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Performance of ternary PtRuRh/C electrocatalyst with varying Pt:Ru:Rh ratio for methanol electro-oxidation

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Abstract

Highly dispersed ternary PtRuRh/C anode catalysts for direct methanol fuel cells were prepared with various contents and their electro-catalytic activities towards methanol oxidation at 25 °C and 60 °C were examined to investigate the influence of the catalyst composition. Electrocatalysts were prepared by a co-impregnation method using ethanolic solutions of metal precursors and carbon black followed by pyrolysis under reducing conditions. X-ray diffraction analysis revealed that the fcc peaks shifted to higher diffraction angles with increasing Rh content, indicating the alloying of Rh into the fcc structure. In terms of the mass specific current density, the activity towards methanol oxidation differed significantly depending on the catalysts composition and cell temperature. The catalyst prepared at a ratio of Pt:Ru:Rh = 1:1:2 exhibited the highest activity at 60 °C of 155 A (g-Pt)−1 at 0.5 V vs. RHE.

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References

  1. Narayanan S.R., Valdez T.I. (2003) Portable direct methnol fuel cell systems. In: Vielstich W., Lamm A., Gasteiger H.A. (eds), Handbook of Fuel Cells Fundamentals Technology and Applications, Vol. 4. John Wiley & Sons Ltd, Chichester, pp. 1133–1141

    Google Scholar 

  2. Waszcuk P., Lu G.-Q., Wiecowski A., Lu C., Rice C., Masel R.I. (2002) Electrochim. Acta 47:3637

    Article  Google Scholar 

  3. Watanabe M., Motoo S. (1975) J. Electroanal. Chem. 60:267

    Article  CAS  Google Scholar 

  4. Iwasita T., Nart F.C., Vielstich W. (1990) Ber. Bunsen-Ges. Phys. Chem. 94:1030

    CAS  Google Scholar 

  5. Krausa M., Vielstich W. (1994) J. Electroanal. Chem. 379:307

    Article  Google Scholar 

  6. Tong Y.Y., Kim H.S., Babu P.K., Waszczuk P., Wieckowski A., Oldfield E. (2002) J. Am. Chem. Soc. 124:468

    Article  CAS  Google Scholar 

  7. Bockris J.O’M., Wroblowa H. (1964) J. Electroanal. Chem. 7:428

    Article  Google Scholar 

  8. Takasu Y., Fujiwara T., Murakami Y., Oguri M., Asaki T., Sugimoto W. (2000) J. Electrochem. Soc. 147:4421

    Article  CAS  Google Scholar 

  9. Gasteiger H.A., Markovic N., Ross P.N., Cairns E.J. Jr (1994) J. Phys. Chem. 98:617

    Article  CAS  Google Scholar 

  10. Friedrich A.K., Geyzers K.P., Linke U., Stimming U., Stumper J. (1996) J. Electroanal. Chem. 402:123

    Article  Google Scholar 

  11. Schmidt T.J., Noeske M., Gasteiger H.A., Behm R.J., Britz P., Brijoux W., Bonnemann H. (1997) Langmuir 13:2591

    Article  CAS  Google Scholar 

  12. Dinh H.N., Ren X., Garzon F.H., Zelenay P., Gottesfeld S. (2000) J. Electroanal. Chem. 491:222

    Article  CAS  Google Scholar 

  13. Kawaguchi T., Sugimoto W., Murakami Y., Takasu Y. (2004) Electrochem. Commun. 6:480

    Article  CAS  Google Scholar 

  14. Takasu Y., Itaya H., Iwazaki T., Miyoshi R., Ohnuma T., Sugimoto W., Murakami Y. (2001) Chem. Commun. 2001:341

    Article  Google Scholar 

  15. Takasu Y., Sugimoto W., Murakami Y. (2003) Catal. Surv. Asia 7:21

    Article  CAS  Google Scholar 

  16. Morimoto Y., Yeager E.B. (1998) J. Electroanal. Chem. 444:95

    Article  CAS  Google Scholar 

  17. Frelink T., Visscher W., Van Veen J.A.R. (1995) Surf. Sci. 335:353

    Article  CAS  Google Scholar 

  18. Gotz M., Wendt H. (1998) Electrochim. Acta 43:3637

    Article  CAS  Google Scholar 

  19. Koch D.F.A., Rand D.A.J., Woods R. (1976) J. Electroanal. Chem. 70:73

    Article  CAS  Google Scholar 

  20. Lei H.W., Suh S., Gurau B., Workie B., Liu R., Smotkin E.S. (2002) Electrochim. Acta 47:2913

    Article  CAS  Google Scholar 

  21. Janssen M.M.P., Moolhuysen J. (1976) Electrochim. Acta 21:861

    Article  CAS  Google Scholar 

  22. Frelink T., Visscher W., van Veen J.A.R. (1994) Electrochim. Acta 39:1871

    Article  CAS  Google Scholar 

  23. Frelink T., Visscher W., Cox A.P., van Veen J.A.R. (1995) Electrochim. Acta 40:1537

    Article  CAS  Google Scholar 

  24. Wang K., Gasteiger H.A., Markovic N.M., Ross P.N., Jr (1996) Electrochim. Acta 41:2587

    Article  CAS  Google Scholar 

  25. Beden B., Kadirgan F., Lamy C., Leger J.M. (1981) J. Electroanal. Chem. 127:75

    Article  CAS  Google Scholar 

  26. Shibata M., Motoo S. (1986) J. Electroanal. Chem. 209:151

    Article  CAS  Google Scholar 

  27. Bittins-Cattaneo B., Iwasita T. (1987) J. Electroanal. Chem. 238:151

    Article  CAS  Google Scholar 

  28. Aricò A.S., Antonucci V., Giordano N., Shukla A.K., Ravikumar M.K., Roy A., Barman S., Sarma D.D. (1994) J. Power Sources 50:295

    Article  Google Scholar 

  29. Stalnionis G., Tamašauskaitė-Tamašiūnaitė L., Pautienienė V., Jusys Z. (2004) J. Solid State Electrochem. 8:900

    Article  CAS  Google Scholar 

  30. Haner A.N., Ross P.N. (1991) J. Phys Chem. 95:3740

    Article  CAS  Google Scholar 

  31. Shukla A.K., Aricò A.S., El-Khatib K.M., Kim H., Antonucci P.L., Antonucci V. (1999) Appl. Surf. Sci. 137:20

    Article  CAS  Google Scholar 

  32. Kita H., Nalajima H., Shimizu K. (1988) J. Electroanal. Chem. 248:181

    Article  CAS  Google Scholar 

  33. Samjeské G., Wang H., Löffler T., Baltruschat H. (2002) Electrochim. Acta 47:3681

    Article  Google Scholar 

  34. Mukerjee S., Urian R.C. (2002) Electrochim Acta 47:3219

    Article  CAS  Google Scholar 

  35. Oliveira R.T.S., Santos M.C., Marcussi B.G., Nascente P.A.P., Bulhões L.O.S., Pereira E.C. (2005) J. Electroanal. Chem 575:177

    Article  CAS  Google Scholar 

  36. He C., Kunz H.R., Fenton J.M. (1997) J. Electrochem. Soc. 144:970

    Article  Google Scholar 

  37. He C., Kunz H.R., Fenton J.M. (2003) J. Electrochem. Soc. 150:A1017

    Article  CAS  Google Scholar 

  38. Venkataraman D.R., Kunz H.R., Fenton J.M. (2003) J. Electrochem. Soc. 150:A278

    Article  CAS  Google Scholar 

  39. Guau B., Viswanathan R., Liu R., Lafrenz T.J., Ley K.L., Smotkin E.S., Reddington E., Sapienza A., Chan B.C., Mallouk T.E., Sarangapani S. (1998) J. Phys. Chem. B 102:9997

    Article  Google Scholar 

  40. Ley K.L., Liu R., Pu C., Fan Q., Leyarovska N., Segre C., Smotkin E.S. (1997) J. Electrochem. Soc. 144:1543

    Article  CAS  Google Scholar 

  41. Lima A., Coutanceau C., Leger J.M., Lamy C. (2001) J. Appl. Electrochem. 31:379

    Article  CAS  Google Scholar 

  42. Umeda M., Ojima H., Mohamedi M., Uchida I. (2004) J. Power Sources 136:10

    Article  CAS  Google Scholar 

  43. Park K.-W., Choi J.-H., Kwon B.-K., Lee S.-A., Sung Y.-E., Ha H.-Y., Hong S.-A., Kim H., Wieckowski A. (2002) J. Phys. Chem. B 106:1869

    Article  CAS  Google Scholar 

  44. Choi J.-H., Park K.-W., Park I.-S., Nam W.-H., Sung Y.-E. (2004) Electrochim. Acta 50:787

    Article  CAS  Google Scholar 

  45. Aramata A., Masuda M. (1991) J. Electrochem. Soc. 138:1949

    Article  CAS  Google Scholar 

  46. Choi W.C., Kim J.D., Woo S.I. (2002) Catal. Today 74:235

    Article  CAS  Google Scholar 

  47. Park K.-W., Choi J.-H., Lee S.-A., Pak C., Chang H., Sung Y.-E. (2004) J. Catal. 224:236

    Article  CAS  Google Scholar 

  48. Dickinson A.J., Carrette L.P.L., Collins J.A., Friedrich K.A., Stimming U. (2004) J. Appl. Electrochem. 34:975

    Article  CAS  Google Scholar 

  49. Ren X., Zelenay P., Thomas S., Davey J., Gottesfeld S. (2000) J. Power Sources 86:111

    Article  CAS  Google Scholar 

  50. Gasteiger H.A., Markovic N., Ross P.N., Jr, Cairns E.J. (1994) J. Electrochem. Soc. 141:1795

    Article  CAS  Google Scholar 

  51. Wakabayashi N., Uchida H., Watanabe M. (2002) Electrochem. Solid-State Lett. 5:E62

    Article  CAS  Google Scholar 

  52. Aricò A.S., Baglio V., Di Blasi A., Modica E., Antonucci P.L., Antonucci V. (2003) J. Electroanal. Chem. 557:167

    Article  Google Scholar 

  53. Massalski T.B. (1990) Binary Alloy Phase Diagrams. ASM International, Materials Park, Ohio

    Google Scholar 

  54. Schmidt T.J., Noeske M., Gasteiger H.A., Behm R.J., Britz P., Bönnemann H.J. (1998) J. Electrochem. Soc. 145:925

    Article  CAS  Google Scholar 

  55. Schmidt T.J., Gasteiger H.A., Stäb G.D., Urban P.M., Kolb D.M., Behm R.J. (1998) J. Electrochem. Soc. 145:2354

    Article  CAS  Google Scholar 

  56. Schultz T., Zhou S., Sundmacher K. (2001) Chem. Eng. Technol. 24:1223

    Article  CAS  Google Scholar 

  57. Wasmus S., Küver A. (1999) J. Electroanal. Chem. 461:14

    Article  CAS  Google Scholar 

  58. Arico A.S., Srinivasan S., Antonucci V. (2001) Fuel Cells 1:133

    Article  CAS  Google Scholar 

  59. Friedrich K.A., Geyzers K.P., Dickinson A.J., Stimming U. (2002) J. Electroanal. Chem. 524–525:261

    Article  Google Scholar 

  60. Kardash D., Korzeniewski C., Markovic N. (2001) J. Electroanal. Chem. 500:518

    Article  CAS  Google Scholar 

  61. Batista E.A., Hoster H., Iwasita T. (2003) J. Electroanal. Chem. 554:265

    Article  Google Scholar 

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Acknowledgements

This work was supported in part by the “Polymer Electrolyte Fuel Cell Program” from the New Energy and Industrial Technology Development Organization (NEDO) of Japan, in collaboration with Toray Industries, Inc., and a 21st Century COE Program from MEXT, Japan. The Pt(NH3)2(NO2)2 complex was a gift from Ishihuku Metal Industry Co., Ltd. We gratefully acknowledge their help.

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Authors and Affiliations

  1. Department of Fine Materials Engineering, Faculty of Textile Science and Technology, Shinshu University, 3-15-1 Tokida, Ueda, 386-8567, Japan

    Tomoyuki Kawaguchi, Yasuhiro Rachi, Wataru Sugimoto, Yasushi Murakami & Yoshio Takasu

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  1. Tomoyuki Kawaguchi
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  2. Yasuhiro Rachi
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  3. Wataru Sugimoto
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  4. Yasushi Murakami
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  5. Yoshio Takasu
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Correspondence to Yoshio Takasu.

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Kawaguchi, T., Rachi, Y., Sugimoto, W. et al. Performance of ternary PtRuRh/C electrocatalyst with varying Pt:Ru:Rh ratio for methanol electro-oxidation. J Appl Electrochem 36, 1117–1125 (2006). https://doi.org/10.1007/s10800-006-9195-y

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  • DOI: https://doi.org/10.1007/s10800-006-9195-y

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