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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 Scontaining 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 (70 8C and 7 bar H2) the catalyst shows high selectivity to g-valerolactone (GVL; >95%) and high stability on recycling. However, under more severe conditions (200 8C and pH2=40 bar) Ru/OMC-P is particularly able to promote GVL ring-opening and the consecutive hydrogenation to pentanoic acid.

Authors:
 [1];  [1];  [1];  [2];  [3];  [4];  [5];  [5];  [1]
  1. Univ. of Milan (Italy)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Puerto Rico, San Juan (Puerto Rico)
  3. Univ. of Puerto Rico, San Juan (Puerto Rico)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1265712
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
ChemSusChem
Additional Journal Information:
Journal Volume: 8; Journal Issue: 15; Journal ID: ISSN 1864-5631
Publisher:
ChemPubSoc Europe
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Villa, Alberto, Schiavoni, Marco, Chan-Thaw, Carine E., Fulvio, Pasquale F., Mayes, Richard T., Dai, Sheng, More, Karren L., Veith, Gabriel M., and Prati, Laura. Acid-Functionalized Mesoporous Carbon: An Efficient Support for Ruthenium-Catalyzed γ-Valerolactone Production. United States: N. p., 2015. Web. doi:10.1002/cssc.201500331.
Villa, Alberto, Schiavoni, Marco, Chan-Thaw, Carine E., Fulvio, Pasquale F., Mayes, Richard T., Dai, Sheng, More, Karren L., Veith, Gabriel M., & Prati, Laura. Acid-Functionalized Mesoporous Carbon: An Efficient Support for Ruthenium-Catalyzed γ-Valerolactone Production. United States. doi:10.1002/cssc.201500331.
Villa, Alberto, Schiavoni, Marco, Chan-Thaw, Carine E., Fulvio, Pasquale F., Mayes, Richard T., Dai, Sheng, More, Karren L., Veith, Gabriel M., and Prati, Laura. Thu . "Acid-Functionalized Mesoporous Carbon: An Efficient Support for Ruthenium-Catalyzed γ-Valerolactone Production". United States. doi:10.1002/cssc.201500331. https://www.osti.gov/servlets/purl/1265712.
@article{osti_1265712,
title = {Acid-Functionalized Mesoporous Carbon: An Efficient Support for Ruthenium-Catalyzed γ-Valerolactone Production},
author = {Villa, Alberto and Schiavoni, Marco and Chan-Thaw, Carine E. and Fulvio, Pasquale F. and Mayes, Richard T. and Dai, Sheng and More, Karren L. and Veith, Gabriel M. and Prati, Laura},
abstractNote = {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 Scontaining 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 (70 8C and 7 bar H2) the catalyst shows high selectivity to g-valerolactone (GVL; >95%) and high stability on recycling. However, under more severe conditions (200 8C and pH2=40 bar) Ru/OMC-P is particularly able to promote GVL ring-opening and the consecutive hydrogenation to pentanoic acid.},
doi = {10.1002/cssc.201500331},
journal = {ChemSusChem},
number = 15,
volume = 8,
place = {United States},
year = {2015},
month = {6}
}

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    Works referencing / citing this record:

    Quantifying Morphology and Diffusion Properties of Mesoporous Carbon From High-Fidelity 3D Reconstructions
    journal, June 2019