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Title: Highly Crystalline Multimetallic Nanoframes with Three-Dimensional Electrocatalytic Surfaces

Control of structure at the atomic level can precisely and effectively tune catalytic properties of materials, enabling enhancement in both activity and durability. We synthesized a highly active and durable class of electrocatalysts by exploiting the structural evolution of platinum-nickel (Pt-Ni) bimetallic nanocrystals. The starting material, crystalline PtNi3 polyhedra, transforms in solution by interior erosion into Pt3Ni nanoframes with surfaces that offer three-dimensional molecular accessibility. The edges of the Pt-rich PtNi3 polyhedra are maintained in the final Pt3Ni nanoframes. Both the interior and exterior catalytic surfaces of this open-framework structure are composed of the nanosegregated Pt-skin structure, which exhibits enhanced oxygen reduction reaction (ORR) activity. The Pt3Ni nanoframe catalysts achieved a factor of 36 enhancement in mass activity and a factor of 22 enhancement in specific activity, respectively, for this reaction (relative to state-of-the-art platinum-carbon catalysts) during prolonged exposure to reaction conditions.
Authors:
 [1] ;  [2] ;  [3] ;  [3] ;  [3] ;  [4] ;  [2] ;  [2] ;  [5] ;  [5] ;  [6] ;  [6] ;  [7] ;  [2] ;  [3] ;  [8] ;  [2]
  1. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Tsinghua Univ., Beijing (China)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
  3. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  5. Univ. of Wisconsin, Madison, WI (United States)
  6. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  7. Tsinghua Univ., Beijing (China)
  8. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); King Abdulaziz Univ., Jeddah (Saudia Arabia)
Publication Date:
OSTI Identifier:
1227053
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Science; Journal Volume: 343; Journal Issue: 6177
Publisher:
AAAS
Research Org:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE Environmental Molecular Sciences Laboratory