A unidirectional and multidirectional composite material with orderly arranged fiber filaments and preparation method thereof

Abstract

The present invention discloses a unidirectional and multidirectional composite material with orderly arranged fiber filaments and a preparation method thereof, belonging to the field of composite material preparation. The present invention arranges reinforcing fibers in an orderly and regular manner through a uniform fiber laying mechanism, and the orderly and regular arrangement refers to that the distance between the reinforcing fibers is adjustable and the orientation is controllable; the composite material resin matrix is ​​prepared by liquid molding or other advanced processes. Through this method, without changing the preparation process of the composite material matrix, the uniformity of the composite material organization can be effectively improved, and the occurrence of local fiber clusters can be avoided, thereby effectively improving its mechanical properties; in addition, the distance between the reinforcing fibers is adjustable and the orientation is controllable, which can improve the designability and predictability of the composite material performance, thereby broadening its application in the fields of aerospace, transportation, etc.

Description

Technical Field

[0001] The invention belongs to the technical field of composite material preparation, and particularly relates to a unidirectional and multidirectional composite material with orderly arranged fiber filaments and a preparation method thereof. Background Art

[0002] Fiber-reinforced resin-based composite materials are often widely used in primary and secondary load-bearing structures in aerospace, transportation and other fields, such as aircraft engine fan blades, containment casings, etc., due to their excellent specific strength and specific stiffness, good designability, excellent damping and vibration reduction performance, and easy integrated molding.

[0003] However, the current preparation process of resin-based composites does not perform fixed-distance and directional control on the spatial position distribution of fibers during the preparation process, resulting in a disordered distribution of the fiber structure in the composite material, which often contains resin-rich areas and fiber cluster areas. This uncertain random distribution of fibers reduces the uniformity of the resin-based composite structure, increases its local stress concentration, and the probability of crack initiation and propagation, severely reduces the macroscopic mechanical properties of the resin-based composite, shortens its life, and is not conducive to its application in various fields. Summary of the invention

[0004] In view of the problem of uneven distribution of reinforcing fibers in traditional resin-based composite materials in the prior art, the present invention provides a unidirectional and multidirectional composite material with orderly arranged fiber filaments and a preparation method thereof, which adopts a reinforcing fiber layer or a three-dimensional preform with fixed-distance and directional arrangement of fibers, and then prepares a resin-based composite material on the basis of the preform. The process can effectively improve the uniformity of the composite material structure, reduce the probability of stress concentration, crack initiation and propagation, thereby improving the mechanical properties of the resin-based composite material; at the same time, the process can improve the designability and predictability of the performance of the resin-based composite material, and expand its application in aerospace, transportation and other fields.

[0005] The technical solution of the present invention is as follows:

[0006] A method for preparing unidirectional and multidirectional composite materials with orderly arranged fiber filaments, wherein the reinforcing fibers are arranged in an orderly and regular manner by a fiber laying mechanism that can evenly lay the fibers, wherein the orderly and regular arrangement means that the distance between the reinforcing fibers is adjustable and the orientation is controllable; the composite material resin matrix is ​​prepared by liquid molding or other advanced processes.

[0007] The purpose of the present invention is achieved through the following technical solutions:

[0008] A method for preparing a unidirectional and multidirectional composite material with orderly arranged fiber filaments, comprising the following steps:

[0009] S1. Laying of reinforcing fibers: firstly, orderly lay out a reinforcing fiber array with 1 to 100 layers and 5 to 500 fibers in each layer; wherein, the reinforcing fibers in each layer are parallelly distributed and the distance between them is 10 μm to 1000 μm; the spacing between adjacent layers is 10 μm to 1000 μm, and the fiber stagger angle is 0 to 90 degrees;

[0010] The orderly laying is to arrange the reinforcing fibers in an orderly and regular manner by using a fiber uniform laying device. The orderly and regular arrangement means that the distance between the reinforcing fibers is adjustable and the orientation is controllable;

[0011] The reinforcing fiber is selected from carbon fiber, glass fiber, aramid fiber, ultra-high molecular weight polyethylene fiber and other fibers used in the field of composite materials;

[0012] S2. Selection of resin-based composite material matrix: selecting one of epoxy resin, bismaleimide resin, polyimide resin, cyanate resin, phenolic resin, polyurethane acrylic resin, polyester acrylic resin as the resin-based composite material matrix;

[0013] S3, 3D light-curing printing: Without changing the distance between the single-layer reinforcement fibers, bond the single-layer reinforcement fibers to the moving table on the 3D light-curing printing device, place 2ml-1000ml of the selected resin on the fixed table, and then print according to the set parameters: slice height 100μm, light intensity range 1mW / cm 2 -15mW / cm 2 ; Exposure time 1s-20s; Number of base layers 1-5; Base exposure time 3s-30s, printing thickness 5mm, to obtain a unidirectional and multidirectional composite material with orderly fiber arrangement;

[0014] The fiber filaments are orderly arranged. The reinforcing fibers in the unidirectional and multidirectional composite materials are arranged in a fixed distance and direction. The distance between fibers in the same layer ranges from 10 μm to 1000 μm, the spacing between adjacent layers and between adjacent layers is 10 μm to 1000 μm, and the fiber stagger angle is 0-90 degrees.

[0015] Furthermore, the surface of the reinforcing fiber described in step S1 is in an untreated state or a pretreated state, and the purpose is to enhance the interfacial bonding between the fiber and the resin matrix, or to enhance the conductivity of the fiber and undergo surface treatment, such as cryogenic treatment, silane coupling agent pretreatment, electroplating copper, chemical chromium plating, etc.;

[0016] The glass fiber is preferably alkali-free glass fiber, high-strength glass fiber, or quartz glass fiber.

[0017] Furthermore, the fiber uniform laying device is any mechanical device that can achieve fixed-distance and directional laying between reinforcing fiber filaments, and has adjustable distance and controllable orientation, and is also a mechanical mechanism that can achieve fixed-distance and directional arrangement between single fibers.

[0018] Furthermore, the composite material matrix described in step S2 is prepared by a liquid molding process or a 3D photocuring printing process; the liquid molding process is specifically a resin transfer molding process, a resin film infiltration process, and a vacuum-assisted infiltration process.

[0019] Furthermore, the epoxy resin is selected from one of bisphenol A diglycidyl ether epoxy resin, bisphenol F diglycidyl ether epoxy resin, linear phenol polyglycidyl ether epoxy resin, 4,4-diaminodiphenylmethane glycidylamine epoxy resin, phthalic acid diglycidyl ester epoxy resin, dimethyl vinyl cyclohexene dioxide, and bisphenol A type epoxy acrylate.

[0020] Furthermore, the process parameters of the 3D light-curing printing described in step S3 are: light intensity 4mW / cm 2 , exposure time 5s, number of base layers 4, base layer exposure time 8s.

[0021] The present invention also relates to a unidirectional and multidirectional composite material with orderly arranged fiber filaments, which is obtained by adopting the preparation method of the above-mentioned unidirectional and multidirectional composite material with orderly arranged fiber filaments. The resin matrix of the unidirectional and multidirectional composite material with orderly arranged fiber filaments is one of epoxy resin, bismaleimide resin, polyimide resin, cyanate resin, phenolic resin, polyurethane acrylic resin and polyester acrylic resin; the reinforcing fibers in the unidirectional and multidirectional composite material with orderly arranged fiber filaments are arranged in a fixed distance and in a directional manner, the distance between fibers in the same layer ranges from 10μm to 1000μm, the spacing between adjacent layers and between adjacent layers is 10μm to 1000μm, and the fiber staggered angle is 0 degree to 90 degrees.

[0022] Compared with the prior art, the present invention has the following advantages:

[0023] The reinforcing fibers in the resin-based composite material prepared by the present invention are arranged in a fixed distance and in a directional manner, and the distance is adjustable and the orientation is controllable. The orderly arrangement of the reinforcing fibers can effectively improve the uniformity of the composite material's organization, avoid the phenomenon of local fiber clusters, reduce the inhomogeneity of mechanical properties, thereby avoiding stress concentration, effectively improving its mechanical properties (such as elastic modulus, strength, stiffness, etc.), and improving its service life; in addition, the distance between the reinforcing fibers is adjustable and the orientation is controllable, which enhances the designability and predictability of the performance of traditional resin-based composite materials. At the same time, the arrangement design of the reinforcing fibers can also give it functional material properties, such as filtering, wave absorption, etc., which is conducive to expanding its application in the fields of aviation, transportation, etc. BRIEF DESCRIPTION OF THE DRAWINGS

[0024] Figure 1 It is a fiber uniformly laying device used in the method for preparing a unidirectional and multidirectional composite material with orderly arranged fiber filaments described in the present invention (including: 1, base; 2, horizontal moving platform; 3, horizontal mounting table; 4, inner horizontal moving frame; 5, single-layer fiber fixing device; 6, single fiber fixing device; 7, vertical lifting plate; 8, progressive motor; 9, vertical moving platform; 10, screw rod; 11, vertical moving beam; 12, outer fixed reinforcing plate; 13, outer moving frame; 14, horizontal mounting plate);

[0025] Figure 2 It is a schematic diagram of a single fiber used in a method for preparing a unidirectional and multidirectional composite material with orderly arranged fiber filaments according to Example 1 of the present invention;

[0026] Figure 3 This is an example diagram of laying a single layer of reinforcing fibers in a method for preparing a unidirectional and multidirectional composite material with orderly arranged fiber filaments in Example 1 of the present invention (the distance x between the fiber filaments can be adjusted);

[0027] Figure 4 This is an example diagram of laying multiple layers of reinforcing fibers in a method for preparing a unidirectional and multidirectional composite material with orderly arranged fiber filaments according to Example 1 of the present invention ( Figure 4 middle, Figure 4 a is the front view of the reinforcement fiber laying, Figure 4 b is the bottom view from the A direction in the left figure; the angle between the fiber layers , height h can be adjusted respectively);

[0028] Figure 5 Schematic diagram of 3D light-curing printing process in a method for preparing a unidirectional and multidirectional composite material with orderly arranged fiber filaments in Example 1 of the present invention ( Figure 5 middle, Figure 5 a is the front view, Figure 5 b is the bottom view from the A direction in the left figure);

[0029] Figure 6 This is an enlarged view of the actual laying of glass fibers in a method for preparing a unidirectional and multidirectional composite material with orderly arranged fiber filaments in Example 1 of the present invention;

[0030] Figure 7 It is an enlarged view of a resin-based composite material after 3D photocuring printing in a method for preparing a unidirectional and multidirectional composite material with orderly arranged fiber filaments in Example 1 of the present invention;

[0031] Figure 8 is a schematic cross-sectional view of the polyester acrylic resin-based composite material prepared in Example 2;

[0032] Fig. 9 It is the microstructure distribution diagram of the resin-based composite material obtained in the comparative example. DETAILED DESCRIPTION

[0033] The present invention is further described in detail below by way of examples, but these examples should not be considered as limiting the present invention.

[0034] Embodiment 1:

[0035] A method for preparing a unidirectional and multidirectional composite material with orderly arranged fibers, combined with Figure 1 The fiber uniformly laying device used in the method for preparing unidirectional and multidirectional composite materials with orderly arranged fiber filaments (Chinese patent application number CN202210062439.1 A method and device for preparing micron-level regularly arranged fiber bundles, the mentioned device for preparing regular fiber bundles) comprises the following steps:

[0036] S1. Glass fiber laying:

[0037] pass Figure 1 The mechanical mechanism horizontally lays a single layer of 125 glass fibers, which are parallel and spaced 100 μm apart.

[0038] S2. Selection of resin-based composite material matrix:

[0039] Polyurethane acrylic resin is selected as the matrix of the resin-based composite material;

[0040] S3, 3D light-curing printing:

[0041] Without changing the distance between the single-layer glass fibers, they were bonded to the mobile stage of the 3D light-curing printing device. 20 ml of polyurethane acrylic resin was placed on the fixed stage, and then printing was performed according to the set parameters: slice height 100 μm; light intensity 4 mW / cm 2 ; Exposure time 5s; Number of base layers 4; Base exposure time 8s, printing thickness 5mm.

[0042] Figure 2 is a schematic diagram of a single fiber used in Example 1;

[0043] Figure 3 This is an example diagram of laying a single layer of reinforcing fibers in Example 1 (the distance x between the fiber filaments can be adjusted);

[0044] Figure 4 This is an example diagram of laying out multiple layers of reinforcing fibers in Example 1 ( Figure 4 middle, Figure 4 a is the front view of the reinforcement fiber laying, Figure 4b is the bottom view from the A direction in the left figure; the angle between the fiber layers , height h can be adjusted respectively);

[0045] Figure 5 is a schematic diagram of the 3D light-curing printing process in Example 1 ( Figure 5 middle, Figure 5 a is the front view, Figure 5 b is the bottom view from the A direction in the left figure);

[0046] Figure 6 is an enlarged view of the glass fibers laid at a distance of 100 μm in Example 1; Figure 6 As shown, the distance between fibers is uniform, ranging from 100 μm ± 10 μm;

[0047] Figure 7 This is a partial enlarged view of the resin-based composite material of the 3D light-cured printing substrate on a single layer of glass fiber laid at a fixed distance in Example 1;

[0048] like Figure 7 As shown in the figure, after 3D light-curing printing, the distance between the glass fibers did not change much and still maintained good uniformity.

[0049] Embodiment 2:

[0050] A method for preparing a unidirectional and multidirectional composite material with orderly arranged fiber filaments, comprising the following steps:

[0051] S1. Glass fiber laying:

[0052] pass Figure 1 The mechanism in the horizontally lays a fixed-distance and oriented glass fiber preform, wherein the number of single-layer fibers is 125, the number of layers is 4, the distance between glass fibers in a layer is 100 μm, the distance between adjacent glass fiber layers is 100 μm, and the fiber stagger angle θ is 45 degrees;

[0053] S2. Selection of resin-based composite material matrix:

[0054] Polyester acrylic resin is selected as the matrix of the resin-based composite material;

[0055] S3, 3D light-curing printing:

[0056] Without changing the distance between the glass fibers, they were bonded to the moving table of the 3D light-curing printing device; a certain amount of photopolymer acrylic resin was placed on the fixed surface, and then printed according to the set parameters: slice height 100μm; light intensity 5W / cm 2 ; Exposure time 6s; Number of base layers 4; Base exposure time 8s, printing thickness 5mm.

[0057] Figure 8 It is a schematic diagram of the transverse cross-section of the polyester acrylic resin-based composite material prepared in Example 2.

[0058] Comparative Example:

[0059] The existing process for preparing the resin-based composite material comprises the following steps;

[0060] S1. Place the glass fiber mesh on the moving table of the 3D light-curing printing device;

[0061] S2. Place 20 ml of polyurethane acrylic resin on the fixed table and then print according to the set parameters: slice height 100 μm; light intensity 4 mW / cm 2 ; Exposure time 5s; Number of base layers 4; Base exposure time 8s, printing thickness 5mm.

[0062] Fig. 9 This is the microstructure distribution diagram of the obtained resin-based composite material. As shown in the figure, the distribution form of the glass fibers and the distance between the fibers are random and uncontrollable.

[0063] Summary and analysis:

[0064] 1. Through Example 1 and Example 2, it can be seen that the fiber filaments are orderly arranged in the prepared unidirectional and multidirectional composite materials. The reinforcing fibers are evenly distributed and orderly arranged, and the spacing between the fibers remains unchanged before and after the photocuring process.

[0065] 2. By comparing Examples 1-2 with the comparative example, it can be seen that for traditional resin-based composite materials, their microstructures are prone to local fiber clusters or resin-rich areas. However, through the technology of the present application, the orderly and regular arrangement of reinforcing fibers in resin-based composite materials can be achieved, avoiding the occurrence of resin-rich areas and local fiber clusters, thereby reducing the probability of stress concentration when subjected to force and increasing the service life of the composite material.

[0066] The above are only preferred implementations of the present invention. The protection scope of the present invention is not limited to the above embodiments. Various process schemes that are not substantially different from the concept of the present invention are within the protection scope of the present invention.

Claims

1. A method for preparing unidirectional and multidirectional composite materials with orderly arranged fiber filaments, characterized in that: The following steps are involved: S1. Laying of reinforcing fibers: firstly, orderly lay out a reinforcing fiber array with 1 to 100 layers and 5 to 500 fibers in each layer; wherein, the reinforcing fibers in each layer are parallelly distributed and the distance between them is 10 μm to 1000 μm; the spacing between adjacent layers is 10 μm to 1000 μm, and the fiber stagger angle is 0 to 90 degrees; The orderly laying is to arrange the reinforcing fibers in an orderly and regular manner by using a fiber uniform laying device. The orderly and regular arrangement means that the distance between the reinforcing fibers is adjustable and the orientation is controllable; The reinforcing fiber is selected from carbon fiber, glass fiber, aramid fiber, ultra-high molecular weight polyethylene fiber and other fibers used in the field of composite materials; the glass fiber is selected from alkali-free glass fiber, high-strength glass fiber and quartz glass fiber; S2. Selection of resin-based composite material matrix: Select one of epoxy resin, bismaleimide resin, polyimide resin, cyanate resin, phenolic resin, polyurethane acrylic resin, and polyester acrylic resin as the resin-based composite material matrix; the epoxy resin is selected from one of bisphenol A diglycidyl ether epoxy resin, bisphenol F diglycidyl ether epoxy resin, linear phenolic polyglycidyl ether epoxy resin, 4,4-diaminodiphenylmethane glycidylamine epoxy resin, phthalic acid diglycidyl ester epoxy resin, dimethyl cyclohexene dioxide, and bisphenol A type epoxy acrylate; S3, 3D light-curing printing: Without changing the distance between the single-layer reinforcement fibers, bond the single-layer reinforcement fibers to the moving table on the 3D light-curing printing device, place 2ml-1000ml of the selected resin on the fixed table, and then print according to the set parameters: slice height 100μm, light intensity range 1 mW / cm 2 -15 mW / cm 2 ; Exposure time 1s-20s; Number of base layers 1-5; Base exposure time 3s-30s, printing thickness 5mm, to obtain a unidirectional and multidirectional composite material with orderly fiber arrangement; The fiber filaments are orderly arranged. The reinforcing fibers in the unidirectional and multidirectional composite materials are arranged in a fixed distance and direction. The distance between fibers in the same layer ranges from 10 μm to 1000 μm, the spacing between adjacent layers and between adjacent layers is 10 μm to 1000 μm, and the fiber stagger angle is 0 degree to 90 degrees.

2. The method for preparing a unidirectional and multidirectional composite material with orderly arranged fiber filaments according to claim 1, characterized in that: The composite material matrix described in step S2 is prepared by a liquid molding process or a 3D light-curing printing process; the liquid molding process is a resin transfer molding process, a resin film infiltration process, or a vacuum-assisted infiltration process.

3. The method for preparing a unidirectional and multidirectional composite material with orderly arranged fiber filaments according to claim 1, characterized in that: The process parameters of 3D light-curing printing described in step S3 are: light intensity 4 mW / cm 2 , exposure time 5s, number of base layers 4, base layer exposure time 8s.

4. A unidirectional and multidirectional composite material with orderly arranged fiber filaments, characterized in that: The method for preparing a unidirectional and multidirectional composite material with orderly arranged fiber filaments as described in any one of claims 1 to 3 is adopted to obtain the composite material, wherein the resin matrix of the unidirectional and multidirectional composite material with orderly arranged fiber filaments is one of epoxy resin, bismaleimide resin, polyimide resin, cyanate resin, phenolic resin, polyurethane acrylic resin and polyester acrylic resin; the reinforcing fibers in the unidirectional and multidirectional composite material with orderly arranged fiber filaments are arranged in a fixed distance and in a directional manner, the distance between fibers in the same layer ranges from 10μm to 1000μm, the spacing between adjacent layers and between adjacent layers is 10μm to 1000μm, and the fiber stagger angle is 0 degree to 90 degrees.

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