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Article
Shape Stability of Truncated Octahedral fcc Metal Nanocrystals
Ames Laboratory Accepted Manuscripts
  • King C. Lai, Iowa State University and Ames Laboratory
  • Minda Chen, Iowa State University
  • Jiaqi Yu, Iowa State University
  • Yong Han, Iowa State University and Ames Laboratory
  • Wenyu Huang, Iowa State University and Ames Laboratory
  • James W. Evans, Iowa State University and Ames Laboratory
Publication Date
7-7-2021
Department
Ames Laboratory; Chemistry; Physics and Astronomy
Report Number
IS-J 10557
DOI
10.1021/acsami.1c07894
Journal Title
ACS Applied Materials & Interfaces
Abstract

Metallic nanocrystals (NCs) can be synthesized with tailored nonequilibrium shapes to enhance desired properties, e.g., octahedral fcc metal NCs optimize catalytic activity associated with {111} facets. However, maintenance of optimized properties requires stability against thermal reshaping. Thus, we analyze the reshaping of truncated fcc metal octahedra mediated by surface diffusion using a stochastic atomistic-level model with energetic input parameters for Pd. The model describes NC thermodynamics by an effective nearest-neighbor interaction and includes a realistic treatment of diffusive hopping for undercoordinated surface atoms. Kinetic Monte Carlo simulation reveals that the effective barrier, Eeff, for the initial stage of reshaping is strongly tied to the degree of truncation of the vertices in the synthesized initial octahedral shapes. This feature is elucidated via exact analytic determination of the energy variation along the optimal reshaping pathway at low-temperature (T), which involves transfer of atoms from truncated {100} vertex facets to form new layers on {111} side facets. Deviations from predictions of the low-T analysis due to entropic effects are more prominent for higher T and larger NC sizes.

DOE Contract Number(s)
AC02-07CH11358
Language
en
Publisher
Iowa State University Digital Repository, Ames IA (United States)
Citation Information
King C. Lai, Minda Chen, Jiaqi Yu, Yong Han, et al.. "Shape Stability of Truncated Octahedral fcc Metal Nanocrystals" (2021)
Available at: http://works.bepress.com/wenyu_huang/86/