On the Structural Origin of the Catalytic Properties of Inherently Strained Ultrasmall Decahedral Gold Nanoparticles

Michael J. Walsh; Kenta Yoshida; Akihide Kuwabara; Mungo L. Pay; Pratibha L. Gai; Edward D. Boyes

doi:10.1021/nl300067q

On the Structural Origin of the Catalytic Properties of Inherently Strained Ultrasmall Decahedral Gold Nanoparticles

Michael J. Walsh, Kenta Yoshida, Akihide Kuwabara, Mungo L. Pay, Pratibha L. Gai^*, Edward D. Boyes

^*Corresponding author for this work

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

Abstract

A new mechanism for reactivity of multiply twinned gold nanoparticles resulting from their inherently strained structure provides a further explanation of the surprising catalytic activity of small gold nanoparticles. Atomic defect structural studies of surface strains and quantitative analysis of atomic column displacements in the decahedral structure observed by aberration corrected transmission electron microscopy reveal an average expansion of surface nearest neighbor distances of 5.6%, with many strained by more than 10%. Density functional theory calculations of the resulting modified gold d-band states predict significantly enhanced activity for carbon monoxide oxidation. The new insights have important implications for the applications of nanoparticles in chemical process technology, including for heterogeneous catalysis.

Original language	English
Pages (from-to)	2027-2031
Number of pages	5
Journal	Nano Letters
Volume	12
Issue number	4
DOIs	https://doi.org/10.1021/nl300067q
Publication status	Published - 11 Apr 2012

Keywords

transmission electron microscopy
TRANSITION
strain
AU NANOPARTICLES
TRANSMISSION ELECTRON-MICROSCOPY
TEMPERATURE CO OXIDATION
METAL-SURFACES
CLUSTERS
RESOLUTION
catalysis
Gold
MULTIPLY-TWINNED PARTICLES
REACTIVITY
ADSORPTION
decahedra
nanoparticles

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title = "On the Structural Origin of the Catalytic Properties of Inherently Strained Ultrasmall Decahedral Gold Nanoparticles",

abstract = "A new mechanism for reactivity of multiply twinned gold nanoparticles resulting from their inherently strained structure provides a further explanation of the surprising catalytic activity of small gold nanoparticles. Atomic defect structural studies of surface strains and quantitative analysis of atomic column displacements in the decahedral structure observed by aberration corrected transmission electron microscopy reveal an average expansion of surface nearest neighbor distances of 5.6%, with many strained by more than 10%. Density functional theory calculations of the resulting modified gold d-band states predict significantly enhanced activity for carbon monoxide oxidation. The new insights have important implications for the applications of nanoparticles in chemical process technology, including for heterogeneous catalysis.",

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author = "Walsh, {Michael J.} and Kenta Yoshida and Akihide Kuwabara and Pay, {Mungo L.} and Gai, {Pratibha L.} and Boyes, {Edward D.}",

year = "2012",

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doi = "10.1021/nl300067q",

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AU - Walsh, Michael J.

AU - Yoshida, Kenta

AU - Kuwabara, Akihide

AU - Pay, Mungo L.

AU - Gai, Pratibha L.

AU - Boyes, Edward D.

PY - 2012/4/11

Y1 - 2012/4/11

N2 - A new mechanism for reactivity of multiply twinned gold nanoparticles resulting from their inherently strained structure provides a further explanation of the surprising catalytic activity of small gold nanoparticles. Atomic defect structural studies of surface strains and quantitative analysis of atomic column displacements in the decahedral structure observed by aberration corrected transmission electron microscopy reveal an average expansion of surface nearest neighbor distances of 5.6%, with many strained by more than 10%. Density functional theory calculations of the resulting modified gold d-band states predict significantly enhanced activity for carbon monoxide oxidation. The new insights have important implications for the applications of nanoparticles in chemical process technology, including for heterogeneous catalysis.

AB - A new mechanism for reactivity of multiply twinned gold nanoparticles resulting from their inherently strained structure provides a further explanation of the surprising catalytic activity of small gold nanoparticles. Atomic defect structural studies of surface strains and quantitative analysis of atomic column displacements in the decahedral structure observed by aberration corrected transmission electron microscopy reveal an average expansion of surface nearest neighbor distances of 5.6%, with many strained by more than 10%. Density functional theory calculations of the resulting modified gold d-band states predict significantly enhanced activity for carbon monoxide oxidation. The new insights have important implications for the applications of nanoparticles in chemical process technology, including for heterogeneous catalysis.

KW - transmission electron microscopy

KW - TRANSITION

KW - strain

KW - AU NANOPARTICLES

KW - TRANSMISSION ELECTRON-MICROSCOPY

KW - TEMPERATURE CO OXIDATION

KW - METAL-SURFACES

KW - CLUSTERS

KW - RESOLUTION

KW - catalysis

KW - Gold

KW - MULTIPLY-TWINNED PARTICLES

KW - REACTIVITY

KW - ADSORPTION

KW - decahedra

KW - nanoparticles

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U2 - 10.1021/nl300067q

DO - 10.1021/nl300067q

M3 - Article

SN - 1530-6984

VL - 12

SP - 2027

EP - 2031

JO - Nano Letters

JF - Nano Letters

IS - 4

ER -

On the Structural Origin of the Catalytic Properties of Inherently Strained Ultrasmall Decahedral Gold Nanoparticles

Abstract

Keywords

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