MXPA00001774A - Coated, long fiber reinforcing composite structure and process of preparation thereof - Google Patents

Abstract

A process for the continuous preparation of a coated, long fiber reinforcing composite structure suitable for the preparation of shaped articles. The process is characterized by impregnating a plurality of continuous lengths of reinforcing fiber strands with a first thermoplastic resin material while continuously drawing the fiber strands to produce a long fiber reinforcing composite structure followed by coating a second thermoplastic resin material containing additives onto the long fiber reinforcing composite structure to produce a coated, long fiber reinforcing composite structure. The coating additives may be selected from mineral reinforcing agents, lubricants, flame retardants, blowing agents, foaming agents, ultraviolet light resistant agents, heat sensitive pigments, etc. The coated, long fiber reinforcing composite structure prepared according to the process is suitable for the preparation of shaped articles exhibiting good physical and chemical properties.

Description

STRUCTURE OF MIXED MATERIAL FOR REINFORCING LONG FIBER, REVESTIDA AND PROCEDURE TO PREPARE THE SAME FIELD OF THE INVENTION The present invention relates to a structure of mixed long-fiber reinforced material, coated and to a process for preparing it. The preparation process eliminates the need to combine selected additives such as pigments, reinforcing agents, flame retardants, etc. with the structure during or after manufacturing it as configured items.

BACKGROUND OF THE INVENTION The composite long-fiber reinforcement material structures are characterized as continuous fiber threads of material impregnated with a thermoplastic resin material, converted into pellets for easy handling and molded as shaped articles. The configured articles, ranging from zippers for recreational vehicles to bicycle frames, have good impact resistance and rigidity due to the unidirectional orientation of the reinforcing fiber strands in the configured article. Mixed long fiber reinforced material structures suitable for the preparation of shaped articles having good impact strength and stiffness can be prepared in accordance with the patent E.U.A. No. Re. 32,772, to Hawley, incorporated herein by reference. Hawley describes a process in which a mass of thermoplastic resin is extruded through a stationary die of impregnation as a plurality of continuous lengths of reinforcing fiber yarns passing through the die to produce a cylindrically shaped structure. Simultaneously, the resin material is extruded through the die and the reinforcing fibers are stretched across the die at speeds sufficient to cause complete impregnation of the individual fiber strands with the resin material. The structure of mixed long fiber reinforcement material, described in the patent E.U.A. No. 4,312,917 to Hawley, incorporated herein by reference, can be cut into individual inserts, placed in a two-piece stationary mold connected to an extruder, in which a thermoplastic resin is heated and injected into the mold to provide a resin coating on the cylindrical inserts to produce a combined structure of mixed material. Hawley's procedure for placing a thermoplastic resin coating on the long fiber reinforced composite material structure has resulted in more work and insufficient production of composite composite structures to meet the requirements of manufacturers of articles configured with reinforced thermoplastics. prepared from it.

In an attempt to overcome the intense work procedure of Hawley, and to increase the appearance as well as the physical and chemical properties of the shaped articles prepared from the mixed fiber reinforcement material structure, physical pellets have been physically mixed. the same with additive materials, and the resulting product is molded into shaped articles. Generally, the desired additive materials are cut into pellets, physically mixed with pellets of the mixed long fiber reinforcing material structure, and molded as shaped articles. This physical mixing process has failed to provide suitable molding materials. Due to certain incompatibilities between the two substances, perhaps the shape, density and size of the pellet, it has been difficult to prepare uniform physical mixtures of the mixed long fiber reinforcing material structure and the additives. Typically, the non-uniform combinations prepared from these mixtures have resulted in shaped articles having localized surface areas containing high or low concentrations of any component. Another method for incorporating additives into the composite long fiber reinforcement material structure prior to the manufacture of articles formed therefrom requires the addition of the additive to the thermoplastic impregnation resin. Nevertheless, due to the high temperatures required to melt some of the resins to ensure proper impregnation of the fiber strands, sometimes when approaching the degradation temperature of the resins, temperature sensitive additives typically degrade and emit volatile vapors during the heating and extrusion processes.

BRIEF DESCRIPTION OF THE INVENTION The present invention is directed to a process for the continuous preparation of a structure of mixed long-fiber reinforcement material, coated suitable for preparing shaped articles, characterized by the steps of: a) extruding a mass of a first thermoplastic resin material in fluid state having no discrete shape in and longitudinally through a first elongated stationary die having no relatively mobile components, said die having a central, fully open, continuous passage extending longitudinally from one side to the other thereof, and a plurality of lobes projecting radially inwardly toward said central passage from separate sites along the length of the opposite internal side walls of said central passage in interleaved relation to each other to form an intricate passageway through which said fluid flows. first thermoplastic resin material; b) simultaneously introducing a plurality of continuous lengths of reinforcing fiber yarns into said central passage of the first die at different places therein; c) separately passing each of said fiber strands longitudinally within and along the length of said central passage over and between said interspersed lobes in the presence of said fluid mass of the first thermoplastic resin material to come into contact and completely permeate each one of said fiber yarns with said first thermoplastic resin material to produce a long fiber composite structure; d) stretching the composite structure of long fiber reinforcing material from said first die longitudinally thereto, whereby the mixed material structure is characterized by containing continuous fiber yarns extending in said first thermoplastic resin material generally parallel to the longitudinal axis of the structure; e) extruding a mass of a second thermoplastic resin material and an additive material to produce a second thermoplastic resin-additive material, wherein said second thermoplastic resin-additive material is in a fluid state without having a discrete form, in and longitudinally through a second elongated stationary die having no relatively mobile components, said die having a central, fully open, continuous passage extending longitudinally from one side to the other thereof to form a passage through which said second thermoplastic resin flows; additive material; f) simultaneously introducing the structure of mixed long fiber reinforcing material into said central passage of the second stationary die; g) contacting and coating the long fiber reinforced composite material structure with the second thermoplastic resin-additive material to produce a long, coated fiber reinforced composite material structure, in which the first and second resin materials thermoplastic are bonded at the interface of the first and second thermoplastic resin materials; h) stretching the structure of mixed long fiber reinforcement material, coated from the second die; and i) cutting the structure of mixed, long-fiber reinforced composite material as pellets. The present invention is also directed to a long, coated, fiber reinforced composite structure characterized as a core element of mixed long fiber reinforcement material composed of a first thermoplastic resin material having a plurality of embedded fiber strands. and which extend therein generally parallel to the longitudinal axis of the central element; a thermoplastic coating element composed of a second thermoplastic resin material and an additive material, in which the coating element surrounds the central element; and an intermediate mixing zone between the coating and core elements which join the first and second thermoplastic resin materials.

BRIEF DESCRIPTION OF THE DRAWINGS Although the specification concludes with claims that particularly claim and distinctly claim the present invention, the invention will be better understood from the following description along with the accompanying drawings in which: Figure 1 is a schematic elevation view of an apparatus used for produce structures of mixed, long-fiber reinforced, coated material; and Figure 2 is an elevation and cross-sectional view of a mixed, long-fiber reinforced structure prepared in accordance with the process.

DETAILED DESCRIPTION OF THE INVENTION In accordance with the present invention there is disclosed a structure of mixed long-fiber reinforcing material, coated as well as a process for the preparation thereof. The process is useful for incorporating additives into the composite structure of long fiber reinforcing material that can not be added to thermoplastic resins used to impregnate long fiber reinforcing yarns. The impregnation step of the process requires a resin having low viscosity and high flow properties to ensure complete impregnation of the individual fiber strands. Since many additives will increase the viscosity of the resin, decreasing the flow and desirable impregnation properties, it is not advantageous to incorporate such additives into the impregnation resin. However, it is possible to incorporate these viscosity enhancing additives as well as other additives into the mixed long fiber reinforcement material structures after the impregnation step has been completed by means of the novel process of the present invention. Generally, the invention is a stretch extrusion process for the continuous preparation of a thermoplastic structure of mixed long fiber reinforcing material characterized by the steps of extruding a mass of a first thermoplastic resin material in a fluid state in a impregnation die while at the same time introducing a plurality of continuous lengths of reinforcing fiber yarns into the die, contacting and impregnating each fiber yarn with the first thermoplastic resin material to provide a structure of mixed reinforcement material. of long fiber, comprising improving the steps of: a) heating a second thermoplastic resin material and an additive material to a temperature to produce a second thermoplastic resin-fluid additive material combination without degrading the additive material in the combination; b) extruding the combination of second thermoplastic resin-additive material in a stationary casing die having no relatively mobile components, said casing die having a central, fully open, continuous passage extending longitudinally from one side to the other, walls opposite sides of said central passage through which said combination of second thermoplastic resin-additive material flows; c) introducing simultaneously the structure of mixed long-fiber reinforcing material into said central passage of the coating die; d) contacting the structure of mixed long-fiber reinforcement material with the combination of second thermoplastic resin-additive material to form an outer coating of the combination of second thermoplastic resin-additive material on the structure of mixed fiber reinforcing material long to produce a structure of mixed, long-fiber reinforced, coated material; e) stretching the composite structure of long fiber reinforcing material, coated from the coating die; and f) cutting as a pellet the structure of mixed, long-fiber reinforced, coated material. Referring to FIG. 1, a schematic top elevation view of a typical apparatus in FIG. which the novel process of the invention is conducted. The process can be characterized as a stretch extrusion process in which a mass of a first thermoplastic resin material in a fluid state having no discrete shape is extruded longitudinally through a first stationary die of elongate impregnation 11 while at the same time the reinforcing fiber strands 12 are stretched through the die 11 by a stretching assembly 18. The die 11 can be characterized as having a central passage completely open, continuous extending longitudinally from one side to another thereof, and a plurality of lobes projecting radially inward toward the central passage from separate sites along the length of the opposite, inner side walls of said central passage in relation interleaved with one another to form an intricate passage in which the first thermoplastic resin material flows. The lobes work by allowing the individual fiber strands to pass over at least one lobe such that the first thermoplastic resin material completely impregnates the strands. The die 11 is attached to the extruder 13 in which the first thermoplastic resin material is heated and formed into a fluid mass. The continuous length of the reinforcing fiber yarns 12 is stretched across the central passage of the die 11 and impregnated with the first thermoplastic resin material to produce the mixed fiber reinforcement material structure 14. Optionally, although the first The thermoplastic resin material is still in the fluid state, the impregnated yarns are stretched through a dosing device in which the cross-sectional shape and diameter can be defined to form the mixed long fiber reinforcement material structure. After this, the long fiber reinforcement mixed material structure 14 is drawn through a stationary coating die 15. The coating die 15 is attached to the extruder 16 through which a second thermoplastic resin material and a material additives are heated and extruded through the die onto the structure of mixed long-fiber reinforcing material 14. Optionally, a second metering device can be placed after the coating die 15 to define the cross-sectional diameter of the material structure mixed long fiber reinforced, coated 17 produced by the process. The structure of the mixed long reinforced fiber reinforced material 17 is cut as pellets in the granulator 19. Referring to FIG. 2, the front and side elevational views of a structure of mixed reinforcement material are illustrated therein. long, coated fiber 20. The composite, long-fiber reinforced composite structure 20, is characterized as a core element of mixed long-fiber reinforcing material 22 having a plurality of continuous fiber strands 24 embedded and extending from one side to another of the same parallel to the longitudinal axis of the structure. The central element 22 is composed of a first thermoplastic resin material of sufficient volume to completely impregnate and surround the continuous fiber strands 24. The central element 26, characterized as a second solid thermoplastic resin material, containing an additive material, the which surrounds and encloses the surface of the central element 22. An intermediate mixing zone 28, characterized as an interface of the first and second thermoplastic materials joins the first and second thermoplastic resin materials together to form an integral structure. Although it will be readily apparent to one skilled in the art that many thermoplastic resin materials, fibers and additive materials may be suitable for use in the process of the present invention for preparing structures of mixed, long-fiber reinforced material, in the present some processing conditions, resins, fibers and additive materials suitable for use in the process are described. Generally, the first thermoplastic resin material must exhibit high flux and low viscosity when heated and extruded through the impregnation die. This should not degrade when heated to temperatures above the melting temperature that might be necessary to ensure complete impregnation of the fibers therewith. The first thermoplastic resin material can be selected from nylon 6, nylon 66, polyethylenes, polyacetals, polyphenylene sulfide, polyurethanes, polypropylene, polycarbonates, polyesters, acrylonitrile-butadiene-styrene and combinations thereof. The continuous lengths of the fiber yarns necessary to provide the reinforcement qualities to the mixed material structure can be selected from glass, amorphous carbon, graphite carbon, aramides, stainless steel, ceramics, alumina, titanium, magnesium, metal-coated carbons , rock wool and combinations thereof. Generally, the yarns, which can be obtained as skeins of many filaments on spools, are generally separated by the lobes inside the impregnating die and impregnated during the process. Optionally, the fiber strands can be heated prior to impregnation to increase the separation of the strands from the skein and improve impregnation. The second thermoplastic resin material must be compatible with the first thermoplastic resin material. The two resins should have compatible thermal expansion coefficients as well as bonding forces so that the intermediate mixing zone is formed at the interface of the resins during the process of preparing the coated, long fiber reinforced composite structure. The coefficients of thermal expansion of the two resin materials must be within the same range with each other to ensure that the resin materials within the structure of mixed, long-fiber reinforced composite material expand and contract at the same speeds. Otherwise, deformation of the mixed material structure may occur. The second thermoplastic resin material is a vehicle for the additive material and must be easily mixed therewith. Although the second thermoplastic resin material can be selected from nylon 6, nylon 66, polyethylenes, polyacetals, polyphenylene sulfide, polyurethanes, polypropylene, polycarbonates, polyesters, acrylonitrile-butadine-styrene and combinations thereof, it is not essential that the first and second thermoplastic resin materials are identical. The second thermoplastic resin material must mix well with the additive material, bond with the first thermoplastic resin material and have a relatively low melting temperature so that a coating of the mixture does not cause melting of the first thermoplastic resin material of the structure of mixed material of long fiber reinforcement. The additive materials are generally selected from components that provide improved molding properties as well as physical and chemical properties of shaped articles prepared therefrom. The additive materials can also be selected from components that are not suitable for incorporation into the first thermoplastic resin material due to their viscosity enhancing characteristics. It might be desirable to add pigments to the mixed material structure to reduce the finishing work of the shaped articles, or it might be desirable to add flame retardant agents to the mixed material structure to increase the flame retardancy characteristics of the shaped article. Since many additive materials are sensitive to heat, an excessive amount of heat can cause them to decompose and produce volatile gases. Therefore, if a heat sensitive additive material is extruded with an impregnation resin under high heating conditions, the result could be a complete degradation of the additive material. The additive materials of the invention can be selected from mineral-based reinforcing agents, lubricants, flame retardants, blowing agents, foaming agents, ultraviolet light resistant agents, heat sensitive pigments and combinations thereof. Mineral-based reinforcing agents can be selected from calcium carbonate, silica, mica, clays, talc, calcium silicate, graphite, wollastonite, calcium silicate, alumina trihydrate, ferrite barium and combinations thereof. The second thermoplastic resin-additive material composition is a combination of the second thermoplastic resin and additive materials. Generally, the composition may contain from about 10 to about 90% by weight of the additive material and from about 90 to 10% by weight of the second thermoplastic resin material. Typically, the second thermoplastic resin-additive material composition may contain from about 15 to about 85% by weight of the additive material and from about 85 to about 15% by weight of the second thermoplastic resin material, and preferably, from about 25 to about 75% by weight of the additive material and from about 75% to about 25% by weight of the second thermoplastic resin material. The composition can be prepared by melt-mixing the components in an extruder to form appropriate mixtures of the components before feeding them to the coating die of the process. Generally, the first stationary impregnation die of the present invention is operated at temperatures that are sufficient to cause melting and impregnation of the first thermoplastic resin material on the long fiber reinforcement yarns. Typically, the operating temperatures of the impregnation die are greater than the melting temperature of the first thermoplastic resin material, and preferably, the impregnation die is operated at temperatures from about 204.4 to about 426.6 ° C. Generally, the second stationary coating die of the invention is operated at temperatures sufficient to ensure fusion of the second thermoplastic resin-additive material combination without degradation of the additive material in the combination. Typically, the coating die is operated at temperatures from about 121.1 to about 371.1 ° C. Generally, shaped articles are prepared from pellets of long fiber reinforced mixed material structures, coated by molding processes. The pellets are placed in an extruder-die assembly and molded as shaped articles. Since pigments and other agents can be applied to the mixed material structure during the coating portion of the process, there is little need for a finish or for applying additives to the surface of the shaped article.

Claims (24)

NOVELTY OF THE INVENTION CLAIMS

1. - A process for the continuous preparation of a structure of mixed long reinforced fiber material, suitable for preparing shaped articles, comprising the steps of: a) extruding a mass of a first thermoplastic resin material in a fluid state that does not have discrete shape in and longitudinally through a first elongated stationary die having no relatively mobile components, said die having a central, fully open, continuous passage extending longitudinally from one side to the other thereof, and a plurality of projecting lobes radially inwardly towards said central passage from separate sites along the length of the opposite internal side walls of said central passage in interleaved relation to each other to form an intricate passage through which said first thermoplastic resin material flows.; b) simultaneously introducing a plurality of continuous lengths of reinforcing fiber yarns into said central passage of the first die at different places therein; c) separately passing each of said fiber strands longitudinally within and along the length of said central passage over and between said interspersed lobes in the presence of said fluid mass of the first thermoplastic resin material to come into contact and completely permeate each one of said fiber yarns with said first thermoplastic resin material to produce a long fiber composite structure; d) stretching the composite structure of long fiber reinforcing material from said first die longitudinally thereto, whereby the mixed material structure is characterized by containing continuous fiber yarns extending in said first thermoplastic resin material generally parallel to the longitudinal axis of the structure; e) extruding a mass of a second thermoplastic resin material and an additive material to produce a second thermoplastic resin-additive material, wherein said second thermoplastic resin-additive material is in a fluid state without having a discrete form, in and longitudinally through a second elongated stationary die having no relatively mobile components, said die having a central, fully open, continuous passage extending longitudinally from one side to the other thereof to form a passage through which said second thermoplastic resin flows; additive material; f) simultaneously introducing the structure of mixed long fiber reinforcing material into said central passage of the second stationary die; g) contacting and coating the long fiber reinforced composite material structure with the second thermoplastic resin-additive material to produce a long, coated fiber reinforced composite material structure, in which the first and second resin materials thermoplastic are bonded at the interface of the first and second thermoplastic resin materials; h) stretching the structure of mixed long fiber reinforcement material, coated from the second die; and i) cutting the structure of mixed, long-fiber reinforced composite material as pellets.

2. The method according to claim 1, further characterized in that the temperature of the first stationary die is sufficient to melt and impregnate the first thermoplastic resin material over the continuous lengths of reinforcing fiber yarns.

3. The method according to claim 2, further characterized in that the temperature of the first stationary die is at least 65.5 ° C higher than the melting temperature of the first thermoplastic resin material.

4. The method according to claim 3, further characterized in that the temperature of the first stationary die is from about 204.4 to about 426.6 ° C.

5. The method according to claim 4, further characterized in that the second stationary die is at a temperature sufficient to coat the second thermoplastic resin-additive material combination on the mixed long fiber reinforcement material structure, without degrading the additive material.

6. The method according to claim 5, further characterized in that the second stationary die is at a temperature of about 121.1 to about 371.1 ° C.

7. The process according to claim 6, further characterized in that the first and second thermoplastic resin materials are selected from the group consisting of nylons, polyethylenes, polyacetals, polyphenylene sulfide, polyurethanes, polypropylene, polycarbonates, polyesters, acrylonitrile- butadiene-styrene and combinations thereof.

8. The process according to claim 7, further characterized in that the continuous length of fiber strands are selected from the group consisting of glass, amorphous carbon, graphite carbon, aramides, stainless steel, ceramics, alumina, titanium, magnesium, coals coated with metal, rock wool and combinations thereof.

9. The process according to claim 8, further characterized in that the additive material is selected from the group consisting of heat-sensitive pigments, mineral-based reinforcing agents, lubricants, flame retardants, blowing agents, foaming agents , agents resistant to ultraviolet light and combinations thereof.

10. The process according to claim 9, further characterized in that the mineral-based reinforcing agents are selected from the group consisting of calcium carbonate, silica, mica, clays, talc, calcium silicate, graphite, wollastonite, calcium silicate, alumina trihydrate, ferrite baric and combinations thereof.

11. The method according to claim 10, further characterized in that the first and second thermoplastic resin materials have compatible thermal expansion coefficients.

12. - A structure of mixed long-fiber reinforced composite material prepared according to the method according to claim 11.

13. A shaped article prepared from the structure of mixed long-fiber reinforcement material, coated in accordance with Claim 12 which exhibits good stiffness and impact resistance.

14. A stretch extrusion process for the continuous preparation of a thermoplastic structure of mixed long-fiber reinforcing material characterized in that a mass of a first thermoplastic resin material is extruded in a fluid state in an impregnation die while at the same time a plurality of continuous lengths of reinforcing fiber yarns are introduced into the die, contacting and impregnating each fiber yarn with the first thermoplastic resin material to produce a long fiber reinforced composite material structure. , the improvement comprising the steps of: a) heating a second thermoplastic resin material and an additive material to a temperature sufficient to produce a fluid combination of second thermoplastic resin-additive material without degrading the combination; b) extruding the combination of second thermoplastic resin-additive material in a stationary casing die having no relatively mobile components, said casing die having a central, fully open, continuous passage extending longitudinally from one side to the other, walls opposite sides of said central passage through which said combination of second thermoplastic resin-additive material flows; c) introducing simultaneously the structure of mixed long-fiber reinforcing material into said central passage of the coating die; d) contacting the structure of mixed long-fiber reinforcement material with the combination of second thermoplastic resin-additive material to form an outer coating of the combination of second thermoplastic resin-additive material on the structure of mixed fiber reinforcing material long to produce a structure of mixed, long-fiber reinforced, coated material; e) stretching the composite structure of long fiber reinforcing material, coated from the coating die; and f) cutting as a pellet the structure of mixed, long-fiber reinforced, coated material.

15. The method according to claim 14, further characterized in that the stationary coating die is operated at a temperature from about 121.1 to about 371.1 ° C.

16. The process according to claim 15, further characterized in that the first and second thermoplastic resin materials are selected from the group consisting of nylons, polyethylenes, polyacetals, polyphenylene sulfides, polycarbonates, polyurethanes, polyesters, acrylonitrile-butadiene- styrene and combinations thereof.

17. The process according to claim 16, further characterized in that the continuous length of the reinforcing fiber yarns are selected from the group consisting of glass, amorphous carbon, graphite carbon, aramides, stainless steel, ceramics, alumina, titanium , magnesium, carbons coated with metal, rock wool and combinations thereof.

18. The process according to claim 17, further characterized in that the additive material is selected from the group consisting of heat sensitive pigments, flame retardants, blowing agents, foaming agents, ultraviolet light resistant agents, lubricants, mineral-based reinforcing agents and combinations thereof.

19. A structure of mixed long fiber reinforced coated material, comprising: a central element of mixed long fiber reinforcement material structure composed of a first thermoplastic resin material having a plurality of continuous lengths embedded therein of fiber strands extending therein generally parallel to the longitudinal axis of the central element; a coating element composed of a second thermoplastic resin material and an additive material, characterized in that the coating element surrounds the central element; and an intermediate mixing zone between the central and facing elements, wherein the first thermoplastic resin material and the second thermoplastic resin material are joined together to form an integral structure.

20. The structure of mixed long-fiber reinforcement material coated according to claim 19, further characterized in that the first and second thermoplastic resin materials are selected from the group consisting of nylons, polyethylenes, polyacetals, polyphenylene sulfide, polyurethanes , polypropylene, polycarbonates, polyesters, acrylonitrile-butadiene-styrene and combinations thereof.

21. The structure of mixed long-fiber reinforcement material, coated, according to claim 20, further characterized in that the continuous length of the reinforcing fiber yarns are selected from the group consisting of glass, amorphous carbon, graphite carbon , aramids, stainless steel, ceramics, alumina, titanium, magnesium, metal-coated carbons, rock wool and combinations thereof.

22. The structure of mixed long-fiber reinforcement material, coated, according to claim 21, further characterized in that the additive material is selected from the group consisting of heat-sensitive pigments, mineral-based reinforcing agents, lubricants , flame retardants, blowing agents, foaming agents, ultraviolet light resistant agents, mineral-based reinforcing agents and combinations thereof.

23. The mixed long fiber reinforced material according to claim 22, further characterized in that the coefficients of thermal expansion of the first and second thermoplastic resin materials are compatible.

24. - A shaped article prepared from the structure of mixed long-fiber reinforcement material, coated in accordance with claim 23, which exhibits good impact resistance and rigidity. APPENDIX SHEET SUMMARY OF THE INVENTION A process for the continuous preparation of a structure of mixed, long-fiber reinforced composite material suitable for preparing shaped articles; the process is characterized by impregnating a plurality of continuous lengths of reinforcing fiber yarns with a first thermoplastic resin material while at the same time continuously stretching the fiber yarns to produce a long fiber reinforced composite material structure followed by coating with a second thermoplastic resin material containing additives on the long fiber reinforced composite material structure to produce a composite long reinforced fiber reinforced material structure; the coating additives may be selected from mineral-based reinforcing agents, lubricants, flame retardants, blowing agents, foaming agents, ultraviolet light resistant agents, heat sensitive pigments, etc .; the structure of mixed, long-fiber reinforced, coated material prepared in accordance with the method is suitable for preparing shaped articles having good physical and chemical properties. P00 / 162F