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Originally published in Science Express on 11 January 2007
Science 26 January 2007:
Vol. 315. no. 5811, pp. 493 - 497
DOI: 10.1126/science.1135941
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Reports

Improved Oxygen Reduction Activity on Pt3Ni(111) via Increased Surface Site Availability

Vojislav R. Stamenkovic,1,2* Ben Fowler,3 Bongjin Simon Mun,2 Guofeng Wang,4 Philip N. Ross,2 Christopher A. Lucas,3 Nenad M. Markovic1*

The slow rate of the oxygen reduction reaction (ORR) in the polymer electrolyte membrane fuel cell (PEMFC) is the main limitation for automotive applications. We demonstrated that the Pt3Ni(111) surface is 10-fold more active for the ORR than the corresponding Pt(111) surface and 90-fold more active than the current state-of-the-art Pt/C catalysts for PEMFC. The Pt3Ni(111) surface has an unusual electronic structure (d-band center position) and arrangement of surface atoms in the near-surface region. Under operating conditions relevant to fuel cells, its near-surface layer exhibits a highly structured compositional oscillation in the outermost and third layers, which are Pt-rich, and in the second atomic layer, which is Ni-rich. The weak interaction between the Pt surface atoms and nonreactive oxygenated species increases the number of active sites for O2 adsorption.

1 Materials Science Division, Argonne National Laboratory, Argonne, IL 60439, USA.
2 Materials Sciences Division, Lawrence Berkeley National Laboratory, University of California, Berkeley, CA 94720, USA.
3 Oliver Lodge Laboratory, Department of Physics, University of Liverpool, Liverpool, L69 7ZE, UK.
4 Department of Chemistry and Physics, University of South Carolina, Aiken, SC 29801, USA.

* To whom correspondence should be addressed. E-mail: vrstamenkovic{at}anl.gov (V.R.S.); nmmarkovic{at}anl.gov (N.M.M.)

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