A combined theoretical and experimental EXAFS study of the structure and dynamics of Au147 nanoparticles

Zhiyao Duan; Yuanyuan Li; Janis Timoshenko; Samuel T. Chill; Rachel M. Anderson; David F. Yancey; Anatoly I. Frenkel; Richard M. Crooks; Graeme Henkelman

doi:10.1039/c6cy00559d

A combined theoretical and experimental EXAFS study of the structure and dynamics of Au₁₄₇ nanoparticles

Zhiyao Duan, Yuanyuan Li, Janis Timoshenko, Samuel T. Chill, Rachel M. Anderson, David F. Yancey, Anatoly I. Frenkel, Richard M. Crooks, Graeme Henkelman

Surface Chemistry & Catalysis Group

Research output: Contribution to journal › Article › peer-review

29 Scopus citations

Abstract

In this study, we present a framework for characterizing the structural and thermal properties of small nanoparticle catalysts by combining precise synthesis, extended X-ray absorption fine structure (EXAFS) spectroscopy, and density functional theory (DFT) calculations. We demonstrate the capability of this approach by characterizing the atomic structure and vibrational dynamics of Au₁₄₇. With the combination of EXAFS spectroscopy and DFT, the synthesized Au₁₄₇ nanoparticles are determined to have an icosahedral structure. A decrease in the Einstein temperature of the Au₁₄₇ particles compared to their bulk value was observed and interpreted in terms of softer vibration modes of surface bonds.

Original language	English
Pages (from-to)	6879-6885
Number of pages	7
Journal	Catalysis Science and Technology
Volume	6
Issue number	18
DOIs	https://doi.org/10.1039/c6cy00559d
State	Published - 2016

Funding

This work was supported by the National Science Foundation under the DMREF program Grant 1534177 (RMC and GH) and 1534184 (AIF). RMC and GH thank the Robert A. Welch Foundation (Grants F-0032 and F-1841) for support. The authors acknowledge the facilities support provided at the Synchrotron Catalysis Consortium (U.S. DOE Grant No. DE-SC0012335). The atomic structures were rendered using Speck (http://wwwtyro.github.io/speck/), a program authored by Rye Terrell. The computational work was done at the National Energy Research Scientific Computing Center and the Texas Advanced Computing Center.

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abstract = "In this study, we present a framework for characterizing the structural and thermal properties of small nanoparticle catalysts by combining precise synthesis, extended X-ray absorption fine structure (EXAFS) spectroscopy, and density functional theory (DFT) calculations. We demonstrate the capability of this approach by characterizing the atomic structure and vibrational dynamics of Au147. With the combination of EXAFS spectroscopy and DFT, the synthesized Au147 nanoparticles are determined to have an icosahedral structure. A decrease in the Einstein temperature of the Au147 particles compared to their bulk value was observed and interpreted in terms of softer vibration modes of surface bonds.",

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AU - Li, Yuanyuan

AU - Timoshenko, Janis

AU - Chill, Samuel T.

AU - Anderson, Rachel M.

AU - Yancey, David F.

AU - Frenkel, Anatoly I.

AU - Crooks, Richard M.

AU - Henkelman, Graeme

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AB - In this study, we present a framework for characterizing the structural and thermal properties of small nanoparticle catalysts by combining precise synthesis, extended X-ray absorption fine structure (EXAFS) spectroscopy, and density functional theory (DFT) calculations. We demonstrate the capability of this approach by characterizing the atomic structure and vibrational dynamics of Au147. With the combination of EXAFS spectroscopy and DFT, the synthesized Au147 nanoparticles are determined to have an icosahedral structure. A decrease in the Einstein temperature of the Au147 particles compared to their bulk value was observed and interpreted in terms of softer vibration modes of surface bonds.

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A combined theoretical and experimental EXAFS study of the structure and dynamics of Au₁₄₇ nanoparticles

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