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Published Online January 11, 2007
Science DOI: 10.1126/science.1135941

Submitted on October 5, 2006
Accepted on December 11, 2006

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

Vojislav R. Stamenkovic 1*, Ben Fowler 2, Bongjin Simon Mun 3, Guofeng Wang 4, Philip N. Ross 3, Christopher A. Lucas 2, Nenad M. Markovic 5*

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

* To whom correspondence should be addressed.
Vojislav R. Stamenkovic , E-mail: vrstamenkovic{at}anl.gov
Nenad M. Markovic , E-mail: nmmarkovic{at}anl.gov

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 show that the Pt3Ni(111) 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 are Pt rich and the second atomic layer is Ni rich. The weak interaction between the Pt surface atoms and non-reactive oxygenated species increases the number of active sites for O2 adsorption.


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Science. ISSN 0036-8075 (print), 1095-9203 (online)