mt9b00646_si_001.pdf (1.15 MB)
Confinement of Candida Antarctica Lipase B in a Multifunctional Cyclodextrin-Derived Silicified Hydrogel and Its Application as Enzymatic Nanoreactor
journal contribution
posted on 2019-11-20, 15:30 authored by Cédric Decarpigny, Rudina Bleta, Anne Ponchel, Eric MonflierSupramolecular
hydrogels with a three-dimensional cross-linked
macromolecular network have attracted growing scientific interest
in recent years because of their ability to incorporate high loadings
of bioactive molecules such as drugs, proteins, antibodies, peptides,
and genes. Herein, we report a versatile approach for the confinement
of Candida antarctica lipase B (CALB) within a silica-strengthened
cyclodextrin-derived supramolecular hydrogel and demonstrate its potential
application in the selective oxidation of 2,5-diformylfuran (DFF)
to 2,5-furandicarboxylic acid (FDCA) under mild conditions. The enzymatic
nanoreactor was deeply characterized using thermogravimetric analysis,
Fourier transform infrared spectroscopy, N2-adsorption,
dynamic light scattering, UV–visible spectroscopy, transmission
electron microscopy, scanning electron microscopy, and confocal laser
scanning microscopy, while the reaction products were established
on the basis of 1H nuclear magnetic resonance spectroscopy
combined with high-performance liquid chromatography. Our results
revealed that while CALB immobilized in conventional sol–gel
silica yielded exclusively 5-formylfuran-2-carboxylic acid (FFCA),
confinement of the enzyme in the silicified hydrogel imparted a 5-fold
increase in DFF conversion and afforded 67% FDCA yield in 7 h and
almost quantitative yields in less than 24 h. The hierarchically interconnected
pore structure of the host matrix was found to provide a readily accessible
diffusion path for reactants and products, while its flexible hydrophilic–hydrophobic
interface was extremely beneficial for the interfacial activation
of the immobilized lipase.
History
Usage metrics
Categories
Keywords
thermogravimetric analysisbioactive moleculessilica-strengthened cyclodextrin-derived supramolecular hydrogelCandida antarctica lipase BN 25- formylfuran -2-carboxylic acidMultifunctional Cyclodextrin-Derived Silicified Hydrogel7 hUVDFF conversionpore structureresonance spectroscopysilicified hydrogelEnzymatic Nanoreactor Supramolecular hydrogels1 Hscanning electron microscopytransmission electron microscopydiffusion pathFFCAFDCACandida Antarctica Lipase Bhost matrixconfocal laser scanning microscopy24 hreaction productsconfinementCALB
Licence
Exports
RefWorks
BibTeX
Ref. manager
Endnote
DataCite
NLM
DC