 41:1689–1701CrossRefGoogle Scholar
- 40.Fu S, Zhu C, Li H, Du D, Lin Y (2015) One-step synthesis of cobalt and nitrogen co-doped carbon nanotubes and their catalytic activity for the oxygen reduction reaction. J Mater Chem A 3(12718):12722Google Scholar
- 41.Mamtani K, Singh D, Tian J, Millet MJ-M, Miller JT, Co AC, Ozkan US (2016) Evolution of N-coordinated iron–carbon (FeNC) catalysts and their oxygen reduction (ORR) performance in acidic media at various stages of catalyst synthesis: an attempt at benchmarking. Catal Lett 146:1749–1770CrossRefGoogle Scholar
- 49.Rouquerol F, Rouquerol J, Sing K (1999) Adsorption by powders and porous solids, principles, methodology and applications. Academic Press, LondonGoogle Scholar
- 50.Wei G, Wainright JS, Savinell RF (2000) Catalytic activity for oxygen reduction reaction of catalysts consisting of carbon, nitrogen and cobalt. J New Mater Electrochem Syst 3:121–129Google Scholar
- 65.Deraz NM (2013) Formation and characterization of cobalt aluminate nano-particles. Int J Electrochem Sci 8:4036–4046Google Scholar
- 68.Niwa H, Kobayashi M, Horiba K, Harada Y, Oshima M, Terakura K, Ikeda T, Koshigoe Y, Ozaki J, Miyata S, Ueda S, Yamashita Y, Yoshikawa H, Kobayashi K (2011) X-ray photoemission spectroscopy analysis of N-containing carbon-based cathode catalysts for polymer electrolyte fuel cells. J Power Sources 196:1006–1011CrossRefGoogle Scholar
- 73.Bagotsky VS (2006) Fundamentals of electrochemistry. Wiley, HobokenGoogle Scholar