Rate enhancement by Cu in NixCu1-x/ZrO2 bimetallic catalysts for hydrodeoxygenation of stearic acid

Christoph Denk; Sebastian Foraita; Libor Kovarik; Kelsey Stoerzinger; Yue Liu; Eszter Baráth; Johannes A. Lercher

doi:10.1039/c9cy00181f

Rate enhancement by Cu in Ni_xCu_1-x/ZrO₂ bimetallic catalysts for hydrodeoxygenation of stearic acid

Christoph Denk, Sebastian Foraita, Libor Kovarik, Kelsey Stoerzinger, Yue Liu, Eszter Baráth, Johannes A. Lercher

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

19 Scopus citations

Abstract

Hydrodeoxygenation of stearic acid on Ni/ZrO₂ to n-heptadecane occurs via the reduction to 1-octadecanal, followed by decarbonylation of the aldehyde to n-heptadecane. Stearic acid binds stronger than 1-octadecanal on Ni, causing decarbonylation to start only once stearic acid is almost fully converted. This first step is enhanced by addition of Cu either in the form of Cu/ZrO₂ or in the form of a ZrO₂ supported Ni_xCu_1-x nano-alloy. Cu has not only a higher activity for the reduction of stearic acid, it also increases the activity of Ni for decarbonylation of 1-octadecanal by increasing the electron density of Ni in the bimetal catalyst. The combination of these two effects leads to high activity of Ni-Cu bimetallic catalysts.

Original language	English (US)
Pages (from-to)	2620-2629
Number of pages	10
Journal	Catalysis Science and Technology
Volume	9
Issue number	10
DOIs	https://doi.org/10.1039/c9cy00181f
State	Published - 2019
Externally published	Yes

Bibliographical note

Funding Information:
The financial support is highly appreciated of the AlgenFlugKraft (FKZ LABAY74A) project, sponsored by Bavarian Ministry of Economic Affairs and Media, Energy and Technology (“Bayerisches Staatsministerium für Wirtschaft und Medien, Energie und Technologie”) and Bavarian State Ministry of Education, Science and the Arts (“Bayerisches Staatsministerium für Bildung und Kultus, Wissenschaft und Kunst”). C. D., L. K., K. S., and J. A. L. were supported by the US Department of Energy (DOE), Office of Basic Energy Sciences (BES), Division of Chemical Sciences, Geosciences & Biosciences. A portion of the research was performed using EMSL, a national scientific user facility sponsored by the Department of Energy's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory. We thank Franz-Xaver Hecht for help with N2-sorption and H2-chemisorption, Martin Neukamm for AAS measurements.

Publisher Copyright:
© 2019 The Royal Society of Chemistry.

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title = "Rate enhancement by Cu in NixCu1-x/ZrO2 bimetallic catalysts for hydrodeoxygenation of stearic acid",

abstract = "Hydrodeoxygenation of stearic acid on Ni/ZrO2 to n-heptadecane occurs via the reduction to 1-octadecanal, followed by decarbonylation of the aldehyde to n-heptadecane. Stearic acid binds stronger than 1-octadecanal on Ni, causing decarbonylation to start only once stearic acid is almost fully converted. This first step is enhanced by addition of Cu either in the form of Cu/ZrO2 or in the form of a ZrO2 supported NixCu1-x nano-alloy. Cu has not only a higher activity for the reduction of stearic acid, it also increases the activity of Ni for decarbonylation of 1-octadecanal by increasing the electron density of Ni in the bimetal catalyst. The combination of these two effects leads to high activity of Ni-Cu bimetallic catalysts.",

author = "Christoph Denk and Sebastian Foraita and Libor Kovarik and Kelsey Stoerzinger and Yue Liu and Eszter Bar{\'a}th and Lercher, {Johannes A.}",

note = "Funding Information: The financial support is highly appreciated of the AlgenFlugKraft (FKZ LABAY74A) project, sponsored by Bavarian Ministry of Economic Affairs and Media, Energy and Technology (“Bayerisches Staatsministerium f{\"u}r Wirtschaft und Medien, Energie und Technologie”) and Bavarian State Ministry of Education, Science and the Arts (“Bayerisches Staatsministerium f{\"u}r Bildung und Kultus, Wissenschaft und Kunst”). C. D., L. K., K. S., and J. A. L. were supported by the US Department of Energy (DOE), Office of Basic Energy Sciences (BES), Division of Chemical Sciences, Geosciences & Biosciences. A portion of the research was performed using EMSL, a national scientific user facility sponsored by the Department of Energy's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory. We thank Franz-Xaver Hecht for help with N2-sorption and H2-chemisorption, Martin Neukamm for AAS measurements. Publisher Copyright: {\textcopyright} 2019 The Royal Society of Chemistry.",

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AU - Stoerzinger, Kelsey

AU - Liu, Yue

AU - Baráth, Eszter

AU - Lercher, Johannes A.

N1 - Funding Information: The financial support is highly appreciated of the AlgenFlugKraft (FKZ LABAY74A) project, sponsored by Bavarian Ministry of Economic Affairs and Media, Energy and Technology (“Bayerisches Staatsministerium für Wirtschaft und Medien, Energie und Technologie”) and Bavarian State Ministry of Education, Science and the Arts (“Bayerisches Staatsministerium für Bildung und Kultus, Wissenschaft und Kunst”). C. D., L. K., K. S., and J. A. L. were supported by the US Department of Energy (DOE), Office of Basic Energy Sciences (BES), Division of Chemical Sciences, Geosciences & Biosciences. A portion of the research was performed using EMSL, a national scientific user facility sponsored by the Department of Energy's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory. We thank Franz-Xaver Hecht for help with N2-sorption and H2-chemisorption, Martin Neukamm for AAS measurements. Publisher Copyright: © 2019 The Royal Society of Chemistry.

PY - 2019

Y1 - 2019

N2 - Hydrodeoxygenation of stearic acid on Ni/ZrO2 to n-heptadecane occurs via the reduction to 1-octadecanal, followed by decarbonylation of the aldehyde to n-heptadecane. Stearic acid binds stronger than 1-octadecanal on Ni, causing decarbonylation to start only once stearic acid is almost fully converted. This first step is enhanced by addition of Cu either in the form of Cu/ZrO2 or in the form of a ZrO2 supported NixCu1-x nano-alloy. Cu has not only a higher activity for the reduction of stearic acid, it also increases the activity of Ni for decarbonylation of 1-octadecanal by increasing the electron density of Ni in the bimetal catalyst. The combination of these two effects leads to high activity of Ni-Cu bimetallic catalysts.

AB - Hydrodeoxygenation of stearic acid on Ni/ZrO2 to n-heptadecane occurs via the reduction to 1-octadecanal, followed by decarbonylation of the aldehyde to n-heptadecane. Stearic acid binds stronger than 1-octadecanal on Ni, causing decarbonylation to start only once stearic acid is almost fully converted. This first step is enhanced by addition of Cu either in the form of Cu/ZrO2 or in the form of a ZrO2 supported NixCu1-x nano-alloy. Cu has not only a higher activity for the reduction of stearic acid, it also increases the activity of Ni for decarbonylation of 1-octadecanal by increasing the electron density of Ni in the bimetal catalyst. The combination of these two effects leads to high activity of Ni-Cu bimetallic catalysts.

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