GB2168361A - Impregnating fibres reinforcement with polymer materials - Google Patents
Impregnating fibres reinforcement with polymer materials Download PDFInfo
- Publication number
- GB2168361A GB2168361A GB08530124A GB8530124A GB2168361A GB 2168361 A GB2168361 A GB 2168361A GB 08530124 A GB08530124 A GB 08530124A GB 8530124 A GB8530124 A GB 8530124A GB 2168361 A GB2168361 A GB 2168361A
- Authority
- GB
- United Kingdom
- Prior art keywords
- polymer material
- fibres
- reinforcement
- fibres reinforcement
- impregnating
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Withdrawn
Links
- 239000002861 polymer material Substances 0.000 title claims abstract description 43
- 230000002787 reinforcement Effects 0.000 title claims abstract description 40
- 238000000034 method Methods 0.000 claims abstract description 24
- 239000002245 particle Substances 0.000 claims abstract description 16
- 239000006185 dispersion Substances 0.000 claims abstract description 14
- 239000000463 material Substances 0.000 claims abstract description 14
- 229920001169 thermoplastic Polymers 0.000 claims abstract description 10
- 239000004416 thermosoftening plastic Substances 0.000 claims abstract description 9
- 239000007788 liquid Substances 0.000 claims abstract description 8
- 238000005470 impregnation Methods 0.000 claims abstract description 6
- 230000009477 glass transition Effects 0.000 claims abstract description 5
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 5
- 239000004696 Poly ether ether ketone Substances 0.000 claims abstract description 4
- 239000004952 Polyamide Substances 0.000 claims abstract description 4
- 239000004697 Polyetherimide Substances 0.000 claims abstract description 4
- 239000004793 Polystyrene Substances 0.000 claims abstract description 4
- 229920001643 poly(ether ketone) Polymers 0.000 claims abstract description 4
- 229920002492 poly(sulfone) Polymers 0.000 claims abstract description 4
- 229920002647 polyamide Polymers 0.000 claims abstract description 4
- 229920002530 polyetherether ketone Polymers 0.000 claims abstract description 4
- 229920001601 polyetherimide Polymers 0.000 claims abstract description 4
- -1 polyethersulphone Polymers 0.000 claims abstract description 4
- 229920002223 polystyrene Polymers 0.000 claims abstract description 4
- 238000009835 boiling Methods 0.000 claims abstract description 3
- UCKMPCXJQFINFW-UHFFFAOYSA-N Sulphide Chemical compound [S-2] UCKMPCXJQFINFW-UHFFFAOYSA-N 0.000 claims description 3
- 229920000642 polymer Polymers 0.000 abstract description 7
- 239000002270 dispersing agent Substances 0.000 abstract description 2
- 239000002904 solvent Substances 0.000 description 5
- 238000000465 moulding Methods 0.000 description 4
- 238000001035 drying Methods 0.000 description 3
- 239000002243 precursor Substances 0.000 description 3
- 238000007654 immersion Methods 0.000 description 2
- 238000005507 spraying Methods 0.000 description 2
- 229920001187 thermosetting polymer Polymers 0.000 description 2
- 239000004604 Blowing Agent Substances 0.000 description 1
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 238000013019 agitation Methods 0.000 description 1
- 125000003118 aryl group Chemical group 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 229940000425 combination drug Drugs 0.000 description 1
- 239000002131 composite material Substances 0.000 description 1
- 238000001704 evaporation Methods 0.000 description 1
- 230000008020 evaporation Effects 0.000 description 1
- 239000004744 fabric Substances 0.000 description 1
- 238000009730 filament winding Methods 0.000 description 1
- 239000000945 filler Substances 0.000 description 1
- 239000012467 final product Substances 0.000 description 1
- 239000011521 glass Substances 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 238000010348 incorporation Methods 0.000 description 1
- 238000004898 kneading Methods 0.000 description 1
- 238000009940 knitting Methods 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 239000000049 pigment Substances 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 239000000047 product Substances 0.000 description 1
- 239000010453 quartz Substances 0.000 description 1
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 1
- 239000004634 thermosetting polymer Substances 0.000 description 1
- 238000009941 weaving Methods 0.000 description 1
Classifications
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
- C08J5/00—Manufacture of articles or shaped materials containing macromolecular substances
- C08J5/04—Reinforcing macromolecular compounds with loose or coherent fibrous material
Landscapes
- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Materials Engineering (AREA)
- Health & Medical Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Medicinal Chemistry (AREA)
- Polymers & Plastics (AREA)
- Organic Chemistry (AREA)
- Reinforced Plastic Materials (AREA)
Abstract
Method of impregnating fibres reinforcement with polymer material including the steps of: mixing the polymer material in particle form with a liquid in which the polymer material does not dissolve to form a dispersion; and impregnating the fibres reinforcement with the dispersion. The fibres reinforcement is said to be dried after impregnation with the dispersent. The use of the processes described with any polymer material is disclosed, however, the preferred polymers are said to be thermoplastics materials such as polysulphone, polyethersulphone, polyetheretherketone, polyetherketone, polyetherimide, polystyrene, polyphenelene suphide and polyamides. Any suitable liquid dispersant having a boiling point below the glass transition temperature of the thermoplastics material may be used and water is said to be preferred for the polymers enumerated. The particle size of the polymer used is said to vary in accordance with the characteristics of the fibres reinforcement used but a typical particle size not exceeding 5 microns is disclosed. The specification discloses in addition articles made from a fibres reinforced polymer material as described.
Description
SPECIFICATION
Impregnating fibres reinforcement with polymer materials
The invention concerns the impregnation of fibres reinforcement with polymer material.
Throughout this specification the term fibres reinforcement encompasses filaments, fibres or tows of filaments or fibres, mats of filaments or fibres or cloths prepared by weaving, knitting, laying-up or the like such filaments, fibres or tows, for use as reinforcement of a polymer material.
The use of thermosetting polymer material with fibres reinforcement to form articles is more extensive than the use of fibres reinforced thermosplastics materials despite the fact that the advantages of using a thermoplastics material are well known.
The production of a basic precursor (i.e. fibres reinforcement impregnated with a thermoplastics material) from which composite article can be made by moulding has proved difficult and costly (especially when the precursor must include 100% of the final desired polymer content).
An extensively used way of impregnating fibres reinforcement with a thermoplastics materials polymer material is to dissolve the polymer material and immerse the fibres reinforcement in the solution; after immersion the fibres reinforcement is dried to drive off all (or a desired part) of the solvent leaving the fibres reinforcement impregnated with the polymer material (or a solution thereof). In using this process difficulties are met in ensuring that all (or the required amount) of the solvent is removed. The presence of the solvent, even at very low levels can affect the further processing of the material (for example leading to the formation of voids in the finished article) and can seriously alter the characteristics of the finished article (for example the strength of the article).
Again, the known precursors tend to be inflexible and difficult to handle in moulding processes I the stiffness of the impregnated fibres reinforcement making them difficult to drape I that is to say difficult to conform to the shape of any mould in which they are placed.
To meet these and other problems we now propose a novel method of impregnating fibres reinforcement with a polymer material in particular a thermoplastic polymer material.
One aspect of the invention provides a method of impregnating fibres reinforcement with polymer material including the steps of: mixing the polymer material in particle form with a liquid in which the polymer material does not dissolve to form a dispersion: and impregnating the fibres reinforcement with the dispersion.
With advantage the polymer material is a thermoplastics material and the dispersent therefor has a boiling point below the glass transition temperature of the thermosplastics material. The polymer material may be an aromatic polymer material selected from the group comprising: polysulphone, polyethersulphone, polyetheretherketone, polyetherketone, polyetherimide, polystyrene, polyphenelene sulphide and a polyamide.
Preferably the dispersent is water.
Desirably the particle size of the polymer material is 5 microns or less.
A second aspect of the invention provides a reinforced polymer material made in accordance with of any of the methods noted above.
A third aspect of the invention provides an article and/or structure made from a fibres reinforced polymer material as noted above.
The impregnation of the fibres reinforcement in the liquid dispersent may be by immersion of the fibres reinforcement therein with together, if necessary, mechanical agitation, kneading or the like.
Drying of the fibres reinforcement after impregnation may be effected by evaporation at room temperature, mechanical drying or by heating to a temperature below the glass transition temperature of the polymer material. For example when the dispersent is water the impregnated fibres reinforcement may be dried rapidly in an oven at a temperature below the glass transition temperature of the polymer material - say 75 to 150"C if the polymer material is polyethersulphone.
The impregnated fibres reinforcement (either taken directly from the dispersion or after partial drying) may readily be laid up in a mould. As the liquid dispersent is not a solvent for the particular polymer material the particles of polymer material in the fibres reinforcement remain relatively mobile enabling the fibres reinforcement to be easily "draped" in a mould. Should the impregnated fibres reinforcement be completely dry (that is to say with all the liquid dispersant driven off) it is possible for the impregnated fibres reinforcement to be re-wetted, e.g. by spraying with the dispersent, should it be necessary to enable it to be readily "draped".
An advantage of the process now described is that impregnated cloths or mats of fibres reinforcement may be draped on a former or shaper for use in a moulding process whilst wet. Further, it is possible for several layers of fabric to be laid up on top of one another to form complex double curvature shapes. Fibres reinforcement impregnated in the described process may be used in vacuum or positive pressure moulding processes.
Pultrusion, filament winding spraying and impregnation of knitted or woven shapes may also readily be accomplished with the present invention.
The dispersion of the polymer material may contain any thermosetting or thermosplastics material; however, we have found that the process is of particular advantage with polymer materials such as polysulphone, polyethersulphone, polyetheretherketone, polyetherketone, polyetherimide, polystyrene, polyphenelene sulphide, polyamides or other thermoplastics material obtainable in fine powder form.
Although water is described as the preferred dispersent it will be appreciated that any other liquid which is not a solvent for the polymer material may be used, for example, various different forms of Freeon may be used either alone or in combina tion.
Although as described the invention is of particular advantage when used with the particular polymer materials recited it will be appreciated that the methods described herein are utilisable with any polymer material having a particle size enabling it to form a dispersion and in that form be impregnated into fibres reinforcement. The maximum particle size will, it will be appreciated, vary in accordance with the polymer used and the physical size of essential requirement is that the size of the majority of the particles be sufficiently small to permit the particles of the polymer to fully pass into the interstices of the fibres reinforcement.
In normal cases it will be desired that all the polymer material be of a size enabling it to percolate between the fibres of the reinforcement, that is to say that all the particles in the dispersion be below the (critical) maximum size for the fibres reinforcement being used - typically 5 Microns for commercially available glass, carbon or quartz fibres however, in some applications it is possible that a proportion of the polymer particles in the dispersion may be above that critical size I providing always that there are sufficient particles in the dispersion below that critical size to enable the fibres reinforcement to be impregnated to the level desired in the particular application under consideration.
It will also be appreciated that the fibres to be impregnated by the methods disclosed in this specification must not have been heavily pretreated (e.g. sized) to an extent preventing the dispersion entering the interstices of the fibres. If in fact the fibres reinforcement have been so pretreated it is necessary for them to be cleaned before they are impregnated by the methods disclosed herein.
It will be'appreciated that the process now described may be modified by the incorporation in the dispersion (and therefore in the finished product) of other desired particles and elements, such as blowing agents, pigments, other additives and/ or fillers having decorative and/or functional characteristics in the final product.
Claims (9)
1. A method of impregnating fibres reinforcement with polymer material including the steps of: mixing the polymer material in particle form with a liquid in which the polymer material does not dissolve to form a dispersion; and impregnating the fibres reinforcement with the dispersion.
2. A method as claimed in claim 1, wherein the fibres reinforcement is at least partially dried after impregnation with the dispersent.
3. A method as claimed in claim 1 or claim 2, wherein the polymer material is a thermoplastics material and the dispersent therefor has a boiling point below the glass transition temperature of the thermoplastics material.
4. A method as claimed in claim 1, claim 2 or claim 3, wherein the polymer material is selected from the group comprising polysulphone, polyethersulphone, polyetheretherketone, polyetherketone, polyetherimide, polystyrene, polyphenelene sulphide and a polyamide.
5. A method as claimed in any one of the preceding claims wherein the dispersent is water.
6. A method as claimed in any one of the preceding claim wherein the particle size of the polymer material is 5 microns or less.
7. A method of impregnating fibres reinforcement with a polymer material as claimed in claim 1 and substantially as herein described.
8. A fibres reinforced polymer material made in accordance with the method of any one of the preceding claims.
9. An article made from a fibres reinforced polymer material as claimed in claim 8.
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| GB848430949A GB8430949D0 (en) | 1984-12-07 | 1984-12-07 | Impregnating fibre reinforcements |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| GB8530124D0 GB8530124D0 (en) | 1986-01-15 |
| GB2168361A true GB2168361A (en) | 1986-06-18 |
Family
ID=10570840
Family Applications (2)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| GB848430949A Pending GB8430949D0 (en) | 1984-12-07 | 1984-12-07 | Impregnating fibre reinforcements |
| GB08530124A Withdrawn GB2168361A (en) | 1984-12-07 | 1985-12-06 | Impregnating fibres reinforcement with polymer materials |
Family Applications Before (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| GB848430949A Pending GB8430949D0 (en) | 1984-12-07 | 1984-12-07 | Impregnating fibre reinforcements |
Country Status (4)
| Country | Link |
|---|---|
| EP (1) | EP0203985A1 (en) |
| AU (1) | AU5235686A (en) |
| GB (2) | GB8430949D0 (en) |
| WO (1) | WO1986003449A1 (en) |
Cited By (10)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| EP0275382A1 (en) * | 1986-12-22 | 1988-07-27 | General Electric Company | Method for preparing composite felt preforms |
| EP0209391A3 (en) * | 1985-07-17 | 1988-08-31 | Sumitomo Chemical Company, Limited | Resin composition and circuit board moulded from the same |
| US4792481A (en) * | 1986-11-28 | 1988-12-20 | Phillips Petroleum Company | Reinforced plastic |
| EP0272648A3 (en) * | 1986-12-20 | 1989-11-08 | Toho Rayon Co., Ltd. | Method for producing carbon fiber reinforced thermoplastic resin product |
| EP0368412A3 (en) * | 1988-11-10 | 1990-09-12 | Stamicarbon B.V. | Method for the production of flexible, polymer-impregnated reinforcing materials, the polymer-impregnated reinforcing materials produced and shaped articles produced on the basis of these reinforcing materials |
| WO1993002127A1 (en) * | 1991-07-16 | 1993-02-04 | Dsm N.V. | Process for making a preimpregnated material |
| US5480603A (en) * | 1994-05-19 | 1996-01-02 | The Dow Chemical Company | Method for preparing preforms for molding processes |
| RU2153981C2 (en) * | 1995-02-24 | 2000-08-10 | Биоксид Ой | Fibrous polymer prepreg, methods for preparation and utilization thereof |
| EP2813539A1 (en) * | 2013-06-11 | 2014-12-17 | Johns Manville | Fiber-reinforced composite articles and methods of making them |
| WO2017004112A1 (en) * | 2015-06-30 | 2017-01-05 | Sabic Global Technologies B.V. | Methods of manufacture of prepregs and composites from polyimide particles, and articles prepared therefrom |
Families Citing this family (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US4894105A (en) * | 1986-11-07 | 1990-01-16 | Basf Aktiengesellschaft | Production of improved preimpregnated material comprising a particulate thermoplastic polymer suitable for use in the formation of substantially void-free fiber-reinforced composite article |
| US4919739A (en) * | 1986-11-07 | 1990-04-24 | Basf Aktiengesellschaft | Production of improved preimpregnated material comprising a particulate thermosetting resin suitable for use in the formation of a substantially void-free fiber-reinforced composite article |
| US5128198A (en) * | 1986-11-07 | 1992-07-07 | Basf Aktiengesellschaft | Production of improved preimpregnated material comprising a particulate thermoplastic polymer suitable for use in the formation of a substantially void-free fiber-reinforced composite article |
| DE3738749A1 (en) * | 1987-11-14 | 1989-05-24 | Basf Ag | FIBER COMPOSITES |
| US4943472A (en) * | 1988-03-03 | 1990-07-24 | Basf Aktiengesellschaft | Improved preimpregnated material comprising a particulate thermosetting resin suitable for use in the formation of a substantially void-free fiber-reinforced composite article |
| DE69907907T2 (en) | 1998-06-08 | 2004-03-11 | Complastik Corp., Lowell | COMPOSITE ITEMS, IN PARTICULAR PREPREGS, PREFORMS, LAMINATES AND SANDWICH MOLDED PARTS, AND METHOD FOR THE PRODUCTION THEREOF |
| AU2002241584A1 (en) | 2000-12-06 | 2002-06-18 | Complastik Corporation | Hybrid composite articles and methods for their production |
Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| GB439884A (en) * | 1934-06-07 | 1935-12-09 | Deutsche Celluloid Fabrik | Manufacture of textile fabrics coated or impregnated with polymerisation products |
| GB1253291A (en) * | 1968-01-11 | 1971-11-10 | Asahi Glass Kabushiki Kaisha | Method of producing mouldable reinforced thermoplastic granular material |
| US4163742A (en) * | 1978-02-09 | 1979-08-07 | E. I. Du Pont De Nemours And Company | Process and product prepared from tetrafluoroethylene resin and graphite fibers |
Family Cites Families (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS5750654B2 (en) * | 1973-03-28 | 1982-10-28 | ||
| US4292105A (en) * | 1978-12-28 | 1981-09-29 | Union Carbide Corporation | Method of impregnating a fibrous textile material with a plastic resin |
| US4402780A (en) * | 1981-04-27 | 1983-09-06 | Hiroyuki Ogoe | Process for preparing laminates with thermoplastic resins |
| FR2516441A1 (en) * | 1981-11-18 | 1983-05-20 | Spie Batignolles | PROCESS FOR PRODUCING FIBER-LOADED THERMOPLASTIC RESIN PROFILES, INSTALLATION FOR IMPLEMENTATION, PROFILES OBTAINED AND USE THEREOF |
| EP0102711A3 (en) * | 1982-07-28 | 1986-01-15 | Imperial Chemical Industries Plc | Process for producing fibre-reinforced polymer compositions |
| CA1257157A (en) * | 1983-07-12 | 1989-07-11 | Chen-Chi M. Ma | Stampable sheets of fiber mat reinforced poly(arylene sulfide) and method of preparation |
-
1984
- 1984-12-07 GB GB848430949A patent/GB8430949D0/en active Pending
-
1985
- 1985-12-06 AU AU52356/86A patent/AU5235686A/en not_active Abandoned
- 1985-12-06 EP EP19860900182 patent/EP0203985A1/en not_active Withdrawn
- 1985-12-06 WO PCT/GB1985/000558 patent/WO1986003449A1/en not_active Ceased
- 1985-12-06 GB GB08530124A patent/GB2168361A/en not_active Withdrawn
Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| GB439884A (en) * | 1934-06-07 | 1935-12-09 | Deutsche Celluloid Fabrik | Manufacture of textile fabrics coated or impregnated with polymerisation products |
| GB1253291A (en) * | 1968-01-11 | 1971-11-10 | Asahi Glass Kabushiki Kaisha | Method of producing mouldable reinforced thermoplastic granular material |
| US4163742A (en) * | 1978-02-09 | 1979-08-07 | E. I. Du Pont De Nemours And Company | Process and product prepared from tetrafluoroethylene resin and graphite fibers |
| GB2014158A (en) * | 1978-02-09 | 1979-08-22 | Du Pont | Tetrafluroethylene resin compositions and process for their preparation |
Non-Patent Citations (1)
| Title |
|---|
| NOTE! GB A 2014158 AND US 4163742 ARE EQUIVALENT * |
Cited By (14)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| EP0209391A3 (en) * | 1985-07-17 | 1988-08-31 | Sumitomo Chemical Company, Limited | Resin composition and circuit board moulded from the same |
| US4792481A (en) * | 1986-11-28 | 1988-12-20 | Phillips Petroleum Company | Reinforced plastic |
| EP0272648A3 (en) * | 1986-12-20 | 1989-11-08 | Toho Rayon Co., Ltd. | Method for producing carbon fiber reinforced thermoplastic resin product |
| EP0275382A1 (en) * | 1986-12-22 | 1988-07-27 | General Electric Company | Method for preparing composite felt preforms |
| EP0368412A3 (en) * | 1988-11-10 | 1990-09-12 | Stamicarbon B.V. | Method for the production of flexible, polymer-impregnated reinforcing materials, the polymer-impregnated reinforcing materials produced and shaped articles produced on the basis of these reinforcing materials |
| BE1005106A3 (en) * | 1991-07-16 | 1993-04-20 | Dsm Nv | PROCESS FOR MAKING A MATERIAL BY VOORGEIMPREGNEERD impregnating a fibrous reinforcement with a dispersion. |
| WO1993002127A1 (en) * | 1991-07-16 | 1993-02-04 | Dsm N.V. | Process for making a preimpregnated material |
| US5480603A (en) * | 1994-05-19 | 1996-01-02 | The Dow Chemical Company | Method for preparing preforms for molding processes |
| US5593758A (en) * | 1994-05-19 | 1997-01-14 | The Dow Chemical Company | Method for preparing preforms for molding processes |
| RU2153981C2 (en) * | 1995-02-24 | 2000-08-10 | Биоксид Ой | Fibrous polymer prepreg, methods for preparation and utilization thereof |
| EP2813539A1 (en) * | 2013-06-11 | 2014-12-17 | Johns Manville | Fiber-reinforced composite articles and methods of making them |
| US9855680B2 (en) | 2013-06-11 | 2018-01-02 | Johns Manville | Fiber-reinforced composite articles and methods of making them |
| US10780609B2 (en) | 2013-06-11 | 2020-09-22 | Jonhs Manville | Fiber-reinforced composite articles and methods of making them |
| WO2017004112A1 (en) * | 2015-06-30 | 2017-01-05 | Sabic Global Technologies B.V. | Methods of manufacture of prepregs and composites from polyimide particles, and articles prepared therefrom |
Also Published As
| Publication number | Publication date |
|---|---|
| GB8430949D0 (en) | 1985-01-16 |
| AU5235686A (en) | 1986-07-01 |
| WO1986003449A1 (en) | 1986-06-19 |
| GB8530124D0 (en) | 1986-01-15 |
| EP0203985A1 (en) | 1986-12-10 |
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Legal Events
| Date | Code | Title | Description |
|---|---|---|---|
| WAP | Application withdrawn, taken to be withdrawn or refused ** after publication under section 16(1) |