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

62 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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10.1002/cssc.201500331

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@article{c3597039112b48cfa762982d3f151778,

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,

day = "10",

doi = "10.1002/cssc.201500331",

language = "English",

volume = "8",

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journal = "ChemSusChem",

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T1 - Acid-Functionalized Mesoporous Carbon

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

UR - https://www.scopus.com/pages/publications/84939463794

U2 - 10.1002/cssc.201500331

DO - 10.1002/cssc.201500331

M3 - Article

C2 - 26089180

AN - SCOPUS:84939463794

SN - 1864-5631

VL - 8

SP - 2520

EP - 2528

JO - ChemSusChem

JF - ChemSusChem

IS - 15

ER -

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

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Keywords

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