4.8 Article

Highly Stable and Active Pt-Cu Oxygen Reduction Electrocatalysts Based on Mesoporous Graphitic Carbon Supports

Journal

CHEMISTRY OF MATERIALS
Volume 21, Issue 19, Pages 4515-4526

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/cm901203n

Keywords

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Funding

  1. National Science Foundation [CHE-9876674]
  2. Department of Energy Office of Basic Energy Sciences
  3. Robert A. Welch Foundation [F-1319, F-1529]

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The activity of oxygen reduction catalysts for fuel cells often decreases markedly (30-70%) during potential cycling tests designed to accelerate catalyst degradation. Herein we achieved essentially no loss in electrochemical surface area and catalyst activity during potential cycling from 0.5 to 1.2 V for presynthesized Pt-Cu nanoparticles of controlled composition that were infused into highly graphitic disordered mesoporous carbons (DMC). The high stability is favored by the strong metal-support interactions and low tendency for carbon oxidation, which mitigates the mechanisms of degradation. Electrochemical dealloying transforms the composition from Pt20Cu80 to Pt85Cu15 with a strained Pt-rich shell, which exhibits an enhanced ORR activity of 0.46 A/mg(Pt), > 4 fold that of pure Pt catalysts. The high uniformity in particle size and composition both before and after dealloying, as a consequence of the presynthesis/infusion technique, is beneficial For elucidating the mechanism of catalyst activity and, ultimately, for designing more active catalysts.

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