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Supported Supramolecular Hydrogel Nanoarchitectonics for Tunable Biocatalytic Flow Activity
Shahaji H More1,2, Jean-Yves Runser1,2, Aymeric Ontani2
1Inserm UMR_S 1121, CNRS EMR 7003, Biomaterials and Bioengineering, Centre de Recherche en Biomédecine de Strasbourg, 1 rue Eugène Boeckel, Strasbourg, F-67000, France.
Small (Weinheim an Der Bergstrasse, Germany)
|October 12, 2024
Summary
Enzymatically-active polyelectrolyte multilayers create supported biocatalytic hydrogels from peptides. These enzyme-decorated hydrogels offer enhanced stability and tunable activity for multi-catalytic transformations.
Area of Science:
- Biomaterials Science
- Supramolecular Chemistry
- Enzyme Engineering
Background:
- Enzymatically-active polyelectrolyte multilayers (APn-PEM) are explored for biocatalytic applications.
- Supramolecular hydrogels offer unique properties for enzyme encapsulation and controlled release.
Purpose of the Study:
- To investigate the formation and properties of supported biocatalytic supramolecular hydrogels induced by APn-PEM.
- To evaluate the stability, activity, and tunability of enzyme-encapsulated hydrogels.
- To demonstrate the utility of these hydrogels in multi-catalytic transformations.
Main Methods:
- Formation of APn-PEM and subsequent hydrogelation with Fmoc-FFpY precursor.
- Cryo scanning electron microscopy (cryo-SEM) for structural analysis.
- Fluorescence confocal microscopy and transmission electron microscopy (TEM) for enzyme localization and self-assembly visualization.
- Activity assays and continuous flow experiments.
Main Results:
- APn-PEM induced spatially-localized hydrogelation with thicknesses dependent on the number of enzyme layers (n).
- Cryo-SEM revealed a dense nanofibrous network of peptide fibrils.
- Enzymes (AP) were observed to decorate the peptide nanofibers, enhancing long-term stability and biocatalytic activity.
- Hydrogel bioactivity was tunable by the number of enzyme layers (n) and demonstrated in continuous flow multi-catalytic reactions.
Conclusions:
- Enzyme-functionalized polyelectrolyte multilayers effectively create supported biocatalytic supramolecular hydrogels.
- These hydrogels exhibit enhanced enzyme stability and activity, with tunable properties.
- The developed strategy is versatile for applications in continuous flow multi-catalytic transformations.
