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Title: Thermal Stability of Metal Nanocrystals: An Investigation of the Surface and Bulk Reconstructions of Pd Concave Icosahedra [On the Thermal Stability of Metal Nanocrystals: An Investigation of the Surface and Bulk Reconstructions of Pd Concave Icosahedra]

Despite the remarkable success in controlling the synthesis of metal nanocrystals, it still remains a grand challenge to stabilize and preserve the shapes or internal structures of metastable kinetic products. In this work, we address this issue by systematically investigating the surface and bulk reconstructions experienced by a Pd concave icosahedron when subjected to heating up to 600 °C in vacuum. We used in situ high-resolution transmission electron microscopy to identify the equilibration pathways of this far-from-equilibrium structure. We were able to capture key structural transformations occurring during the thermal annealing process, which were mechanistically rationalized by implementing self-consistent plane-wave density functional theory (DFT) calculations. Specifically, the concave icosahedron was found to evolve into a regular icosahedron via surface reconstruction in the range of 200–400 °C, and then transform into a pseudospherical crystalline structure through bulk reconstruction when further heated to 600 °C. As a result, the mechanistic understanding may lead to the development of strategies for enhancing the thermal stability of metal nanocrystals.
ORCiD logo [1] ;  [2] ; ORCiD logo [1] ;  [2] ;  [3] ; ORCiD logo [2] ; ORCiD logo [1]
  1. Georgia Inst. of Technology and Emory Univ., Atlanta, GA (United States)
  2. Univ. of Wisconsin-Madison, Madison, WI (United States)
  3. Hitachi High-Technologies Canada, Toronto, ON (Canada)
Publication Date:
Grant/Contract Number:
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 17; Journal Issue: 6; Journal ID: ISSN 1530-6984
American Chemical Society
Research Org:
Univ. of Wisconsin-Madison, Madison, WI (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Contributing Orgs:
Environmental Molecular Sciences Laboratory; the Center for Nanoscale Materials at Argonne National Laboratory; the National Energy Research Scientific Computing Center (NERSC); and the UW-Madison Center for High Throughput Computing (CHTC)
Country of Publication:
United States
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; concave icosahedron; density functional theory; in situ electron microscopy; nanocrystal; Palladium; thermal stability
OSTI Identifier: