Journal
JOURNAL OF PHYSICAL CHEMISTRY C
Volume 118, Issue 35, Pages 20496-20503Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jp507204k
Keywords
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Funding
- Fuel Cell Technology Program of the Office of Energy Efficiency and Renewable Energy of the U.S. Department of Energy [DE-EE0000458]
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-98CH10886]
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To truly understand the origin of the enhanced oxygen reduction reaction (ORR) activity of Pt-based electrocatalysts over pure Pt, it is essential to characterize the electrocatalysts under ORR operating conditions. Herein, we report a dealloyed Pt1Co1 NP catalyst with Pt mass activity similar to 4 times higher than that of Pt/C and with superior stability in proton exchange membrane fuel cells (PEMFCs). Advanced microscopy and in situ spectroscopy are combined to show that this electrocatalyst possesses a unique ordered PtCo core-ultrathin with nonporous Pt shell structure, and the structure maintains the desired compositional profiles in the near-surface region even during the ORR in acid. Ab initio FEFF8 calculations based on experimentally derived structures reveal that the catalytic enhancements result from cooperative compressive-strain and ligand effects induced by the Co enrichment in the compact core and near subsurface.
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