Hydrodeoxygenation of Levulinic Acid to γ-Valerolactone over Mesoporous Silica-Supported Cu-Ni Composite Catalysts

Monometallic (Cu, Ni) and bimetallic (Cu-Ni) catalysts supported on KIT-6 based mesoporous silica/zeolite composites were prepared using the wet impregnation method. The catalysts were characterized using X-ray powder diffraction, N<sub>2</sub> physisorption, SEM, solid state NMR and H&l...

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Main Authors: Margarita Popova, Ivalina Trendafilova, Manuela Oykova, Yavor Mitrev, Pavleta Shestakova, Magdolna R. Mihályi, Ágnes Szegedi
Format: Article
Language:English
Published: MDPI AG 2022-08-01
Series:Molecules
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Online Access:https://www.mdpi.com/1420-3049/27/17/5383
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author Margarita Popova
Ivalina Trendafilova
Manuela Oykova
Yavor Mitrev
Pavleta Shestakova
Magdolna R. Mihályi
Ágnes Szegedi
author_facet Margarita Popova
Ivalina Trendafilova
Manuela Oykova
Yavor Mitrev
Pavleta Shestakova
Magdolna R. Mihályi
Ágnes Szegedi
author_sort Margarita Popova
collection DOAJ
description Monometallic (Cu, Ni) and bimetallic (Cu-Ni) catalysts supported on KIT-6 based mesoporous silica/zeolite composites were prepared using the wet impregnation method. The catalysts were characterized using X-ray powder diffraction, N<sub>2</sub> physisorption, SEM, solid state NMR and H<sub>2</sub>-TPR methods. Finely dispersed NiO and CuO were detected after the decomposition of impregnating salt on the silica carrier. The formation of small fractions of ionic Ni<sup>2+</sup> and/or Cu<sup>2+</sup> species, interacting strongly with the silica supports, was found. The catalysts were studied in the gas-phase upgrading of lignocellulosic biomass-derived levulinic acid (LA) to γ-valerolactone (GVL). The bimetallic, CuNi-KIT-6 catalyst showed 100% LA conversion at 250 °C and atmospheric pressure. The high LA conversion and GVL yield can be attributed to the high specific surface area and finely dispersed Cu-Ni species in the catalyst. Furthermore, the catalyst also exhibited high stability after 24 h of reaction time with a GVL yield above 80% without any significant change in metal dispersion.
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spelling doaj.art-1c4bb03043514175a51a5dfbcf97c0882023-11-23T13:41:02ZengMDPI AGMolecules1420-30492022-08-012717538310.3390/molecules27175383Hydrodeoxygenation of Levulinic Acid to γ-Valerolactone over Mesoporous Silica-Supported Cu-Ni Composite CatalystsMargarita Popova0Ivalina Trendafilova1Manuela Oykova2Yavor Mitrev3Pavleta Shestakova4Magdolna R. Mihályi5Ágnes Szegedi6Institute of Organic Chemistry with Centre of Phytochemistry, Bulgarian Academy of Sciences, 1113 Sofia, BulgariaInstitute of Organic Chemistry with Centre of Phytochemistry, Bulgarian Academy of Sciences, 1113 Sofia, BulgariaInstitute of Organic Chemistry with Centre of Phytochemistry, Bulgarian Academy of Sciences, 1113 Sofia, BulgariaInstitute of Organic Chemistry with Centre of Phytochemistry, Bulgarian Academy of Sciences, 1113 Sofia, BulgariaInstitute of Organic Chemistry with Centre of Phytochemistry, Bulgarian Academy of Sciences, 1113 Sofia, BulgariaResearch Centre for Natural Sciences, Magyar Tudósok Körútja 2., 1117 Budapest, HungaryResearch Centre for Natural Sciences, Magyar Tudósok Körútja 2., 1117 Budapest, HungaryMonometallic (Cu, Ni) and bimetallic (Cu-Ni) catalysts supported on KIT-6 based mesoporous silica/zeolite composites were prepared using the wet impregnation method. The catalysts were characterized using X-ray powder diffraction, N<sub>2</sub> physisorption, SEM, solid state NMR and H<sub>2</sub>-TPR methods. Finely dispersed NiO and CuO were detected after the decomposition of impregnating salt on the silica carrier. The formation of small fractions of ionic Ni<sup>2+</sup> and/or Cu<sup>2+</sup> species, interacting strongly with the silica supports, was found. The catalysts were studied in the gas-phase upgrading of lignocellulosic biomass-derived levulinic acid (LA) to γ-valerolactone (GVL). The bimetallic, CuNi-KIT-6 catalyst showed 100% LA conversion at 250 °C and atmospheric pressure. The high LA conversion and GVL yield can be attributed to the high specific surface area and finely dispersed Cu-Ni species in the catalyst. Furthermore, the catalyst also exhibited high stability after 24 h of reaction time with a GVL yield above 80% without any significant change in metal dispersion.https://www.mdpi.com/1420-3049/27/17/5383lignocellulosic biomasslevulinic acidmesoporous silica compositesγ-valerolactonegas-phase hydrogenationsolid state NMR
spellingShingle Margarita Popova
Ivalina Trendafilova
Manuela Oykova
Yavor Mitrev
Pavleta Shestakova
Magdolna R. Mihályi
Ágnes Szegedi
Hydrodeoxygenation of Levulinic Acid to γ-Valerolactone over Mesoporous Silica-Supported Cu-Ni Composite Catalysts
Molecules
lignocellulosic biomass
levulinic acid
mesoporous silica composites
γ-valerolactone
gas-phase hydrogenation
solid state NMR
title Hydrodeoxygenation of Levulinic Acid to γ-Valerolactone over Mesoporous Silica-Supported Cu-Ni Composite Catalysts
title_full Hydrodeoxygenation of Levulinic Acid to γ-Valerolactone over Mesoporous Silica-Supported Cu-Ni Composite Catalysts
title_fullStr Hydrodeoxygenation of Levulinic Acid to γ-Valerolactone over Mesoporous Silica-Supported Cu-Ni Composite Catalysts
title_full_unstemmed Hydrodeoxygenation of Levulinic Acid to γ-Valerolactone over Mesoporous Silica-Supported Cu-Ni Composite Catalysts
title_short Hydrodeoxygenation of Levulinic Acid to γ-Valerolactone over Mesoporous Silica-Supported Cu-Ni Composite Catalysts
title_sort hydrodeoxygenation of levulinic acid to γ valerolactone over mesoporous silica supported cu ni composite catalysts
topic lignocellulosic biomass
levulinic acid
mesoporous silica composites
γ-valerolactone
gas-phase hydrogenation
solid state NMR
url https://www.mdpi.com/1420-3049/27/17/5383
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