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Topics in Catalysis

, Volume 46, Issue 3–4, pp 249–262 | Cite as

Platinum Monolayer Fuel Cell Electrocatalysts

  • R. R. Adzic
  • J. Zhang
  • K. Sasaki
  • M. B. Vukmirovic
  • M. Shao
  • J. X. Wang
  • A. U. Nilekar
  • M. Mavrikakis
  • J. A. Valerio
  • F. Uribe
Original Paper

Abstract

We describe a new class of electrocatalysts for the O2 reduction, and H2 and methanol oxidation reactions, consisting of a monolayer of Pt deposited on a metal or alloy carbon-supported nanoparticles. These electrocatalysts show up to a 20-fold increase in Pt mass activity compared with conventional all-Pt electrocatalysts. The origin of their increased activity was identified through a combination of experimental methods, employing electrochemical and surface science techniques, X-ray absorption spectroscopy, and density functional theory calculations. The long-term tests in fuel cells demonstrated excellent stability of the anode and good stability of the cathode electrocatalysts. We also describe the stabilization of Pt electrocatalysts against dissolution under potential cycling regimes effected by a submonolayer of Au clusters deposited on Pt surfaces. These new electrocatalysts promise to alleviate some of the major problems of existing fuel cell technology.

Keywords

Hydrogen oxidation CO oxidation Oxygen reduction Platinum monolayer Fuel cells Electrocatalysis Density functional theory 

Notes

Acknowledgments

This work is supported by U.S. Department of Energy, Divisions of Chemical and Material Sciences, under the Contract No. DE-AC02-98CH10886. Work at UW-Madison was supported by DOE-BES, Chemical Sciences Office, and by S. C. Johnson through a fellowship to AUN. Supercomputing time at NERSC, PNNL, and ORNL resources is gratefully acknowledged.

References

  1. 1.
    Cleghorn SJC, Ren X, Springer TE. Wilson MS, Zawodzinski C, Zawodzinski TA, Gottesfeld S (1997) Int J Hydrogen Energy 22:1137–1144CrossRefGoogle Scholar
  2. 2.
    Inoue H, Wang JX, Sasaki K, Adzic RR (2003) J Electroanal Chem 554:77–85CrossRefGoogle Scholar
  3. 3.
    Tarasevich MR, Sadkowski A, Eager E (1983) In: Conway BE (ed) Comprehensive treatise of electrochemistry. Plenum, New York, pp 301–398Google Scholar
  4. 4.
    Adzic RR (1998) In: Jacek Lipkowski PNR (ed) Electrocatalysis. Wiley–VCH, Inc., p 197Google Scholar
  5. 5.
    Markovic NM, Ross PN (1999) In: Wieckowski A (ed) Interfacial electrochemistry. Marcel Dekker, New York, pp 821Google Scholar
  6. 6.
    Brankovic SR, Wang JX, Adzic RR (2001) Electrochem Solid-State Lett 4:A217–A220CrossRefGoogle Scholar
  7. 7.
    Zhang J, Lima FHB, Shao MH, Sasaki K, Wang JX, Hanson J, Adzic RR (2005) J Phys Chem B 109:22701–22704CrossRefGoogle Scholar
  8. 8.
    Zhang J, Vukmirovic MB, Sasaki K, Uribe F, Adzic RR, Serb J (2005) Chem Soc 70:513–525Google Scholar
  9. 9.
    Hammer B, Norskov JK (2000) Advance catalysis. Academic Press Inc., San Diego, pp 71–129Google Scholar
  10. 10.
    Sasaki K, Wang JX, Balasubramanian M, McBreen J, Uribe F, Adzic RR (2004) Electrochim Acta 49:3873–3877CrossRefGoogle Scholar
  11. 11.
    Zhang J, Mo Y, Vukmirovic MB, Klie R, Sasaki K, Adzic RR (2004) J Phys Chem B 108:10955–10964CrossRefGoogle Scholar
  12. 12.
    Brankovic SR, Wang JX, Adzic RR (2001) Surf Sci 474:L173–L179CrossRefGoogle Scholar
  13. 13.
    Brankovic SR, Wang JX, Adzic RR (2001) J Serb Chem Soc 66:887–898Google Scholar
  14. 14.
    Vanderbilt D (1990) Phys Rev B 41:7892–7895CrossRefGoogle Scholar
  15. 15.
    Greeley J, Norskov JK, Mavrikakis M (2002) Annu Rev Phys Chem 53:319–348CrossRefGoogle Scholar
  16. 16.
    Hammer M, Hansen LB, Norskov JK (1999) Phys Rev B 59:7413–7421CrossRefGoogle Scholar
  17. 17.
    Greeley J, Mavrikakis M (2004) Nature Mater 3:810–815CrossRefGoogle Scholar
  18. 18.
    Xu Y, Ruban AV, Mavrikakis M (2004) J Am Chem Soc 126:4717–4725CrossRefGoogle Scholar
  19. 19.
    Ashcroft NW, Mermin ND (1976) Solid state physics. Saunders College, Orlando FLGoogle Scholar
  20. 20.
    Wang JX, Springer TE, Adzic RR (2006) J Electrochem Soc 153:A1732–A1740CrossRefGoogle Scholar
  21. 21.
    Brankovic SR, Marinkovic NS, Wang JX, Adzic RR (2002) J Electroanal Chem 532:57–66CrossRefGoogle Scholar
  22. 22.
    Koper MTM, Shubina TE, van Santen RA (2002) J Phys Chem B 106:686CrossRefGoogle Scholar
  23. 23.
    de Mongeot FB, Scherer M, Gleich B, Kopatzki E, Behm RJ (1998) Surf Sci 411:249–62CrossRefGoogle Scholar
  24. 24.
    Chen SL, Kucernak A (2004) J Phys Chem B 108:13984–13994CrossRefGoogle Scholar
  25. 25.
    Zhang JL, Vukmirovic MB, Xu Y, Mavrikakis M, Adzic RR (2005) Angew Chem Int Ed 44:2132–2135CrossRefGoogle Scholar
  26. 26.
    Zhang JL, Vukmirovic MB, Sasaki K, Nilekar AU, Mavrikakis M, Adzic RR (2005) J Am Chem Soc 127:12480–12481CrossRefGoogle Scholar
  27. 27.
    Rodriguez JA (1996) Surf Sci Rep 24:225–287CrossRefGoogle Scholar
  28. 28.
    Kitchin JR, Norskov JK, Barteau MA, Chen JG (2004) J Chem Phys 120:10240–10246CrossRefGoogle Scholar
  29. 29.
    Mukerjee S, Srinivasan S, Soriaga MP, McBreen J (1995) J Phys Chem 99:4577–4589CrossRefGoogle Scholar
  30. 30.
    Ruckman MW, Strongin M (1994) Acc Chem Res 27:250–256CrossRefGoogle Scholar
  31. 31.
    Markovic NM, Schmidt TJ, Stamenkovic V, Ross PN (2001) Fuel Cells 1:105CrossRefGoogle Scholar
  32. 32.
    Murthi VS, Urian RC, Mukerjee S (2004) J Phys Chem B 108:11011–11023CrossRefGoogle Scholar
  33. 33.
    Shao M, Liu P, Zhang J, Adzic RR (2007) J Phys Chem 111:6772–6775Google Scholar
  34. 34.
    Zhang J, Sutter SKE. Adzic RR (2007) Science 315:220CrossRefGoogle Scholar
  35. 35.
    Woods R (1976) In: Bard AJ (ed) Electroanalytical chemistry. Marcel Dekker, New York, pp 1–162Google Scholar
  36. 36.
    Roudgar A, Groβ A (2004) Surf Sci 559:L180–L186CrossRefGoogle Scholar
  37. 37.
    Del Popolo MG, Leiva EPM, Mariscal M, Schmickler W (2005) Surf Sci 597:133–155CrossRefGoogle Scholar

Copyright information

© Springer Science+Business Media, LLC 2007

Authors and Affiliations

  • R. R. Adzic
    • 1
  • J. Zhang
    • 1
  • K. Sasaki
    • 1
  • M. B. Vukmirovic
    • 1
  • M. Shao
    • 1
  • J. X. Wang
    • 1
  • A. U. Nilekar
    • 2
  • M. Mavrikakis
    • 2
  • J. A. Valerio
    • 3
  • F. Uribe
    • 3
  1. 1.Chemistry Department Brookhaven National LaboratoryUptonUSA
  2. 2.Department of Chemical and Biological EngineeringUniversity of Wisconsin-Madison MadisonUSA
  3. 3.Los Alamos National Laboratory Los AlamosUSA

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