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Effect of Electrochemical Reduction of Ruthenium Black Cathode Catalyst on the Performance of Polymer Electrolyte Membrane Fuel Cells

캐소드 루테늄 촉매의 전기화학적 환원 처리가 고분자 전해질 연료전지 성능에 미치는 영향

  • Choi, Jong-Ho (Dept. of New and Renewable Energy, Kyungil University)
  • 최종호 (경일대학교 신재생에너지학과)
  • Received : 2011.05.20
  • Accepted : 2011.05.27
  • Published : 2011.05.31

Abstract

Ru black was used for cathode catalyst in polymer electrolyte membrane fuel cell which showed low performance at the initial test. However, it was observed that the performance of Ru black cathode was dramatically enhanced after certain kind of experiment compared with initial one. It might be due to an electrochemical treatment in which a voltage was applied to the Ru cathode for constant period time. When a constant potential of 0.1 V was applied to Ru cathode for 30 min, the fuel cell performance of Ru cathode showed the best results. In order to investigate the effect of electrochemical treatment on the performance enhancement, the characteristics of electrochemically treated Ru black was compared with that of Ru black which was reduced under $H_2$ atmosphere. From XRD results, it was turned out that Ru black was not completely converted to metallic Ru by electrochemical treatment, but it is sufficient to be one of reasons for the performance enhancement. According to the results of CO stripping voltammetry, it was observed that some Ru was removed from Ru electrode by electrochemical treatment which might have a bad effect on the fuel cell performance. The removal of some Ru from as-received Ru black by electrochemical treatment is also another reason for the enhancement of fuel cell performance.

Acknowledgement

Supported by : 경일대학교

References

  1. S. Arico, S. Srinivasan, and V. Antonucci. 'DMFCs: From Fundamental Aspects to Technology Development' Fuel Cells, 1, 133 (2001). https://doi.org/10.1002/1615-6854(200107)1:2<133::AID-FUCE133>3.0.CO;2-5
  2. K. Kordesch and G. Simader, "Fuel Cells and their Applications" Wiley-VCH, Weinheim (1996).
  3. S. Wasmus and A. Kuver, 'Methanol oxidation and direct methanol fuel cells: a selective review' J. Electroanal. Chem., 461, 14 (1999). https://doi.org/10.1016/S0022-0728(98)00197-1
  4. M. P. Hogarth and G. A. Hards, 'Direct Methanol Fuel Cells : Technological Advances and Further requirements' Plat. Met. Rev., 40, 150 (1996).
  5. D. Chu and S. Gilman, 'The Influence of Methanol on $O_2$ Electroreduction at a Rotating Pt Disk Electrode in Acid Electrolyte' J. Electrochem. Soc., 141, 1770 (1994). https://doi.org/10.1149/1.2055002
  6. P. S. Kauranen and E. Skou, 'Mixed methanol oxidation/ oxygen reduction currents on a carbon supported Pt catalyst' J. Electroanal. Chem., 408, 189 (1996). https://doi.org/10.1016/0022-0728(96)04515-9
  7. S. C. Thomas, X. Ren, S. Gottesfeld, and P. Zelenay, 'Direct methanol fuel cells: progress in cell performance and cathode research' Electrochim. Acta, 47, 3741 (2002). https://doi.org/10.1016/S0013-4686(02)00344-4
  8. B. Wang, 'Recent development of non-platinum catalysts for oxygen reduction reaction' J. Power Sources, 152, 1 (2005). https://doi.org/10.1016/j.jpowsour.2005.05.098
  9. L. Zhang, J. Zhang, D. P. Wilkinson, and H. Wang, 'Progress in preparation of non-noble electrocatalysts for PEM fuel cell reactions' J. Power Sources, 156, 171 (2006). https://doi.org/10.1016/j.jpowsour.2005.05.069
  10. A. K. Shukla, R. K. Raman, and K. Scott, 'Advances in Mixed-Reactant Fuel Cells' Fuel Cells, 5, 436 (2005). https://doi.org/10.1002/fuce.200400075
  11. S. C. Barton, T. Pattern, E. Wang, T. F. Fuller, and A. C. West, 'Mixed-reactant, strip-cell direct methanol fuel cells' J. Power Sources, 96, 329 (2001). https://doi.org/10.1016/S0378-7753(00)00663-7
  12. R. W. Reeve, P. A. Christensen, A. J. Dickinson, A. Hamnett, and K. Scott, 'Methanol-tolerant oxygen reduction catalysts based on transition metal sulfides and their application to the study of methanol permeation' Electrochim. Acta, 45, 4237 (2000). https://doi.org/10.1016/S0013-4686(00)00556-9
  13. K. -W. Park, Y. -M. Kim, B. -K. Kwon, J. -H. Choi, I. -S. Park, and Y. -E. Sung, 'Characterization of Methanol Crossover through Nafion Membranes by Direct Cell Performance Measurement' J. Kor. Electrochem. Soc., 5, 226 (2002). https://doi.org/10.5229/JKES.2002.5.4.226
  14. M. Hayashi, H. Uemura, K. Shimanoe, N. Miura, and N. Yamazoe, 'Reverse Micelle Assisted Dispersion of Lanthanum Manganite on Carbon Support for Oxygen Reduction Cathode' J. Electrochem. Soc., 151, A158 (2004). https://doi.org/10.1149/1.1633266
  15. R. Bashyam, P. Zelenay, 'A class of non-precious metal composite catalysts for fuel cells' Nature, 443, 63 (2006). https://doi.org/10.1038/nature05118
  16. N. AlonsoVante, P. Bogdanoff, and H. Tributsch, 'On the Origin of the Selectivity of Oxygen Reduction of Ruthenium-Containing Electrocatalysts in Methanol-Containing Electrolyte' J. Cat, 190, 240 (2000). https://doi.org/10.1006/jcat.1999.2728
  17. T. J. Schmidt, U. A. Paulus, and H. A. Gasteiger, N. Alonso-Vante, R. J. Behm, 'Oxygen Reduction on $Ru_{1.92}Mo_{0.08}SeO_4$, Ru/Carbon, and Pt/Carbon in Pure and Methanol-Containing Electrolytes' J. Electrochem. Soc., 147, 2620 (2000). https://doi.org/10.1149/1.1393579
  18. M. Lefevre, J. P. Dodelet, and P. Bertrand, '$O_2$ 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, 11238 (2000). https://doi.org/10.1021/jp002444n
  19. M. Johnston, J.-H. Choi, P. K. Babu, A. Wieckowski, and P. Zelenay, 'Performance and Durability of Chalcogen-Modified Ruthenium Catalysts for Oxygen Reduction: Hydrogen-Air MEA and RRDE Studies' ECS Trans., 6, 117 (2008). https://doi.org/10.1149/1.2943230
  20. K. -H. Choi, K. -S. Lee, T. -Y Jeon, H. -Y. Park, N. Jung, Y. -H. Chung, and Y. -E. Sung, 'High Alloying Degree of Carbon Supported Pt-Ru Alloy Nanoparticles Applying Anhydrous Ethanol as a Solvent' J. Electrochem. Sci. Tech., 1, 19 (2010). https://doi.org/10.5229/JECST.2010.1.1.019
  21. P. Piela, C. Eikes, E. Brosha, F. Garzon, and P. Zelenay, 'Ruthenium Crossover in Direct Methanol Fuel Cell with Pt-Ru Black Anode' J. Electrochem. Soc., 151, A2053 (2004). https://doi.org/10.1149/1.1814472
  22. C. M. Johnston and J. -H. Choi, Yu Seung Kim, P. Zelenay, 'Towards Understanding Ruthenium Crossover Effects: Oxygen Reduction Reaction on Ru-modified Platinum Surfaces' Abstract 1122, 209th Meeting of Electrochemical Society, Denver, CO, May 7-11 (2006).
  23. K. -A. Starz, K. Ruth, P. Biberbach, and R. Mclntoch, 'Process for preparing an anode catalyst for fuel cells and the anode catalyst prepared therewith' US Patent 6,797,667 (2004).
  24. K. Hiroshima, T. Asaoka, Y. Ohya, T. Noritake, H. Kato, and T. Nagami, 'Electrode catalyst for fuel cell and process for producing the same' US Patent 6,911,278 (2005).
  25. Y. S. Kim, J. -H. Choi, and P. Zelenay, 'Method of improving fuel cell performance by removing at least one metal oxide contaminant from a fuel cell electrode' US Patent 7,575,824 (2009).
  26. J. -H. Choi, Y. S. Kim, R. Bashyam, and P. Zelenay, 'Oxygen Reduction Electrocatalysis at Chalcogen-modified Ruthenium Cathodes' ECS Trans., 1, 437 (2006).
  27. H. A. Gasteiger, N. Markoviæ, P. N. Ross, and E. J. Cairns Jr., 'Carbon monoxide electrooxidation on well-characterized platinum-ruthenium alloys' J. Phys. Chem., 98, 617 (1994). https://doi.org/10.1021/j100053a042
  28. H. N. Dinh, X. Ren, F. Garzon, P. Zelenay, and S. Gottesfeld, 'Electrocatalysis in direct methanol fuel cells: in-situ probing of PtRu anode catalyst surfaces' J. Electroanal. Chem., 491, 222 (2000). https://doi.org/10.1016/S0022-0728(00)00271-0

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