# US 2016/0355652 A1 · Methods of reducing the amount of colorant in a multilayer film

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- Number: US 2016/0355652 A1
- Document ID: US20160355652A1
- Status: Published application
- Kind: A1
- Application number: 15/238,163
- Filed: 2016-08-16
- Published: 2016-12-08
- Earliest claimed: 2013-12-17
- Assignees: E. I. Du Pont de Nemours and Company
- Applicants: E I Du Pont De Nemours and Company
- Inventors: THOMAS EDWARD CARNEY; JEFFREY MICHAEL BARTOLIN; CHRISTOPHER ROBERT BECKS
- Web page: https://patentgrep.com/patent/US20160355652A1

## CPC

- B32B 27/281: {comprising polyimides}
- B05D 7/52: {Two layers}
- C08J 7/0427: {with only one layer of a composition containing a polymer binder (with more layers C08J7/042)}
- C08J 7/043: Improving the adhesiveness of the coatings per se, e.g. forming primers (adhesives in the form of films or foils characterised by the primer layers between the polymer carriers and the adhesives C09J7/50)
- C08J 7/046: Forming abrasion-resistant coatings; Forming surface-hardening coatings
- C08J 7/05: Forming flame retardant coatings or fire resistant coatings
- C09D 7/42: Gloss-reducing agents
- C09D 7/61: inorganic
- C09D 179/08: Polyimides; Polyester-imides; Polyamide-imides; Polyamide acids or similar polyimide precursors
- B32B 2457/00: Electrical equipment
- C08J 2379/08: Polyimides; Polyester-imides; Polyamide-imides; Polyamide acids or similar polyimide precursors
- C08J 2479/08: Polyimides; Polyester-imides; Polyamide-imides; Polyamide acids or similar polyimide precursors
- C08K 3/04: Carbon
- C08K 3/22: of metals
- C08K 3/36: Silica
- C08K 2003/2227: {of aluminium}
- Y10T 428/24967: Absolute thicknesses specified
- B32B: LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B05D: PROCESSES FOR APPLYING FLUENT MATERIALS TO SURFACES, IN GENERAL (conveying articles or workpieces through baths of liquid B65G, e.g. B65G49/02)
- C08J: WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H (working, e.g. shaping, of plastics B29)
- C09D: COATING COMPOSITIONS, e.g. PAINTS, VARNISHES OR LACQUERS; FILLING PASTES; CHEMICAL PAINT OR INK REMOVERS; INKS; CORRECTING FLUIDS; WOODSTAINS; PASTES OR SOLIDS FOR COLOURING OR PRINTING; USE OF MATERIALS THEREFOR (cosmetics A61K; processes for applying liquids or other fluent materials to surfaces, in general, B05D; staining wood B27K5/02; glazes or vitreous enamels C03C; natural resins, French polish, drying-oils, driers, turpentine, per se, C09F; polishing compositions other than French polish, ski waxes C09G; adhesives or use of materials as adhesives C09J; materials for sealing or packing joints or covers C09K3/10; materials for stopping leaks C09K3/12; processes for the electrolytic or electrophoretic production of coatings C25D)
- C08K: Use of inorganic or non-macromolecular organic substances as compounding ingredients (paints, inks, varnishes, dyes, polishes, adhesives C09)
- Y10T: TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION

## Abstract

The present disclosure is directed to methods of reducing the amount of colorant in a multilayer film and achieving an L* color less than 30 and a 60 degree gloss value less than 10. The multilayer film has a first polyimide layer and a second polyimide layer containing a matting agent, submicron carbon black and submicron fumed metal oxide.

## Claims

### Claim 1

A method of reducing the amount of colorant in a multilayer film and achieving an L* color less than 30 and a 60 degree gloss value less than 10, the method comprising:
a) providing a first polyimide layer;
b) providing a polyamic acid solution containing polyamic acid, silica matting agent, and submicron carbon black for forming a second polyimide layer;
c) adding at least one submicron fumed metal oxide to the polyamic acid solution;
d) coating the polyamic acid solution on to the first polyimide layer; and
e) imidizing the coating to form the second polyimide layer on the first polyimide layer.

### Claim 2 (depends on 1)

The method of claim 1, wherein the first polyimide layer is derived from pyromellitic dianhydride and 4,4′-oxydianiline, or derived from pyromellitic dianhydride, 4,4′-oxydianiline and paraphenylenediamine.

### Claim 3 (depends on 1)

The method of claim 1, wherein the polyamic acid is derived from pyromellitic dianhydride and 4,4′-oxydianiline, or derived from 3,3′,4,4′-biphenyl tetracarboxylic dianhydride and paraphenylenediamine, or derived from pyromellitic dianhydride, 4,4′-oxydianiline and paraphenylenediamine, or derived from 3,3′,4,4′-biphenyl tetracarboxylic dianhydride, pyromellitic dianhydride, 4,4′-oxydianiline, or derived from 3,3′,4,4′-biphenyl tetracarboxylic dianhydride, pyromellitic dianhydride, 4,4′-oxydianiline and paraphenylenediamine, or derived from i) blocks of pyromellitic dianhydride and 4,4′-oxydianiline and ii) blocks of pyromellitic dianhydride and paraphenylenediamine, or derived from pyromellitic dianhydride, oxydiphthalic dianhydride and 1,3-bis-(4-aminophenoxy) benzene, or a mixture thereof.

### Claim 4 (depends on 1)

The method of claim 1, wherein the submicron fumed metal oxide comprises fumed alumina, fumed silica or a mixture thereof.

### Claim 5

A method of reducing the amount of colorant in a multilayer film and achieving an L* color less than 30 and a 60 degree gloss value less than 10, the method comprising:
a) providing a polyamic acid green film for forming a first polyimide layer;
b) providing a polyamic acid solution containing polyamic acid, silica matting agent, and submicron carbon black for forming a second polyimide layer;
c) adding at least one submicron fumed metal oxide to the polyamic acid solution;
d) coating the polyamic acid solution on to the polyamic acid green film; and
e) imidizing the coating and the polyamic acid green film to form the first and second polyimide layers.

### Claim 6 (depends on 5)

The method of claim 5, wherein the polyamic acid green film is derived from pyromellitic dianhydride and 4,4′-oxydianiline, or derived from pyromellitic dianhydride, 4,4′-oxydianiline and paraphenylenediamine.

### Claim 7 (depends on 5)

The method of claim 5, wherein the polyamic acid is derived from pyromellitic dianhydride and 4,4′-oxydianiline, or derived from 3,3′,4,4′-biphenyl tetracarboxylic dianhydride and paraphenylenediamine, or derived from pyromellitic dianhydride, 4,4′-oxydianiline and paraphenylenediamine, or derived from 3,3′,4,4′-biphenyl tetracarboxylic dianhydride, pyromellitic dianhydride, 4,4′-oxydianiline, or derived from 3,3′,4,4′-biphenyl tetracarboxylic dianhydride, pyromellitic dianhydride, 4,4′-oxydianiline and paraphenylenediamine, or derived from i) blocks of pyromellitic dianhydride and 4,4′-oxydianiline and ii) blocks of pyromellitic dianhydride and paraphenylenediamine, or derived from pyromellitic dianhydride, oxydiphthalic dianhydride and 1,3-bis-(4-aminophenoxy) benzene, or a mixture thereof.

### Claim 8 (depends on 5)

The method of claim 5, wherein the submicron fumed metal oxide comprises fumed alumina, fumed silica or a mixture thereof.

### Claim 9

A method of reducing the amount of colorant in a multilayer film and achieving an L* color less than 30 and a 60 degree gloss value less than 10, the method comprising:
a) providing a first polyamic acid solution containing a first polyamic acid for forming a first polyimide layer;
b) providing a second polyamic acid solution containing a second polyamic acid, silica matting agent, and submicron carbon black for forming a second polyimide layer;
c) adding at least one submicron fumed metal oxide to the second polyamic acid solution;
d) coextruding the second polyamic acid solution and the first polyamic acid solution; and
e) imidizing the coextruded layers to form the first and second polyimide layers.

### Claim 10 (depends on 9)

The method of claim 9, wherein the first polyamic acid is derived from pyromellitic dianhydride and 4,4′-oxydianiline, or derived from pyromellitic dianhydride, 4,4′-oxydianiline and paraphenylenediamine.

### Claim 11 (depends on 6)

The method of claim 6, wherein the second polyamic acid is derived from pyromellitic dianhydride and 4,4′-oxydianiline, or derived from 3,3′,4,4′-biphenyl tetracarboxylic dianhydride and paraphenylenediamine, or derived from pyromellitic dianhydride, 4,4′-oxydianiline and paraphenylenediamine, or derived from 3,3′,4,4′-biphenyl tetracarboxylic dianhydride, pyromellitic dianhydride, 4,4′-oxydianiline, or derived from 3,3′,4,4′-biphenyl tetracarboxylic dianhydride, pyromellitic dianhydride, 4,4′-oxydianiline and paraphenylenediamine, or derived from i) blocks of pyromellitic dianhydride and 4,4′-oxydianiline and ii) blocks of pyromellitic dianhydride and paraphenylenediamine, or derived from pyromellitic dianhydride, oxydiphthalic dianhydride and 1,3-bis-(4-aminophenoxy) benzene, or a mixture thereof.

### Claim 12 (depends on 9)

The method of claim 9, wherein the submicron fumed metal oxide comprises fumed alumina, fumed silica or a mixture thereof.

### Claim 13

A method of reducing the amount of colorant in a multilayer film and achieving an L* color less than 30 and a 60 degree gloss value less than 10, the method comprising:
a) providing a first polyamic acid solution containing a first polyamic acid for forming a first polyimide layer;
b) providing a second polyamic acid solution containing a second polyamic acid, a first silica matting agent, and a first submicron carbon black for forming a second polyimide layer;
c) providing a third polyamic acid solution containing a third polyamic acid, a second silica matting agent, and a second submicron carbon black for forming a third polyimide layer;
d) adding at least one first submicron fumed metal oxide to the second polyamic acid solution;
e) adding at least one second submicron fumed metal oxide to the third polyamic acid solution;
f) coextruding the first, second and third polyamic acid solutions, wherein the second and third polyamic acid solutions are in direct contact with opposite sides of the first polyamic acid solution; and
g) imidizing the coextruded layers to form the first, second and third polyimide layers.

### Claim 14 (depends on 13)

The method of claim 13, wherein the first polyamic acid is derived from pyromellitic dianhydride and 4,4′-oxydianiline, or derived from pyromellitic dianhydride, 4,4′-oxydianiline and paraphenylenediamine.

### Claim 15 (depends on 13)

The method of claim 13, wherein the second polyamic acid is derived from pyromellitic dianhydride and 4,4′-oxydianiline, or derived from 3,3′,4,4′-biphenyl tetracarboxylic dianhydride and paraphenylenediamine, or derived from pyromellitic dianhydride, 4,4′-oxydianiline and paraphenylenediamine, or derived from 3,3′,4,4′-biphenyl tetracarboxylic dianhydride, pyromellitic dianhydride, 4,4′-oxydianiline, or derived from 3,3′,4,4′-biphenyl tetracarboxylic dianhydride, pyromellitic dianhydride, 4,4′-oxydianiline and paraphenylenediamine, or derived from i) blocks of pyromellitic dianhydride and 4,4′-oxydianiline and ii) blocks of pyromellitic dianhydride and paraphenylenediamine, or derived from pyromellitic dianhydride, oxydiphthalic dianhydride and 1,3-bis-(4-aminophenoxy) benzene, or a mixture thereof.

### Claim 16 (depends on 13)

The method of claim 13, wherein the third polyamic acid is derived from pyromellitic dianhydride and 4,4′-oxydianiline, or derived from 3,3′,4,4′-biphenyl tetracarboxylic dianhydride and paraphenylenediamine, or derived from pyromellitic dianhydride, 4,4′-oxydianiline and paraphenylenediamine, or derived from 3,3′,4,4′-biphenyl tetracarboxylic dianhydride, pyromellitic dianhydride, 4,4′-oxydianiline, or derived from 3,3′,4,4′-biphenyl tetracarboxylic dianhydride, pyromellitic dianhydride, 4,4′-oxydianiline and paraphenylenediamine, or derived from i) blocks of pyromellitic dianhydride and 4,4′-oxydianiline and ii) blocks of pyromellitic dianhydride and paraphenylenediamine, or derived from pyromellitic dianhydride, oxydiphthalic dianhydride and 1,3-bis-(4-aminophenoxy) benzene, or a mixture thereof.

### Claim 17 (depends on 13)

The method of claim 13, wherein the first submicron fumed metal oxide comprises fumed alumina, fumed silica or a mixture thereof.

### Claim 18 (depends on 13)

The method of claim 13, wherein the second submicron fumed metal oxide comprises fumed alumina, fumed silica or a mixture thereof.

### Claim 19 (depends on 13)

The method of claim 13, wherein the second and third polyimide layers are the same.