Reshaping of Truncated Pd Nanocubes: Energetic and Kinetic Analysis Integrating Transmission Electron Microscopy with Atomistic-Level and Coarse-Grained Modeling

Lai, King C.; Chen, Minda; Williams, Benjamin; Han, Yong; Tsung, Chia-Kuang; Huang, Wenyu; Evans, James W.

doi:10.1021/acsnano.0c02864

Reshaping of Truncated Pd Nanocubes: Energetic and Kinetic Analysis Integrating Transmission Electron Microscopy with Atomistic-Level and Coarse-Grained Modeling

Journal Article · Wed Jul 08 00:00:00 EDT 2020 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.0c02864· OSTI ID:1638689

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Ames Lab., Ames, IA (United States); Iowa State Univ., Ames, IA (United States)
Iowa State Univ., Ames, IA (United States)
Boston College, Chestnut Hill, MA (United States)

Stability against reshaping of metallic fcc nanocrystals synthesized with tailored far-from-equilibrium shapes is key to maintaining optimal properties for applications such as catalysis. Yet Arrhenius analysis of experimental reshaping kinetics, and appropriate theory and simulation, is lacking. As such, we use TEM to monitor the reshaping of Pd nanocubes of ~25 nm side length between 410 °C (over ~4.5 h) and 440 °C (over ~0.25 h), extracting a high effective energy barrier of E_eff ≈ 4.6 eV. We also provide an analytic determination of the energy variation along the optimal pathway for reshaping that involves transfer of atoms across the nanocube surface from edges or corners to form new layers on side {100} facets. The effective barrier from this analysis is shown to increase strongly with the degree of truncation of edges and corners in the synthesized nanocube. Theory matches experiment for the appropriate degree of truncation. In addition, we perform simulations of a stochastic atomistic-level model incorporating a realistic description of diffusive hopping for undercoordinated surface atoms, thereby providing a visualization of the initial reshaping process.

View Accepted Manuscript (DOE)

Research Organization:: Ames Laboratory (AMES), Ames, IA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Science Foundation (NSF)

Grant/Contract Number:: AC02-07CH11358; AC02-05CH11231

OSTI ID:: 1638689

Report Number(s):: IS--J-10,188

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 7 Vol. 14; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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