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Title: Pd@Pt core-shell concave decahedra: A class of catalysts for the oxygen reduction reaction with enhanced activity and durability

Journal Article · · Journal of the American Chemical Society
DOI:https://doi.org/10.1021/jacs.5b10059· OSTI ID:1279435
 [1];  [2];  [3];  [4];  [4];  [4];  [2];  [5];  [1];  [6];  [7];  [8]
  1. Georgia Institute of Technology, Atlanta, GA (United States); Emory Univ., Atlanta, GA (United States); Xiamen Univ., Fujian (People's Republic of China)
  2. Georgia Institute of Technology, Atlanta, GA (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Georgia Institute of Technology, Atlanta, GA (United States); Emory Univ., Atlanta, GA (United States)
  5. Georgia Inst. of Technology, Atlanta, GA (United States)
  6. Arizona State Univ., Tempe, AZ (United States)
  7. Hitachi High-Technologies Canada, Toronto, ON (Canada)
  8. Xiamen Univ., Fujian (People's Republic of China)

Here, we report a facile synthesis of multiply twinned Pd@Pt core shell concave decahedra by controlling the deposition of Pt on preformed Pd decahedral seeds. The Pt atoms are initially deposited on the vertices of a decahedral seed, followed by surface diffusion to other regions along the edges/ridges and then across the faces. Different from the coating of a Pd icosahedral seed, the Pt atoms prefer to stay at the vertices and edges/ridges of a decahedral seed even when the deposition is conducted at 200 degrees C, naturally generating a core shell structure covered by concave facets. The nonuniformity in the Pt coating can be attributed to the presence of twin boundaries at the vertices, as well as the {100} facets and twin defects along the edges/ridges of a decahedron, effectively trapping the Pt adatoms at these high-energy sites. As compared to a commercial Pt/C catalyst, the Pd@Pt concave decahedra show substantial enhancement in both catalytic activity and durability toward the oxygen reduction reaction (ORR). For the concave decahedra with 29.6% Pt by weight, their specific (1.66 mA/cm2pt) and mass (1.60 A/mg/2pt) ORR activities are enhanced by 4.4 and 6.6 times relative to those of the Pt/C catalyst (0.36 mA/cm2pt and 0.32 A/mgpt, respectively). After 10 000 cycles of accelerated durability test, the concave decahedra still exhibit a mass activity of 0.69 A/mgpt, more than twice that of the pristine Pt/C catalyst.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Organization:
USDOE Office of Science (SC)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1279435
Journal Information:
Journal of the American Chemical Society, Vol. 137, Issue 47; ISSN 0002-7863
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 244 works
Citation information provided by
Web of Science

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The Quasi‐Pt‐Allotrope Catalyst: Hollow PtCo@single‐Atom Pt 1 on Nitrogen‐Doped Carbon toward Superior Oxygen Reduction journal February 2019
Nanoscale kinetics of asymmetrical corrosion in core-shell nanoparticles journal March 2018
Enhanced catalytic activity of Au core Pd shell Pt cluster trimetallic nanorods for CO 2 reduction journal January 2019
Seed-Mediated Growth of Colloidal Metal Nanocrystals journal December 2016
Aqueous Synthesis of Pd–M (M = Pd, Pt, and Au) Decahedra with Concave Facets for Catalytic Applications journal February 2020
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Surface evolution of a Pt–Pd–Au electrocatalyst for stable oxygen reduction journal July 2017
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