X-ray tomography measurements identify structure-reactivity correlations in catalysts for oxygenates coupling reactions

Konstantinos A. Goulas; Shahar Dery; Paul Dietrich; Gregory R. Johnson; Adam Grippo; Young Chung Wang; Elad Gross

doi:10.1016/j.cattod.2018.12.012

X-ray tomography measurements identify structure-reactivity correlations in catalysts for oxygenates coupling reactions

Konstantinos A. Goulas, Shahar Dery, Paul Dietrich, Gregory R. Johnson, Adam Grippo, Young Chung Wang, Elad Gross^*

^*Corresponding author for this work

Institute of Chemistry

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

8 Scopus citations

Abstract

The impact of tandem dehydrogenation-aldol condensation reactions on the structure of oxide-supported PdCu catalysts was studied by a combination of X-ray tomography measurements, ensemble-averaging spectroscopy techniques and reactivity measurements. X-ray tomography measurements generated 3D images at submicron resolution of the packed catalyst in the flow reactor following its exposure to various reaction conditions. Quantitative analysis of the tomography data revealed that exposure of the catalyst to reaction conditions induced structural deformation of the mixed Mg-Al oxide supports, accompanied by sintering of the PdCu nanoparticles into micron-sized aggregates. Improved stability was achieved once the PdCu particles were supported on an oxide, such as anatase TiO₂, which does not undergo restructuring or phase transition under reaction conditions. This study demonstrates that structural information extracted by X-ray tomography measurements may uncover important structure-reactivity correlations and identify the reasons for catalysts deactivation.

Original language	English
Pages (from-to)	186-192
Number of pages	7
Journal	Catalysis Today
Volume	336
DOIs	https://doi.org/10.1016/j.cattod.2018.12.012
State	Published - 1 Oct 2019

Bibliographical note

Publisher Copyright:
© 2018 Elsevier B.V.

Keywords

Aldol-condensation
Hydrotalcite
Metal-oxide
Pd-Cu nanoparticles
X-ray tomography

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10.1016/j.cattod.2018.12.012

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title = "X-ray tomography measurements identify structure-reactivity correlations in catalysts for oxygenates coupling reactions",

abstract = "The impact of tandem dehydrogenation-aldol condensation reactions on the structure of oxide-supported PdCu catalysts was studied by a combination of X-ray tomography measurements, ensemble-averaging spectroscopy techniques and reactivity measurements. X-ray tomography measurements generated 3D images at submicron resolution of the packed catalyst in the flow reactor following its exposure to various reaction conditions. Quantitative analysis of the tomography data revealed that exposure of the catalyst to reaction conditions induced structural deformation of the mixed Mg-Al oxide supports, accompanied by sintering of the PdCu nanoparticles into micron-sized aggregates. Improved stability was achieved once the PdCu particles were supported on an oxide, such as anatase TiO2, which does not undergo restructuring or phase transition under reaction conditions. This study demonstrates that structural information extracted by X-ray tomography measurements may uncover important structure-reactivity correlations and identify the reasons for catalysts deactivation.",

keywords = "Aldol-condensation, Hydrotalcite, Metal-oxide, Pd-Cu nanoparticles, X-ray tomography",

author = "Goulas, {Konstantinos A.} and Shahar Dery and Paul Dietrich and Johnson, {Gregory R.} and Adam Grippo and Wang, {Young Chung} and Elad Gross",

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year = "2019",

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doi = "10.1016/j.cattod.2018.12.012",

language = "אנגלית",

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AU - Goulas, Konstantinos A.

AU - Dery, Shahar

AU - Dietrich, Paul

AU - Johnson, Gregory R.

AU - Grippo, Adam

AU - Wang, Young Chung

AU - Gross, Elad

PY - 2019/10/1

Y1 - 2019/10/1

N2 - The impact of tandem dehydrogenation-aldol condensation reactions on the structure of oxide-supported PdCu catalysts was studied by a combination of X-ray tomography measurements, ensemble-averaging spectroscopy techniques and reactivity measurements. X-ray tomography measurements generated 3D images at submicron resolution of the packed catalyst in the flow reactor following its exposure to various reaction conditions. Quantitative analysis of the tomography data revealed that exposure of the catalyst to reaction conditions induced structural deformation of the mixed Mg-Al oxide supports, accompanied by sintering of the PdCu nanoparticles into micron-sized aggregates. Improved stability was achieved once the PdCu particles were supported on an oxide, such as anatase TiO2, which does not undergo restructuring or phase transition under reaction conditions. This study demonstrates that structural information extracted by X-ray tomography measurements may uncover important structure-reactivity correlations and identify the reasons for catalysts deactivation.

AB - The impact of tandem dehydrogenation-aldol condensation reactions on the structure of oxide-supported PdCu catalysts was studied by a combination of X-ray tomography measurements, ensemble-averaging spectroscopy techniques and reactivity measurements. X-ray tomography measurements generated 3D images at submicron resolution of the packed catalyst in the flow reactor following its exposure to various reaction conditions. Quantitative analysis of the tomography data revealed that exposure of the catalyst to reaction conditions induced structural deformation of the mixed Mg-Al oxide supports, accompanied by sintering of the PdCu nanoparticles into micron-sized aggregates. Improved stability was achieved once the PdCu particles were supported on an oxide, such as anatase TiO2, which does not undergo restructuring or phase transition under reaction conditions. This study demonstrates that structural information extracted by X-ray tomography measurements may uncover important structure-reactivity correlations and identify the reasons for catalysts deactivation.

KW - Aldol-condensation

KW - Hydrotalcite

KW - Metal-oxide

KW - Pd-Cu nanoparticles

KW - X-ray tomography

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SN - 0920-5861

VL - 336

SP - 186

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JO - Catalysis Today

JF - Catalysis Today

ER -

X-ray tomography measurements identify structure-reactivity correlations in catalysts for oxygenates coupling reactions

Abstract

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Keywords

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