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The synthesis and characterization of a Co-N/C composite catalyst for the oxygen reduction reaction in acidic solution

  • Article
  • Physical Chemistry
  • Published:
Chinese Science Bulletin

Abstract

A non-precious metal Co-N/C catalyst for the oxygen reduction reaction (ORR) was synthesized by heating a mechanical mixture of cobalt chloride, urea and acetylene black under a nitrogen atmosphere. The catalyst was characterized by XRD and XPS. The electrocatalytic activity in the ORR was evaluated by linear sweep voltammetry in 0.5 mol L−1 H2SO4 solution. The results show that the Co-N/C catalyst aids the reduction of oxygen. The presence of elemental cobalt in the precursor allows nitrogen atoms to embed themselves in the graphite matrix to form pyridinic and graphitic type C-N structures as the ORR active sites. The effect of heat-treating temperature on the catalytic activity was also investigated. The results also show that the Co-N/C catalyst is most active when pyrolyzed at 600°C. The obtained Co-N/C catalyst loses some activity after initial exposure to the H2SO4 solution because of leaching, but is then stable for up to 20 h immersion. The catalyst is also stable when charged, which is supported by the cyclic voltammetry results.

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References

  1. Thomas S C, Ren X, Gottesfeld S, et al. Direct methanol fuel cells: Progress in cell performance and cathode research. Electrochim Acta, 2002, 47: 3741–3748

    Article  Google Scholar 

  2. Alexey S, Chan K. Review of non-platinum anode catalysts for DMFC and PEMFC application. Appl Catal B: Environ, 2009, 90: 313–320

    Article  Google Scholar 

  3. Yeager E. Electrocatalysts for O2 reduction. Electrochim Acta, 2002, 29: 1527–1537

    Article  Google Scholar 

  4. Nallathambi V, Lee J W, Kumaraguru S P, et al. Development of high performance carbon composite catalyst for oxygen reduction reaction in PEM Proton Exchange Membrane fuel cells. J Power Sources, 2008, 183: 34–42

    Article  Google Scholar 

  5. Gojkovic S L, Gupta S, Savinell R F. Heat-treated iron(III) tetrame-thoxyphenyl porphyrin chloride supported on high-area carbon as an electrocatalyst for oxygen reduction: Part III. Detection of hydrogen-peroxide during oxygen reduction. Electrochim Acta, 1999, 45: 889–897

    Article  Google Scholar 

  6. Ramya K, Dhathathreyan K S. Direct methanol fuel cells: Determination of fuel crossover in a polymer electrolyte membrane. J Electroanal Chem, 2003, 542: 109–115

    Article  Google Scholar 

  7. Jeon M K, Lee K R, Lee W S, et al. Investigation of Pt/WC/C catalyst for methanol electro-oxidation and oxygen electro-reduction. J Power Sources, 2008, 185: 927–931

    Article  Google Scholar 

  8. Jeyabharathi C, Venkateshkumar P, Mathiyarasu J, et al. Platinum-tin bimetallic nanoparticles for methanol tolerant oxygen-reduction activity. Electrochim Acta, 2008, 54: 448–454

    Article  Google Scholar 

  9. Antolini E, Lopes T, Gonzalez E R. An overview of platinum-based catalysts as methanol-resistant oxygen reduction materials for direct methanol fuel cells. J Alloys Compd, 2008, 461: 253–262

    Article  Google Scholar 

  10. Salvador-Pascual J J, Citalan-Cigarroa S, Solorza-Feria O. Kinetics of oxygen reduction reaction on nanosized Pd electrocatalyst in acid media. J Power Sources, 2007, 172: 229–234

    Article  Google Scholar 

  11. Fu Y, Wei Z D, Chen S G, et al. Synthesis of Pd/TiO2 nanotubes/Ti for oxygen reduction reaction in acidic solution. J Power Sources, 2009, 189: 982–987

    Article  Google Scholar 

  12. Kim J, Momm T, Osaka T. Synthesis of carbon-supported Pd-Sn catalyst by ultrasonic irradiation for oxygen reduction reaction. J Power Sources, 2009, 189: 909–915

    Article  Google Scholar 

  13. Tarasevich M R, Bogdanovskaya V A, Kuznetsova L N, et al. Development of platinum-free catalyst and catalyst with low platinum content for cathodic oxygen reduction in acidic electrolytes. J Appl Electrochem, 2007, 37: 1503–1513

    Article  Google Scholar 

  14. Jasinski R. A new fuel cell catlyst. Nature, 1964, 201: 1212–1213

    Article  Google Scholar 

  15. Zagal J H, Bedioui F, Dodelet J P. N4-Macrocyclic Metal Complexes. New York: Springer, 2006. 45

    Book  Google Scholar 

  16. Faubert G, Cote R, Guay D, et al. Iron catalysts prepared by high-temperature pyrolysis of tetraphenylporphyrins adsorbed on carbon black for oxygen reduction in polymer electrolyte fuel cells. Electrochim Acta, 1998, 43: 341–353

    Article  Google Scholar 

  17. Lefevre M, Dodelet J P. O2 reduction in PEM fuel cells: Activity and active site structural information for catalysts obtained by the pyrolysis at high temperature of Fe precursors. J Phys Chem B, 2000, 104: 11238–11247

    Article  Google Scholar 

  18. Lefevre M, Dodelet J P, Bertrand P. Molecular oxygen reduction in PEM fuel cells: Evidence for the simultaneous presence of two active sites in Fe-based catalysts. J Phys Chem B, 2002, 106: 8705–8713

    Article  Google Scholar 

  19. Schulenburg H, Stankov S, Schulnemann V, et al. Catalysts for the oxygen reduction from heat-treated iron(III) tetramethoxyphenylporphyrin chloride: Structure and stability of active sites. J Phys Chem B, 2003, 107: 9034–9041

    Article  Google Scholar 

  20. Niwa H, Horiba K, Harada Y, et al. X-ray absorption analysis of nitrogen contribution to oxygen reduction reaction in carbon alloy cathode catalysts for polymer electrolyte fuel cells. J Power Sources, 2009, 187: 93–97

    Article  Google Scholar 

  21. Wang P, Ma Z, Zhao Z, et al. Oxygen reduction on the electrocatalysts based on pyrolyzed non-noble metal/poly-o-phenylenediamine/carbon black composites: New insight into the active sites. J Electroanal Chem, 2007, 611: 87–95

    Article  Google Scholar 

  22. Matter P H, Wang E, Arias M, et al. Oxygen reduction reaction activity and surface properties of nanostructured nitrogen-containing carbon. J Mol Catal A: Chem, 2007, 264: 73–81

    Article  Google Scholar 

  23. Zhang H J, Yuan X, Wen W, et al. Electrochemical performance of a novel CoTETA/C catalyst for the oxygen reduction reaction. Electrochem Commun, 2009, 11: 206–208

    Article  Google Scholar 

  24. Matter P H, Zhang L, Ozkan U S. The role of nanostructure in nitrogen-containing carbon catalysts for the oxygen reduction reaction. J Catal, 2006, 239: 83–96

    Article  Google Scholar 

  25. Bezerra C W B, Zhang L, Lee K, et al. Novel carbon-supported Fe-N electrocatalysts synthesized through heat treatment of iron tripyridyl triazine complexes for the PEM fuel cell oxygen reduction reaction. Electrochim Acta, 2008, 53: 7703–7710

    Article  Google Scholar 

  26. Herranz J, Lefevre M, Larouche N, et al. Step-by-step synthesis of non-noble metal electrocatalysts for O2 reduction under proton exchange membrane fuel cell conditions. J Phys Chem C, 2007, 111: 19033–19042

    Article  Google Scholar 

  27. Charreteur F, Jaouen F, Ruggeri S, et al. Fe/N/C non-precious catalysts for PEM fuel cells: Influence of the structural parameters of pristine commercial carbon blacks on their activity for oxygen reduction. Electrochim Acta, 2008, 53: 2925–2938

    Article  Google Scholar 

  28. Bashyam R, Zelenay P. A class of non-precious metal composite catalysts for fuel cells. Nature, 2006, 443: 63–66

    Article  Google Scholar 

  29. Millan W M, Thompson T T, Arriaga L G, et al. Characterization of composite materials of electroconductive polymer and cobalt as electrocatalysts for the oxygen reduction reaction. Int J Hydrogen Energ, 2009, 34: 694–702

    Article  Google Scholar 

  30. Lee K, Zhang L, Lui H, et al. Oxygen reduction reaction (ORR) catalyzed by carbon-supported cobalt polypyrrole (Co-PPy/C) electrocatalysts. Electrochim Acta, 2009, 54: 4704–4711

    Article  Google Scholar 

  31. Garsuch A, Yang R, Bonakdarpour A, et al. The effect of boron doping into Co-C-N and Fe-C-N electrocatalysts on the oxygen reduction reaction. Electrochim Acta, 2008, 53: 2423–2429

    Article  Google Scholar 

  32. Yang R, Stevens K, Dahn J R. Investigation of activity of sputtered transition-metal (TM)-C-N (TM=V, Cr, Mn, Co, Ni) catalysts for oxygen reduction reaction. J Electrochem Soc, 2008, 155: B79–B91

    Article  Google Scholar 

  33. Lalande G, Cote R, Tamizhmani G, et al. Physical, chemnical and electrochemical characterization of heat-treated tetracarboxylic cobalt phthalocyanine adsorbed on carbon black as electrocatalyst for oxygen reduction in polymer electrolyte fuel cells. Electrochim Acta, 1995, 40: 2635–2646

    Article  Google Scholar 

  34. Maldonado S, Stevenson K J. Influence of nitrogen doping on oxygen reduction electrocatalysis at carbon nanofiber electrodes. J Phys Chem B, 2005, 109: 4707–4716

    Article  Google Scholar 

  35. Subramanian N P, Li X, Nallathambi V, et al. Nitrogen-modified carbon-based catalysts for oxygen reduction reaction in polymer electrolyte membrane fuel cells. J Power Sources, 2009, 188: 38–44

    Article  Google Scholar 

  36. Nallathambi V, Lee J W, Kumaraguru S P, et al. Development of high performance carbon composite catalyst for oxygen reduction reaction in PEM Proton Exchange Membrane fuel cells. J Power Sources, 2008, 183: 34–42

    Article  Google Scholar 

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Authors and Affiliations

  1. College of Chemistry and Chemical Engineering, Chongqing University, Chongqing, 400044, China

    YuJun Si, ChangGuo Chen, Wei Yin & Hui Cai

  2. College of Chemistry and Pharmaceutical Engineering, Sichuan University of Science and Engineering, Zigong, 643000, China

    YuJun Si

  3. College of Material Science and Engineering, Chongqing University, Chongqing, 400044, China

    YuJun Si & ChangGuo Chen

Authors
  1. YuJun Si
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  2. ChangGuo Chen
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  3. Wei Yin
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  4. Hui Cai
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Correspondence to YuJun Si or ChangGuo Chen.

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Si, Y., Chen, C., Yin, W. et al. The synthesis and characterization of a Co-N/C composite catalyst for the oxygen reduction reaction in acidic solution. Chin. Sci. Bull. 56, 1086–1091 (2011). https://doi.org/10.1007/s11434-011-4434-y

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  • DOI: https://doi.org/10.1007/s11434-011-4434-y

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