IP Library Granted Patent US 8,492,474
Granted Patent B2
US 8,492,474 · App. 12/099,809 · Granted Jul 23, 2013

Methods of making polymer blend compositions

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Quick Facts
Patent No.
US 8,492,474
App. No.
12/099,809
Granted
Jul 23, 2013
Kind
B2
Abstract

Methods of making miscible and compatible immiscible polymer blends are disclosed. The polymer blends have a polyimide as a component. The miscible polymer blends have a single glass transition temperature. The compatible polymer blends have two glass transition temperatures. The polymer blends may optionally include one or more fillers.

Claims (58)

1. A method of making a polymer blend comprising:

melt mixing

(a) a pre-polymer having a component selected from the group consisting of free amine groups, free anhydride groups, and combinations thereof said pre-polymer being an incompletely imidized oligomer having a weight average molecular weight of 2,000 to 20,000 grams/mole and a total reactive end group concentration of 0.5 to 20 mole %, comprising structural units derived from a dianhydride and a diamine,

(b) a polymer having a weight average molecular weight of 10,000 to 80,000 grams/mole and a total reactive end group concentration of from 0.05 to 0.3 mole %, comprising a reactive member reactive with the pre-polymer's free anhydride groups, free amine groups, or combinations thereof and wherein the polymer blend is non-delaminated; and

(c) from 1 to 98 wt. % of at least one filler;

wherein the pre-polymer is present in an amount of 1 weight percent to 98 weight percent, based on the combined weight of the pre-polymer and the polymer and the polymer is present in an amount of 1 weight percent to 98 weight percent, based on the combined weight of the pre-polymer and the polymer, and

wherein the at least one filler and all of the polymer components have a weight loss (under nitrogen) of 10% or less at 300° C., as determined by thermal gravimetric analyses ASTM method E1868.

2. The method of claim 1 , wherein the dianhydride is oxydiphthalic anhydride and the diamine is a diamino diaryl sulfone.

3. The method of claim 1 , wherein the polymer is selected from the group consisting of polyimides, polyetherimides, polyamideimides, polyaryl ether ketones, polyaryl ketones, polyether ketones, polyether ether ketones, polyaryl sulfones, liquid crystal polymers, polyamides, polyesters, polysulfones, polyphenylene sulfides, polybenzimidazoles, and combinations of two or more of the foregoing.

4. The method of claim 1 , wherein the pre-polymer is present in an amount of 20 weight percent to 79 weight percent, based on the combined weight of the pre-polymer and the polymer and the polymer is present in an amount of 20 weight percent to 79 weight percent, based on the combined weight of the pre-polymer and the polymer.

5. The method of claim 1 , wherein the pre-polymer has a ratio of carbon atoms/(nitrogen atoms+oxygen atoms+sulfur atoms) of 2.8 to 4.2.

6. The method of claim 1 , wherein the filler is selected from the group consisting of glass fillers, carbon fillers, aramid fillers, metallic fillers, metal-coated fibers, natural fillers, and nanofillers; and the composition optionally further comprises minerals; stabilizers; colorants; lubricants; impact modifiers; flame retardants; mold release agents; processing aids; coupling agents; and blends and/or mixtures including two or more of the foregoing.

7. A method of making a polymer blend comprising:

melt mixing

(a) a pre-polymer comprising a component selected from the group consisting of free amine groups, free anhydride groups, and combinations thereof said pre-polymer being an incompletely imidized oligomer having a weight average molecular weight of 2,000 to 20,000 grams/mole and a total reactive end group concentration of 0.5 to 20 mole %, further comprising structural units derived from a first dianhydride and a first diamine;

(b) a polymer having a weight average molecular weight of 10,000 to 80,000 grams/mole and a total reactive end group concentration of from 0.05 to 0.3 mole %, comprising a reactive member reactive with the pre-polymer's free anhydride groups, free amine groups, or combinations thereof and said polymer further comprising structural units derived from a second dianhydride and a second diamine; and

(c) from 1 to 98 wt. % of at least one filler;

wherein the first dianhydride is the same as the second dianhydride or the first diamine is the same as the second diamine, and the other is different,

wherein the pre-polymer is present in an amount of 1 weight percent to 98 weight percent, based on the combined weight of the pre-polymer and the polymer and the polymer is present in an amount of 1 weight percent to 98 weight percent, based on the combined weight of the pre-polymer and the polymer, and

wherein the at least one filler and all of the polymer components have a weight loss (under nitrogen) of 10% or less at 300 C, as determined by thermal gravimetric analyses ASTM method E1868.

8. The method of claim 7 , wherein the first dianhydride and the second anhydride is independently selected from the group consisting of oxydiphthalic anhydrides, bisphenol-A dianhydrides, and combinations thereof.

9. The method of claim 7 , wherein the first diamine and the second diamine is independently selected from the group consisting of diamino diaryl sulfones, metaphenylene diamines, paraphenylene diamines, and combinations thereof.

10. The method of claim 7 , wherein the pre-polymer is present in an amount of 20 weight percent to 79 weight percent, based on the combined weight of the pre-polymer and the polymer and the polymer is present in an amount of 20 weight percent to 79 weight percent, based on the combined weight of the pre-polymer and the polymer.

11. The method of claim 7 , wherein the pre-polymer comprises structural units derived from oxydiphthalic anhydrides and diamino diaryl sulfones and the polymer comprises structural units derived from bisphenol-A dianhydrides and diamino diaryl sulfones.

12. The method of claim 7 , wherein the pre-polymer has a ratio of carbon atoms/(nitrogen atoms+oxygen atoms+sulfur atoms) of 2.8 to 4.2.

13. The method of claim 7 , wherein the filler is selected from the group consisting of glass fillers, carbon fillers, aramid fillers, metallic fillers, metal-coated fibers, natural fillers, and nanofillers; and the composition optionally further comprises minerals; stabilizers; colorants; lubricants; impact modifiers; flame retardants; mold release agents; processing aids; coupling agents; and blends and/or mixtures including two or more of the foregoing.

14. A method of making a polymer blend comprising:

melt mixing

a. a pre-polymer comprising a component selected from the group consisting of free amine groups, free anhydride groups, and combinations thereof said pre-polymer being an incompletely imidized oligomer having a weight average molecular weight of 2,000 to 20,000 grams/mole and a total reactive end group concentration of 0.5 to 20 mole %, further comprising structural units derived from a first dianhydride and a first diamine;

b. a polymer having a weight average molecular weight of 10,000 to 80,000 grams/mole and a total reactive end group concentration of from 0.05 to 0.3 mole %, comprising structural units derived from a second dianhydride and a second diamine; and

c. from 1 to 98 wt. % of at least one filler;

wherein the first dianhydride is different from the second dianhydride and the first diamine is different from the second diamine,

wherein the pre-polymer is present in an amount of 1 weight percent to 98 weight percent, based on the combined weight of the pre-polymer and the polymer and the polymer is present in an amount of 1 weight percent to 98 weight percent, based on the combined weight of the pre-polymer and the polymer, and

wherein the at least one filler and all of the polymer components have a weight loss (under nitrogen) of 10% or less at 300 C, as determined by thermal gravimetric analyses ASTM method E1868.

15. The method of claim 14 , wherein the first dianhydride or the second anhydride is selected from the group consisting of oxydiphthalic anhydrides, bisphenol-A dianhydrides, and combinations thereof.

16. The method of claim 14 , wherein the first diamine or the second diamine is selected from the group consisting of diamino diaryl sulfones, metaphenylene diamines, paraphenylene diamines, and combinations thereof.

17. The method of claim 14 , wherein the pre-polymer is present in an amount of 20 weight percent to 79 weight percent, based on the combined weight of the pre-polymer and the polymer and the polymer is present in an amount of 79 weight percent to 80 weight percent, based on the combined weight of the pre-polymer and the polymer.

18. The method of claim 14 , wherein the pre-polymer has a ratio of carbon atoms/(nitrogen atoms+oxygen atoms+sulfur atoms) of 2.8 to 4.2.

19. The method of claim 14 , wherein the filler is selected from the group consisting of glass fillers, carbon fillers, aramid fillers, metallic fillers, metal-coated fibers, natural fillers, and nanofillers; and the composition optionally further comprises minerals; stabilizers; colorants; lubricants; impact modifiers; flame retardants; mold release agents; processing aids; coupling agents; and blends and/or mixtures including two or more of the foregoing.

20. A method of making a polyimide polymer blend having a predetermined glass transition temperature comprising:

selecting a glass transition temperature for the blend; and

melt mixing a pre-polymer, a polymer and at least one filler,

wherein the pre-polymer and polymer are present in amounts sufficient to provide a blend having the selected glass transition temperature,

wherein the pre-polymer comprises a component selected from the group consisting of free amine groups, free anhydride groups, and combinations thereof said pre-polymer being an incompletely imidized oligomer having a weight average molecular weight of 2,000 to 20,000 grams/mole and a total reactive end group concentration of 0.5 to 20 mole %, further comprising structural units derived from a first dianhydride and a first diamine,

wherein the polymer has a weight average molecular weight of 10,000 to 80,000 grams/mole and a total reactive end group concentration of from 0.05 to 0.3 mole %, and comprises a reactive member reactive with the pre-polymer's free anhydride groups, free amine groups, or combinations thereof,

wherein the polymer comprises structural units derived from a second dianhydride and a second diamine,

wherein the first dianhydride is the same as the second dianhydride or the first diamine is the same as the second diamine, and the other is different, and

wherein the at least one filler and all of the polymer components have a weight loss (under nitrogen) of 10% or less at 300 C, as determined by thermal gravimetric analyses ASTM method E1868.

21. The method of claim 20 , wherein the pre-polymer has a ratio of carbon atoms/(nitrogen atoms+oxygen atoms+sulfur atoms) of 2.8 to 4.2.

22. A method of making a polyimide polymer blend having a predetermined glass transition temperature comprising:

selecting a glass transition temperature for the blend; and

melt mixing a pre-polymer, a polymer and at least one filler,

wherein the pre-polymer and polymer are present in amounts sufficient to provide a blend having the selected glass transition temperature,

wherein the pre-polymer comprises a component selected from the group consisting of free amine groups, free anhydride groups, and combinations thereof said pre-polymer being an incompletely imidized oligomer having a weight average molecular weight of 2,000 to 20,000 grams/mole and a total reactive end group concentration of 0.5 to 20 mole %, further comprising structural units derived from a first dianhydride and a first diamine,

wherein the polymer has a weight average molecular weight of 10,000 to 80,000 grams/mole and a total reactive end group concentration of from 0.05 to 0.3 mole %, and comprises a reactive member reactive with the pre-polymer's free anhydride groups, free amine groups, or combinations thereof,

wherein the polymer comprises structural units derived from a second dianhydride and a second diamine,

wherein the first dianhydride is different from the second dianhydride and the first diamine is different from the second diamine, and

wherein the at least one filler and all of the polymer components have a weight loss (under nitrogen) of 10% or less at 300 C, as determined by thermal gravimetric analyses ASTM method E1868.

Assignments (3)
CHANGE OF NAME Recorded Jun 6, 2016
From: SABIC INNOVATIVE PLASTICS IP B.V.
To: SABIC GLOBAL TECHNOLOGIES B.V.
Reel/Frame 038883/0816 →
RELEASE OF SECURITY INTEREST Recorded Mar 17, 2014
From: CITIBANK, N.A.
To: SABIC INNOVATIVE PLASTICS IP B.V.
Reel/Frame 032459/0798 →
CORRECTIVE ASSIGNMENT TO CORRECT THE THE INCORRECT ASSIGNEE ADDRESS OF 1 PLASTICS AVENUE, PITTSFIELD, MA 01201 PREVIOUSLY RECORDED ON REEL 020775 FRAME 0346. ASSIGNOR(S) HEREBY CONFIRMS THE CORRECT ASSIGNEE ADDRESS IS 1 PLASTICSLAAN, 4612 PX BERGEN OP ZOOM, THE NETHERLANDS. Recorded Dec 18, 2012
From: GALLUCCI, ROBERT RUSSELL; MULLEN, TARA J.; ODLE, ROY RAY; SHETH, KAPIL CHANDRAKANT; WHITE, JAMES MITCHELL
To: SABIC INNOVATIVE PLASTICS IP B.V.
Reel/Frame 029486/0409 →