Mesoporous catalysts of magnetic nanoparticles and free-radical-producing enzymes, and methods of use

Patent metadata

Field	Value
Publication number	US-2019309282-A1
Application number	US-201916424584-A
Country	US
Kind code	A1
Filing date	May 29, 2019
Priority date	Mar 10, 2011
Publication date	Oct 10, 2019
Grant date	—

Abstract

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.

First claim

What is claimed is:

1 . A composition comprising mesoporous aggregates of magnetic nanoparticles and free-radical producing enzyme, wherein said mesoporous aggregates of magnetic nanoparticles have mesopores in which said free-radical-producing enzyme is embedded.

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 free-radical-producing enzyme is selected from EC 1.11 oxidoreductases acting with peroxide as an acceptor and EC 1.10 oxidoreductases acting on diphenols and related substances as donors, and combinations thereof.

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 II peroxidase.

10 . The composition of claim 9 , wherein said class II peroxidase is a class II microbial peroxidase.

11 . The composition of claim 10 , wherein said class II microbial peroxidase is selected from lignin peroxidase, manganese peroxidase, and versatile peroxidase.

12 . The composition of claim 8 , wherein said peroxidase is a class III peroxidase.

13 . The composition of claim 12 , wherein said class III peroxidase is selected from horseradish peroxidase, peanut peroxidase, soybean peroxidase, turnip peroxidase, tobacco peroxidase, tomato peroxidase, and barley peroxidase.

14 . The composition of claim 7 , wherein said free-radical-producing enzyme is a laccase.

15 . 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.

16 . The composition of claim 1 , wherein said free-radical-producing enzyme is comprised of an EC 1.1.3 enzyme and a peroxidase.

17 . The composition of claim 16 , wherein said EC 1.1.3 enzyme is glucose oxidase EC 1.1.3.4.

18 . The composition of claim 16 , wherein said peroxidase is horseradish peroxidase.

19 . The composition of claim 1 , wherein said mesoporous aggregates of magnetic nanoparticles and free-radical producing enzyme are surface-coated with gold.

20 . The composition of claim 1 , wherein said mesoporous aggregates of magnetic nanoparticles and free-radical producing enzyme reside on the surface of ferromagnetic submicrometric particles having a size of at least 20 nanometers.

21 . A composition comprising magnetic nanoparticles bound to free-radical-producing enzyme, wherein said magnetic nanoparticles bound to free-radical-producing enzyme are surface-coated with gold.

22 . A composition comprising magnetic nanoparticles bound to free-radical-producing enzyme, wherein said magnetic nanoparticles bound to free-radical-producing enzyme reside on the surface of ferromagnetic submicrometric particles having a size of at least 20 nanometers.

23 . A process for depolymerizing lignin, the method comprising reacting lignin-containing material with a composition comprising magnetic nanoparticles bound to free-radical-producing enzyme to produce depolymerized products from said lignin.

24 . The process of claim 23 , wherein said depolymerized products are selected from coniferyl, sinapyl, and coumaryl alcohols, and derivatives thereof.

25 . The process of claim 23 , wherein said free-radical-producing enzyme is comprised of a peroxidase.

26 . The process of claim 25 , wherein said peroxidase is a lignin-degrading peroxidase.

27 . The process of claim 26 , wherein said lignin-degrading peroxidase is selected from a lignin peroxidase, versatile peroxidase, manganese peroxidase, and combinations thereof.

28 . The process of claim 23 , wherein said process is coupled with a lignocellulosic conversion process in which said lignin to be depolymerized is produced by said lignocellulosic material conversion process.

29 . The process of claim 23 , wherein said magnetic nanoparticles are comprised of mesoporous aggregates of magnetic nanoparticles, wherein said mesoporous aggregates of magnetic nanoparticles have mesopores in which free-radical-producing enzyme is embedded.

30 . The process of claim 23 , wherein said magnetic nanoparticles bound to free-radical-producing enzyme are surface-coated with gold.

31 . The process of claim 23 , wherein said magnetic nanoparticles bound to free-radical-producing enzyme reside on the surface of ferromagnetic submicrometric particles having a size of at least 20 nanometers.

32 . The process of claim 23 , wherein said magnetic nanoparticles bound to free-radical-producing enzyme are captured by magnetic separation after said process and re-used after being captured, wherein said magnetic nanoparticles bound to free-radical-producing enzyme substantially retain their activity after being captured and re-used.

33 . A process for removing aromatic contaminants from water, the method comprising contacting water contaminated with aromatic substances with a composition comprising magnetic nanoparticles bound to free-radical-producing enzyme to remove said aromatic contaminants from said water.

34 . The process of claim 33 , wherein contacting said water with said magnetic nanoparticles bound to free-radical-producing enzyme results in precipitation of an insoluble material derived from said aromatic contaminants.

35 . The process of claim 34 , further comprising removing said insoluble material from said water.

36 . The process of claim 33 , wherein said aromatic contaminants are comprised of phenolic substances.

37 . The process of claim 33 , wherein said free-radical-producing enzyme is comprised of a peroxidase.

38 . The process of claim 33 , wherein said magnetic nanoparticles are comprised of mesoporous aggregates of magnetic nanoparticles, wherein said mesoporous aggregates of magnetic nanoparticles have mesopores in which free-radical-producing enzyme is embedded.

39 . The process of claim 33 , wherein said magnetic nanoparticles bound to free-radical-producing enzyme are surface-coated with gold.

40 . The process of claim 33 , wherein said magnetic nanoparticles bound to free-radical-producing enzyme reside on the surface of ferromagnetic submicrometric

Assignees

• Univ Cornell

Inventors

• Corgie Stephane C
• Kahawong Patarawan
• Giannelis Emmanuel P
• Walker Larry P

Classifications

• C12Y111/01016

  Versatile peroxidase (1.11.1.16) · CPC title

• C12N9/0004

  Oxidoreductases (1.) · CPC title

• C12N9/0055

  acting on diphenols and related substances as donors (1.10) · CPC title

• C12Y111/01007

  Peroxidase (1.11.1.7), i.e. horseradish-peroxidase · CPC title

• C12P2201/00

  Pretreatment of cellulosic or lignocellulosic material for subsequent enzymatic treatment or hydrolysis · CPC title