Oxidation of 2,5-diformfylfuran to 2,5-furandicarboxylic acid catalyzed by Candida antarctica Lipase B immobilized in a cyclodextrin-templated mesoporous silica. The critical role of pore characteristics on the catalytic performance
International audience HypothesisPorous silica has been extensively used as suitable carrier for the immobilization of various enzymes. Randomly Methylated β-Cyclodextrin (RaMeβCD) has surface active properties and very high solubility in water and could therefore be used as template in the fabricat...
Published in: | Colloids and Surfaces B: Biointerfaces |
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Format: | Article in Journal/Newspaper |
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Online Access: | https://hal.archives-ouvertes.fr/hal-03190872 https://doi.org/10.1016/j.colsurfb.2021.111606 |
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ftccsdartic:oai:HAL:hal-03190872v1 2023-05-15T13:48:18+02:00 Oxidation of 2,5-diformfylfuran to 2,5-furandicarboxylic acid catalyzed by Candida antarctica Lipase B immobilized in a cyclodextrin-templated mesoporous silica. The critical role of pore characteristics on the catalytic performance Decarpigny, Cédric Bleta, Rudina Ponchel, Anne Monflier, Eric Unité de Catalyse et Chimie du Solide - UMR 8181 (UCCS) Centrale Lille Institut (CLIL)-Université d'Artois (UA)-Centrale Lille-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Lille 2021-04 https://hal.archives-ouvertes.fr/hal-03190872 https://doi.org/10.1016/j.colsurfb.2021.111606 en eng HAL CCSD Elsevier info:eu-repo/semantics/altIdentifier/doi/10.1016/j.colsurfb.2021.111606 hal-03190872 https://hal.archives-ouvertes.fr/hal-03190872 doi:10.1016/j.colsurfb.2021.111606 ISSN: 0927-7765 Colloids and Surfaces B: Biointerfaces https://hal.archives-ouvertes.fr/hal-03190872 Colloids and Surfaces B: Biointerfaces, Elsevier, 2021, 200, pp.111606. ⟨10.1016/j.colsurfb.2021.111606⟩ [CHIM]Chemical Sciences [CHIM.CATA]Chemical Sciences/Catalysis info:eu-repo/semantics/article Journal articles 2021 ftccsdartic https://doi.org/10.1016/j.colsurfb.2021.111606 2021-12-19T00:18:57Z International audience HypothesisPorous silica has been extensively used as suitable carrier for the immobilization of various enzymes. Randomly Methylated β-Cyclodextrin (RaMeβCD) has surface active properties and very high solubility in water and could therefore be used as template in the fabrication of silica particles with tunable pore size.ExperimentsSilica particles were prepared by sol-gel process in alkaline medium with and without use of RaMeβCD. Lipase Bfrom Candida antarctica (CALB) was either incorporated within the pores of RaMeβCD-derived support or covalently attached on the surface of CD-free silica particles and its catalytic performance was assayed in the oxidation of 2,5-diformylfuran (DFF) to 2,5-furandicarboxylic acid (FDCA). Enzymatic reactors were characterized by N 2 -adsorption analysis, small angle XRD, TG/DSC experiments, ATR-FTIR spectroscopy, HR-TEM and LSCM, while reaction products were determined based on 1H NMR spectroscopy combined with HPLC.FindingsResults showed that the use of RaMeβCD as structure directing agent led to mesoporous silica composed of uniform 8 nm-sized particles with 11 nm-sized mesopores compatible with the dimensions of CALB (3.0 nm × 4.0 nm × 5.0 nm). Incorporation of CALB within the pores of RaMeβCD-derived silica caused almost a two-fold increase in specific activity after 7 h at 40 °C when compared to lipase immobilized on the surface of CD-free silica particles (33.2 μmol g −1 min −1 vs. 14.4 μmol g −1 min −1 ). Moreover, the RaMeβCD-derived biocatalyst demonstrated enhanced operational stability during the recycling experiments, retaining more than 90% of its initial activity after five 24 h-reaction cycles. These findings open up new avenues for future research on the use of cyclodextrins in the development of enzyme-based nanoreactors. Article in Journal/Newspaper Antarc* Antarctica Archive ouverte HAL (Hyper Article en Ligne, CCSD - Centre pour la Communication Scientifique Directe) Colloids and Surfaces B: Biointerfaces 200 111606 |
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Open Polar |
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Archive ouverte HAL (Hyper Article en Ligne, CCSD - Centre pour la Communication Scientifique Directe) |
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ftccsdartic |
language |
English |
topic |
[CHIM]Chemical Sciences [CHIM.CATA]Chemical Sciences/Catalysis |
spellingShingle |
[CHIM]Chemical Sciences [CHIM.CATA]Chemical Sciences/Catalysis Decarpigny, Cédric Bleta, Rudina Ponchel, Anne Monflier, Eric Oxidation of 2,5-diformfylfuran to 2,5-furandicarboxylic acid catalyzed by Candida antarctica Lipase B immobilized in a cyclodextrin-templated mesoporous silica. The critical role of pore characteristics on the catalytic performance |
topic_facet |
[CHIM]Chemical Sciences [CHIM.CATA]Chemical Sciences/Catalysis |
description |
International audience HypothesisPorous silica has been extensively used as suitable carrier for the immobilization of various enzymes. Randomly Methylated β-Cyclodextrin (RaMeβCD) has surface active properties and very high solubility in water and could therefore be used as template in the fabrication of silica particles with tunable pore size.ExperimentsSilica particles were prepared by sol-gel process in alkaline medium with and without use of RaMeβCD. Lipase Bfrom Candida antarctica (CALB) was either incorporated within the pores of RaMeβCD-derived support or covalently attached on the surface of CD-free silica particles and its catalytic performance was assayed in the oxidation of 2,5-diformylfuran (DFF) to 2,5-furandicarboxylic acid (FDCA). Enzymatic reactors were characterized by N 2 -adsorption analysis, small angle XRD, TG/DSC experiments, ATR-FTIR spectroscopy, HR-TEM and LSCM, while reaction products were determined based on 1H NMR spectroscopy combined with HPLC.FindingsResults showed that the use of RaMeβCD as structure directing agent led to mesoporous silica composed of uniform 8 nm-sized particles with 11 nm-sized mesopores compatible with the dimensions of CALB (3.0 nm × 4.0 nm × 5.0 nm). Incorporation of CALB within the pores of RaMeβCD-derived silica caused almost a two-fold increase in specific activity after 7 h at 40 °C when compared to lipase immobilized on the surface of CD-free silica particles (33.2 μmol g −1 min −1 vs. 14.4 μmol g −1 min −1 ). Moreover, the RaMeβCD-derived biocatalyst demonstrated enhanced operational stability during the recycling experiments, retaining more than 90% of its initial activity after five 24 h-reaction cycles. These findings open up new avenues for future research on the use of cyclodextrins in the development of enzyme-based nanoreactors. |
author2 |
Unité de Catalyse et Chimie du Solide - UMR 8181 (UCCS) Centrale Lille Institut (CLIL)-Université d'Artois (UA)-Centrale Lille-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Lille |
format |
Article in Journal/Newspaper |
author |
Decarpigny, Cédric Bleta, Rudina Ponchel, Anne Monflier, Eric |
author_facet |
Decarpigny, Cédric Bleta, Rudina Ponchel, Anne Monflier, Eric |
author_sort |
Decarpigny, Cédric |
title |
Oxidation of 2,5-diformfylfuran to 2,5-furandicarboxylic acid catalyzed by Candida antarctica Lipase B immobilized in a cyclodextrin-templated mesoporous silica. The critical role of pore characteristics on the catalytic performance |
title_short |
Oxidation of 2,5-diformfylfuran to 2,5-furandicarboxylic acid catalyzed by Candida antarctica Lipase B immobilized in a cyclodextrin-templated mesoporous silica. The critical role of pore characteristics on the catalytic performance |
title_full |
Oxidation of 2,5-diformfylfuran to 2,5-furandicarboxylic acid catalyzed by Candida antarctica Lipase B immobilized in a cyclodextrin-templated mesoporous silica. The critical role of pore characteristics on the catalytic performance |
title_fullStr |
Oxidation of 2,5-diformfylfuran to 2,5-furandicarboxylic acid catalyzed by Candida antarctica Lipase B immobilized in a cyclodextrin-templated mesoporous silica. The critical role of pore characteristics on the catalytic performance |
title_full_unstemmed |
Oxidation of 2,5-diformfylfuran to 2,5-furandicarboxylic acid catalyzed by Candida antarctica Lipase B immobilized in a cyclodextrin-templated mesoporous silica. The critical role of pore characteristics on the catalytic performance |
title_sort |
oxidation of 2,5-diformfylfuran to 2,5-furandicarboxylic acid catalyzed by candida antarctica lipase b immobilized in a cyclodextrin-templated mesoporous silica. the critical role of pore characteristics on the catalytic performance |
publisher |
HAL CCSD |
publishDate |
2021 |
url |
https://hal.archives-ouvertes.fr/hal-03190872 https://doi.org/10.1016/j.colsurfb.2021.111606 |
genre |
Antarc* Antarctica |
genre_facet |
Antarc* Antarctica |
op_source |
ISSN: 0927-7765 Colloids and Surfaces B: Biointerfaces https://hal.archives-ouvertes.fr/hal-03190872 Colloids and Surfaces B: Biointerfaces, Elsevier, 2021, 200, pp.111606. ⟨10.1016/j.colsurfb.2021.111606⟩ |
op_relation |
info:eu-repo/semantics/altIdentifier/doi/10.1016/j.colsurfb.2021.111606 hal-03190872 https://hal.archives-ouvertes.fr/hal-03190872 doi:10.1016/j.colsurfb.2021.111606 |
op_doi |
https://doi.org/10.1016/j.colsurfb.2021.111606 |
container_title |
Colloids and Surfaces B: Biointerfaces |
container_volume |
200 |
container_start_page |
111606 |
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