One-pot catalytic hydrolysis/hydrogenation of cellobiose into hexitols over Ru/Al-MCM-48
The simultaneous catalytic hydrolysis and hydrogenation of cellobiose, as a model constituent of biomass has been studied over Ru/Al-MCM-48. The catalyst, presenting both acidic and hydrogenating functions has been synthesized and characterized by means of N2 adsorption-desorption, SAXS, H2-TPR, XRD...
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Published in: | Microporous and mesoporous materials Vol. 271; no. -; pp. 186 - 195 |
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15-11-2018
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Abstract | The simultaneous catalytic hydrolysis and hydrogenation of cellobiose, as a model constituent of biomass has been studied over Ru/Al-MCM-48. The catalyst, presenting both acidic and hydrogenating functions has been synthesized and characterized by means of N2 adsorption-desorption, SAXS, H2-TPR, XRD, TEM and NH3-TPD. A kinetic model is proposed, and possible reaction pathways and key intermediate compounds of conversion of cellobiose to hexitols are discussed. In the kinetic study the effects of pressure, temperature and time on the one-pot reaction were evaluated. A maximum yield around 91% of hexitols was achieved at 180 °C, 5 MPa of H2 and 7 min, where sorbitol was the main compound in the final product with 82% yield. Cellobitol was the main reaction intermediate. Temperatures in the range of 140–180 °C and pressures in the range of 3–5 MPa of H2 were studied and it was concluded that higher temperatures and pressures had a positive effect in order to maximize the production of hexitols. The developed kinetic model predicted with high accuracy the concentration of the different compounds involved in the proposed reaction pathway and served to calculate the reaction rate constant and activation energy values for the different steps of the catalytic process.
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•Ru/Al-MCM-48 exhibited higher activity than most catalytic systems reported.•High temperature and pressure enhance the production of hexitols.•Cellobitol was the main intermediate in the conversion of cellobiose to hexitols.•Development of kinetic model for the catalytic conversion of cellobiose to sorbitol.•Hydrolysis of cellobitol to sorbitol is the rate-determining step. |
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AbstractList | The simultaneous catalytic hydrolysis and hydrogenation of cellobiose, as a model constituent of biomass has been studied over Ru/Al-MCM-48. The catalyst, presenting both acidic and hydrogenating functions has been synthesized and characterized by means of N2 adsorption-desorption, SAXS, H2-TPR, XRD, TEM and NH3-TPD. A kinetic model is proposed, and possible reaction pathways and key intermediate compounds of conversion of cellobiose to hexitols are discussed. In the kinetic study the effects of pressure, temperature and time on the one-pot reaction were evaluated. A maximum yield around 91% of hexitols was achieved at 180 °C, 5 MPa of H2 and 7 min, where sorbitol was the main compound in the final product with 82% yield. Cellobitol was the main reaction intermediate. Temperatures in the range of 140–180 °C and pressures in the range of 3–5 MPa of H2 were studied and it was concluded that higher temperatures and pressures had a positive effect in order to maximize the production of hexitols. The developed kinetic model predicted with high accuracy the concentration of the different compounds involved in the proposed reaction pathway and served to calculate the reaction rate constant and activation energy values for the different steps of the catalytic process.
[Display omitted]
•Ru/Al-MCM-48 exhibited higher activity than most catalytic systems reported.•High temperature and pressure enhance the production of hexitols.•Cellobitol was the main intermediate in the conversion of cellobiose to hexitols.•Development of kinetic model for the catalytic conversion of cellobiose to sorbitol.•Hydrolysis of cellobitol to sorbitol is the rate-determining step. Ru/Al-MCM-48 |
Author | Pinel, C. Essayem, N. Alonso, E. Romero, A. Nieto-Márquez, A. Díaz, J.A. |
Author_xml | – sequence: 1 givenname: A. surname: Romero fullname: Romero, A. organization: High Pressure Processes Group, Chemical Engineering and Environmental Technology Department, Dr. Mergelina s/n, 47011, Valladolid, Spain – sequence: 2 givenname: J.A. surname: Díaz fullname: Díaz, J.A. organization: Catalonia Institute for Energy Research, Jardins de les Dones de Negre, 1 2 Pl, Sant Adria de Besòs, 08930, Spain – sequence: 3 givenname: A. orcidid: 0000-0003-2784-787X surname: Nieto-Márquez fullname: Nieto-Márquez, A. email: antonio.nieto@upm.es organization: Mechanical, Chemical and Industrial Design Engineering Department, Technical University of Madrid (UPM), Ronda de Valencia 3, 28012 Madrid, Spain – sequence: 4 givenname: N. surname: Essayem fullname: Essayem, N. organization: Université Lyon, CNRS, Université Claude Bernard Lyon 1, IRCELYON, UMR 5256, F-69626, Villeurbanne, France – sequence: 5 givenname: E. orcidid: 0000-0002-7995-7993 surname: Alonso fullname: Alonso, E. organization: High Pressure Processes Group, Chemical Engineering and Environmental Technology Department, Dr. Mergelina s/n, 47011, Valladolid, Spain – sequence: 6 givenname: C. surname: Pinel fullname: Pinel, C. organization: Université Lyon, CNRS, Université Claude Bernard Lyon 1, IRCELYON, UMR 5256, F-69626, Villeurbanne, France |
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CitedBy_id | crossref_primary_10_1016_j_micromeso_2019_05_035 crossref_primary_10_1021_acssuschemeng_1c04141 crossref_primary_10_1021_acssuschemeng_2c05412 crossref_primary_10_1016_j_matchemphys_2020_124146 crossref_primary_10_1021_acssuschemeng_4c00749 |
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Keywords | Sorbitol Ru/Al-MCM-48 Cellobiose Hexitols Hydrolysis/hydrogenation |
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Snippet | The simultaneous catalytic hydrolysis and hydrogenation of cellobiose, as a model constituent of biomass has been studied over Ru/Al-MCM-48. The catalyst,... Ru/Al-MCM-48 |
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SubjectTerms | Catalysis Cellobiose Chemical Sciences Environment and Society Environmental Sciences Hexitols Hydrolysis/hydrogenation Ru/Al-MCM-48 Sorbitol |
Title | One-pot catalytic hydrolysis/hydrogenation of cellobiose into hexitols over Ru/Al-MCM-48 |
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