Skip to main content
SpringerLink
Log in

Nitrogen-doped ordered porous carbon catalyst for oxygen reduction reaction in proton exchange membrane fuel cells

  • Original Paper
  • Published:
Journal of Solid State Electrochemistry Aims and scope Submit manuscript

Abstract

Three different N-doped ordered porous carbons (CNx) were produced by a nanocasting process using polyaniline as the carbon and nitrogen precursor. A pyrolysis treatment of iron chloride-impregnated CNx under nitrogen is used in the preparation of the carbon composite catalysts, and this is followed by posttreatments and optimization of the iron loading and the pore size. Exploration of the catalytic activity of the CNx products for catalyzing the oxygen reduction reaction (ORR) using rotating disk electrode measurements and single-cell tests shows that the onset potential for ORR of the most effective catalyst in 0.5 M H2SO4 is as high as 0.9 V vs. the normal hydrogen electrode. A proton exchange membrane fuel cell constructed with the catalyst exhibits a current density as high as 0.52 A cm−2 at 0.6 V with 2 atm back pressure using a cathode catalyst loading of 6 mg cm−2. The average pore diameters of synthesized CNx-12, CNx-15, and CNx-16 are 0.7, 4.3, and 14 nm, respectively. It is observed that the pore size and specific surface area are an important factor for increased catalyst activity. The pore size of the most effective catalysts is found to be 4.3 nm.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Subscribe and save

Springer+ Basic
$34.99 /Month
  • Get 10 units per month
  • Download Article/Chapter or eBook
  • 1 Unit = 1 Article or 1 Chapter
  • Cancel anytime
Subscribe now

Buy Now

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7
Fig. 8
Fig. 9

Similar content being viewed by others

References

  1. Jasinski R (1964) A New Fuel Cell Cathode Catalyst. Nature 201:1212–1213

    Article  CAS  Google Scholar 

  2. Alt H, Binder H, Sandstede G (1973) Mechanism of the electrocatalytic reduction of oxygen on metal chelates. J Catal 28:8–19

    Article  CAS  Google Scholar 

  3. Wiesener K (1986) N4-chelates as electrocatalyst for cathodic oxygen reduction. Electrochim Acta 31:1073–1078

    Article  CAS  Google Scholar 

  4. Schulenburg H, Stankov S, Schunemann V, Radnik J, Dorbandt I, Fiechter S et al (2003) Catalysts for the oxygen reduction from heat-treated iron(III) tetramethoxyphenylporphyrin chloride: Structure and stability of active sites. J Phys Chem B 107(34):9034–9041

    Article  CAS  Google Scholar 

  5. Maldonado S, Stevenson KJ (2004) Direct preparation of carbon nanofiber electrodes via pyrolysis of Iron(II) phthalocyanine: electrocatalytic aspects for oxygen reduction. J Phys Chem B 108(31):11375–11383

    Article  CAS  Google Scholar 

  6. Nallathambi V, Lee JW, Kumaraguru SP, Wu G, Popov BN (2008) Development of high performance carbon composite catalyst for oxygen reduction reaction in PEM Proton Exchange Membrane fuel cells. J Power Sources 183:34–42

    Article  CAS  Google Scholar 

  7. Wood TE, Tan ZS, Schmoeckel AK, O’Neill D, Atanasoski R (2008) Non-precious metal oxygen reduction catalyst for PEM fuel cells based on nitroaniline precursor. J Power Sources 178:510–516

    Article  CAS  Google Scholar 

  8. Wu G, Chen Z, Artyushkova K, Garzon FH, Zelenay P (2008) Polyaniline-derived non-precious catalyst for the polymer electrolyte fuel cell cathode. ECS Trans 16(2):159–170

    Article  CAS  Google Scholar 

  9. Matter PH, Zhang L, Ozkan US (2006) The role of nanostructure in nitrogen-containing carbon catalysts for the oxygen reduction reaction. J Catal 239:83–96

    Article  CAS  Google Scholar 

  10. Lefevre M, Dodelet JP, Bertrand P (2000) 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 104(47):11238–11247

    Article  CAS  Google Scholar 

  11. Koslowski UI, Abs-Wurmbach I, Fiechter S, Bogdanoff P (2008) Nature of the Catalytic Centers of Porphyrin-Based Electrocatalysts for the ORR: A Correlation of Kinetic Current Density with the Site Density of Fe−N4 Centers. J Phys Chem C 112(39):15356–15366

    Article  CAS  Google Scholar 

  12. Kothandaraman R, Nallathambi V, Artyushkova K, Barton SC (2009) Non-precious oxygen reduction catalysts prepared by high-pressure pyrolysis for low-temperature fuel cells. Appl Catal B 92:209–216

    Article  CAS  Google Scholar 

  13. Yeager E (1984) Electrocatalysts for O2 reduction. Electrochim Acta 29(11):1527–1537

    Article  CAS  Google Scholar 

  14. Gouerec P, Savy M, Riga J (1997) Oxygen reduction in acidic media catalyzed by pyrolyzed cobalt macrocycles dispersed on an active carbon: The importance of the content of oxygen surface groups on the evolution of the chelate structure during the heat treatment. Electrochim Acta 43:743–753

    Article  Google Scholar 

  15. Kundu S, Nagaiah TC, Xia W, Wang Y, Dommele SV, Bitter JH et al (2009) Electrocatalytic activity and stability of nitrogen containing carbon nanotubes for oxygen reduction reactions. J Phys Chem C 113:14302–14310

    Article  CAS  Google Scholar 

  16. Gasteiger HA, Markovic NM (2009) Just a dream – or future reality? Science 324:48–49

    Article  CAS  Google Scholar 

  17. Liu G, Li X, Ganesan P, Popov BN (2009) Development of non-precious metal oxygen reduction catalysts for PEM fuel cells based on N-doped ordered porous carbon. Appl Catal B Environ 93:156–165

    Article  CAS  Google Scholar 

  18. Yiu HHP, Keane MA, Lethbridge ZAD, Lees MR, El Haj AJ, Dobson J (2008) Synthesis of novel magnetic iron metal-silica (Fe-SBA-15) and magnetite-silica (Fe3O4-SBA-15) nanocomposites with a high iron content using temperature-programed reduction. Nanotechnology 19:255606–255613

    Article  CAS  Google Scholar 

  19. Mesa M, Sierra L, Guth GL (2008) Contribution to the study of the formation mechanism of mesoporous SBA-15 and SBA-16 type silica particles in aqueous acid solutions. Micropor Mesopor Mater 112:338–350

    Article  CAS  Google Scholar 

  20. Pel JR, Kapteijn F, Moulijn JA, Zhu Q, Thomas KM (1995) Evolution of nitrogen functionalities in carbonaceous materials during pyrolysis. Carbon 33:1641–1653

    Article  Google Scholar 

  21. Torres J, Perry CC, Bransfield SJ, Fairbrother DH (2003) Low-Temperature Oxidation of Nitrided Iron Surfaces. J Phys Chem B 107:5558–5567

    Article  CAS  Google Scholar 

  22. Okada T, Katou K, Hirose T, Yuasa M, Sekine I (1999) Oxygen Reduction on Pyrolytic Graphite Electrodes Modified with Electropolymerized Cobalt Salen Compounds. J Electrochem Soc 146(7):2562–2568

    Google Scholar 

  23. Ikeda T, Boero M, Huang S-F, Terakura K, Oshima M, Ozaki J-I (2008) Carbon Alloy Catalysts: Active Sites for Oxygen Reduction Reaction. J Phys Chem C 112:14706–14709

    Google Scholar 

  24. Gong K, Chakrabarti S, Dai L (2008) Electrochemistry at Carbon Nanotube Electrodes: Is the Nanotube Tip More Active Than the Sidewall? Angew Chem Int Ed 47:5446–5450

    Google Scholar 

Download references

Acknowledgments

This work was supported by the National Research Foundation of Korea Grant funded by the Korean Government (MEST: NRF-C1AAA001-2009-0092926).

Author information

Authors and Affiliations

  1. Department of Chemical and Biomolecular Engineering, Yonsei University, Seoul, South Korea

    Altansukh Dorjgotov, Jinhee Ok, YuKwon Jeon & Yong Gun Shul

  2. Institute for Materials Chemistry and Engineering, Kyushu University, Fukuoka, Japan

    Seong-Ho Yoon

Authors
  1. Altansukh Dorjgotov
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Jinhee Ok
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. YuKwon Jeon
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Seong-Ho Yoon
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Yong Gun Shul
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Yong Gun Shul.

Rights and permissions

Reprints and permissions

About this article

Cite this article

Dorjgotov, A., Ok, J., Jeon, Y. et al. Nitrogen-doped ordered porous carbon catalyst for oxygen reduction reaction in proton exchange membrane fuel cells. J Solid State Electrochem 17, 2567–2577 (2013). https://doi.org/10.1007/s10008-013-2135-y

Download citation

  • Received:

  • Revised:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10008-013-2135-y

Keywords

Search

Navigation