Environmental Molecular Sciences Laboratory

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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.

Chen C, Y Kang, Z Huo, Z Zhu, W Huang, H Xin, J Snyder, D Li, JA Herron, M Mavrikakis, M Chi, KL More, Y Li, NM Markovic, GA Somorjai, P Yang, and VR Stamenkovic.2014."Highly Crystalline Multimetallic Nanoframes with Three-Dimensional Electrocatalytic Surfaces."Science 343(6177):1339-1343. doi:10.1126/science.1249061
C Chen
Y Kang
Z Huo
Z Zhu
W Huang
H Xin
J Snyder
D Li
JA Herron
M Mavrikakis
M Chi
KL More
Y Li
NM Markovic
GA Somorjai
P Yang
VR Stamenkovic