期刊
ADVANCED FUNCTIONAL MATERIALS
卷 30, 期 35, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.202002990
关键词
aromatics biodegradation; artificial metabolic channels; cascade reactions; chemoenzymatic nanoreactors; responsive nanomaterials
类别
资金
- Spanish Ministry of Economy and Competitiveness (MINECO)
- FEDER funds [MAT2017-88808-R]
- Maria de Maeztu Units of Excellence Programme [MDM-2016-0618]
- Spanish Research Agency (AEI)
- Basque Government
- Spanish Ministry of Economy and Competitiveness (MINECO) [MAT2016-77393-R]
- FEDER funds
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.
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