Intracluster Atomic and Electronic Structural Heterogeneities in Supported Nanoscale Metal Catalysts

Annika Elsen; Ulrich Jung; Fernando Vila; Yuanyuan Li; Olga V. Safonova; Rowena Thomas; Moniek Tromp; John J. Rehr; Ralph G. Nuzzo; Anatoly I. Frenkel

doi:10.1021/acs.jpcc.5b08267

Intracluster Atomic and Electronic Structural Heterogeneities in Supported Nanoscale Metal Catalysts

Annika Elsen, Ulrich Jung, Fernando Vila, Yuanyuan Li, Olga V. Safonova, Rowena Thomas, Moniek Tromp, John J. Rehr, Ralph G. Nuzzo, Anatoly I. Frenkel

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

9 Scopus citations

Abstract

This work reveals and quantifies the inherent intracluster heterogeneity in the atomic structure and charge distribution present in supported metal catalysts. The results demonstrate that these distributions are pronounced and strongly coupled to both structural and dynamic perturbations. They also serve to clarify the nature of the dynamic bonding of nanoscale catalytic metal clusters with their supports, and the mediation of these properties due to the presence of adsorbates. These findings are supported by theoretical modeling and experimental data measured for an exemplary supported metal catalyst, Pt supported on silica, using in situ high energy resolution X-ray absorption and emission spectroscopies; in situ diffuse reflectance infrared Fourier transform spectroscopy; and ex situ scanning transmission electron microscopy.

Original language	English
Pages (from-to)	25615-25627
Number of pages	13
Journal	Journal of Physical Chemistry C
Volume	119
Issue number	45
DOIs	https://doi.org/10.1021/acs.jpcc.5b08267
State	Published - Oct 20 2015
Externally published	Yes

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Publisher Copyright:
© 2015 American Chemical Society.

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title = "Intracluster Atomic and Electronic Structural Heterogeneities in Supported Nanoscale Metal Catalysts",

abstract = "This work reveals and quantifies the inherent intracluster heterogeneity in the atomic structure and charge distribution present in supported metal catalysts. The results demonstrate that these distributions are pronounced and strongly coupled to both structural and dynamic perturbations. They also serve to clarify the nature of the dynamic bonding of nanoscale catalytic metal clusters with their supports, and the mediation of these properties due to the presence of adsorbates. These findings are supported by theoretical modeling and experimental data measured for an exemplary supported metal catalyst, Pt supported on silica, using in situ high energy resolution X-ray absorption and emission spectroscopies; in situ diffuse reflectance infrared Fourier transform spectroscopy; and ex situ scanning transmission electron microscopy.",

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doi = "10.1021/acs.jpcc.5b08267",

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AU - Elsen, Annika

AU - Jung, Ulrich

AU - Vila, Fernando

AU - Li, Yuanyuan

AU - Safonova, Olga V.

AU - Thomas, Rowena

AU - Tromp, Moniek

AU - Rehr, John J.

AU - Nuzzo, Ralph G.

AU - Frenkel, Anatoly I.

PY - 2015/10/20

Y1 - 2015/10/20

N2 - This work reveals and quantifies the inherent intracluster heterogeneity in the atomic structure and charge distribution present in supported metal catalysts. The results demonstrate that these distributions are pronounced and strongly coupled to both structural and dynamic perturbations. They also serve to clarify the nature of the dynamic bonding of nanoscale catalytic metal clusters with their supports, and the mediation of these properties due to the presence of adsorbates. These findings are supported by theoretical modeling and experimental data measured for an exemplary supported metal catalyst, Pt supported on silica, using in situ high energy resolution X-ray absorption and emission spectroscopies; in situ diffuse reflectance infrared Fourier transform spectroscopy; and ex situ scanning transmission electron microscopy.

AB - This work reveals and quantifies the inherent intracluster heterogeneity in the atomic structure and charge distribution present in supported metal catalysts. The results demonstrate that these distributions are pronounced and strongly coupled to both structural and dynamic perturbations. They also serve to clarify the nature of the dynamic bonding of nanoscale catalytic metal clusters with their supports, and the mediation of these properties due to the presence of adsorbates. These findings are supported by theoretical modeling and experimental data measured for an exemplary supported metal catalyst, Pt supported on silica, using in situ high energy resolution X-ray absorption and emission spectroscopies; in situ diffuse reflectance infrared Fourier transform spectroscopy; and ex situ scanning transmission electron microscopy.

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JO - Journal of Physical Chemistry C

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ER -

Intracluster Atomic and Electronic Structural Heterogeneities in Supported Nanoscale Metal Catalysts

Abstract

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