Highly Crystalline Multimetallic Nanoframes with Three-Dimensional Electrocatalytic Surfaces

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Science  27 Feb 2014:
DOI: 10.1126/science.1249061

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Control of structure at the atomic level can precisely and effectively tune catalytic properties of materials, enabling enhancement in both activity and durability. We report synthesis of a highly active and durable class of electrocatalysts by exploiting the structural evolution of Pt-Ni bimetallic nanocrystals. The starting material, crystalline PtNi3 polyhedra, transformed in solution by interior erosion into Pt3Ni nanoframes with surfaces that have three-dimensional molecular accessibility. The edges of these PtNi3 polyhedra, which were Pt rich, are maintained in the final Pt3Ni nanoframes. Both the interior and exterior catalytic surfaces of this open framework structure are composed of the nano-segregated Pt-Skin structure that exhibits enhanced oxygen reduction reaction (ORR) activity. The Pt3Ni nanoframe catalysts achieved over 36 and 22-fold enhancement in mass and specific activities, respectively, for this reaction versus ORR in comparison to state-of-the-art Pt/C catalysts during prolonged exposure to reaction conditions.

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