Magnetic hierarchical catalysts of nanoparticles and enzymes forming mesoporous assemblies embedded in macroporous scaffolds, and their use with magnetically-driven reactors and in chemical reactions
US-2015252352-A1 · Sep 10, 2015 · US
US9597672B2 · US · B2
| Field | Value |
|---|---|
| Publication number | US-9597672-B2 |
| Application number | US-201214004311-A |
| Country | US |
| Kind code | B2 |
| Filing date | Mar 9, 2012 |
| Priority date | Mar 10, 2011 |
| Publication date | Mar 21, 2017 |
| Grant date | Mar 21, 2017 |
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A composition comprising mesoporous aggregates of magnetic nanoparticles and free-radical producing enzyme (i.e., enzyme-bound mesoporous aggregates), wherein the mesoporous aggregates of magnetic nanoparticles have mesopores in which the free-radical-producing enzyme is embedded. Methods for synthesizing the enzyme-bound mesoporous aggregates are also described. Processes that use said enzyme-bound mesoporous aggregates for depolymerizing lignin, removing aromatic contaminants from water, and polymerizing monomers polymerizable by a free-radical reaction are also described.
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What is claimed is: 1. A composition comprising self-assembled mesoporous aggregates of magnetic nanoparticles and a first free-radical producing enzyme, wherein said first enzyme is magnetically-entrapped without a bonding agent in mesopores formed by said aggregates of magnetic nanoparticles and said first enzyme functions by converting a diffusible substrate into a diffusible product. 2. The composition of claim 1 , wherein said mesoporous aggregates of magnetic nanoparticles have an iron oxide composition. 3. The composition of claim 1 , wherein said mesoporous aggregates of magnetic nanoparticles have a magnetic nanoparticle size distribution in which at least 90% of magnetic nanoparticles have a size of at least 3 nm and up to 30 nm, and an aggregated particle size distribution in which at least 90% of said mesoporous aggregates of magnetic nanoparticles have a size of at least 10 nm and up to 500 nm. 4. The composition of claim 1 , wherein said mesoporous aggregates of magnetic nanoparticles possess a saturated magnetization of at least 10 emu/g. 5. The composition of claim 1 , wherein said mesoporous aggregates of magnetic nanoparticles possess a remanent magnetization up to 5 emu/g. 6. The composition of claim 1 , wherein said free-radical-producing enzyme is contained in said mesoporous aggregates of magnetic nanoparticles in up to 100% of saturation capacity. 7. The composition of claim 1 , wherein said first free-radical-producing enzyme is an EC 1.11 oxidoreductase. 8. The composition of claim 7 , wherein said free-radical-producing enzyme is comprised of a peroxidase. 9. The composition of claim 8 , wherein said peroxidase is a class III peroxidase. 10. The composition of claim 9 , wherein said class III peroxidase is horseradish peroxidase. 11. The composition of claim 1 , wherein said mesopores are characterized by a pore size distribution in which at least 90% of the pore volume is attributed to pores having a pore size of at least 2 nm and up to 20 nm. 12. The composition of claim 1 , further comprising a second enzyme that is an EC 1.1.3 enzyme, and wherein said first enzyme is a peroxidase. 13. The composition of claim 12 , wherein said EC 1.1.3 enzyme is glucose oxidase EC 1.1.3.4. 14. The composition of claim 12 , wherein said peroxidase is horseradish peroxidase. 15. The composition of claim 1 , wherein said mesoporous aggregates of magnetic nanoparticles and free-radical producing enzyme further comprise a metallic surface layer. 16. Microparticles comprising the composition of claim 1 . 17. The microparticles of claim 16 , wherein said microparticles comprise magnetite. 18. The microparticles of claim 16 , wherein said microparticles are ferromagnetic submicrometric particles having a size of at least 20 nanometers. 19. The composition of claim 1 , wherein said mesoporous aggregates of magnetic nanoparticles have a magnetic nanoparticle size distribution in which at least 50% of magnetic nanoparticles have a size of at least 1 nm and up to 50 nm, and an aggregated particle size distribution in which at least 90% of said mesoporous aggregates of magnetic nanoparticles have a size of at least 10 nm and up to 500 nm, and wherein said free-radical producing enzyme is an oxidoreductase belonging to the EC1 family of enzymes.
characterised by the enzymes used · CPC title
Oxidoreductases (1.) · CPC title
Peroxidase (1.11.1.7), i.e. horseradish-peroxidase · CPC title
L-Ascorbate--cytochrome-b5 reductase (1.10.2.1) · CPC title
Enzymes or microbial cells immobilised on or in an inorganic carrier · CPC title
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