Acid-Functionalized Mesoporous Carbon: An Efficient Support for Ruthenium-Catalyzed γ-Valerolactone Production

Alberto Villa; Marco Schiavoni; Carine E. Chan-Thaw; Pasquale F. Fulvio; Richard T. Mayes; Sheng Dai; Karren L. More; Gabriel M. Veith; Laura Prati

doi:10.1002/cssc.201500331

Acid-Functionalized Mesoporous Carbon: An Efficient Support for Ruthenium-Catalyzed γ-Valerolactone Production

Alberto Villa, Marco Schiavoni, Carine E. Chan-Thaw, Pasquale F. Fulvio, Richard T. Mayes, Sheng Dai, Karren L. More, Gabriel M. Veith, Laura Prati

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

58 Scopus citations

Abstract

The hydrogenation of levulinic acid has been studied using Ru supported on ordered mesoporous carbons (OMCs) prepared by soft-templating. P- and S-containing acid groups were introduced by postsynthetic functionalization before the addition of 1 Ru by incipient wetness impregnation. These functionalities and the reaction conditions mediate the activity and selectivity of the levulinic acid hydrogenation. The presence of S-containing groups (Ru/OMC-S and Ru/OMC-P/S) deactivates the Ru catalysts strongly, whereas the presence of P-containing groups (Ru/OMC-P) enhances the activity compared to that of pristine Ru/OMC. Under mild conditions (70C and 7bar H₂) the catalyst shows high selectivity to γ-valerolactone (GVL; >95) and high stability on recycling. However, under more severe conditions (200C and pH2=40bar) Ru/OMC-P is particularly able to promote GVL ring-opening and the consecutive hydrogenation to pentanoic acid.

Original language	English
Pages (from-to)	2520-2528
Number of pages	9
Journal	ChemSusChem
Volume	8
Issue number	15
DOIs	https://doi.org/10.1002/cssc.201500331
State	Published - Aug 10 2015

Keywords

carbon
hydrogenation
mesoporous materials
ruthenium
supported catalysts

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This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1002/cssc.201500331

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title = "Acid-Functionalized Mesoporous Carbon: An Efficient Support for Ruthenium-Catalyzed γ-Valerolactone Production",

abstract = "The hydrogenation of levulinic acid has been studied using Ru supported on ordered mesoporous carbons (OMCs) prepared by soft-templating. P- and S-containing acid groups were introduced by postsynthetic functionalization before the addition of 1 Ru by incipient wetness impregnation. These functionalities and the reaction conditions mediate the activity and selectivity of the levulinic acid hydrogenation. The presence of S-containing groups (Ru/OMC-S and Ru/OMC-P/S) deactivates the Ru catalysts strongly, whereas the presence of P-containing groups (Ru/OMC-P) enhances the activity compared to that of pristine Ru/OMC. Under mild conditions (70C and 7bar H2) the catalyst shows high selectivity to γ-valerolactone (GVL; >95) and high stability on recycling. However, under more severe conditions (200C and pH2=40bar) Ru/OMC-P is particularly able to promote GVL ring-opening and the consecutive hydrogenation to pentanoic acid.",

keywords = "carbon, hydrogenation, mesoporous materials, ruthenium, supported catalysts",

author = "Alberto Villa and Marco Schiavoni and Chan-Thaw, {Carine E.} and Fulvio, {Pasquale F.} and Mayes, {Richard T.} and Sheng Dai and More, {Karren L.} and Veith, {Gabriel M.} and Laura Prati",

note = "Publisher Copyright: {\textcopyright} 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.",

year = "2015",

month = aug,

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doi = "10.1002/cssc.201500331",

language = "English",

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T2 - An Efficient Support for Ruthenium-Catalyzed γ-Valerolactone Production

AU - Villa, Alberto

AU - Schiavoni, Marco

AU - Chan-Thaw, Carine E.

AU - Fulvio, Pasquale F.

AU - Mayes, Richard T.

AU - Dai, Sheng

AU - More, Karren L.

AU - Veith, Gabriel M.

AU - Prati, Laura

PY - 2015/8/10

Y1 - 2015/8/10

N2 - The hydrogenation of levulinic acid has been studied using Ru supported on ordered mesoporous carbons (OMCs) prepared by soft-templating. P- and S-containing acid groups were introduced by postsynthetic functionalization before the addition of 1 Ru by incipient wetness impregnation. These functionalities and the reaction conditions mediate the activity and selectivity of the levulinic acid hydrogenation. The presence of S-containing groups (Ru/OMC-S and Ru/OMC-P/S) deactivates the Ru catalysts strongly, whereas the presence of P-containing groups (Ru/OMC-P) enhances the activity compared to that of pristine Ru/OMC. Under mild conditions (70C and 7bar H2) the catalyst shows high selectivity to γ-valerolactone (GVL; >95) and high stability on recycling. However, under more severe conditions (200C and pH2=40bar) Ru/OMC-P is particularly able to promote GVL ring-opening and the consecutive hydrogenation to pentanoic acid.

AB - The hydrogenation of levulinic acid has been studied using Ru supported on ordered mesoporous carbons (OMCs) prepared by soft-templating. P- and S-containing acid groups were introduced by postsynthetic functionalization before the addition of 1 Ru by incipient wetness impregnation. These functionalities and the reaction conditions mediate the activity and selectivity of the levulinic acid hydrogenation. The presence of S-containing groups (Ru/OMC-S and Ru/OMC-P/S) deactivates the Ru catalysts strongly, whereas the presence of P-containing groups (Ru/OMC-P) enhances the activity compared to that of pristine Ru/OMC. Under mild conditions (70C and 7bar H2) the catalyst shows high selectivity to γ-valerolactone (GVL; >95) and high stability on recycling. However, under more severe conditions (200C and pH2=40bar) Ru/OMC-P is particularly able to promote GVL ring-opening and the consecutive hydrogenation to pentanoic acid.

KW - carbon

KW - hydrogenation

KW - mesoporous materials

KW - ruthenium

KW - supported catalysts

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JO - ChemSusChem

JF - ChemSusChem

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ER -

Acid-Functionalized Mesoporous Carbon: An Efficient Support for Ruthenium-Catalyzed γ-Valerolactone Production

Abstract

Keywords

UN SDGs

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