Processes for manufacturing fiber composite materials

Abstract

(b) forming a film from the resin of step (a) on one surface of a release substrate sheet; (c) providing a fiber woven substrate sheet having a cross-sectional thickness with a varying fiber areal weight; (d) contacting at least one surface of the fiber woven substrate sheet of step (c) with the film of step (b); (e) applying pressure to the other surface of the release substrate sheet facing the resin film of step (b) to impregnate the fiber woven substrate sheet of step (c) with the resin composition of step (a); and (f) partially curing the fiber woven substrate sheet impregnated with the resin composition of step (e) to form a prepreg product. Also disclosed is an S-wrap compression roll assembly having at least three rolls, wherein a second nip roller positioned between the other two rolls has a varied diameter.

Description

[Technical field]

[0001] The present invention relates to a process for manufacturing fiber composite materials, more particularly, the present invention relates to a process for preparing carbon fiber epoxy resin composite materials having various fiber areal weights. [Background technology]

[0002] It is generally known to manufacture carbon fiber composites by first impregnating a fiber or fabric with a resin formulation, such as an epoxy resin formulation, to form a prepreg structure, and then curing the impregnated prepreg structure to form a carbon fiber composite. Carbon fiber epoxy composites can be used in many applications, including, for example, the manufacture of automotive parts. Automotive applications require carbon fiber epoxy composites to be made in a continuously aligned fabric, where the fiber areal weight (FAW) can vary across the entire width of the fabric. To be useful in automotive applications, the impregnated fiber or fabric must (1) be compression molded and cured in less than five minutes, (2) maintain a high glass transition temperature, and (3) use an internal mold release agent to achieve high strength and stiffness and allow easy release of the cured part from the mold.

[0003] So far, impregnation methods used to impregnate textiles, such as those disclosed in EP 2 692 783 B1 and EP 3 216 496 A1, have been carried out on prepregs with uniform FAW, and the known methods assume a singular thickness of the reinforcing layers of the prepregs. Problems arise when using the known impregnation methods, namely when such known impregnation methods are used to impregnate textiles of various fiber areal weights (of various thicknesses), i.e. textiles having both high and low areal weight portions, with resin. For example, when the known impregnation methods are used on textiles of various fiber areal weights, the high areal weight portions of the textile are distorted or the low areal weight portions of the textile are not infused with resin. Typically, textiles of variable carbon fiber areal weight braided structure have a high fiber areal weight (e.g., 588 grams per square meter (g / m)) in the center of the textile. 2)) at the ends of the fabric, with low fiber areal weight (e.g., 520 g / m 2 ). Summary of the Invention [Problem to be solved by the invention]

[0004] It would be desirable to provide a method or process for impregnating carbon fabric with an epoxy resin formulation, where the carbon fibers have a variable carbon fiber areal weight braided structure by preparing a prepreg from the epoxy resin impregnated carbon fabric, without the distortion problems mentioned above.

[0005] One embodiment of the present invention is directed to an inventive process for producing a prepreg product, the process comprising the steps of: (a) providing a fast-curing resin composition; (b) forming a film of the resin from step (a) on one surface of a sheet of release substrate; (c) providing a sheet of fibrous fabric substrate having a cross-sectional thickness of various fiber areal weights; (d) contacting at least one surface of the sheet of fibrous fabric substrate of step (c) with the resin of the sheet of resin film of step (b); (e) applying pressure to the other surface of the sheet of release substrate opposite the resin film to impregnate the fibrous fabric substrate with the fast-curing resin composition; and (f) partially curing the fibrous fabric substrate impregnated with the fast-curing resin composition of step (e) to form a prepreg product.

[0006] In another embodiment, the process of the present invention includes impregnating woven carbon fabrics having various fiber areal weights with epoxy resin and then forming prepregs from the woven carbon fiber fabrics impregnated with epoxy resin.

[0007] In yet another preferred embodiment, the process of the present invention is carried out at a target average film thickness (e.g., 540 grams / m 2) is used to prepreg a fabric with a variable fiber areal weight carbon fiber construction, and pressure is equalized by adding release paper in the desired locations (low fiber areal weight) to produce the uniform pressure required for impregnation (e.g., across a 12 inch (30.48 centimeter (cm)) width of the fabric) without distorting the fabric.

[0008] In yet another preferred embodiment, the present invention comprises a nip roll assembly apparatus for producing a resin impregnated prepreg product.

[0009] The present invention utilizes a single ply broadgood prepreg (all fiber angles contained within the same prepreg) of varying thickness across its width to mold complex cross-sectional tubular shapes with non-uniform diameters.

[0010] Advantageously, the prepregs produced by the process of the present invention can be molded to form shaped fiber reinforced composite structures with complex cross sections, such as tubular non-uniform diameter parts. [Brief description of the drawings]

[0011] [Figure 1] FIG. 1 is a perspective view of a schematic diagram of an S-nip roller system apparatus that can be used to form prepreg products such as the prepreg shown in FIG. 3 described below. [Diagram 2] FIG. 2 is a cross-sectional view taken along line 2-2 of FIG. [Diagram 3] FIG. 3 is an enlarged cross-sectional view of a "dumbbell" shaped prepreg product formed by impregnating a woven carbon fiber substrate with epoxy resin using the apparatus of FIG. [Figure 4] FIG. 4 is an enlarged cross-sectional view of another molded prepreg product formed by impregnating a woven carbon fiber substrate with an epoxy resin. DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS

[0012] "Broadgood" is a term used in the textile industry for fabrics woven in standard or wider widths, especially as distinguished from ribbons, bands, or trimmings, and usually includes fabrics over 18 inches (450 mm) wide.

[0013] "Infusion," "impregnation," and "prepregging" are used interchangeably herein with respect to a resin composition in contact with a fibrous material, and herein mean flowing the resin composition into the body of the fibrous material to fill, permeate, or saturate the fibrous material with the resin composition.

[0014] In a broad embodiment, the process for making the prepreg product of the present invention includes impregnating a woven fiber substrate having a cross-sectional thickness of various fiber areal weights with a fast-curing resin composition, applying a pressure that varies along a horizontal axis of the resin-impregnated woven fiber substrate, and partially curing the fast-curing resin composition-impregnated woven fiber substrate to form a prepreg product.

[0015] The fast-curing resin composition useful in the process of the present invention may include, for example, a fast-curing epoxy resin system, formulation, or composition. In one preferred embodiment, for example, the fast-curing epoxy resin composition described in WO2017 / 066056 can be used in the process of the present invention. The fast-curing epoxy resin composition useful in the present invention includes an epoxy resin composition that provides more uniform infusion of resin into fiber materials to form prepregs or composite articles.

[0016] As described in WO2017 / 066056, the fast curing epoxy resin composition useful in the present invention includes an epoxy resin composition comprising a solid epoxy resin containing an oxazolidone as a first epoxy component, a second epoxy component, a soluble latent catalyst, and a latent curing agent having a particle distribution in which at least 35 weight percent (wt%) of the particles have an average particle size of less than 2 microns (μm), based on the total weight of the curing agent. By using a latent curing agent with a desired particle distribution (e.g., at least 35 percent (%) of the particles have a diameter of less than 2 μm), a more uniform infusion of the epoxy resin composition into the fiber material can be achieved. This, in turn, provides an epoxy resin composition with a faster curing rate, thereby shortening the molding cycle time and thereby increasing the speed at which molded articles and parts can be prepared from the prepreg.

[0017] In one typical embodiment, the epoxy resin composition selected for infusion desirably has a glass transition temperature (Tg) between 0 degrees Celsius (° C.) and less than 15° C. At these Tg levels, the epoxy resin composition can advantageously be rapidly infused into the fibrous material while minimizing and reducing voids (e.g., air bubble pockets) within the prepreg.

[0018] The above epoxy formulations advantageously (1) provide prepregs with relatively fast cure rates (e.g., curable in 3 minutes at 150° C.), (2) provide carbon fiber prepregs with low to negligible tack, (3) provide prepregs with long shelf life (e.g., greater than 40 days at 23° C. and at least 1 year at −20° C.), and (4) provide final cured fiber reinforced composites with high Tg (onset), e.g., greater than 100° C., and Tg (peak loss factor), e.g., greater than 140° C. Another advantage of using the above epoxy resin systems is that the resins are curable without the use of external mold release agents.

[0019] Once the epoxy resin composition is prepared, it can be infused into a fibrous material in the form of a tow or fabric (e.g., rolls of carbon fiber fabric) according to the process of the present invention to form a prepreg. The epoxy resin composition according to the embodiments of the present invention can be combined with a wide variety of different reinforcing fibers. The fibers of the fabric used in the present invention can include, for example, carbon fibers, graphite fibers, glass fibers, ceramic fibers, aramid fibers, natural fibers (such as basalt, hemp, seaweed, hay, flax, straw, jute or coconut). In one preferred embodiment, the carbon fibers used can be in the form of a fabric, which can be random, knitted, non-woven, multiaxial (e.g., unbonded fabric), braided, or any other suitable pattern. The fabric must be thermally and chemically stable under the conditions of prepreg formation (e.g., curing of the epoxy resin composition), and the fabric must be compatible with the resin selected for use in the fabric infusion process.

[0020] In one preferred embodiment, the process of the present invention for producing a prepreg product includes the steps of: (a) providing a fast-curing resin composition; (b) forming a film of the resin from step (a) on one surface of a sheet of release substrate; (c) providing a sheet of fibrous fabric substrate having cross-sectional thicknesses of various fiber areal weights; (d) contacting at least one surface of the sheet of fibrous fabric substrate of step (c) with the resin of the sheet of resin film of step (b); (e) applying pressure to the other surface of the sheet of release substrate facing the resin film to impregnate the fibrous fabric substrate with the fast-curing resin composition; and (f) partially curing the fibrous fabric substrate impregnated with the fast-curing resin composition of step (e) to form a prepreg product.

[0021] Generally, the process of preparing the prepreg of the present invention includes forming a film or sheet of the fast-curing resin composition from step (a) above on one surface of a sheet material. For example, this step (b) can be accomplished by extruding a resin composition, such as an epoxy resin, onto the sheet material to form a film resin coating on the sheet material. The thickness of the resulting film resin can vary depending on the final prepreg product to be produced. For example, in one general embodiment, but not limited thereto, the thickness can be 0.0119 inches (0.03 cm) to 0.0125 inches (0.032 cm) for FAW materials. In general, the thickness of the film resin can be such that the resin is at least 30% to 50% by weight of the prepreg composite in one embodiment, and 35% to 45% by weight in another embodiment. In a preferred embodiment, the thickness of the film resin can be at least 40% by weight of the prepreg composite, and the fiber substrate can be at least 60% by weight of the prepreg composite.

[0022] The sheet material may be a release film or paper from which a film coating of the epoxy resin composition is transferred to the fiber material during the contacting step (prepregging) of the process. Sheet materials including films or papers may be made, for example, from sheets of paper or sheets of Telfon material coated with a release agent. In one general embodiment, but not limited thereto, the thickness of the sheet material may be, in one embodiment, 0.007 inches (0.018 cm) to 0.009 inches (0.023 cm).

[0023] After the film of the epoxy resin composition is deposited on the sheet material, the sheet material with the film resin coating can be passed through a chill roll to cool the epoxy resin composition. The sheet material containing the cooled epoxy resin composition can then be wound into a roll for immediate or future use. In one preferred embodiment, the release paper or film on which the epoxy resin composition is coated as a film can be rewound into a roll for later use following the step of cooling the epoxy resin composition.

[0024] In one embodiment of the process, the sheet material having the epoxy resin composition film coating can be contacted with a surface of the fibrous fabric substrate or fibrous material (e.g., NCF, braided, or unidirectional woven) described above from step (c) above. Pressure can then be applied to the fibrous material and the sheet material having the epoxy resin composition film coating after or during the contacting step to infuse the epoxy resin into the fibrous material.

[0025] Standard conventional prepreg lines and auxiliary equipment for prepreg lines known in the art can be used for the contacting step and the subsequent or simultaneous impregnation step. The prepreg line used in the process of the present invention can be any known prepreg line including, for example, (1) an unwinding station, (2) a heated table (with insulation pad), (3) an S-wrap compression roller, and (4) a pull roller for controlling the speed.

[0026] In one preferred embodiment, a sheet of fibrous material can be sandwiched between two sheet materials on which a film coating of the epoxy resin composition has been deposited, and the fibrous material coated with the epoxy resin composition and the sheet material can be provided as continuous tapes from respective supply rolls. The contacting step of the inventive process can be carried out with the above-mentioned film forming equipment used to form sheets of different substrates and to compress the sheets together using an S-wrap nip compression roll system apparatus. However, in a preferred embodiment of the present invention, the apparatus is modified to accommodate desired fibrous woven substrates having various fiber areal weights. In addition, the apparatus is modified to provide uniform pressure along the thickness of the fibrous woven substrates having various fiber areal weights.

[0027] 1 and 2, a preferred modified embodiment of an S-wrap compression roller for use in the present invention is shown and is generally designated by reference numeral 10 and includes a series of nip rollers, such as an upper nip roller 11, a middle nip roller 12, and a lower nip roller 13. In one embodiment, nipped material is fed into roller system 10 as indicated by directional arrow A. The nipped material passes / rotates through roller system 10 in a direction as indicated by directional rotation arrows B and C (shown in FIG. 2). And, the injected fibrous material exits roller system 10 as indicated by directional arrow D.

[0028] In a preferred modified embodiment of the S-wrap compression roller, the central nip roller 12 varies in size as shown by edges 12a and 12b that are integral with the middle portion 12c. In general, the shape of the nip roller member 12 can be described as two cylindrical members joined together by and integral with a middle bar portion, or, simply, the nip roller member 12 can be in the shape of a "dumbbell weight" or "dumbbell-shaped" member 12 when the member 12 is viewed in a front perspective view as shown in FIG. 1. The middle roller 12 can be made by using one or more release papers of a predetermined thickness on the edges of a regular nip roller of a certain diameter and length, and "building up" the diameter of the edges 12a and 12b of the nip roller 12 to the desired diameter to provide the preferred shape of the nip roller 12 to accommodate the resin impregnated fiber fabric.

[0029] A dumbbell-shaped roller, i.e., intermediate nip roller 12, disposed between nip rollers 11 and 13, provides a first gap 14 and a second gap 15, which allows a desired pressure to be applied to supply film 21 (shown in FIG. 2).

[0030] After the contacting step to bring the sandwiched materials together (i.e., the combined sheet of resin and fiber material), the sandwiched materials can be passed through a pair of nip rolls that press the epoxy resin composition into both surfaces of the fiber material. The prepreg of the present invention can be produced by injecting (or impregnating) the fiber material (or woven carbon fiber substrate) with the epoxy resin composition by applying pressure to the sandwiched materials. In one preferred embodiment, this step (e) of applying pressure is performed to impregnate (or infuse) the woven carbon fiber substrate with the fast-curing epoxy resin composition. In another embodiment, a woven fiber substrate having variable fiber areal weight regions is impregnated with the fast-curing resin composition to obtain uniform impregnation across the width of the variable fiber areal weight composite material. "Uniform impregnation" in reference to impregnation of the fiber material with resin means herein that a given level of impregnation is the same across the entire width of the variable fiber areal weight composite material, including in low fiber areal weight regions and high fiber areal weight regions.

[0031] In the process of impregnating the above carbon fiber woven substrates having various fiber areal weights with the above epoxy resin composition, the above nip roller system can be used to provide the desired impregnated fiber woven substrate to form a prepreg. The impregnation step of the present process includes, for example, feeding the carbon fiber woven substrate disposed between two films of fast-curing epoxy resin composition into the nip roller system (as shown by arrow A in FIG. 1), with the resin of the upper sheet of resin contacting the upper surface of the fiber woven substrate and the resin of the lower sheet of resin contacting the lower surface of the fiber woven substrate. The carbon fiber woven substrate impregnated with the fast-curing epoxy resin composition then exits the roller system (as shown by arrow D in FIG. 1).

[0032] Referring to Figure 3, there is shown a molded prepreg, generally designated by reference numeral 30, including a resin matrix 31 infused with a weave of fibers 32. The prepreg shown in Figure 3 is the result of being processed through the S-wrap roller system 10 shown in Figure 1. An upper release paper sheet 33 and a lower release paper sheet 34 are disposed between the upper and lower layers 33, 34, respectively, sandwiching the prepreg 30. The prepreg 30 includes an edge portion generally designated by reference numeral 40A and an edge portion generally designated by reference numeral 40B, both integral with a middle portion generally designated by reference numeral 50. As shown in Figure 3, the edge portions 40A and 40B are more compressed than the middle portion 50.

[0033] Referring to FIG. 4, another embodiment of a molded prepreg, generally designated by reference numeral 60, is shown, including a resin matrix 61 infused into a weave of fibers 62. An upper release paper sheet 63 and a lower release paper sheet 64 are disposed between upper and lower layers 63 and 64, respectively, sandwiching the prepreg 60. The prepreg 60 includes an edge portion generally designated by reference numeral 70A and an edge portion generally designated by reference numeral 70B, both integral with a middle portion generally designated by reference numeral 80. As shown in FIG. 4, the middle portion 80 is more compressed than the edge portions 70A and 70B. The prepreg shown in FIG. 4 may also be the result of being processed through another alternative S-wrap roller system (not shown) having a series of nip rollers (not shown), such as an upper nip roller, a middle nip roller, and a lower nip roller, providing a modified middle nip roller (not shown) to the roller system to provide the shape of the middle portion 80 of the prepreg 60.

[0034] In one embodiment, the infusion process can be carried out at an elevated temperature so that the viscosity of the epoxy resin composition can be further reduced, and thus the heating step can facilitate rapid infusion of the epoxy resin composition into the fibrous material. For example, the sandwiched material can be subjected to heating to increase the temperature of the epoxy resin composition by passing the combination of the fibrous material and the epoxy resin composition over a heated plate to heat the epoxy resin composition. However, the temperature should not be so high for such a long time that an undesirable level of curing of the epoxy resin composition occurs. For example, during the impregnation step (e), the infusion of the epoxy resin composition into the fibrous material can be carried out at a temperature ranging from 100°C to 130°C in one embodiment, from 100°C to 125°C in another embodiment, and from 110°C to 120°C in yet another embodiment. The above heating for infusing the epoxy resin composition into the fibrous material can be carried out using a heated table and a heated nip roll.

[0035] It should be appreciated that temperature ranges outside the above ranges can also be used. However, the use of higher or lower injection temperatures typically requires adjustments to the machine speed at which the infusion process is carried out. For example, at temperatures above about 120°C, it may be necessary to carry out the infusion process at a higher machine speed to reduce the time that the epoxy resin composition is exposed to high temperatures to avoid undesired crosslinking of the epoxy resin composition. Similarly, the use of lower injection temperatures typically requires a lower machine speed for infusing the epoxy resin composition into the fiber material to obtain a desired level of infusion, thereby reducing voids within the prepreg. In one preferred embodiment, the epoxy resin composition can be applied to the fiber material at a temperature in the above range, and the epoxy resin composition can be solidified into the fiber material by pressure. For example, pressure on the combination of fiber material and resin can be applied by passing the combination through one or more pairs of nip rollers.

[0036] In a preferred embodiment, the combination of fibrous material and epoxy resin composition may be subjected to the further step of passing the combination through a heated plate, followed by passing the combination through a second nip to further infuse the epoxy resin composition into the fibrous material to form a resin-infused prepreg. The prepreg may then be cooled, for example, by passing the material through a chill roll or chill plate. After cooling, the prepreg may be wound onto a supply roll for future use.

[0037] As mentioned above, the infusion step can be carried out at an elevated temperature to reduce the viscosity of the epoxy resin composition. Additionally, the infused epoxy resin composition can be subjected to a partial curing step (advancing) to increase the glass transition temperature of the epoxy resin composition in the prepreg. The prepreg can then be packaged, stored, or shipped as required. As previously mentioned, in some embodiments, it may be desirable to subject the prepreg to an advancing step to increase the Tg of the epoxy resin, thereby reducing the tackiness of the prepreg.

[0038] In another preferred embodiment, a "nip roll" action of the compression rollers can be used during the impregnation step (e). During the "nip roll" action of the compression rollers of a standard prepreg line, additional pressure needs to be applied to the thinner parts of the prepreg. The nip gap is set to accommodate the thickest parts to reduce the distortion seen in this area. A portion of release paper with a predetermined thickness (e.g., 0.008 inch (0.02 cm) thick) can be added to the middle roller (S-wrap action allowing two nip gaps with three rollers) in the thinner areas of the broadgood. The use of release paper allows uniform pressure despite thickness variations to optimally infuse the epoxy resin into the carbon fiber fabric substrate to form a prepreg with minimal distortion.

[0039] The conditions of the impregnation process of the present invention may vary and may depend on various factors, including, for example, the type of fabric used, the size of the fabric used, the FAW of the fabric used, and the design and dimensions of the prepreg product to be produced. As an illustration of the process of the present invention, but not limited thereby, in one particular embodiment, a broadgood carbon fiber fabric sheet is fed between two sheets of epoxy resin film deposited on one side of each of two release papers, so that the resin contacts the fabric. The combined sheets are fed into an S-wrap nip roll assembly device, and the infusion or prepregging step is carried out, for example, as follows:

[0040] (1) The nip temperature range may be, for example, 100°C to 130°C in one embodiment, 100°C to 125°C in another embodiment, and 110°C to 120°C in yet another embodiment.

[0041] (2) The table temperature range may be 100°C to 130°C in one embodiment, 100°C to 125°C in another embodiment, and 110°C to 120°C in yet another embodiment.

[0042] (3) The first nip gap between the top roll and the middle roll, and between the bottom roll and the middle roll, is generally indicated by reference numeral 14 in FIG. 1 and, in one embodiment, can be 0.022 inches to 0.026 inches (0.056 cm to 0.066 cm).

[0043] (4) A second nip gap between the upper roll and the middle roll, and between the lower roll and the middle roll, is generally indicated by reference numeral 15 in FIG. 1 and, in one embodiment, may be 0.022 inches to 0.025 inches (0.056 cm to 0.064 cm).

[0044] (5) The speed of the feed material to the nip roll system can be from 1.0 ft / min to 2.4 ft / min (0.305 m / min to 0.732 m / min) in one embodiment, from 1.0 ft / min to 2.0 ft / min (0.305 m / min to 0.610 m / min) in another embodiment, and from 1.5 ft / min to 2.0 ft / min (0.457 m / min to 0.610 m / min) in yet another embodiment.

[0045] The release paper used in the process may have a thickness of, for example, 0.007 inches (0.018 cm) to 0.009 inches (0.023 cm) in one embodiment. Any standard release paper known in the art may be used in the present invention. The release paper may be used to keep the material being processed from adhering to the metal roller. Alternatively, the compression roller may be modified to account for thickness variations. For example, instead of adding release paper to a metal roller, the metal roller may be machined to compensate for thickness variations.

[0046] The parameters useful in the present invention may be "fixed" parameters, i.e., parameters that do not change throughout the sequence of processing steps of the fabric and resin sheet. For example, the nip temperature and table temperature described above may be fixed parameters. To illustrate the present invention, but without being limited thereto, in one embodiment, a nip gap range of 0.023 inches to 0.026 inches (0.058 cm to 0.066 cm), the addition of release paper, and a slower speed of 1.8 ft / min (0.549 m / min) may be used to demonstrate the utility of the present invention. The nip temperature and table temperature may remain fixed throughout the process of the present invention.

[0047] As the fiber fabric substrate impregnated with the fast curing epoxy resin composition of step (e) exits the nip roller system, the impregnated fabric is allowed to partially cure to form a prepreg product. The produced prepreg can then be rolled up onto a core, and the roll of prepreg can then be transferred to a storage location (as noted above, the prepreg is stable during storage) or the prepreg can be used in a molding process.

[0048] Prepregs produced by the process of the present invention advantageously exhibit low tack, i.e., the prepregs are easily handleable and do not stick to each other at room temperature when used or stored in a roll.

[0049] Using the process of the present invention, the prepreg is advantageously not over-crosslinked, i.e., the prepreg has a Tg less than 20° C., so the prepreg does not exhibit problems such as the creation of voids in the prepreg. Prepregs processed using injection at high prepregging temperatures can result in undesirable "overcooked" prepregs having a Tg greater than 20° C., which can exhibit undesirable surface quality and can become stiff and difficult to work with.

[0050] In one broad embodiment, the carbon fiber reinforced composite material of the present invention is a fully cured composite material formed by fully curing the prepreg produced as described above. For example, in a broad embodiment, a process for producing a carbon fiber reinforced composite material includes the steps of (A) providing a resin impregnated fiber prepreg made by the process described above, and (B) curing the impregnated woven prepreg of step (A) to form a fiber reinforced composite article.

[0051] In one embodiment, the curing step (or advancing step) to fully cure the prepreg may be carried out by heating the prepreg at a temperature between 140° C. and 155° C. for a cure time between 3 minutes and 5 minutes.

[0052] One of the objectives of the present invention is to produce fiber reinforced composites (e.g., carbon fiber reinforced composites) with a variable cross-section along the width of the composite. For example, in one preferred embodiment, the fiber reinforced composites can be tubular members with a variable cross-section along the diameter. The production of carbon fiber reinforced composites with FAW of the present invention has not been possible using prior art methods until now. Advantageously, the carbon fiber composites of the present invention can now be used to produce automotive composites, such as interior and exterior parts, where such parts are of different shapes, sizes, and dimensions. For example, in one preferred embodiment, the carbon fiber composites of the present invention can be used to produce composite parts that can be used in steering columns of automobiles. EXAMPLES

[0053] The following examples are presented to further illustrate the invention, but should not be construed as limiting the scope of the claims. All parts and percentages are by weight unless otherwise indicated.

[0054] The various raw materials used in the following inventive examples (Inv. Ex.) and comparative examples (Comp. Ex.) are set forth in Table I below. [Table 1]

[0055] Examples 1 and 2 and Comparative Examples A to C An experimental prepreg line was used with standard prepregging conditions used in the manufacture of conventional prepregs to produce prepregs using the VORAFUSE™ P6300 resin system and carbon fiber hybrid broadgoods provided by A&P. This resulted in insufficient infusion on the outside (thin areas) and distortion in the center (thick areas) related to appearance / distortion levels. Materials were only tested when they reached an acceptable subjective visible appearance as judged according to the rating scale (described below). The nip gap was then set to the average thickness of the prepreg (Comp.Ex.B). Similar results were seen in the first trial (Comp.Ex.A). Next, release paper was added to the middle roller to compensate for the variable fiber areal weight across the width of the material and the nip gap was opened and set to the thickest part of the material (Comp.Ex.C). This showed a slight improvement compared to (Comp.Ex.A) and (Comp.Ex.B). The nip gap was reduced and the speed slowed down (Inv.Ex.1) for additional pressure and time, at a temperature which improved injection and distortion. This level of tolerance and distortion was acceptable and the material was tested in both lower and higher FAW regions. In the final step, the nip gap was opened slightly (Inv.Ex.2) to further reduce distortion. This further improved the appearance level and the material was tested again. However, due to the uniqueness of the material, the material was tested in the intended part orientation (horizontal vs. vertical pre-test) and therefore differences in storage modulus were expected (more fibers running in the direction of the test). [Table 2]

[0056] A rating scale was developed to indicate the "Appearance / Distortion Level" of the samples to determine whether the samples passed the criteria required for them to undergo further testing. The rating scale included numerical rating levels from "1" to "4," with "1" being the least acceptable and "4" being the most acceptable. A detailed description of rating levels 1-4 is provided in Table IV. Samples with an appearance / distortion rating level of 3 are required for further testing. [Table 3]

Claims

1. 1. A process for producing a prepreg product, comprising: (a) providing a fast curing resin composition; (b) forming a film of the resin from step (a) on one surface of a sheet of release substrate; (c) providing a sheet of fibrous woven substrate having cross-sectional thicknesses of various fiber areal weights; (d) contacting at least one surface of the sheet of fiber woven substrate of step (c) with a resin side of the sheet of resin film of step (b) such that the resin contacts the fiber woven substrate; (e) applying pressure to the other surface of the sheet of release substrate facing the resin film using a nip roll assembly device to impregnate the fiber fabric substrate with the fast curing resin composition to obtain uniform impregnation of the resin across the width of the variable fiber areal weight fiber fabric substrate; (f) allowing the fiber fabric substrate impregnated with the fast curing resin composition of step (e) to at least partially cure the resin to form a prepreg product; Including, The fast-curing resin composition comprises a solid epoxy resin containing an oxazolidone as a first epoxy component; a second epoxy component; and a soluble latent catalyst; a latent curing agent having a particle distribution in which at least 35 weight percent of the particles have an average particle size of less than 2 μm, based on the total weight of the latent curing agent; The epoxy resin composition includes the nip roll assembly apparatus comprises an S-wrap compression roll assembly including a combination of at least first, second, and third nip rollers in rolling contact with one another; the second nip roller is disposed between the first and third nip rollers to provide a first nip gap and a second nip gap; In step (e), the nip roll assembly device applies uniform pressure across the width of the variable fiber areal weight fibrous fabric substrate by adjusting the first and second nip gaps, adding release paper to a low fiber areal weight portion of the variable fiber areal weight fibrous fabric substrate, and setting a feed speed of the variable fiber areal weight fibrous fabric substrate between 0.305 m / min and 0.610 m / min.

2. The process of claim 1 , wherein the woven fiber substrate is a woven carbon fiber substrate.

3. 10. The process of claim 1, wherein the woven fiber substrate impregnated with the fast curing resin composition of step (f) is heated at a temperature sufficient to at least partially cure the resin to form a prepreg product.

4. 4. The process of claim 3, wherein the temperature is from 100° C. to 130° C.

5. 2. The process of claim 1, wherein the fiber woven substrate is a fiber areal weight hybrid carbon fiber broadgood.

6. 1. A process for producing a fiber-reinforced composite article, comprising: (A) providing a resin impregnated woven prepreg made by the process of claim 1; (B) curing the impregnated woven prepreg of step (A) to form a fiber reinforced composite article.

7. 1. A process for making a carbon fiber reinforced composite material, comprising: (a) providing a fast curing resin composition; (b) forming a film of the resin from step (a) on one surface of a sheet of release substrate; (c) providing a sheet of fibrous woven substrate having cross-sectional thicknesses of various fiber areal weights; (d) contacting the surface of at least one side of the sheet of fibrous fabric substrate of step (c) with the resin of the sheet of resin film of step (b); (e) applying pressure to the other surface of the sheet of release substrate opposite the resin film using a nip roll assembly device to impregnate the fiber fabric substrate with the fast curing resin composition to obtain uniform impregnation of the resin across the width of the variable fiber areal weight fiber fabric substrate; (f) partially curing the fiber fabric substrate impregnated with the fast curing resin composition of step (e) to allow for the formation of a prepreg product; (g) curing the prepreg product of step (f) to form a cured carbon fiber reinforced composite material; Including, The fast-curing resin composition comprises a solid epoxy resin containing an oxazolidone as a first epoxy component; a second epoxy component; and a soluble latent catalyst; a latent curing agent having a particle distribution in which at least 35 weight percent of the particles have an average particle size of less than 2 μm, based on the total weight of the latent curing agent; The epoxy resin composition includes the nip roll assembly apparatus comprises an S-wrap compression roll assembly including a combination of at least first, second, and third nip rollers in rolling contact with one another; the second nip roller is disposed between the first and third nip rollers to provide a first nip gap and a second nip gap; In step (e), the nip roll assembly device applies uniform pressure across the width of the variable fiber areal weight fibrous fabric substrate by adjusting the first and second nip gaps, adding release paper to a low fiber areal weight portion of the variable fiber areal weight fibrous fabric substrate, and setting a feed speed of the variable fiber areal weight fibrous fabric substrate between 0.305 m / min and 0.610 m / min.

8. 8. The process of claim 7, wherein the temperature of the curing step (g) is from 140°C to 155°C.

9. 8. The process of claim 7, wherein the curing time of the curing step (g) is from 3 minutes to 5 minutes.

10. 1. A nip roll assembly apparatus for receiving a plurality of sheet members including at least one sheet of fibrous woven substrate having a cross-sectional thickness of varying fiber areal weight and at least one sheet of release substrate containing a film of a fast curing resin composition releasably attached to the sheet of release substrate, comprising: The nip roll assembly apparatus is used for the process for producing the prepreg product according to claim 1, the nip roll assembly apparatus comprises an S-wrap compression roll assembly including a combination of at least first, second, and third nip rollers in rolling contact with one another; the second nip roller is disposed between the first and third nip rollers to provide a first nip gap and a second nip gap; the nip roll assembly device applies uniform pressure across the width of the variable fiber areal weight fibrous fabric substrate by adjusting the first and second nip gaps, adding release paper to the low fiber areal weight portion of the variable fiber areal weight fibrous fabric substrate, and setting the feed speed of the variable fiber areal weight fibrous fabric substrate at 0.305 m / min to 0.610 m / min; the second roller provides uniform pressure across the surface of one side of the sheet of release substrate opposite the side of the resin film to impregnate the fibrous fabric substrate with the fast curing resin composition and includes a diameter that is modified to obtain uniform impregnation of the resin across the width of the fibrous fabric substrate with variable fiber areal weight; The fast-curing resin composition comprises a solid epoxy resin containing an oxazolidone as a first epoxy component; a second epoxy component; and a soluble latent catalyst; a latent curing agent having a particle distribution in which at least 35 weight percent of the particles have an average particle size of less than 2 μm, based on the total weight of the latent curing agent; A nip roll assembly apparatus comprising an epoxy resin composition comprising:

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