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Platinum-based nanocages with subnanometer-thick walls and well-defined, controllable facets

Lei ZhangState Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, and Department of Chemistry, Xiamen University, Xiamen, Fujian 361005, P. R. ChinaLuke T. RolingDepartment of Chemical and Biological Engineering, University of Wisconsin–Madison, Madison, WI 53706, USAXue WangState Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, and Department of Chemistry, Xiamen University, Xiamen, Fujian 361005, P. R. ChinaMadeline VaraSchool of Chemistry and Biochemistry, Georgia Institute of Technology, Atlanta, GA 30332, USAMiaofang ChiCenter for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USAJingyue LiuDepartment of Physics, Arizona State University, Tempe, AZ 85287, USASang‐Il ChoiWallace H. Coulter Department of Biomedical Engineering, Georgia Institute of Technology and Emory University, Atlanta, GA 30332, USAJinho ParkSchool of Chemistry and Biochemistry, Georgia Institute of Technology, Atlanta, GA 30332, USAJeffrey A. HerronDepartment of Chemical and Biological Engineering, University of Wisconsin–Madison, Madison, WI 53706, USAZhaoxiong XieState Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, and Department of Chemistry, Xiamen University, Xiamen, Fujian 361005, P. R. ChinaManos MavrikakisDepartment of Chemical and Biological Engineering, University of Wisconsin–Madison, Madison, WI 53706, USAYounan XiaSchool of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, GA 30332, USA
2015en
ABI

Аннотация

A cost-effective catalyst should have a high dispersion of the active atoms, together with a controllable surface structure for the optimization of activity, selectivity, or both. We fabricated nanocages by depositing a few atomic layers of platinum (Pt) as conformal shells on palladium (Pd) nanocrystals with well-defined facets and then etching away the Pd templates. Density functional theory calculations suggest that the etching is initiated via a mechanism that involves the formation of vacancies through the removal of Pd atoms incorporated into the outermost layer during the deposition of Pt. With the use of Pd nanoscale cubes and octahedra as templates, we obtained Pt cubic and octahedral nanocages enclosed by {100} and {111} facets, respectively, which exhibited distinctive catalytic activities toward oxygen reduction.

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