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Title: Probing Structural Reconstruction of Metal Nanoparticles under Annealing and Water Vapor Conditions: A Theoretical Study

Abstract

Knowing the structural reconstruction of metal nanoparticles (NPs) under working conditions is of great importance to catalytic processes. Here, using Wulff construction combined with density functional theory (DFT) and molecular dynamics (MD) simulation, we investigated truncated octahedron-based Rh and Ir NPs (3.5, 5.5, and 9.5 nm in size) with different morphology for their structural reconstruction under annealing and water vapor conditions. Our MD results show that the NPs with lower average atomic coordination number ($$\overline{CN}$$) of surface atoms have lowered structural transformation inertness and thermal stability, resulting in more severe structural transition especially for smaller-sized NPs and Ir NPs. Under water vapor conditions, the competition between the interfacial tension ($$γ^{\overline{int}}_{hkl}$$) of (111) and (110) facets plays a major role in driving the shape evolution of Rh and Ir NPs by minimizing the total surface tension. It is revealed that annealing in vacuum/water vapor condition is an irreversible/reversible process on Rh and Ir NPs. We identified that the total adsorbate–metal ($$γ^{\overline{int}}_{hkl}$$) can serve as a key stability parameter for describing the potential energy surface of adsorbate–metal NP system in a variable gaseous environment (P, T).

Authors:
 [1]; ORCiD logo [1];  [1]; ORCiD logo [2]
  1. Shanghai Univ. of Engineering Science (China)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1581954
Report Number(s):
BNL-213515-2020-JAAM
Journal ID: ISSN 1932-7447; TRN: US2100675
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 123; Journal Issue: 49; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Wang, Zeming, An, Wei, Sun, Yangang, and Hybertsen, Mark S. Probing Structural Reconstruction of Metal Nanoparticles under Annealing and Water Vapor Conditions: A Theoretical Study. United States: N. p., 2019. Web. doi:10.1021/acs.jpcc.9b09678.
Wang, Zeming, An, Wei, Sun, Yangang, & Hybertsen, Mark S. Probing Structural Reconstruction of Metal Nanoparticles under Annealing and Water Vapor Conditions: A Theoretical Study. United States. https://doi.org/10.1021/acs.jpcc.9b09678
Wang, Zeming, An, Wei, Sun, Yangang, and Hybertsen, Mark S. Mon . "Probing Structural Reconstruction of Metal Nanoparticles under Annealing and Water Vapor Conditions: A Theoretical Study". United States. https://doi.org/10.1021/acs.jpcc.9b09678. https://www.osti.gov/servlets/purl/1581954.
@article{osti_1581954,
title = {Probing Structural Reconstruction of Metal Nanoparticles under Annealing and Water Vapor Conditions: A Theoretical Study},
author = {Wang, Zeming and An, Wei and Sun, Yangang and Hybertsen, Mark S.},
abstractNote = {Knowing the structural reconstruction of metal nanoparticles (NPs) under working conditions is of great importance to catalytic processes. Here, using Wulff construction combined with density functional theory (DFT) and molecular dynamics (MD) simulation, we investigated truncated octahedron-based Rh and Ir NPs (3.5, 5.5, and 9.5 nm in size) with different morphology for their structural reconstruction under annealing and water vapor conditions. Our MD results show that the NPs with lower average atomic coordination number ($\overline{CN}$) of surface atoms have lowered structural transformation inertness and thermal stability, resulting in more severe structural transition especially for smaller-sized NPs and Ir NPs. Under water vapor conditions, the competition between the interfacial tension ($γ^{\overline{int}}_{hkl}$) of (111) and (110) facets plays a major role in driving the shape evolution of Rh and Ir NPs by minimizing the total surface tension. It is revealed that annealing in vacuum/water vapor condition is an irreversible/reversible process on Rh and Ir NPs. We identified that the total adsorbate–metal ($γ^{\overline{int}}_{hkl}$) can serve as a key stability parameter for describing the potential energy surface of adsorbate–metal NP system in a variable gaseous environment (P, T).},
doi = {10.1021/acs.jpcc.9b09678},
journal = {Journal of Physical Chemistry. C},
number = 49,
volume = 123,
place = {United States},
year = {2019},
month = {11}
}

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