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Title: Platinum and Palladium Overlayers Dramatically Enhance the Activity of Ruthenium Nanotubes for Alkaline Hydrogen Oxidation

Abstract

Templated vapor synthesis and thermal annealing were used to synthesize unsupported metallic Ru nanotubes with Pt or Pd overlayers. By controlling the elemental composition and thickness of these overlayers, we obtain nanostructures with very high alkaline hydrogen oxidation activity. For nanotubes with a nominal atomic composition of Ru0.90Pt0.10 display a surface-specific activity (2.4 mA/cm2) that is 35 times greater than that of pure Ru nanotubes at a 50 mV overpotential and 2.5 times greater than that of pure Pt nanotubes (0.98 mA/cm2). The surface-segregated structure also confers dramatically increased Pt utilization efficiency. We find a platinum-mass-specific activity of 1240 A/gPt for the optimized nanotube versus 280 A/gPt for carbon-supported Pt nanoparticles and 109 A/gPt for monometallic Pt nanotubes. Here, we attribute the enhancement of both area- and platinum-mass-specific activity to the atomic-scale homeomorphism of the nanotube form factor with adlayer-modified polycrystals. Subsurface ligand and bifunctional effects previously observed on segregated, adlayer-modified polycrystals are translated to nanoscale catalysts.

Authors:
 [1];  [1];  [2];  [1];  [3];  [1]
+ Show Author Affiliations
  1. Univ. of Tennessee, Knoxville, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1286948
Grant/Contract Number:  
AC05-00OR22725; AC02-06CH11357; N0014-12-1-0887
Resource Type:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 5; Journal Issue: 11; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; alkaline anode; chemical vapor deposition; electrocatalysts; fuel cell; nanoparticle alloy; ruthenium-rich

Citation Formats

St. John, Samuel, Atkinson, Robert W., Unocic, Kinga A., Unocic, Raymond R., Zawodzinski, Thomas A., and Papandrew, Alexander B. Platinum and Palladium Overlayers Dramatically Enhance the Activity of Ruthenium Nanotubes for Alkaline Hydrogen Oxidation. United States: N. p., 2015. Web. doi:10.1021/acscatal.5b01432.
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St. John, Samuel, Atkinson, Robert W., Unocic, Kinga A., Unocic, Raymond R., Zawodzinski, Thomas A., & Papandrew, Alexander B. Platinum and Palladium Overlayers Dramatically Enhance the Activity of Ruthenium Nanotubes for Alkaline Hydrogen Oxidation. United States. https://doi.org/10.1021/acscatal.5b01432
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St. John, Samuel, Atkinson, Robert W., Unocic, Kinga A., Unocic, Raymond R., Zawodzinski, Thomas A., and Papandrew, Alexander B. Sun . "Platinum and Palladium Overlayers Dramatically Enhance the Activity of Ruthenium Nanotubes for Alkaline Hydrogen Oxidation". United States. https://doi.org/10.1021/acscatal.5b01432. https://www.osti.gov/servlets/purl/1286948.
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@article{osti_1286948,
title = {Platinum and Palladium Overlayers Dramatically Enhance the Activity of Ruthenium Nanotubes for Alkaline Hydrogen Oxidation},
author = {St. John, Samuel and Atkinson, Robert W. and Unocic, Kinga A. and Unocic, Raymond R. and Zawodzinski, Thomas A. and Papandrew, Alexander B.},
abstractNote = {Templated vapor synthesis and thermal annealing were used to synthesize unsupported metallic Ru nanotubes with Pt or Pd overlayers. By controlling the elemental composition and thickness of these overlayers, we obtain nanostructures with very high alkaline hydrogen oxidation activity. For nanotubes with a nominal atomic composition of Ru0.90Pt0.10 display a surface-specific activity (2.4 mA/cm2) that is 35 times greater than that of pure Ru nanotubes at a 50 mV overpotential and 2.5 times greater than that of pure Pt nanotubes (0.98 mA/cm2). The surface-segregated structure also confers dramatically increased Pt utilization efficiency. We find a platinum-mass-specific activity of 1240 A/gPt for the optimized nanotube versus 280 A/gPt for carbon-supported Pt nanoparticles and 109 A/gPt for monometallic Pt nanotubes. Here, we attribute the enhancement of both area- and platinum-mass-specific activity to the atomic-scale homeomorphism of the nanotube form factor with adlayer-modified polycrystals. Subsurface ligand and bifunctional effects previously observed on segregated, adlayer-modified polycrystals are translated to nanoscale catalysts.},
doi = {10.1021/acscatal.5b01432},
journal = {ACS Catalysis},
number = 11,
volume = 5,
place = {United States},
year = {Sun Oct 18 00:00:00 EDT 2015},
month = {Sun Oct 18 00:00:00 EDT 2015}
}
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https://doi.org/10.1021/acscatal.5b01432
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