Journal
NANO LETTERS
Volume 12, Issue 10, Pages 5230-5238Publisher
AMER CHEMICAL SOC
DOI: 10.1021/nl302404g
Keywords
Fuel cell; ORR; electrocatalyst; ordered intermetallic nanoparticle; dealloying
Categories
Funding
- Department of Energy [DE-FG02-87ER45298]
- Energy Materials Center at Cornel
- Energy Frontier Research Center
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001086]
- U.S. Department of Energy [DE-AC02-05CH11231]
- American Chemical Society (ACS) Division of Analytical Chemistry (ACS)
- Eastman Chemical Company
- CCMR
- Research Experience for Undergraduates program [DMR-1063059]
- Division Of Materials Research
- Direct For Mathematical & Physical Scien [1063059] Funding Source: National Science Foundation
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A promising electrocatalyst prototype of low Pt mole fraction, intermetallic nanoparticles of Cu3Pt, has been prepared using a simple impregnation-reduction method, followed by a post heat-treatment. Two dealloying methods (electrochemical and chemical) were implemented to control the atomic-level morphology and improve performance for the oxygen reduction reaction (ORR). The morphology and elemental composition of the dealloyed nanoparticles were characterized at angstrom resolution using an aberration-corrected scanning transmission electron microscope equipped with an electron energy loss spectrometer. We found that the electrochemical dealloying method led to the formation of a thin Pt skin of ca. 1 nm in thickness with an ordered Cu3Pt core structure, while chemical leaching gave rise to a spongy structure with no ordered structure being preserved. A three-dimensional tomographic reconstruction indicated that numerous voids were formed in the chemically dealloyed nanoparticles. Both dealloying methods yielded enhanced specific and mass activities toward the ORR and higher stability relative to Pt/C. The spongy nanoparticles exhibited better mass activity with a slightly lower specific activity than the electrochemically dealloyed nanoparticles after 50 potential cycles. In both cases, the mass activity was still enhanced after 5000 potential cycles.
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