CN114478053A

CN114478053A - Aluminum-based silicon carbide composite material and preparation method thereof

Info

Publication number: CN114478053A
Application number: CN202210113833.3A
Authority: CN
Inventors: 闫春泽; 王长顺; 刘桂宙; 杨潇; 史玉升
Original assignee: Huazhong University of Science and Technology
Current assignee: Huazhong University of Science and Technology
Priority date: 2022-01-30
Filing date: 2022-01-30
Publication date: 2022-05-13

Abstract

The invention belongs to the technical field of aluminum-based silicon carbide composite materials, and discloses an aluminum-based silicon carbide composite material and a preparation method thereof, wherein the preparation method comprises the following steps: (1) curing the silicon carbide composite material blank to obtain a porous silicon carbide/carbon blank; (2) carrying out reaction sintering on the porous silicon carbide/carbon blank; (3) carrying out silicon carbide densification treatment on the porous silicon carbide blank to ensure that the porosity of the porous silicon carbide blank is within a preset range so as to obtain a porous silicon carbide preform; (4) carrying out sol-gel interface modification on the porous silicon carbide preform; (5) and (3) carrying out aluminum alloy infiltration on the modified porous silicon carbide preform, and filling the pores inside the porous silicon carbide preform with aluminum alloy liquid to obtain the aluminum-based silicon carbide composite material with the preset aluminum alloy volume fraction. The aluminum-based silicon carbide component with adjustable silicon carbide-aluminum volume fraction, controllable structural complexity and size meeting the requirement can be obtained by the method, and has wide application prospect.

Description

Aluminum-based silicon carbide composite material and preparation method thereof

Technical Field

The invention belongs to the technical field of aluminum-based silicon carbide composite materials, and particularly relates to an aluminum-based silicon carbide composite material and a preparation method thereof.

Background

The aluminum-based silicon carbide composite material has the characteristics of low density, high heat conductivity, high strength, good thermal stability, good wear resistance and the like, and is widely applied to important fields of aerospace, automobiles, ships and the like. The aluminum-based silicon carbide integrates the advantages of aluminum alloy and silicon carbide, has the advantages of high toughness and plasticity of metal and high hardness and modulus of silicon carbide, is generally 1/3 of steel in density, higher than pure aluminum and medium carbon steel in strength, good in wear resistance and capable of stably working at the high temperature of 300-350 ℃. At present, the traditional preparation methods of the aluminum-based silicon carbide composite material comprise a pressure casting method, a jet coprecipitation method, a liquid method, a semi-solid stirring and melting composite method and the like, and the methods can theoretically prepare the isotropic aluminum-based silicon carbide composite material with uniformly distributed particles. However, with the rapid development of science and technology, the demand of various fields for aluminum-based silicon carbide complex profiled members is higher and higher, however, the aluminum-based silicon carbide material prepared by the traditional method still needs to be processed by secondary machinery to obtain the required product, thereby increasing the manufacturing cost. And moreover, by adopting the traditional forming method, certain complex special-shaped aluminum-based silicon carbide composite material components are difficult to prepare or even cannot be integrally prepared.

The additive manufacturing technology can form a complex structure through three-dimensional model data without a die, and is an effective way for realizing integration, light weight and complex forming of complex components at present. The patent with application number 201810333525.5 discloses a method for preparing high-performance aluminum-based carbide, which comprises the steps of carrying out surface coupling modification and aluminum nanoshell coating on silicon carbide powder to obtain composite powder, and pressing to obtain aluminum-based silicon carbide. For this reason, some aluminum-based silicon carbide composite material preparation schemes based on additive manufacturing techniques have been proposed in the prior art. For example, the application No. 201910011326.7 discloses a method for preparing a SiC/Al composite structural member by selective laser sintering, which comprises the steps of uniformly coating modified silicon carbide powder with an aluminum alloy liquid by a gas atomization powder preparation method to obtain aluminum alloy coated silicon carbide composite powder with uniformly distributed particle sizes, and sintering and forming the aluminum-based silicon carbide composite material by selective laser sintering under the protection of inert gas. The patent with the application number of 201910579799.7 discloses a ceramic-aluminum composite material for additive manufacturing, a preparation method and a ceramic-aluminum composite material structural member additive manufacturing method, wherein an electrostatic assembly method is adopted to enable nano ceramic powder with negative electricity to be stably adsorbed on aluminum alloy powder with positive electricity, and the ceramic-aluminum composite material is obtained through selective laser melting forming. The two methods can only prepare the silicon carbide reinforced aluminum-based composite material with low volume fraction, and limit the application range of the aluminum-based silicon carbide composite material.

Disclosure of Invention

Aiming at the defects or improvement requirements of the prior art, the invention provides the aluminum-based silicon carbide composite material and the preparation method thereof, which can realize material system regulation and control of the aluminum-based silicon carbide composite material and integrated forming of a complex structure, well solve the problem that a complex component is difficult or even cannot be formed in the traditional preparation method, and simultaneously solve the problems that the material preparation process is complex and a blank body is difficult to form in the traditional additive manufacturing method; meanwhile, the method can be used for preparing the silicon carbide reinforced aluminum-based composite material with high/low volume fraction, realizes the preparation of small-sized high-precision large-sized integrated complex aluminum-based silicon carbide components, can be used for manufacturing corresponding aluminum-based silicon carbide products according to different requirements, and has wide application prospect.

To achieve the above object, according to one aspect of the present invention, there is provided a method for preparing an aluminum-based silicon carbide composite material, the method comprising the steps of:

(1) selecting a silicon carbide material as a base material, a carbon material as an auxiliary material and resin as a binder, and forming a silicon carbide composite material blank body with a required structure by adopting an additive manufacturing technology;

(2) curing the silicon carbide composite material blank at 600-1000 ℃ to obtain a porous silicon carbide/carbon blank;

(3) performing reaction sintering on the porous silicon carbide/carbon blank to enable carbon in the porous silicon carbide/carbon blank to react with silicon to generate a porous silicon carbide blank;

(4) carrying out silicon carbide densification treatment on the porous silicon carbide blank to enable the porosity of the porous silicon carbide blank to be within a preset range so as to obtain a porous silicon carbide preform;

(5) carrying out sol-gel interface modification on the porous silicon carbide preform to improve the interface compatibility between the porous silicon carbide preform and the aluminum alloy;

(6) and (3) carrying out aluminum alloy infiltration on the modified porous silicon carbide preform, and filling the pores inside the porous silicon carbide preform with aluminum alloy liquid to obtain the aluminum-based silicon carbide composite material with the preset aluminum alloy volume fraction.

Further, liquid-phase siliconizing or gas-phase siliconizing is adopted in the reaction sintering; the silicon carbide densification treatment adopts chemical vapor infiltration or precursor impregnation cracking; and the aluminum alloy liquid infiltration adopts pressureless infiltration, vacuum infiltration or pressure infiltration.

Further, the silicon carbide material is one or more of silicon carbide micro powder, chopped silicon carbide fiber, silicon carbide whisker and silicon carbide nanowire; the carbon material is one or more of spherical graphite, flake graphite, diamond micro powder, graphene and carbon fiber; the resin is epoxy resin powder, phenolic resin powder, nylon powder, liquid phenolic resin or liquid photosensitive resin.

Furthermore, in the step (1), the silicon carbide material, the carbon material and the resin are 55-85 parts, 5-25 parts and 10-20 parts respectively.

Further, the additive manufacturing technique is stereolithography, powder bed melting, material extrusion, directed energy deposition, adhesive jetting, or thin-material lamination.

Further, the porosity of the porous silicon carbide/carbon blank is 60-65%.

Further, in the step (3), the reaction sintering is performed by gas-phase siliconizing, the gas-phase siliconizing is performed in vacuum or protective atmosphere, the protective atmosphere is one or more of nitrogen, argon and helium, the vacuum degree is 100Pa, the gas-phase siliconizing temperature is 1550 ℃ to 1700 ℃, the temperature rise rate of the gas-phase siliconizing is 5 ℃/min to 15 ℃/min, and the gas-phase siliconizing time is 0.5h to 5 h.

Further, the porosity of the porous silicon carbide preform is 30-65%.

Further, in the step (5), the porous silicon carbide preform is placed into silica sol with the concentration of 10% -30%, and is soaked for 15 min-60 min under the vacuum condition, then the porous silicon carbide preform soaked with the silica sol is placed into a muffle furnace, and is heated to 600-1200 ℃, and the temperature is kept for 30 min-120 min.

According to another aspect of the present invention, there is provided an aluminum-based silicon carbide composite material prepared by the method for preparing an aluminum-based silicon carbide composite material as described above.

Generally, compared with the prior art, the aluminum-based silicon carbide composite material and the preparation method thereof provided by the invention have the following beneficial effects:

1. the porosity of the porous silicon carbide body can be adjusted through chemical vapor infiltration or precursor impregnation and cracking, so that the porous silicon carbide preform with the required volume fraction is obtained.

2. The surface of the silicon carbide preform is improved by a sol-gel method, so that the poor interface reaction between the aluminum alloy and the silicon carbide is eliminated, and the interface bonding strength of the aluminum-based silicon carbide composite material is improved.

3. According to the invention, the mass of the aluminum alloy ingot/particle is calculated quantitatively through the porosity of the porous silicon carbide preform, an aluminum-based silicon carbide product can be obtained through aluminizing once, and the post-treatment process is reduced as much as possible.

4. The preparation method of the aluminum-based silicon carbide composite material based on the additive manufacturing technology has the advantages of adjustable aluminum-silicon carbide ratio, controllable aluminum-silicon carbide distribution gradient, capability of forming complex components and the like, and has wide application prospects.

5. According to the invention, carbon in the porous silicon carbide/carbon blank body can react with silicon to generate silicon carbide through a reaction sintering process, so that residual carbon can be removed and fine crystal grain silicon carbide can be generated, and the strength of the aluminum-based silicon carbide composite material can be improved.

6. The additive technology used by the invention comprises processes of three-dimensional light curing, powder bed melting, material extrusion, directional energy deposition, adhesive spraying, thin material lamination and the like, wherein the three-dimensional light curing can form a small-size high-precision component, the powder bed melting process can form a medium-size component, and the adhesive spraying process can form a large-size component, so that the requirements of different application scenes on the sizes of aluminum-based silicon carbide products are met.

7. The invention has wide range of selected raw materials, and can design and prepare the silicon carbide particle reinforced aluminum matrix composite with high/low volume fraction according to application requirements, thereby realizing the diversified application of the aluminum matrix silicon carbide composite.

8. The invention provides a preparation method of an aluminum-based silicon carbide composite material based on an additive manufacturing technology and a product, and provides a new thought and a new method for the design and preparation of the aluminum-based silicon carbide composite material.

Drawings

Fig. 1 is a schematic flow chart of a preparation method of an aluminum-based silicon carbide composite material provided by the invention.

Detailed Description

In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is described in further detail below with reference to the accompanying drawings and embodiments. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention. In addition, the technical features involved in the embodiments of the present invention described below may be combined with each other as long as they do not conflict with each other.

Referring to fig. 1, the present invention provides a method for preparing an aluminum-based silicon carbide composite material, wherein the method comprises the steps of manufacturing a silicon carbide composite material blank by additive manufacturing, preparing a porous silicon carbide/carbon blank by high temperature curing, preparing a silicon carbide blank by reaction sintering, obtaining porous silicon carbide by chemical vapor infiltration or precursor impregnation and cracking, and obtaining the aluminum-based silicon carbide composite material by an aluminum alloy impregnation process.

The preparation method mainly comprises the following steps:

selecting a silicon carbide material as a base material, a carbon material as an auxiliary material and resin as a binder, and forming a silicon carbide composite material blank body with a required structure by adopting an additive manufacturing technology.

Wherein, the additive manufacturing technology forming process of the silicon carbide composite material blank comprises the following steps:

(1) according to the mass fractions of the silicon carbide material, the carbon material and the binder, composite powder, slurry, sheets, wires and the like suitable for additive manufacturing are prepared by adopting methods such as mechanical mixing, solvent evaporation or stirring defoaming and the like.

(2) And establishing a corresponding three-dimensional model by adopting modeling software according to a required product.

(3) And forming the silicon carbide composite material blank body by the composite powder, the slurry, the sheets, the wires and the like according to the three-dimensional model through a corresponding additive manufacturing technology.

The silicon carbide material is preferably one or more of composite materials of silicon carbide micro powder, chopped silicon carbide fibers, silicon carbide whiskers and silicon carbide nanowires, the carbon material is preferably one or more of composite materials of spherical graphite, flake graphite, diamond micro powder, graphene and carbon fibers, and the resin is preferably epoxy resin powder, phenolic resin powder, nylon powder, liquid phenolic resin and liquid photosensitive resin.

In the embodiment, the silicon carbide material is 55-85 parts, the carbon material is 5-25 parts, and the resin/aluminum alloy is 10-20 parts; the additive manufacturing techniques include stereolithography, powder bed melting, material extrusion, directed energy deposition, adhesive jetting, thin material lamination, and the like.

And secondly, curing the silicon carbide composite material blank at high temperature to obtain a porous silicon carbide/carbon blank. Wherein the high temperature curing comprises the following steps: and (3) placing the silicon carbide composite material blank in an alumina crucible, embedding the silicon carbide composite material blank by using silicon carbide coarse powder, and heating the silicon carbide composite material blank under an inert atmosphere or vacuum condition to crack organic matters in the blank and melt aluminum alloy to obtain a porous silicon carbide/carbon blank. The particle size of the silicon carbide coarse powder is 0.2-1 mm, the inert atmosphere is one or more of nitrogen, argon, helium and neon, the heating temperature is 600-1000 ℃, the heating rate is 0.1-5 ℃/min, and the heat preservation time is 2-10 h. In the present embodiment, the porosity of the porous silicon carbide/carbon green body is preferably 60% to 65%.

And step three, performing reaction sintering on the porous silicon carbide/carbon blank to enable carbon in the porous silicon carbide/carbon blank to react with silicon to generate the porous silicon carbide blank, wherein the reaction sintering adopts liquid phase siliconizing or gas phase siliconizing.

The liquid phase siliconizing comprises the following steps: covering a layer of graphite paper inside the graphite crucible, placing the porous silicon carbide/carbon blank in the graphite crucible, embedding the porous silicon carbide/carbon blank with silicon particles, heating the porous silicon carbide/carbon blank under a vacuum condition to melt the silicon particles and uniformly infiltrate the silicon particles into the porous silicon carbide/carbon blank, and reacting the silicon particles with carbon in the porous silicon carbide/carbon blank to generate silicon carbide to obtain the porous silicon carbide blank. Wherein the vacuum degree under the vacuum condition is 100 Pa-200 Pa, the particle size of the silicon particles is 1 mm-5 mm, the mass of the silicon particles is 3-3.5 times of that of the carbon material, the heating temperature is 1450-1600 ℃, the heating rate is 5-20 ℃/min, and the heat preservation time is 0.5-3 h.

The gas phase siliconizing comprises the following steps: and placing the porous silicon carbide/carbon blank on a porous graphite support, placing the porous silicon carbide/carbon blank in a graphite crucible with a boron nitride coating coated on the surface, placing silicon particles in the graphite crucible, heating under a vacuum condition to melt the silicon particles, generating silicon vapor, uniformly penetrating the silicon vapor into the porous silicon carbide/carbon blank, and reacting the silicon vapor with the carbon in the porous silicon carbide/carbon blank to generate silicon carbide to obtain the porous silicon carbide blank. The vacuum degree under the vacuum condition is 100Pa, the particle size of the silicon particles is 1-5 mm, the mass of the silicon particles is 3-3.5 times of that of the carbon material, the heating temperature is 1550-1700 ℃, the heating rate is preferably 5-15 ℃/min, and the heat preservation time is preferably 0.5-5 h.

And step four, carrying out silicon carbide densification treatment on the porous silicon carbide pre-blank body to enable the porosity of the porous silicon carbide blank body to be in a controllable range so as to obtain the porous silicon carbide pre-blank body, wherein the silicon carbide densification treatment adopts chemical gas phase permeation and precursor impregnation cracking.

The chemical vapor infiltration comprises the following steps: placing the porous silicon carbide green body in a chemical vapor deposition furnace, conveying a precursor solution into a hearth under the conveying of hydrogen, uniformly permeating the precursor solution into the green body, heating to crack the precursor to generate silicon carbide, and obtaining a porous silicon carbide preform with the porosity within a required range; the precursor is methyl trichlorosilane, the heating temperature is 900-1200 ℃, the heating rate is 2-5 ℃/min, and the heating time is 5-15 h.

The precursor impregnation cracking comprises the following steps: placing the porous silicon carbide green body in a precursor solution, vacuumizing to enable the precursor solution to be impregnated into the green body, curing the green body, transferring the green body to a tubular furnace, heating to enable the precursor to be cracked to generate silicon carbide, and obtaining a porous silicon carbide prefabricated body with the porosity within a required range; the precursor is polycarbosilane, the heating temperature is 1000-1500 ℃, the heating rate is 0.5-5 ℃/min, the heating time is 2-5 h, and the porosity of the porous silicon carbide is preferably 30-65%.

And fifthly, carrying out sol-gel interface modification on the porous silicon carbide preform to improve the interface compatibility between the porous silicon carbide preform and the aluminum alloy.

The sol-gel interface modification comprises the following steps: and placing the porous silicon carbide preform into 10-30% silica sol, dipping for 15-60 min under a vacuum condition, then placing the porous silicon carbide preform dipped with the silica sol into a muffle furnace, heating to 600-1200 ℃, and preserving heat for 30-120 min.

And sixthly, performing aluminum alloy infiltration on the porous silicon carbide preform to fill the pores in the porous silicon carbide preform with aluminum alloy liquid so as to obtain the aluminum-based silicon carbide composite material. The aluminum alloy liquid infiltration adopts pressureless infiltration, vacuum infiltration or pressure infiltration.

The pressureless infiltration comprises the following steps: embedding the porous silicon carbide preform by adopting aluminum alloy ingots/particles, placing the embedded porous silicon carbide preform in an alumina crucible, placing the alumina crucible in a vacuum atmosphere sintering furnace, introducing protective gas, heating to a set temperature to melt aluminum alloy, infiltrating aluminum alloy liquid into the porous silicon carbide preform under the action of capillary force, and finally cooling along with the furnace to obtain an aluminum-based silicon carbide composite material; the aluminum alloy is preferably one or more of aluminum-silicon alloy, aluminum-magnesium alloy, aluminum-iron alloy, aluminum-copper alloy, aluminum-zinc alloy and aluminum-silicon-magnesium alloy, the mass of the aluminum alloy is 0.4-1.6 times that of porous silicon carbide, the heating temperature is 650-800 ℃, and the heating rate is 5-10 ℃/min.

The vacuum infiltration comprises the following steps: embedding the porous silicon carbide preform by adopting aluminum alloy ingots/particles, placing the porous silicon carbide preform in an alumina crucible, placing the alumina crucible in a vacuum atmosphere sintering furnace, introducing protective gas, heating to a set temperature, vacuumizing to 100Pa to melt aluminum alloy, infiltrating aluminum alloy liquid into the porous silicon carbide preform under the action of capillary force and pressure difference, and finally cooling along with the furnace to obtain an aluminum-based silicon carbide composite material; the aluminum alloy is preferably one or more of aluminum-silicon alloy, aluminum-magnesium alloy, aluminum-iron alloy, aluminum-copper alloy, aluminum-zinc alloy and aluminum-silicon-magnesium alloy, the mass of the aluminum alloy is 0.4-1.6 times that of porous silicon carbide, the heating temperature is 650-800 ℃, and the heating rate is 5-10 ℃/min.

The pressure infiltration comprises the following steps: placing the porous silicon carbide preform in a crucible resistance furnace, adding a proper amount of aluminum alloy ingots/particles, introducing protective gas, heating to a set temperature to melt the aluminum alloy, vacuumizing to 1000Pa, maintaining the pressure for 15-30 min, introducing inert gas to pressurize to 0.5-2 MPa, maintaining the pressure for 30-60 min, and finally releasing the pressure and cooling along with the furnace to obtain the aluminum-based silicon carbide composite material; the aluminum alloy is preferably one or more of aluminum-silicon alloy, aluminum-magnesium alloy, aluminum-iron alloy, aluminum-copper alloy, aluminum-zinc alloy and aluminum-silicon-magnesium alloy, the mass of the aluminum alloy is 0.4-1.6 times that of porous silicon carbide, the heating temperature is 650-800 ℃, and the heating rate is 5-10 ℃/min.

In the embodiment, the volume fraction of the aluminum alloy in the aluminum-based silicon carbide composite material is preferably 33-68%; the embodiment mainly comprises five aspects: firstly, a designed material system is adopted to form a silicon carbide composite material blank body with a required shape through additive manufacturing; secondly, the prepared silicon carbide composite material green body is cured at high temperature to obtain a porous silicon carbide/carbon green body; thirdly, reacting the prepared porous silicon carbide/carbon blank by adopting reactive sintering to generate a porous silicon carbide blank; fourthly, preparing the prepared silicon carbide prefabricated body into a porous silicon carbide prefabricated body with proper volume fraction by a chemical vapor infiltration or precursor impregnation cracking method; and fifthly, obtaining the aluminum-based silicon carbide composite material by the porous silicon carbide preform through an aluminum alloy infiltration process, and finally preparing the complex aluminum-based silicon carbide part with adjustable material volume fraction and controllable structure.

The invention also provides an aluminum-based silicon carbide composite material, which is prepared by adopting the preparation method of the aluminum-based silicon carbide composite material.

The present invention will be described in further detail below with reference to several specific examples.

Example 1

The preparation method of the aluminum-based silicon carbide composite material provided by the embodiment 1 of the invention mainly comprises the following steps:

(a) selecting 55 parts, 25 parts and 10 parts of silicon carbide micro powder, spherical graphite and epoxy resin powder, respectively, constructing a three-dimensional model, and sintering by adopting a selective laser region to form a silicon carbide composite material blank body with a required structure.

(b) And (2) curing the silicon carbide composite material blank at high temperature, placing the silicon carbide composite material blank in an alumina crucible, embedding the silicon carbide composite material blank by using silicon carbide coarse powder with the particle size of 0.2mm, heating to 600 ℃ under the condition of nitrogen to crack organic matters, wherein the heating rate is 0.1 ℃/min, and preserving heat for 2 hours to obtain the porous silicon carbide/carbon blank.

(c) And carrying out liquid phase siliconizing on the porous silicon carbide/carbon blank, covering a layer of graphite paper inside the graphite crucible, placing the porous silicon carbide/carbon blank in the graphite crucible, embedding the porous silicon carbide/carbon blank by using silicon particles with the particle size of 1mm, wherein the mass of the silicon particles is 3 times that of the carbon material, heating the porous silicon carbide/carbon blank to 1450 ℃ at the heating rate of 5 ℃/min under the vacuum degree of 100Pa so as to melt the silicon particles, uniformly impregnating the porous silicon carbide/carbon blank, reacting the porous silicon carbide/carbon blank with carbon in the porous silicon carbide/carbon blank to generate silicon carbide to obtain the porous silicon carbide blank, and keeping the temperature for 0.5 h.

(d) And carrying out chemical vapor infiltration densification treatment on the porous silicon carbide blank, placing the silicon carbide blank in a chemical vapor deposition furnace, conveying a methyltrichlorosilane solution into a hearth under the condition of hydrogen, uniformly infiltrating the methyl trichlorosilane solution into the preform, heating the hearth to 900 ℃/min at the heating rate of 2 ℃/min to crack the precursor to generate silicon carbide, and heating for 5h to obtain the porous silicon carbide preform with the porosity of 65%.

(e) And putting the porous silicon carbide preform into 10% silica sol, soaking for 15min under a vacuum condition, then putting the porous silicon carbide preform soaked with the silica sol into a muffle furnace, heating to 600 ℃, and preserving heat for 30 min.

(f) And (2) carrying out aluminum alloy infiltration on the porous silicon carbide preform, embedding the porous silicon carbide preform by adopting an aluminum-silicon alloy ingot/particle which is 1.6 times that of the porous silicon carbide, placing the porous silicon carbide preform in an alumina crucible, putting the porous silicon carbide preform in a vacuum atmosphere sintering furnace, introducing protective gas, heating to 650 ℃ at a heating rate of 5 ℃/min to melt the aluminum alloy, infiltrating aluminum alloy liquid into the porous silicon carbide preform under the action of capillary force, and finally cooling along with the furnace to obtain the aluminum-based silicon carbide composite material.

Example 2

The preparation method of the aluminum-based silicon carbide composite material provided by the embodiment 2 of the invention mainly comprises the following steps:

(a) selecting short-cut silicon carbide fiber, flake graphite and phenolic resin powder in the proportion of 85 parts, 5 parts and 10 parts respectively, preparing composite powder suitable for additive manufacturing by adopting a solvent evaporation method, constructing a three-dimensional model, and sintering and forming a silicon carbide composite material blank body with a required structure by adopting a selective laser sintering method.

(b) And (2) curing the silicon carbide composite material blank at high temperature, placing the silicon carbide composite material blank in an alumina crucible, embedding the silicon carbide composite material blank by using silicon carbide coarse powder with the particle size of 1mm, heating to 1000 ℃ under the condition of nitrogen to crack organic matters, wherein the heating rate is 0.1 ℃/min, and keeping the temperature for 5 hours to obtain the porous silicon carbide/carbon blank.

(c) And carrying out liquid phase siliconizing on the porous silicon carbide/carbon blank, covering a layer of graphite paper inside the graphite crucible, placing the porous silicon carbide/carbon blank in the graphite crucible, embedding the porous silicon carbide/carbon blank by using silicon particles with the particle size of 5mm, wherein the mass of the silicon particles is 3.5 times that of the carbon material, heating the porous silicon carbide/carbon blank to 1600 ℃ at the heating rate of 5 ℃/min under the vacuum degree of 50Pa so as to melt the silicon particles and uniformly infiltrate the silicon particles into the porous silicon carbide/carbon blank, reacting the silicon particles with carbon in the porous silicon carbide/carbon blank to generate silicon carbide so as to obtain the porous silicon carbide blank, and keeping the temperature for 2 hours.

(d) And carrying out chemical vapor infiltration densification treatment on the porous silicon carbide blank, placing the silicon carbide blank in a chemical vapor deposition furnace, conveying a methyltrichlorosilane solution into a hearth under the condition of hydrogen, uniformly infiltrating the solution into the preform, heating the preform to 1200 ℃ at the heating rate of 2 ℃/min, cracking the precursor to generate silicon carbide, and heating for 5h to obtain the porous silicon carbide preform with the porosity of 30%.

(e) And putting the porous silicon carbide preform into silica sol with the concentration of 30%, soaking for 60min under a vacuum condition, then putting the porous silicon carbide preform soaked with the silica sol into a muffle furnace, heating to 1200 ℃, and preserving heat for 120 min.

(f) And (2) carrying out aluminum alloy impregnation on the porous silicon carbide preform, embedding the porous silicon carbide preform by adopting an aluminum-silicon-magnesium alloy ingot/particle aluminum alloy ingot/particle with the mass of 0.4 time of that of the porous silicon carbide preform, placing the porous silicon carbide preform in an aluminum oxide crucible, putting the porous silicon carbide preform in a vacuum atmosphere sintering furnace, introducing protective gas, heating to 800 ℃ at the heating rate of 5 ℃/min, vacuumizing to 100Pa to melt aluminum alloy, infiltrating aluminum alloy liquid into the porous silicon carbide preform under the action of capillary force and pressure difference, and finally cooling along with the furnace to obtain the aluminum-based silicon carbide composite material.

Example 3

The preparation method of the aluminum-based silicon carbide composite material provided by the embodiment 3 of the invention mainly comprises the following steps:

(a) selecting 55 parts, 20 parts and 25 parts of silicon carbide whiskers, diamond micropowder and photosensitive resin respectively, preparing composite powder suitable for additive manufacturing by adopting a stirring defoaming method, constructing a three-dimensional model, and forming a silicon carbide composite material blank body with a required structure by adopting three-dimensional photocuring.

(b) And (2) curing the silicon carbide composite material blank at high temperature, placing the silicon carbide composite material blank in an alumina crucible, embedding the silicon carbide composite material blank by using silicon carbide coarse powder with the particle size of 1mm, heating to 800 ℃ under the condition of nitrogen to crack organic matters, wherein the heating rate is 0.1 ℃/min, and keeping the temperature for 5 hours to obtain the porous silicon carbide/carbon blank.

(c) And carrying out gas-phase siliconizing on the porous silicon carbide/carbon blank, placing the porous silicon carbide/carbon blank on a porous graphite support, placing the porous silicon carbide/carbon blank in a graphite crucible with a boron nitride coating coated on the surface, placing the silicon particles in the graphite crucible, heating under a vacuum condition to melt the silicon particles, generate silicon vapor, uniformly permeate the silicon vapor into the porous silicon carbide/carbon blank, and reacting the silicon vapor with carbon in the porous silicon carbide/carbon blank to generate silicon carbide so as to obtain the porous silicon carbide blank. The vacuum degree of the vacuum condition is 0Pa, the particle size of the silicon particles is 5mm, the mass of the silicon particles is 3 times that of the carbon material, the heating temperature is 1700 ℃, the heating rate is preferably 5 ℃/min, and the heat preservation time is preferably 5 h.

(d) And carrying out precursor impregnation cracking densification treatment on the porous silicon carbide blank, placing the porous silicon carbide blank into a precursor solution, vacuumizing to enable the precursor solution to infiltrate into the blank, curing the blank, transferring the blank into a tube furnace, heating to enable the precursor to crack so as to generate silicon carbide, and obtaining the porous silicon carbide preform with the porosity within the required range. The precursor is polycarbosilane, the heating temperature is 1000 ℃, the heating rate is 0.5 ℃/min, the heating time is 2h, and the porosity of the porous silicon carbide is preferably 65%.

(e) And (3) putting the porous silicon carbide preform into 20% silica sol, soaking for 30min under a vacuum condition, then putting the porous silicon carbide preform soaked in the silica sol into a muffle furnace, heating to 800 ℃, and preserving heat for 60 min.

(f) And (2) carrying out aluminum alloy infiltration on the porous silicon carbide preform, placing the porous silicon carbide preform in a crucible resistance furnace, adding aluminum-silicon alloy ingots/particles with the mass 1.6 times that of the porous silicon carbide, introducing protective gas, heating to 800 ℃ at the heating rate of 5 ℃/min to melt the aluminum alloy, vacuumizing to 1000Pa, maintaining the pressure for 15min, introducing inert gas to pressurize to 0.5MPa, maintaining the pressure for 30min, and finally, releasing the pressure and cooling along with the furnace to obtain the aluminum-based silicon carbide composite material.

Example 4

The preparation method of the aluminum-based silicon carbide composite material provided by the embodiment 4 of the invention mainly comprises the following steps:

(a) selecting 55 parts, 20 parts and 30 parts of silicon carbide whiskers, diamond micropowder and photosensitive resin respectively, preparing composite powder suitable for additive manufacturing by adopting a stirring defoaming method, constructing a three-dimensional model, and forming a silicon carbide composite material blank body with a required structure by adopting three-dimensional photocuring.

(b) And (2) curing the silicon carbide composite material blank at high temperature, placing the silicon carbide composite material blank in an alumina crucible, embedding the silicon carbide composite material blank by using silicon carbide coarse powder with the particle size of 1mm, heating to 800 ℃ under the condition of nitrogen to crack organic matters, wherein the heating rate is 0.1 ℃/min, and preserving heat for 5 hours to obtain the porous silicon carbide/carbon blank.

(c) And carrying out gas-phase siliconizing on the porous silicon carbide/carbon blank, placing the porous silicon carbide/carbon blank on a porous graphite support, placing the porous silicon carbide/carbon blank in a graphite crucible with a boron nitride coating coated on the surface, placing the silicon particles in the graphite crucible, heating under a vacuum condition to melt the silicon particles, generate silicon vapor, uniformly permeate the silicon vapor into the porous silicon carbide/carbon blank, and reacting the silicon vapor with carbon in the porous silicon carbide/carbon blank to generate silicon carbide to obtain the porous silicon carbide blank. The vacuum degree of the vacuum condition is 0Pa, the particle size of the silicon particles is 5mm, the mass of the silicon particles is 3 times that of the carbon material, the heating temperature is 1700 ℃, the heating rate is preferably 5 ℃/min, and the heat preservation time is preferably 5 h.

(d) And carrying out precursor impregnation cracking densification treatment on the porous silicon carbide blank, placing the silicon carbide blank in a precursor solution, vacuumizing to enable the precursor solution to infiltrate into the blank, curing the blank, transferring the blank into a tube furnace, heating to enable the precursor to crack to generate silicon carbide, and obtaining the porous silicon carbide preform with the porosity within the required range. The precursor is polycarbosilane, the heating temperature is 1000 ℃, the heating rate is 0.5 ℃/min, the heating time is 2h, and the porosity of the porous silicon carbide blank is preferably 65%.

(e) And putting the porous silicon carbide preform into 15% silica sol, soaking for 20min under a vacuum condition, then putting the porous silicon carbide preform soaked with the silica sol into a muffle furnace, heating to 1000 ℃, and preserving heat for 45 min.

(f) And (2) carrying out aluminum alloy infiltration on the porous silicon carbide preform, placing the porous silicon carbide preform in a crucible resistance furnace, adding a proper amount of aluminum-silicon alloy ingot/particle with the mass 1.6 times that of the porous silicon carbide, introducing protective gas, heating to 800 ℃ at the heating rate of 5 ℃/min to melt the aluminum alloy, vacuumizing to 1000Pa, maintaining the pressure for 15min, introducing inert gas to pressurize to 0.5MPa, maintaining the pressure for 30min, and finally, releasing the pressure and cooling along with the furnace to obtain the aluminum-based silicon carbide composite material.

Example 5

The preparation method of the aluminum-based silicon carbide composite material provided by the embodiment 5 of the invention mainly comprises the following steps:

(a) selecting 70 parts, 25 parts and 5 parts of silicon carbide nanowires, flake graphite and liquid phenolic resin respectively, preparing composite powder suitable for additive manufacturing by adopting a mechanical mixing method, constructing a three-dimensional model, and spray-forming a silicon carbide composite material blank body with a required structure by adopting a binder.

(b) And (2) curing the silicon carbide composite material blank at high temperature, placing the silicon carbide composite material blank in an alumina crucible, embedding the silicon carbide composite material blank by using silicon carbide coarse powder with the particle size of 0.5mm, heating to 1000 ℃ under the condition of nitrogen to crack organic matters, wherein the heating rate is 0.1 ℃/min, and preserving heat for 2 hours to obtain the porous silicon carbide/carbon blank.

(c) And carrying out gas-phase siliconizing on the porous silicon carbide/carbon blank, placing the porous silicon carbide/carbon blank on a porous graphite support, placing the porous silicon carbide/carbon blank in a graphite crucible with a boron nitride coating coated on the surface, placing the silicon particles in the graphite crucible, heating under a vacuum condition to melt the silicon particles, generate silicon vapor, uniformly permeate the silicon vapor into the porous silicon carbide/carbon blank, and reacting the silicon vapor with the carbon in the porous silicon carbide/carbon blank to generate silicon carbide to obtain the porous silicon carbide blank. The vacuum degree of the vacuum condition is 0Pa, the particle size of the silicon particles is 5mm, the mass of the silicon particles is 3 times that of the carbon material, the heating temperature is 1550 ℃, the heating rate is preferably 10 ℃/min, and the heat preservation time is preferably 5 h.

(d) And carrying out precursor impregnation cracking densification treatment on the porous silicon carbide blank, placing the porous silicon carbide blank in a precursor solution, vacuumizing to enable the precursor solution to infiltrate into the blank, curing the blank, transferring the blank into a tube furnace, heating to enable the precursor to crack to generate silicon carbide, and obtaining the porous silicon carbide preform with the porosity within the required range. The precursor is polycarbosilane, the heating temperature is 1000 ℃, the heating rate is 0.5 ℃/min, the heating time is 2h, and the porosity of the porous silicon carbide is preferably 65%.

(e) And putting the porous silicon carbide preform into 25% silica sol, soaking for 35min under a vacuum condition, then putting the porous silicon carbide preform soaked with the silica sol into a muffle furnace, heating to 700 ℃, and preserving heat for 60 min.

Example 6

The preparation method of the aluminum-based silicon carbide composite material provided by the embodiment 6 of the invention mainly comprises the following steps:

(a) selecting 70 parts of silicon carbide micro powder, 10 parts of carbon fiber and 20 parts of liquid phenolic resin, preparing composite powder suitable for additive manufacturing by adopting a stirring defoaming method, constructing a three-dimensional model, and spraying and forming a silicon carbide composite material blank body with a required structure by adopting a binder.

(b) And (3) curing the silicon carbide composite material blank at high temperature, placing the silicon carbide composite material blank in an alumina crucible, embedding the silicon carbide composite material blank by using silicon carbide coarse powder with the particle size of 0.5mm, heating to 800 ℃ under the condition of argon to crack an organic matter, and keeping the temperature for 10 hours at the heating rate of 2 ℃/min to obtain the porous silicon carbide/carbon blank.

(c) And (2) leading the porous silicon carbide/carbon blank to enter a liquid phase for siliconizing, covering a layer of graphite paper inside the graphite crucible, placing the porous silicon carbide/carbon blank in the graphite crucible, embedding the porous silicon carbide/carbon blank with silicon particles, heating the porous silicon carbide/carbon blank under a vacuum condition to melt the silicon particles, uniformly impregnating the porous silicon carbide/carbon blank, and reacting the porous silicon carbide/carbon blank with carbon in the porous silicon carbide/carbon blank to generate silicon carbide so as to obtain the porous silicon carbide blank. The vacuum degree under the vacuum condition is 100-200 Pa, the particle size of the silicon particles is 1-5 mm, the mass of the silicon particles is 3-3.5 times of that of the carbon material, the heating temperature is 1450-1600 ℃, the heating rate is 5-20 ℃/min, and the heat preservation time is 0.5-3 h.

(d) And carrying out precursor impregnation cracking densification treatment on the porous silicon carbide blank, placing the porous silicon carbide blank in a precursor solution, vacuumizing to enable the precursor solution to infiltrate into the blank, transferring the blank into a tubular furnace after curing, and heating to enable the precursor to crack to generate silicon carbide so as to obtain the porous silicon carbide preform with the porosity within the required range. The precursor is polycarbosilane, the heating temperature is 1000 ℃, the heating rate is 0.5 ℃/min, the heating time is 2h, and the porosity of the porous silicon carbide is preferably 65%.

(e) And putting the porous silicon carbide preform into 10% silica sol, soaking for 60min under a vacuum condition, then putting the porous silicon carbide preform soaked with the silica sol into a muffle furnace, heating to 900 ℃, and preserving heat for 30 min.

Example 7

The preparation method of the aluminum-based silicon carbide composite material provided by the embodiment 7 of the invention mainly comprises the following steps:

(a) selecting 85 parts of silicon carbide micro powder, 5 parts of graphene and 10 parts of liquid phenolic resin, preparing composite powder suitable for additive manufacturing by adopting a mechanical mixing method, constructing a three-dimensional model, and spray-forming a silicon carbide composite material blank body with a required structure by adopting a binder.

(c) And carrying out liquid phase siliconizing on the porous silicon carbide/carbon blank, covering a layer of graphite paper inside the graphite crucible, placing the porous silicon carbide/carbon blank in the graphite crucible, embedding the porous silicon carbide/carbon blank by using silicon particles with the particle size of 5mm, wherein the mass of the silicon particles is 3 times that of the carbon material, heating the porous silicon carbide/carbon blank to 1600 ℃ at the heating rate of 5 ℃/min under the vacuum degree of 100Pa so as to melt the silicon particles, uniformly impregnating the porous silicon carbide/carbon blank, reacting the porous silicon carbide/carbon blank with carbon in the porous silicon carbide/carbon blank to generate silicon carbide so as to obtain the porous silicon carbide blank, and keeping the temperature for 2 h.

(d) And carrying out precursor impregnation cracking densification treatment on the porous silicon carbide blank, placing the porous silicon carbide blank in a precursor solution, vacuumizing to enable the precursor solution to infiltrate into the blank, transferring the blank into a tubular furnace after curing, and heating to enable the precursor to crack to generate silicon carbide so as to obtain the porous silicon carbide preform with the porosity within the required range. The precursor is polycarbosilane, the heating temperature is 1500 ℃, the heating rate is 0.5 ℃/min, the heating time is 5h, and the porosity of the porous silicon carbide is preferably 50%.

(e) And putting the porous silicon carbide preform into 20% silica sol, soaking for 30min under a vacuum condition, then putting the porous silicon carbide preform soaked with the silica sol into a muffle furnace, heating to 1000 ℃, and preserving heat for 60 min.

Example 8

The preparation method of the aluminum-based silicon carbide composite material provided by the embodiment 8 of the invention mainly comprises the following steps:

(d) And carrying out precursor impregnation cracking densification treatment on the porous silicon carbide blank, placing the silicon carbide blank in a precursor solution, vacuumizing to enable the precursor solution to infiltrate into the blank, transferring the blank into a tubular furnace after curing, and heating to enable the precursor to crack to generate silicon carbide so as to obtain the porous silicon carbide preform with the porosity within the required range. The precursor is polycarbosilane, the heating temperature is 1500 ℃, the heating rate is 0.5 ℃/min, the heating time is 5h, and the porosity of the porous silicon carbide preform is preferably 50%.

(e) And putting the porous silicon carbide preform into silica sol with the concentration of 30%, soaking for 20min under a vacuum condition, then putting the porous silicon carbide preform soaked with the silica sol into a muffle furnace, heating to 1100 ℃, and preserving heat for 75 min.

Example 9

The preparation method of the aluminum-based silicon carbide composite material provided by the embodiment 9 of the invention mainly comprises the following steps:

(a) selecting 85 parts of silicon carbide micro powder, 5 parts of spherical graphite and 10 parts of liquid phenolic resin, preparing composite powder suitable for additive manufacturing by adopting a mechanical mixing method, constructing a three-dimensional model, and forming a silicon carbide composite material blank body with a required structure by adopting directional energy deposition.

(b) And (2) curing the silicon carbide composite material blank at high temperature, placing the silicon carbide composite material blank in an alumina crucible, embedding the silicon carbide composite material blank by using silicon carbide coarse powder with the particle size of 1mm, heating to 800 ℃ under the condition of nitrogen to crack organic matters, wherein the heating rate is 1 ℃/min, and the temperature is kept for 5 hours to obtain the porous silicon carbide/carbon blank.

(c) And carrying out liquid phase siliconizing on the porous silicon carbide/carbon blank, covering a layer of graphite paper inside the graphite crucible, placing the porous silicon carbide/carbon blank in the graphite crucible, embedding the porous silicon carbide/carbon blank by using silicon particles with the particle size of 5mm, wherein the mass of the silicon particles is 3.5 times that of the carbon material, heating the porous silicon carbide/carbon blank to 1600 ℃ at the heating rate of 10 ℃/min under the vacuum degree of 100Pa so as to melt the silicon particles, uniformly impregnating the porous silicon carbide/carbon blank, reacting the silicon particles with carbon in the porous silicon carbide/carbon blank to generate silicon carbide so as to obtain a silicon carbide blank, and keeping the temperature for 2 h.

(d) And carrying out precursor impregnation cracking densification treatment on the porous silicon carbide blank, placing the silicon carbide blank in a precursor solution, vacuumizing to enable the precursor solution to infiltrate into the blank, transferring the blank into a tubular furnace after curing, and heating to enable the precursor to crack to generate silicon carbide so as to obtain the porous silicon carbide preform with the porosity within the required range. The precursor is polycarbosilane, the heating temperature is 1500 ℃, the heating rate is 5 ℃/min, the heating time is 3h, and the porosity of the porous silicon carbide is preferably 45%.

(e) And putting the porous silicon carbide preform into 20% silica sol, soaking for 30min under a vacuum condition, then putting the porous silicon carbide preform soaked with the silica sol into a muffle furnace, heating to 900 ℃, and preserving heat for 60 min.

(f) And (2) carrying out aluminum alloy infiltration on the porous preform, placing the porous silicon carbide in a crucible resistance furnace, adding a proper amount of aluminum-silicon alloy ingot/particle with the mass 1 time that of the porous silicon carbide, introducing protective gas, heating to 700 ℃ at the heating rate of 10 ℃/min to melt the aluminum alloy, vacuumizing to 0Pa, maintaining the pressure for 15min, introducing inert gas to pressurize to 0.5MPa, maintaining the pressure for 30min, and finally, releasing the pressure and cooling along with the furnace to obtain the aluminum-based silicon carbide composite material.

The relationship between the porosity and the volume fraction of the aluminum alloy of the preform and the concentration of the impregnation solution is shown in table 1, and the relationship between the porosity and the volume fraction of the aluminum alloy of the preform and the number of times of impregnation is shown in table 2.

TABLE 1

TABLE 2

It will be understood by those skilled in the art that the foregoing is only a preferred embodiment of the present invention, and is not intended to limit the invention, and that any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the scope of the present invention.

Claims

1. The preparation method of the aluminum-based silicon carbide composite material is characterized by comprising the following steps of:

2. The method of preparing an aluminum-based silicon carbide composite material according to claim 1, wherein: the reaction sintering adopts liquid phase siliconizing or gas phase siliconizing; the silicon carbide densification treatment adopts chemical vapor infiltration or precursor impregnation cracking; and the aluminum alloy liquid infiltration adopts pressureless infiltration, vacuum infiltration or pressure infiltration.

3. The method of preparing an aluminum-based silicon carbide composite material according to claim 1, wherein: the silicon carbide material is one or more of silicon carbide micro powder, chopped silicon carbide fiber, silicon carbide whisker and silicon carbide nanowire; the carbon material is one or more of spherical graphite, flake graphite, diamond micro powder, graphene and carbon fiber; the resin is epoxy resin powder, phenolic resin powder, nylon powder, liquid phenolic resin or liquid photosensitive resin.

4. The method of preparing an aluminum-based silicon carbide composite material according to claim 1, wherein: in the step (1), the silicon carbide material, the carbon material and the resin are 55-85 parts, 5-25 parts and 10-20 parts respectively.

5. The method of preparing an aluminum-based silicon carbide composite material according to claim 1, wherein: the additive manufacturing technique is stereolithography, powder bed melting, material extrusion, directed energy deposition, adhesive jetting, or thin-sheet lamination.

6. The method of preparing an aluminum-based silicon carbide composite material according to claim 1, wherein: the porosity of the porous silicon carbide/carbon blank is 60-65%.

7. The method of preparing an aluminum-based silicon carbide composite material according to claim 1, wherein: in the step (3), the reaction sintering adopts gas-phase siliconizing, the gas-phase siliconizing is carried out in vacuum or protective atmosphere, the protective atmosphere is one or more of nitrogen, argon and helium, the vacuum degree is-100 Pa, the gas-phase siliconizing temperature is 1550-1700 ℃, the temperature rise rate of the gas-phase siliconizing is 5-15 ℃/min, and the gas-phase siliconizing time is 0.5-5 h.

8. The method of producing an aluminum-based silicon carbide composite material according to any one of claims 1 to 7, wherein: the porosity of the porous silicon carbide preform is 30-65%.

9. The method of producing an aluminum-based silicon carbide composite material according to any one of claims 1 to 7, wherein: in the step (5), the porous silicon carbide preform is placed into silica sol with the concentration of 10% -30%, and is soaked for 15 min-60 min under the vacuum condition, then the porous silicon carbide preform soaked with the silica sol is placed into a muffle furnace, and is heated to 600-1200 ℃, and the temperature is kept for 30 min-120 min.

10. An aluminum-based silicon carbide composite material is characterized in that: the aluminum-based silicon carbide composite material is prepared by the preparation method of the aluminum-based silicon carbide composite material according to any one of claims 1 to 9.