Oxidation of 2,5-diformfylfuran to ...
Document type :
Article dans une revue scientifique: Article original
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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
Author(s) :
Decarpigny, Cedric [Auteur]
Bleta, Rudina [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Ponchel, Anne [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Monflier, Eric [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Bleta, Rudina [Auteur]

Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Ponchel, Anne [Auteur]

Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Monflier, Eric [Auteur]

Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Journal title :
Colloids and surfaces. B, Biointerfaces
Abbreviated title :
Colloids Surf B Biointerfaces
Volume number :
200
Pages :
111606
Publication date :
2021-02-05
ISSN :
1873-4367
HAL domain(s) :
Chimie/Catalyse
English abstract : [en]
Hypothesis: Porous 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 ...
Show more >Hypothesis: Porous 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. Experiments: Silica 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 N2-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. Findings: Results 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-1vs. 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.Show less >
Show more >Hypothesis: Porous 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. Experiments: Silica 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 N2-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. Findings: Results 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-1vs. 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.Show less >
Language :
Anglais
Audience :
Internationale
Popular science :
Non
Administrative institution(s) :
CNRS
Centrale Lille
ENSCL
Univ. Artois
Université de Lille
Centrale Lille
ENSCL
Univ. Artois
Université de Lille
Collections :
Research team(s) :
Catalyse et chimie supramoléculaire (CASU)
Submission date :
2022-03-02T07:13:03Z
2023-12-15T19:50:58Z
2023-12-15T19:50:58Z
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