Nanoconfined (Bio)Catalysts as Efficient Glucose‐Responsive Nanoreactors. (9th July 2020)

• Record Type: Journal Article
• Authors: Rodriguez‐Abetxuko, Andoni; Muñumer, Pablo; Okuda, Mitsuhiro; Calvo, Javier; Knez, Mato; Beloqui, Ana
• Is Part Of: Advanced functional materials. Volume 30:Number 35(2020)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2020-07-09
• Subjects: aromatics biodegradation -- artificial metabolic channels -- cascade reactions -- chemoenzymatic nanoreactors -- responsive nanomaterials; Materials -- Periodicals; Chemical vapor deposition -- Periodicals; 620.11
• DOI: 10.1002/adfm.202002990
• Languages: English
• ISSNs: 1616-301X

Abstract

Abstract: Herein, the design, synthesis, and characterization of bifunctional hybrid nanoreactors used for concurrent one‐pot chemoenzymatic reactions are shown. In the design, the enzyme, glucose oxidase, is wrapped with a peroxidase‐mimetic catalytic polymer. Hemin, the organic catalyst, is linked to the flexible polymeric scaffold through coordination to the imidazole groups that hang out the network. This spatial arrangement, which works as a metabolic channel, is optimized for cooperative chemoenzymatic reactions in which the enzyme catalyzes first. A deep characterization of the integrated nanoreactors demonstrates that the confinement of two distinct catalytic sites in the nanospace is very effective in one‐pot reactions. Moreover, besides its role as scaffold material, the polymeric mantel protects both the biocatalyst and the chemical catalyst from degradation and inactivation in the presence of organic solvents. Furthermore, the polymeric environment of the nanoreactors can be tailored in order to trigger the assembly of those into highly active heterogeneous hybrid catalysts. Finally, the new nanoreactors are applied to the efficient degradation of organic aromatic compounds using glucose as the only fuel. Abstract : Herein, a new type of chemoenzymatic nanoreactor in which the (bio)catalysts are confined in the nanospace and conveniently arranged is shown. The encapsulation of glucose oxidase into a peroxidase‐mimetic catalytic polymer gives rise to the fabrication of a highly stable and robust bifunctional nanoreactor used for the concurrent degradation of aromatic compounds using glucose as the only fuel.