Metabolic engineering of polyhydroxyalkanoate monomer synthases
원문보기
IPC분류정보
국가/구분
United States(US) Patent
등록
국제특허분류(IPC7판)
C07H-021/04
C12P-007/52
C12P-007/44
C12P-007/62
C12N-015/63
출원번호
US-0091609
(1700-01-01)
국제출원번호
PCT/US96/20119
(1996-12-18)
발명자
/ 주소
Sherman, David H.
Williams, Mark D.
Xue, Yongquan
출원인 / 주소
Regents of the University of Minnesota
대리인 / 주소
Schwegman, Lundberg, Woessner & Kluth, P.A.
인용정보
피인용 횟수 :
6인용 특허 :
38
초록▼
A novel pathway for the synthesis of polyhydroxyalkanoate is provided. A method of synthesizing a recombinant polyhydroxyalkanoate monomer synthase is also provided. These recombinant polyhydroxyalknoate synthases are derived from multifunctional fatty acid synthases or polyketide synthases and gene
A novel pathway for the synthesis of polyhydroxyalkanoate is provided. A method of synthesizing a recombinant polyhydroxyalkanoate monomer synthase is also provided. These recombinant polyhydroxyalknoate synthases are derived from multifunctional fatty acid synthases or polyketide synthases and generate hydroxyacyl acids capable of polymerization by a polyhydroxyalknoate synthase.
대표청구항▼
A novel pathway for the synthesis of polyhydroxyalkanoate is provided. A method of synthesizing a recombinant polyhydroxyalkanoate monomer synthase is also provided. These recombinant polyhydroxyalknoate synthases are derived from multifunctional fatty acid synthases or polyketide synthases and gene
A novel pathway for the synthesis of polyhydroxyalkanoate is provided. A method of synthesizing a recombinant polyhydroxyalkanoate monomer synthase is also provided. These recombinant polyhydroxyalknoate synthases are derived from multifunctional fatty acid synthases or polyketide synthases and generate hydroxyacyl acids capable of polymerization by a polyhydroxyalknoate synthase. kylene, aryl and heteroaryl groups being substituted with H or C1-3 alkyl; R1and R2are independently selected from the group consisting of H, nitro, halo and C1-6alkoxy; R3and R4are independently selected from the group consisting of H, C1-6 alkyl, C5-10 aryl and C5-10 heteroaryl, said alkyl, aryl and heteroaryl groups being substituted; and W is selected from the group consisting of OH, NH2and NHpg where pg is a protecting group. 13. A method for preparing the multiftnctionalized support resin of claim 1, comprising: a) coupling a diamino carboxylic acid template to a resin backbone, wherein each of the two amino groups of the diamino acid template are protected; b) deprotecting one of the two protected amino groups of the template to generate a first deprotected amino group; c) reacting the first deprotected amino group with a first benzyl linker moiety under conditions effective to covalently bond the benzyl linker moiety to the first deprotected amino group; d) deprotecting the remaining protected amino group of the diamine carboxylic acid template to generate a second deprotected amino group; e) reacting the second deprotected amino group with a second benzyl moiety under conditions effective to covalently bond the second benzyl linker moiety to the second deprotected amino group thereby to forming the multifunctionalized resin of claim 1; and f) recovering the multifunctionalized resin of claim 1. one monohydric alcohol selected from the group consisting of 2,4-dibromophenol, 2,4,6-tribromophenol, dibromopropanol, and tribromoneopentyl alcohol. 5. A process according to claim 3, wherein said reacting (b) comprises propagating a ring-opening polymerization reaction to provide the bromine-containing, hydroxy-functional copolymer with a polyester block, wherein the polyester block has at least two ester repeating units and a hydroxy functionality. 6. A process according to claim 1, wherein the initiator comprises a glycol, and wherein the bromine-containing copolymer comprises an ABA triblock copolymer consisting of two hydroxy-functional A blocks and a B block, wherein the process comprises forming the B block from the glycol and forming each of the A blocks from at least a respective one of the lactone monomers, each of the A blocks independently comprising an ester or a polyester. 7. A process according to claim 6, wherein the initiator comprises at least one member selected from the group consisting of tetrabromobisphenol A, tetrabromobisphenol A-bis(2-hydroxy-ethyl ether), dibromoneopentyl glycol, and tetrabromodipentaerythritol. 8. A process according to claim 6, wherein said reacting (b) comprises propagating a ring-opening polymerization reaction to provide the bromine-containing, hydroxy-functional copolymer with at least one polyester block, wherein the polyester block has at least two ester repeating units and a hydroxy functionality. 9. A process according to claim 1, further comprising adding a catalyst that forms a complex with the initiator prior to said reacting (b) so that the initiator is present as the complex during said reacting (b). 10. A process according to claim 1, further comprising adding a catalyst comprising at least one member selected from the group consisting of boron trifluoride, sodium methoxide, calcium methoxide, aluminum isopropoxide, tetrabutyl titanate, titanium chelates, titanium acylates, lead oxides, zinc borates, antimony oxide, sulfuric acid, hydrochloric acid, phosphoric acid, p-toluenesulfonic acid, tin(II) oxide, tin(II) octoate, and tin(II) acetate. 11. A process according to claim 1, wherein the bromine-containing, hydroxy-functional copolymer has an average molecular weight in a range of 300 to 2000. 12. A process according to claim 1, wherein the bromine-containing, hydroxy-functional copolymer has a Gardner color of less than 1.0. 13. A process according to claim 1, wherein the bromine-containing, hydroxy-functional copolymer has a viscosity in a range of 50 cps to 4500 cps at 25° C. 14. A process according to claim 1, wherein the bromine-containing, hydroxyl-functional copolymer has a bromine weight content of 10% to 39%. 15. A process comprising: (a) providing an initiator having at least one bromine atom, the initiator being a solid at room temperature; (b) reacting the initiator with an effective amount of lactone monomers to establish a bromine-containing, hydroxy-functional copolymer that is a liquid at room temperature; and (c) reacting the bromine-containing, hydroxy-functional copolymer with a polymer. 16. A process according to claim 15, wherein the lactone monomers comprise at least one member selected from the group consisting of α,α-bis(chloromethyl) propiolactone, δ-valerolactone, α,β,γ-trimethoxy-δ-valerolactone, 1,4-dioxane-2-one, glycolide, lactide, 1,4-dithiane-2,5-dione, trimethylene carbonate, neopentylene carbonate, ethylene oxalate, propylene oxalate, γ-valerolactone, ε-caprolactone. β-methyl-ε-isopropyl-ε-caprolactone, γ-methyl-ε-caprolactone, ε-methyl-ε-caprolactone, and β,δ-dimethyl-ε-caprolactone. 17. A process according to claim 15, wherein the initiator comprises a monohydric alcohol, and wherein the bromine-containing, hydroxy-functional copolymer comprises an AB diblock copolymer consisting of an A block and a B block, wherein the process comprises forming the B block from the monohydric alcohol and forming the A b lock from one or more of the lactone monomers, wherein the A block is an ester or a polyester. 18. A process according to claim 17, wherein the initiator comprises at least one monohydric alcohol selected from the group consisting of 2,4-dibromophenol, 2,4,6-tribromophenol, dibromopropanol, and tribromoneopentyl alcohol. 19. A process according to claim 17, wherein said reacting (b) comprises propagating a ring-opening polymerization reaction to provide the bromine-containing, hydroxy-functional copolymer with a polyester block, wherein the polyester block has at least two ester repeating units and a hydroxy functionality. 20. A process according to claim 15, wherein the initiator comprises a glycol, and wherein the bromine-containing copolymer comprises an ABA triblock copolymer consisting of two hydroxy-functional A blocks and a B block, wherein the process comprises forming the B block from the glycol and forming each of the A blocks from at least a respective one of the lactone monomers, and wherein the A blocks are each independently selected from the group consisting of an ester and a polyester. 21. A process according to claim 20, wherein the initiator comprises at least one member selected from the group consisting of tetrabromobisphenol A, tetrabromobisphenol A-bis(2-hydroxy-ethyl ether), dibromoneopentyl glycol, and tetrabromodipentaerythritol. 22. A process according to claim 20, wherein said reacting (b) comprises propagating a ring-opening polymerization reaction to provide the bromine-containing, hydroxy-functional copolymer with at least one polyester block, wherein the polyester block has at least two ester repeating units and a hydroxy functionality. 23. A process according to claim 15, wherein said process comprises adding a catalyst to form a complex with the initiator prior to said reacting (b) so that the initiator is present as the complex during said reacting (b). 24. A process according to claim 23, wherein the catalyst comprises at least one member selected from the group consisting of boron trifluoride, sodium methoxide, calcium methoxide, aluminum isopropoxide, tetrabutyl titanate, titanium chelates titanium acylates, lead oxides, zinc borates, antimony oxide, sulfuric acid, hydrochloric acid, phosphoric acid, p-toluenesulfonic acid, tin(II) oxide, tin(II) octoate, and tin(II) acetate. 25. A process according to claim 15, wherein the bromine-containing, hydroxy-functional copolymer has an average molecular weight in a range of 300 to 2000. 26. A process according to claim 15, wherein the bromine-containing, hydroxy-functional copolymer has a Gardner color of less than 1.0. 27. A process according to claim 15, wherein the bromine-containing, hydroxy-functional copolymer has a viscosity in a range of 50 cps to 4500 cps at 25° C. 28. A process according to claim 15, wherein the bromine-containing, hydroxyl-functional copolymer has a bromine weight content of 10% to 39%. 29. A process according to claim 15, wherein the initiator comprises a monohydric alcohol, and wherein said reacting (c) comprises grafting the bromine-containing, hydroxy-functional copolymer to the polymer. 30. A process according to claim 15, wherein the initiator comprises a polyol, and wherein said reacting (c) comprises crosslinking the polymer with the bromine-containing, hydroxy-functional copolymer. 31. A process according to claim 1, wherein said reacting is conducted in a temperature range of 120° C. to 160° C. 32. A process according to claim 1, wherein said reacting is conducted in a temperature range of 130° C. to 150° C. 33. A process according to claim 32, wherein the bromine-containing, hydroxy-functional copolymer has a Gardner color of less than 1.0. 34. A process according to claim 15, wherein said reacting is conducted in a temperature range of 120° C. to 160° C. 35. A process according to claim 15, wherein said reacting is conducted in a temperature range of 130° C. to 150° C. 36. A process according to cla
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