# US 12,759,245 B2 · Method for manufacturing a fibrous material which is made of continuous fibres and impregnated with a thermoplastic polymer

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- Number: US 12,759,245 B2
- Document ID: US12759245B2
- Status: Granted
- Kind: B2
- Application number: 18/258,093
- Filed: 2021-12-15
- Published: 2024-02-15
- Granted: 2026-10-13
- Earliest claimed: 2020-12-17
- Assignees: Arkema France
- Applicants: Arkema France
- Inventors: Thibaut Savart; Arthur Babeau; Axel Salinier
- Web page: https://patentgrep.com/patent/US12759245B2

## CPC

- B29C 70/16: using fibres of substantial or continuous length {(non-woven fabrics per se D04H3/00)}
- B29C 35/0244: {using fluidised bed}
- B29C 70/388: {Tape placement heads, e.g. component parts, details or accessories}
- B29C 70/56: Tensioning reinforcements before or during shaping
- B29C 2035/0822: {using IR radiation}
- B29K 2105/10: {Cords, strands or rovings, e.g.} oriented {cords, strands or rovings}
- B29K 2277/00: Use of {PA, i.e.} polyamides, e.g. polyesteramides {or derivatives thereof,} as reinforcement
- B29K 2307/04: Carbon
- B29K 2507/04: Carbon
- B29C: SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING (making preforms B29B11/00; making laminated products by combining previously unconnected layers which become one product whose layers will remain together B32B37/00 - B32B41/00)
- B29K: INDEXING SCHEME ASSOCIATED WITH SUBCLASSES B29B, B29C OR B29D, RELATING TO MOULDING MATERIALS OR TO MATERIALS FOR {MOULDS, } REINFORCEMENTS, FILLERS OR PREFORMED PARTS, e.g. INSERTS

## Abstract

Impregnation of a fibrous material made from continuous fibres with a thermoplastic polymer matrix, the fibrous material comprising a thermoplastic sizing polymer and, before impregnation, an initial width. The method comprises an expansion step which is carried out by means of at least two tensioning members (E) and a heating system SC for heating the tensioning members and/or the fibrous material, the expansion being from 1.5 to 5 times the initial width. The expanded fibrous material is cooled below the Tg of the thermoplastic sizing polymer by means of a cooling system before being brought into contact with the thermoplastic polymer matrix.

## Claims

### Claim 1

A method for manufacturing an impregnated fibrous material comprising a fibrous material made of continuous fibres and at least one thermoplastic polymer matrix, characterized in that said fibrous material is sized by a sizing thermoplastic polymer and has, before its pre-impregnation with said thermoplastic polymer, an initial width, said method comprising a step of spreading said fibrous material before a pre-impregnation step, said spreading step being carried out by means of at least two tension devices and at least one heating system for heating said tension devices and/or said fibrous material, said spreading, after said fibrous material has passed in contact with said tension devices, being between 1.5 and 5 times the initial width, said spread fibrous material being cooled below a Tg of the sizing thermoplastic polymer by means of a cooling system before it is placed in contact with said thermoplastic polymer matrix in a pre-impregnation system to carry out the pre-impregnation step, the spreading being consistent and always representing 1.5 to 5 times the initial width when said fibrous material is placed in contact with said thermoplastic polymer matrix in the pre-impregnation system.

### Claim 2 (depends on 1)

The method as claimed in claim 1, characterized in that the heating system and the at least two tension devices are located outside or inside the pre-impregnation system.

### Claim 3 (depends on 1)

The method as claimed in claim 1, characterized in that the heating system and the at least two tension devices are located outside the pre-impregnation system and said pre-impregnation step is carried out with a system chosen from among a fluidized bed, spraying through a nozzle, aqueous dispersion and a molten route.

### Claim 4 (depends on 1)

The method as claimed in claim 1, characterized in that the heating system and the at least two tension devices are located inside the pre-impregnation system and said pre-impregnation step is carried out with a system chosen from among a fluidized bed, spraying through a nozzle and aqueous dispersion.

### Claim 5 (depends on 1)

The method as claimed in claim 1, characterized in that said at least two tension devices conduct heat and the heating system is present and integrated in said at least two tension devices.

### Claim 6 (depends on 1)

The method as claimed in claim 1, characterized in that said at least two tension devices conduct heat and the heating system is present above said at least two tension devices for heating the fibrous material and said at least two tension devices.

### Claim 7 (depends on 5)

The method as claimed in claim 5, characterized in that said at least two tension devices conduct heat and a first heating means is present and integrated in said at least two tension devices and a second heating means is present above said at least two tension devices for heating the fibrous material and said at least two tension devices.

### Claim 8 (depends on 7)

The method as claimed in claim 7, characterized in that at least one of the tension devices may be cooled to control a temperature of the fibrous material.

### Claim 9 (depends on 1)

The method as claimed in claim 1, characterized in that said at least two tension devices do not conduct heat and a heating means is present above said at least two tension devices for heating the fibrous material.

### Claim 10 (depends on 1)

The method as claimed in claim 1, characterized in that the at least two tension devices are compression rollers of convex, concave or cylindrical shape.

### Claim 11 (depends on 10)

The method as claimed in claim 10, characterized in that the number of rollers in contact with said fibrous material ranges from 2 to 20.

### Claim 12 (depends on 10)

The method as claimed in claim 10, characterized in that said compression rollers are in co-rotation and/or in counter-rotation.

### Claim 13 (depends on 10)

The method as claimed in claim 10, characterized in that said compression rollers are vibrating.

### Claim 14 (depends on 10)

The method as claimed in claim 10, characterized in that said compression rollers have a surface treatment and/or an apparent surface roughness minimizing friction with the fibrous material.

### Claim 15 (depends on 10)

The method as claimed in claim 10, characterized in that said rollers are separated from one another by a distance of less than 30 cm.

### Claim 16 (depends on 1)

The method as claimed in claim 1, characterized in that said thermoplastic polymer is a non-reactive thermoplastic polymer.

### Claim 17 (depends on 16)

The method as claimed in claim 16, characterized in that it the method comprises a step of heating the pre-impregnated fibrous material to melt the thermoplastic polymer of the matrix and to finalize the impregnation of said fibrous material.

### Claim 18 (depends on 1)

The method as claimed in claim 1, characterized in that said thermoplastic polymer of the matrix is a reactive prepolymer capable of reacting with itself or with another prepolymer, as a function of chain ends borne by said prepolymer, or else with a chain extender.

### Claim 19 (depends on 18)

The method as claimed in claim 18, characterized in that it the method comprises a step of heating the pre-impregnated fibrous material to melt and polymerize the thermoplastic prepolymer of the matrix optionally with said extender and to finalize the impregnation of said fibrous material.

### Claim 20 (depends on 1)

The method as claimed in claim 1, characterized in that said at least one thermoplastic polymer of the matrix is selected from: poly(aryl ether ketone)s, (PAEKs); poly(aryl ether ketone ketone)s, (PAEKKs); aromatic polyetherimides (PEIs); polyaryl sulphones; polyaryl sulphides; polyamides (PAs); polyether block amides (PEBAs); polyacrylates; polyolefins; polylactic acid (PLA); polyvinyl alcohol (PVA); and fluoropolymers; and blends thereof.

### Claim 21 (depends on 1)

The method as claimed in claim 1, characterized in that said at least one thermoplastic polymer of the matrix is a polymer having a glass transition temperature Tg≥80° C., or a semicrystalline polymer having a melting temperature Tm≥150° C.

### Claim 22 (depends on 1)

The method as claimed in claim 1, characterized in that said at least one thermoplastic polymer of the matrix is selected from polyamides, PEKK, PEI, and a blend of PEKK and PEI.

### Claim 23 (depends on 16)

The method as claimed in claim 16, characterized in that the content of fibres in said impregnated fibrous material is from 45% to 65% by volume.

### Claim 24 (depends on 16)

The method as claimed in claim 16, characterized in that the degree of porosity in said impregnated fibrous material is less than 10%.

### Claim 25 (depends on 1)

The method as claimed in claim 1, characterized in that said thermoplastic polymer of the matrix further comprises carbon-based fillers.

### Claim 26 (depends on 1)

The method as claimed in claim 1, characterized in that said fibrous material comprises continuous fibres selected from fibres of mineral origin, natural fibres, or amorphous thermoplastic fibres having a glass transition temperature Tg above the Tg of said thermoplastic polymer of the matrix or of said blend of polymers when the latter is amorphous or above the Tm of said thermoplastic polymer of the matrix or of said blend of polymers when the latter is semicrystalline, or semicrystalline thermoplastic fibres having a melting temperature Tm above the Tg of said thermoplastic polymer of the matrix or of said blend of polymers when the latter is amorphous or above the Tm of said thermoplastic polymer of the matrix or of said blend of polymers when the latter is semicrystalline, or a mixture of two or more of said fibres.

### Claim 27 (depends on 1)

A use of the method as defined in claim 1, for the manufacture of calibrated tapes suitable for the manufacture of three-dimensional composite parts, by automated layup of said tapes using a robot.

### Claim 28 (depends on 27)

The use as claimed in claim 27, characterized in that said composite parts relate to a field selected from the group consisting of transport, oil and gas, hydrogen, gas storage; renewable energy; thermal protection panels; sports; and leisure.
