CN116425548A - Adhesive jet printing silicon carbide ceramic composite material based on particle-size distribution powder and preparation method thereof - Google Patents
Adhesive jet printing silicon carbide ceramic composite material based on particle-size distribution powder and preparation method thereof Download PDFInfo
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Abstract
The invention relates to a binder jet printing silicon carbide ceramic composite material based on particle-grade powder and a preparation method thereof. The preparation method comprises the following steps: respectively mixing silicon carbide powder with the median diameter of 20 mu m, silicon carbide powder with the median diameter of 5 mu m, silicon carbide powder with the median diameter of 10 mu m, silicon carbide powder with the median diameter of 50 mu m and silicon carbide powder with the median diameter of 80 mu m to obtain composite powder; wherein, the mass ratio of the silicon carbide powder with the median diameter of 20 mu m, the median diameter of 5 mu m, the median diameter of 10 mu m, the median diameter of 50 mu m and the median diameter of 80 mu m is 150 (50-60): 50-60; spraying and printing the composite powder with a binder to obtain a ceramic blank; debonding the ceramic blank to obtain a ceramic biscuit; and performing reaction sintering siliconizing treatment on the ceramic biscuit to obtain the silicon carbide ceramic composite material.
Description
Technical Field
The invention belongs to the technical field of preparation of silicon carbide ceramic materials, and particularly relates to a binder jet printing silicon carbide ceramic composite material based on particle-grade powder modification and a preparation method thereof.
Background
The silicon carbide ceramic has the characteristics of high strength, high hardness, high thermal shock resistance, low thermal expansion and the like, and has wide application value in the fields of national defense, military industry and aerospace, such as microreactors, pressure-resistant shells, optical components, nuclear energy application and the like. However, the silicon carbide ceramic has low fracture reliability, so that the application range is limited, and the preparation of the special-shaped structure with the complex shape is particularly limited. Along with the development of scientific technology, the traditional ceramic forming process such as slip casting, dry pressing and the like has the defects of single shape, higher cost and the like, and is difficult to realize high-precision rapid precision processing of the special-shaped silicon carbide ceramic composite material with geometric complexity, and the requirements of modern space technology cannot be met. Aiming at the defects, the silicon carbide ceramic composite material based on the 3D printing rapid prototyping technology becomes the current research hot spot direction, and is based on a three-dimensional model, powder raw materials are processed layer by layer and stacked to be shaped through program control of a computer system, and finally a three-dimensional entity is manufactured. Compared with the traditional material reduction manufacturing technology, the material reduction manufacturing method has the advantages of integration, rapidness, individuation and the like, saves raw materials, and is widely applied to the fields of bioengineering, industrial equipment, transportation and the like.
Adhesive jet printing (BJ) is used as a novel additive manufacturing mode and is suitable for manufacturing high-precision complex components by almost all powders (metals, ceramics and polymers). The adhesive is sprayed on the surface of the powder through a nozzle, a new layer of powder is paved on a roller, and the bonding process is repeated layer by layer. Compared with Fused Deposition Modeling (FDM), the method has the advantages of high molding precision, high printing speed and the like; compared with light curing molding (SL), the method has the advantages of lower requirements on powder and binder, and the like; compared with laser selective sintering (SLS), the method has the advantages of lower equipment requirement, higher molding precision and the like; compared with the direct writing molding technology (DIW), the method has the advantages that a blank is not easy to crack in the curing process, and the like. BJ is an important way for molding silicon carbide ceramic composite materials with high precision and complex shapes.
For BJ, powder-spreading molding technology, powder flowability is an important factor affecting the performance of molded test pieces. Chinese patent CN202210319685 discloses a silicon carbide/carbon/chopped carbon fiber composite powder with good fluidity obtained by ball milling, drying or spray granulation, and a high-density silicon carbide ceramic composite material obtained by degreasing and siliconizing a BJ formed ceramic biscuit. The method is characterized in that BJ paste-spreading type printing is adopted, so that the paste preparation steps are complicated, a series of factors such as paste viscosity, solid content and the like need to be considered, and the method is not friendly for rapid forming. Chinese patent CN202210900589 discloses a composite powder obtained by preparing a slurry from a carbonaceous powder, drying or spray granulating, forming a print biscuit by BJ, de-binding, impregnating, solidifying, cracking, and finally siliconizing to obtain a silicon carbide ceramic material with higher performance. The chopped carbon fiber powder is a rod-shaped cylindrical particle, and because of the large shearing force and plane contact points between the particles, the flowability of the chopped carbon fiber powder is poorer than that of the nearly spherical silicon carbide particles, and the chopped carbon fiber powder is used as an important filler for preparing high-performance ceramics, and can reduce the flowability of composite powder after being mixed with a silicon carbide matrix in the 3D printing process, and has a certain influence on the porosity of the material, so that the silicon carbide powder is required to be treated to improve the flowability of the silicon carbide powder.
Disclosure of Invention
Aiming at the problems in the prior art, the invention adopts orthogonal experimental design optimization to obtain the optimal fluidity of silicon carbide powder with different particle size fractions, and provides a binder jet printing silicon carbide ceramic composite material based on the particle size fraction powder and a preparation method thereof.
In a first aspect, the present invention provides a method for preparing a silicon carbide ceramic composite material, comprising:
(1) Mixing silicon carbide powder with a median diameter of 20 mu m, silicon carbide powder with a median diameter of 5 mu m, silicon carbide powder with a median diameter of 10 mu m, silicon carbide powder with a median diameter of 50 mu m and silicon carbide powder with a median diameter of 80 mu m respectively to obtain composite powder; preferably, the mass ratio of the silicon carbide powder with the median diameter of 20 mu m, the silicon carbide powder with the median diameter of 5 mu m, the silicon carbide powder with the median diameter of 10 mu m, the silicon carbide powder with the median diameter of 50 mu m and the silicon carbide powder with the median diameter of 80 mu m is 150 (50-60): 50-60;
(2) Spraying and printing the composite powder with a binder to obtain a ceramic blank;
(3) Debonding the ceramic blank to obtain a ceramic biscuit;
(4) And performing reaction sintering siliconizing treatment on the ceramic biscuit to obtain the silicon carbide ceramic composite material.
Preferably, the mixing mode is roller ball milling, the rotating speed is 50-70 revolutions per minute, the ball-to-material ratio is 1.5-2:1, and the ball milling time is 1-1.5 h.
Preferably, the bulk density of the composite powder is 1.01-1.15g/cm 3 Tap density of 1.50-1.61g/cm 3 The Calf index is 27.20-35.30, and the Haoshan ratio is 1.28-1.68.
Preferably, the parameters of the adhesive jet printing are as follows: the powder scattering speed is 10-50 mm/s, the printing layer thickness is 20-50 mu m, the roller rotating speed is 300-400 rpm, the base layer for paving powder before printing is set to 15-20 layers, the heater sweeping speed is 15-30 mm/s, and the drainage oscillator speed is 2600-3000 rpm.
Preferably, the spray binder used for the spray printing of the binder is an aqueous organic binder with the saturation of 70-75%, and the spray binder comprises ethylene glycol, ethylene glycol monobutyl ether and phenolic resin.
Preferably, the debonding temperature is 900-1000 ℃ and the debonding time is 9-10h; the porosity of the ceramic body after the debonding is controlled to be 50 to 70 percent and the density is controlled to be 0.98 to 1.22g/cm 3 。
Preferably, the mass ratio of the silicon powder to the ceramic biscuit in the siliconizing sintering is 1-1.2:1.5-2; the siliconizing sintering temperature is 1500-1600 ℃, and the siliconizing sintering time is 4-5h.
Preferably, the preparation method further comprises at least one impregnation and cracking of the ceramic biscuit between debinding and siliconizing sintering; the density of the ceramic biscuit after the dipping and cracking treatment is controlled to be 1.73-2.22 g/cm 3 The bending strength is 3.59-19.24 MPa.
In a second aspect, the invention provides a silicon carbide ceramic composite material obtained by the preparation method, wherein the bending strength of the silicon carbide ceramic composite material is 235-312MPa, the elastic modulus is 216-301GPa, and the fracture toughness is 1.74-2.96 MPa-m 1/2 The density is 97-99%.
The beneficial effects are that:
(1) According to the invention, the composite powder with good fluidity and different particle sizes is obtained through ball milling by orthogonal experimental design, and the composite powder with excellent performance is prepared, so that the binder is favorable for jet printing to obtain ceramic biscuit with uniform pore distribution, and the subsequent reaction siliconizing process is favorable for obtaining silicon carbide ceramic with better performance;
(2) The carbon content of the biscuit is improved through dipping and cracking treatment, and the silicon carbide ceramic composite material with high density is obtained through reaction sintering in a high-temperature vacuumizing environment.
Drawings
FIG. 1 is a schematic diagram of the flowability test of the composite powder in example 1;
FIG. 2 is an SEM image of the polished surface of the silicon carbide ceramic composite prepared in example 1;
FIG. 3 is an SEM image of the polished surface of the silicon carbide ceramic composite prepared in example 3;
FIG. 4 is a schematic diagram showing powder flowability test in comparative example 1;
fig. 5 is an SEM image of the polished surface of the silicon carbide ceramic composite prepared in comparative example 1.
Detailed Description
The invention is further illustrated by the following embodiments, it being understood that the following embodiments are merely illustrative of the invention and not limiting thereof.
In the invention, different grain-size silicon carbide is taken as an investigation factor, a Carr Index and a Hausner ratio are taken as evaluation indexes, and the powder is screened by adopting an orthogonal experiment method. The method comprises the steps of selecting silicon carbide powder with better flow as a reference, taking other powder with grain size as a variable factor, measuring repose angle, bulk density and tap density of the powder by adopting a HYL-1001 type powder comprehensive property tester according to a bulk density measuring method specified in GB/T16913.3-2008 (measurement of bulk density by a natural stacking method) and a tap density measuring method specified in ASTM D6393-99 standard (Karl index), and obtaining the Karl index and Haoshanover of the composite powder according to an evaluation formula of the Karl index and the Haoshanover. Wherein, the smaller the Cal index and the Haoshan ratio, the better the fluidity, the fluidity of each group of powder is measured to obtain the powder mixture ratio with the optimal fluidity. BJ printing is carried out on the powder with different granularity before and after the grain composition, and after-treatment such as debonding and siliconizing is carried out on the printed piece, so that the silicon carbide ceramic composite material with excellent mechanical property can be obtained.
Hereinafter, a method for preparing the silicon carbide ceramic composite material provided by the present invention is exemplified, and the method may include the following steps.
And (5) batching. Silicon carbide powder having a median diameter of 20 [ mu ] m (particle size range may be 15-25 [ mu ] m), silicon carbide powder having a median diameter of 5 [ mu ] m (particle size range may be 2-8 [ mu ] m), silicon carbide powder having a median diameter of 10 [ mu ] m (particle size range may be 8-15 [ mu ] m), silicon carbide powder having a median diameter of 50 [ mu ] m (particle size range may be 30-60 [ mu ] m), and silicon carbide powder having a median diameter of 80 [ mu ] m (particle size range may be 70-100 [ mu ] m) were separately taken, and put into a ball mill grinding pot to be ball-milled, to obtain a uniformly mixed composite powder. Wherein the mass ratio of the silicon carbide powder with the median diameter of 20 mu m, the silicon carbide powder with the median diameter of 5 mu m, the silicon carbide powder with the median diameter of 10 mu m, the silicon carbide powder with the median diameter of 50 mu m and the silicon carbide powder with the median diameter of 80 mu m can be 150 (50-60): 50-60.
The Particle Size Distribution (PSD) of the raw materials is regulated and controlled by a particle grading method, small particles fill gaps among large particles, and the particle size distribution is an important way for obtaining a biscuit with lower porosity, is convenient for efficient forming, and affects the post-treatment densification sintering step. The Furnace theory is a typical discontinuous size particle packing theory that considers that the closest packing is formed when small particles just fill the interstices of large particles. If there are 3 kinds of particles, the medium particles should be just filled in the gaps of the coarse particles, and the fine particles should be filled in the gaps of the medium and coarse particles, thus being promoted to the case of particles of various sizes. The layer thickness for 3D printing is generally controlled between 0 and 100 μm, which requires that the powder particle size be selected not to be greater than 100 μm, which would otherwise lead to reduced print quality, subject to the influence of 3D printing equipment and the basis of existing research. The stacking of particles with various sizes is significant for the regulation and control of the mechanical properties of ceramics, and the invention adopts five particle sizes: 3 sizes of granularity regulation and control in a Furnace theory are carried out by taking medium diameters of 5 and 10 mu m as small particles, 20 mu m as medium particles and 50 and 80 mu m as large particles, and powder with good stacking property and fluidity is prepared by mixing, so as to meet the requirements of different fields on different performances of ceramics.
In some embodiments, the ball milling is roller milling, the rotational speed may be 50-70 revolutions per minute, the ball-to-material ratio may be 1.5-2:1, and the ball milling time may be 1-1.5 hours. The powder is smashed when the ball-material ratio is too large and the ball milling time is too long, so that the particle size of the composite powder is affected, and the later-stage formed powder is too thin to be printed successfully; otherwise, uneven mixing can be caused, and a clamping phenomenon can occur.
In some embodiments, the bulk density of the composite powder may be controlled to be 1.01-1.15g/cm 3 Tap density of 1.50-1.61g/cm 3 The Calf index is 27.20-35.30, and the Haoshan ratio is 1.28-1.68. Preferably, the bulk density of the composite powder is 1.01-1.15g/cm 3 The tap density is 1.50-1.6g/cm 3 The Cal index is 27.80-34.94, and the Haoshan ratio is 1.38-1.59. The powder under the fluidity parameters can ensure certain compressionThe flowability and flowability are beneficial to the powder flowing state during powder paving and the powder compaction after particle grading. The excessive Karl index can lead to the reduction of the compactibility of the powder during the grading process, so that the porosity is too high; the Carl index is too small, the powder fluidity is improved, the pressing performance is reduced, and the quality of the biscuit and the performance of the ceramic after sintering are finally affected.
Printing a blank. And (3) performing binder jet printing on the composite powder to obtain a ceramic blank.
In some embodiments, the parameters of the adhesive jet printing may be: the powder scattering speed is 10-50 mm/s, the printing layer thickness is 20-50 mu m, the roller rotating speed is 300-400 rpm, the base layer for paving powder before printing is set to 15-20 layers, the heater sweeping speed is 15-30 mm/s, and the drainage oscillator speed is 2600-3000 rpm.
In some embodiments, the spray adhesive used for adhesive spray printing is an aqueous organic adhesive, and the components of the spray adhesive may include ethylene glycol, ethylene glycol monobutyl ether, and phenolic resin. The binder of this type is suitable for printing high temperature materials including nonmetallic materials such as carbon, tungsten carbide, silicon carbide and other ceramics, and has a saturation of 70-75%.
The spray binder is an organic binder, and can provide more carbon sources for sintering described later. Too low a saturation of the binder may result in poor adhesion between the powders, and thus the performance of the test piece may be degraded; too high a saturation of the binder and too high a viscosity can cause nozzle clogging, affecting printing efficiency.
And (5) debonding. And (3) performing de-bonding treatment on the ceramic blank at high temperature to obtain a ceramic biscuit.
In some embodiments, the debonding temperature may be 900 to 1000 ℃ and the debonding time may be 9 to 10 hours; the porosity of the ceramic body after the debonding is controlled to be 50 to 70 percent and the density is controlled to be 0.98 to 1.22g/cm 3 . The porosity of the ceramic body after the debonding is maintained between 50 and 70 percent, which is beneficial to obtaining silicon carbide ceramics used in various fields through the subsequent siliconizing process.
Siliconizing and sintering. And (3) performing reaction sintering siliconizing treatment on the ceramic biscuit to obtain the high-density silicon carbide ceramic composite material.
In some embodiments, the mass ratio of the silicon powder to the ceramic biscuit in the siliconizing sintering can be controlled to be 1-1.2:1.5-2.
In some embodiments, the siliconizing sintering temperature may be 1500-1600 ℃ and the siliconizing sintering time may be 4-5 hours.
Densification is realized by adopting a reaction infiltration mode, and silicon is melted and infiltrated into sample pores and can react with carbon to generate silicon carbide.
In some embodiments, at least one impregnation cracking can be performed on the ceramic biscuit between the debinding and siliconizing sintering, and a carbon source can be provided for the densification process of the biscuit through the impregnation cracking, so that the pre-densification effect is achieved, the performance of the sintered part is promoted, and the highly-dense silicon carbide ceramic composite material is obtained.
Wherein, the dipping and cracking process can be as follows: preparing phenolic resin powder and ethanol solution into impregnating solution according to the mass ratio of 1:1, soaking the debonded biscuit in the impregnating solution, vacuumizing, putting into a 120 ℃ oven, drying for 6 hours to obtain a preform, and then continuing debonding, wherein the debonding process is consistent with the debonding process.
In some embodiments, the density of the ceramic greenware after the dip cracking treatment can be controlled to be 1.73-2.22 g/cm 3 The bending strength is 3.59-19.24 MPa.
The invention improves the flow characteristic of the composite powder as a whole after optimizing through grading composition, and the density of the printed biscuit is improved through stacking of various grading powder, thereby improving the density of the de-bonded green body and being beneficial to sintering densification of the silicon carbide material. Meanwhile, through the means of grain composition, the combination of a plurality of grains with different diameters can also improve the sintering driving force in the siliconizing sintering densification stage, thereby more effectively promoting densification and improving the performance of the final sintered body.
The silicon carbide ceramic composite material prepared by the method has the bending strength of 235-312MPa, the elastic modulus of 216-301GPa and the fracture toughness of 1.74-2.96 MPa.m 1/2 The density is 97-99％。
The present invention will be described in more detail by way of examples. It should also be understood that the following examples are given by way of illustration only and are not to be construed as limiting the scope of the invention, since various insubstantial modifications and adaptations of the invention to those skilled in the art based on the foregoing disclosure are intended to be within the scope of the invention and the specific process parameters and the like set forth below are merely one example of a suitable range within which one skilled in the art would choose from the description herein without being limited to the specific values set forth below.
Example 1
Weighing 150g of silicon carbide with the particle size of 20 mu m, 55g of silicon carbide with the particle size of 5 mu m, 60g of silicon carbide with the particle size of 10 mu m, 50g of silicon carbide with the particle size of 50 mu m and 55g of silicon carbide with the particle size of 80 mu m, putting the silicon carbide with the particle size of 55g, 5 mu m and 60g of silicon carbide with the particle size of 50 mu m into a grinding tank of a ball mill, ball-milling the silicon carbide with the particle size of 1.5:1 for 1.5 hours to obtain uniformly mixed composite powder, measuring the bulk density and tap density of the composite powder by using a powder physical property tester, and calculating the Karl index and Hairyranafar.
Adopting adhesive jet printing, selecting an adhesive with the saturation degree of 75%, setting printing parameters, wherein the thickness of a printing layer is 50 mu m, the powder dispersing speed is 50mm/s, the rotating speed of a roller is 300rpm/min, the basic layer for paving powder before printing is 20 layers, the transverse sweeping speed of a heater is 30mm/s, the speed of a drainage oscillator is 2600rpm/min, and printing to obtain a silicon carbide ceramic blank.
High Wen Tuonian at 900 ℃, carrying out dipping treatment by using phenolic resin ethanol solution according to the mass ratio of 1:1, and then carrying out debonding to obtain a biscuit;
siliconizing at 1550 ℃ to obtain the high-density silicon carbide ceramic composite material, and testing the mechanical property of the composite material.
FIG. 1 is a schematic diagram of the flowability test of the composite powder in example 1.
Fig. 2 is an SEM image of the polished surface of the silicon carbide ceramic composite prepared in example 1.
Example 2
Weighing 150g of 20 mu m silicon carbide, 55g of 5 mu m silicon carbide, 60g of 10 mu m silicon carbide, 50g of 50 mu m silicon carbide and 50g of 80 mu m silicon carbide; putting the powder into a grinding tank of a ball mill according to a ball-material ratio of 1.5:1, performing ball milling for 1.5 hours to obtain uniformly mixed composite powder, measuring the bulk density and tap density of the composite powder by using a powder physical property tester, and calculating a Karl index and a Hawsonia ratio.
Adopting adhesive jet printing, selecting an adhesive with the saturation degree of 75%, setting printing parameters, wherein the thickness of a printing layer is 50 mu m, the powder dispersing speed is 50mm/s, the rotating speed of a roller is 300rpm/min, the basic layer for paving powder before printing is 20 layers, the transverse sweeping speed of a heater is 30mm/s, the speed of a drainage oscillator is 2600rpm/min, and printing to obtain a silicon carbide ceramic blank.
Performing high-temperature de-bonding at 900 ℃, performing impregnation treatment by using a phenolic resin ethanol solution according to a mass ratio of 1:1, and performing de-bonding to obtain a biscuit;
siliconizing at 1550 ℃ to obtain the high-density silicon carbide ceramic composite material, and testing the mechanical property of the composite material.
Example 3
Weighing 150g of 20 mu m silicon carbide, 55g of 5 mu m silicon carbide, 60g of 10 mu m silicon carbide, 50g of 50 mu m silicon carbide and 60g of 80 mu m silicon carbide; putting the powder into a grinding tank of a ball mill according to a ball-material ratio of 1.5:1, performing ball milling for 1.5 hours to obtain uniformly mixed composite powder, measuring the bulk density and tap density of the composite powder by using a powder physical property tester, and calculating a Karl index and a Hawsonia ratio.
Adopting adhesive jet printing, selecting an adhesive with the saturation degree of 75%, setting printing parameters, wherein the thickness of a printing layer is 50 mu m, the powder dispersing speed is 50mm/s, the rotating speed of a roller is 300rpm/min, the basic layer for paving powder before printing is 20 layers, the transverse sweeping speed of a heater is 30mm/s, the speed of a drainage oscillator is 2600rpm/min, and printing to obtain a silicon carbide ceramic blank.
And (3) performing high-temperature de-bonding at 900 ℃, performing impregnation treatment by using a phenolic resin ethanol solution according to a mass ratio of 1:1, and performing de-bonding to obtain a biscuit.
Siliconizing at 1550 ℃ to obtain the high-density silicon carbide ceramic composite material, and testing the mechanical property of the composite material.
Fig. 3 is an SEM image of the polished surface of the silicon carbide ceramic composite material prepared in example 3.
Example 4
Weighing 150g of 20 mu m silicon carbide, 60g of 5 mu m silicon carbide, 55g of 10 mu m silicon carbide, 50g of 50 mu m silicon carbide and 60g of 80 mu m silicon carbide, putting into a ball mill grinding tank, ball milling for 1.5 hours according to a ball-material ratio of 1.5:1, obtaining uniformly mixed composite powder, measuring the bulk density and tap density of the composite powder by using a powder physical property tester, and calculating the Karl index and Hawsonia ratio.
Adopting adhesive jet printing, selecting an adhesive with the saturation degree of 75%, setting printing parameters, wherein the thickness of a printing layer is 50 mu m, the powder dispersing speed is 50mm/s, the rotating speed of a roller is 300rpm/min, the basic layer for paving powder before printing is 20 layers, the transverse sweeping speed of a heater is 30mm/s, the speed of a drainage oscillator is 2600rpm/min, and printing to obtain a silicon carbide ceramic blank.
And (3) performing high-temperature de-bonding at 900 ℃, performing impregnation treatment by using a phenolic resin ethanol solution according to a mass ratio of 1:1, and performing de-bonding to obtain a biscuit.
Siliconizing at 1550 ℃ to obtain the high-density silicon carbide ceramic composite material, and testing the mechanical property of the composite material.
Example 5
Weighing 150g of 20 mu m silicon carbide, 60g of 5 mu m silicon carbide, 60g of 10 mu m silicon carbide, 55g of 50 mu m silicon carbide and 50g of 80 mu m silicon carbide, putting into a ball mill grinding tank, ball milling for 1.5 hours according to a ball-material ratio of 1.5:1, obtaining uniformly mixed composite powder, measuring the bulk density and tap density of the composite powder by using a powder physical property tester, and calculating the Karl index and Hawsonia ratio.
Adopting adhesive jet printing, selecting an adhesive with the saturation degree of 75%, setting printing parameters, wherein the thickness of a printing layer is 50 mu m, the powder dispersing speed is 50mm/s, the rotating speed of a roller is 300rpm/min, the basic layer for paving powder before printing is 20 layers, the transverse sweeping speed of a heater is 30mm/s, the speed of a drainage oscillator is 2600rpm/min, and printing to obtain a silicon carbide ceramic blank.
And (3) performing high-temperature de-bonding at 900 ℃, performing impregnation treatment by using a phenolic resin ethanol solution according to a mass ratio of 1:1, and performing de-bonding to obtain a biscuit.
Siliconizing at 1550 ℃ to obtain the high-density silicon carbide ceramic composite material, and testing the mechanical property of the composite material.
Example 6
Weighing 150g of 20 mu m silicon carbide, 55g of 5 mu m silicon carbide, 60g of 10 mu m silicon carbide, 50g of 50 mu m silicon carbide and 55g of 80 mu m silicon carbide, putting into a ball mill grinding tank, ball milling for 1.5 hours according to a ball-material ratio of 1.5:1, obtaining uniformly mixed composite powder, measuring the bulk density and tap density of the composite powder by using a powder physical property tester, and calculating the Karl index and Hawsonia ratio.
Adopting adhesive jet printing, selecting an adhesive with the saturation degree of 75%, setting printing parameters, wherein the thickness of a printing layer is 40 mu m, the powder dispersing speed is 50mm/s, the rotating speed of a roller is 300rpm/min, the basic layer for paving powder before printing is 20 layers, the transverse sweeping speed of a heater is 30mm/s, the speed of a drainage oscillator is 2600rpm/min, and printing to obtain a silicon carbide ceramic blank.
And (3) performing high-temperature de-bonding at 900 ℃, performing impregnation treatment by using a phenolic resin ethanol solution according to a mass ratio of 1:1, and performing de-bonding to obtain a biscuit.
Siliconizing at 1550 ℃ to obtain the high-density silicon carbide ceramic composite material, and testing the mechanical property of the composite material.
Example 7
Weighing 150g of 20 mu m silicon carbide, 55g of 5 mu m silicon carbide, 60g of 10 mu m silicon carbide, 50g of 50 mu m silicon carbide and 55g of 80 mu m silicon carbide, putting into a ball mill grinding tank, ball milling for 1.5 hours according to a ball-material ratio of 1.5:1, obtaining uniformly mixed composite powder, measuring the bulk density and tap density of the composite powder by using a powder physical property tester, and calculating the Karl index and Hawsonia ratio.
Adopting adhesive jet printing, selecting an adhesive with the saturation degree of 75%, setting printing parameters, wherein the thickness of a printing layer is 30 mu m, the powder dispersing speed is 50mm/s, the rotating speed of a roller is 300rpm/min, the basic layer for paving powder before printing is 20 layers, the transverse sweeping speed of a heater is 30mm/s, the speed of a drainage oscillator is 2600rpm/min, and printing to obtain a silicon carbide ceramic blank.
And (3) performing high-temperature de-bonding at 900 ℃, performing impregnation treatment by using a phenolic resin ethanol solution according to a mass ratio of 1:1, and performing de-bonding to obtain a biscuit.
Siliconizing at 1550 ℃ to obtain the high-density silicon carbide ceramic composite material, and testing the mechanical property of the composite material.
Example 8
Weighing 150g of 20 mu m silicon carbide, 55g of 5 mu m silicon carbide, 60g of 10 mu m silicon carbide, 50g of 50 mu m silicon carbide and 55g of 80 mu m silicon carbide, putting into a ball mill grinding tank, ball milling for 1.5 hours according to a ball-material ratio of 1.5:1, obtaining uniformly mixed composite powder, measuring the bulk density and tap density of the composite powder by using a powder physical property tester, and calculating the Karl index and Hawsonia ratio.
Adopting adhesive jet printing, selecting an adhesive with 75% of non-saturation degree, setting printing parameters, wherein the thickness of a printing layer is 20 mu m, the powder dispersing speed is 50mm/s, the rotating speed of a roller is 300rpm/min, the powder spreading base layer before printing is 20 layers, the transverse sweeping speed of a heater is 30mm/s, the speed of a drainage oscillator is 2600rpm/min, and printing to obtain a silicon carbide ceramic blank.
And (3) performing high-temperature de-bonding at 900 ℃, performing impregnation treatment by using a phenolic resin ethanol solution according to a mass ratio of 1:1, and performing de-bonding to obtain a biscuit.
Siliconizing at 1550 ℃ to obtain the high-density silicon carbide ceramic composite material, and testing the mechanical property of the composite material.
Comparative example 1
300g of silicon carbide powder with the median diameter of 20 mu m is weighed, the bulk density and the tap density of the powder are measured by a powder physical property tester, and the Cal index and the Hawsonia ratio are calculated.
Adopting adhesive jet printing, selecting an adhesive with the saturation degree of 75%, setting printing parameters, wherein the thickness of a printing layer is 50 mu m, the powder dispersing speed is 50mm/s, the rotating speed of a roller is 300rpm/min, the basic layer for paving powder before printing is 20 layers, the transverse sweeping speed of a heater is 30mm/s, the speed of a drainage oscillator is 2600rpm/min, and printing to obtain a silicon carbide ceramic blank.
And (3) performing high-temperature de-bonding at 900 ℃, performing impregnation treatment by using a phenolic resin ethanol solution according to a mass ratio of 1:1, and performing de-bonding to obtain a biscuit.
Siliconizing at 1550 ℃ to obtain the high-density silicon carbide ceramic composite material, and testing the mechanical property of the composite material.
FIG. 4 is a schematic diagram showing the powder flowability test in comparative example 1.
Fig. 5 is an SEM image of the polished surface of the silicon carbide ceramic composite prepared in comparative example 1.
Comparative example 2
300g of silicon carbide powder with the median diameter of 50 mu m is weighed, the bulk density and the tap density of the powder are measured by a powder physical property tester, and the Karl index and the Hawsonia ratio are calculated.
Adopting adhesive jet printing, selecting an adhesive with the saturation degree of 75%, setting printing parameters, wherein the thickness of a printing layer is 50 mu m, the powder dispersing speed is 50mm/s, the rotating speed of a roller is 300rpm/min, the basic layer for paving powder before printing is 20 layers, the transverse sweeping speed of a heater is 30mm/s, the speed of a drainage oscillator is 2600rpm/min, and printing to obtain a silicon carbide ceramic blank.
And (3) performing high-temperature de-bonding at 900 ℃, performing impregnation treatment by using a phenolic resin ethanol solution according to a mass ratio of 1:1, and performing de-bonding to obtain a biscuit.
Siliconizing at 1550 ℃ to obtain the high-density silicon carbide ceramic composite material, and testing the mechanical property of the composite material.
Comparative example 3
Weighing 150g of 20 mu m silicon carbide, 55g of 5 mu m silicon carbide, 60g of 10 mu m silicon carbide, 50g of 50 mu m silicon carbide and 0g of 80 mu m silicon carbide, putting into a ball mill grinding tank, ball milling for 1.5 hours according to a ball-material ratio of 1.5:1, obtaining uniformly mixed composite powder, measuring the bulk density and tap density of the composite powder by using a powder physical property tester, and calculating the Karl index and Hawster, wherein the composite powder of the formula has relatively poor compactibility and is unfavorable for improving the performance of the formed biscuit.
Adopting adhesive jet printing, selecting an adhesive with the saturation degree of 75%, setting printing parameters, wherein the thickness of a printing layer is 50 mu m, the powder dispersing speed is 50mm/s, the rotating speed of a roller is 300rpm/min, the basic layer for paving powder before printing is 20 layers, the transverse sweeping speed of a heater is 30mm/s, the speed of a drainage oscillator is 2600rpm/min, and printing to obtain a silicon carbide ceramic blank.
And (3) performing high-temperature de-bonding at 900 ℃, performing impregnation treatment by using a phenolic resin ethanol solution according to a mass ratio of 1:1, and performing de-bonding to obtain a biscuit.
Siliconizing at 1550 ℃ to obtain the high-density silicon carbide ceramic composite material, and testing the mechanical property of the composite material.
Comparative example 4
Weighing 150g of 20 mu m silicon carbide, 55g of 5 mu m silicon carbide, 60g of 10 mu m silicon carbide, 50g of 50 mu m silicon carbide and 40g of 80 mu m silicon carbide, putting into a ball mill grinding tank, ball milling for 1.5 hours according to a ball-material ratio of 1.5:1, obtaining uniformly mixed composite powder, measuring the bulk density and tap density of the composite powder by using a powder physical property tester, and calculating the Karl index and Hawster, wherein the composite powder of the formula has relatively poor compactibility and is unfavorable for improving the performance of the formed biscuit. Adopting adhesive jet printing, selecting an adhesive with the saturation degree of 75%, setting printing parameters, wherein the thickness of a printing layer is 50 mu m, the powder dispersing speed is 50mm/s, the rotating speed of a roller is 300rpm/min, the basic layer for paving powder before printing is 20 layers, the transverse sweeping speed of a heater is 30mm/s, the speed of a drainage oscillator is 2600rpm/min, and printing to obtain a silicon carbide ceramic blank.
And (3) performing high-temperature de-bonding at 900 ℃, performing impregnation treatment by using a phenolic resin ethanol solution according to a mass ratio of 1:1, and performing de-bonding to obtain a biscuit.
Siliconizing at 1550 ℃ to obtain the high-density silicon carbide ceramic composite material, and testing the mechanical property of the composite material.
Comparative example 5
Weighing 150g of 20 mu m silicon carbide, 55g of 5 mu m silicon carbide, 60g of 10 mu m silicon carbide, 50g of 50 mu m silicon carbide and 70g of 80 mu m silicon carbide, putting into a ball mill grinding tank, ball milling for 1.5 hours according to a ball-material ratio of 1.5:1, obtaining uniformly mixed composite powder, measuring the bulk density and tap density of the composite powder by using a powder physical property tester, and calculating the Karl index and Hawsonia ratio.
Adopting adhesive jet printing, selecting an adhesive with the saturation degree of 75%, setting printing parameters, wherein the thickness of a printing layer is 50 mu m, the powder dispersing speed is 50mm/s, the rotating speed of a roller is 300rpm/min, the basic layer for paving powder before printing is 20 layers, the transverse sweeping speed of a heater is 30mm/s, the speed of a drainage oscillator is 2600rpm/min, and printing to obtain a silicon carbide ceramic blank.
And (3) performing high-temperature de-bonding at 900 ℃, performing impregnation treatment by using a phenolic resin ethanol solution according to a mass ratio of 1:1, and performing de-bonding to obtain a biscuit.
Siliconizing at 1550 ℃ to obtain the high-density silicon carbide ceramic composite material, and testing the mechanical property of the composite material.
Comparative example 6
Weighing 150g of 20 mu m silicon carbide, 55g of 5 mu m silicon carbide, 60g of 10 mu m silicon carbide, 50g of 50 mu m silicon carbide and 55g of 80 mu m silicon carbide, putting into a ball mill grinding tank, ball milling for 1.5 hours according to a ball-material ratio of 1.5:1, obtaining uniformly mixed composite powder, measuring the bulk density and tap density of the composite powder by using a powder physical property tester, and calculating the Karl index and Hawsonia ratio.
Adopting adhesive jet printing, selecting an adhesive with the saturation degree of 75%, setting printing parameters, wherein the thickness of a printing layer is 10 mu m, the powder dispersing speed is 50mm/s, the rotating speed of a roller is 300rpm/min, the basic layer for paving powder before printing is 20 layers, the transverse sweeping speed of a heater is 30mm/s, the speed of a drainage oscillator is 2600rpm/min, and printing to obtain a silicon carbide ceramic blank.
And (3) performing high-temperature de-bonding at 900 ℃, performing impregnation treatment by using a phenolic resin ethanol solution according to a mass ratio of 1:1, and performing de-bonding to obtain a biscuit.
Siliconizing at 1550 ℃ to obtain the high-density silicon carbide ceramic composite material, and testing the mechanical property of the composite material.
The following Table 1 shows the compositions of the powders of examples 1 to 8 and comparative examples 1 to 6:
table 2 below shows the bulk density, tap density, cal index and Hawshare ratio parameter values for the powders of examples 1 to 8 and comparative examples 1 to 6.
| Sample of | Bulk Density (g/cm) 3 ) | Tap density (g/cm) 3 ) | Calf index | Haoshan ratio |
| Example 1 | 1.105 | 1.531 | 27.80 | 1.38 |
| Example 2 | 1.092 | 1.529 | 28.35 | 1.40 |
| Example 3 | 1.104 | 1.535 | 27.98 | 1.39 |
| Example 4 | 1.047 | 1.610 | 34.94 | 1.54 |
| Example 5 | 1.099 | 1.571 | 30.05 | 1.43 |
| Example 6 | 1.105 | 1.531 | 27.80 | 1.38 |
| Example 7 | 1.105 | 1.531 | 27.80 | 1.38 |
| Example 8 | 1.105 | 1.531 | 27.80 | 1.38 |
| Comparative example 1 | 1.058 | 1.682 | 37.11 | 1.59 |
| Comparative example 2 | 1.139 | 1.595 | 28.57 | 1.40 |
| Comparative example 3 | 1.021 | 1.522 | 33.89 | 1.49 |
| Comparative example 4 | 1.078 | 1.520 | 29.03 | 1.41 |
| Comparative example 5 | 1.101 | 1.542 | 28.60 | 1.40 |
| Comparative example 6 | 1.105 | 1.531 | 27.80 | 1.38 |
。
Table 3 below shows the mechanical properties such as flexural strength of the green body after primary dip cracking and the ceramic after siliconizing densification of the molded articles of examples 1 to 8 and comparative examples 1 to 6:
referring to the data in tables 1-3, it can be seen that fluidity is significantly improved after grading compared to an ungraded pure 20 μm system of silicon carbideThe flexural strength of the green body and the ceramic printed and formed by various powder BJ is also higher; from the data of examples 1 to 3 and comparative example 3, it is understood that the fluidity after the gradation of five powders (5 μm, 10 μm, 20 μm, 50 μm, 80 μm) is better than that of four powders (5 μm, 10 μm, 20 μm, 50 μm), and the addition of 80 μm silicon carbide increases the popularity and compactibility of the powders, which has an accelerating effect on the properties of the molded green body; secondly, in terms of the quality of the graded powder BJ printing biscuit and the ceramic performance, the flowability and the performance are in a direct proportion relation, the performance of the biscuit after one PIP treatment can reach 19.2MPa optimally, the ceramic performance can reach 285MPa optimally, the elastic modulus can reach 278GPa, and the fracture toughness can reach 2.24 MPa.m 1 /2 Corresponding to the group of powder with the best fluidity.
While the present invention has been described in detail through the foregoing description of the preferred embodiment, it should be understood that the foregoing description is not to be considered as limiting the invention. Many modifications and substitutions of the present invention will become apparent to those of ordinary skill in the art upon reading the foregoing. Accordingly, the scope of the invention should be limited only by the attached claims.
Claims (9)
1. A method for preparing a silicon carbide ceramic composite material, comprising the steps of:
(1) Mixing silicon carbide powder with a median diameter of 20 mu m, silicon carbide powder with a median diameter of 5 mu m, silicon carbide powder with a median diameter of 10 mu m, silicon carbide powder with a median diameter of 50 mu m and silicon carbide powder with a median diameter of 80 mu m respectively to obtain composite powder; preferably, the mass ratio of the silicon carbide powder with the median diameter of 20 mu m, the silicon carbide powder with the median diameter of 5 mu m, the silicon carbide powder with the median diameter of 10 mu m, the silicon carbide powder with the median diameter of 50 mu m and the silicon carbide powder with the median diameter of 80 mu m is 150 (50-60): 50-60;
(2) Spraying and printing the composite powder with a binder to obtain a ceramic blank;
(3) Debonding the ceramic blank to obtain a ceramic biscuit;
(4) And performing reaction sintering siliconizing treatment on the ceramic biscuit to obtain the silicon carbide ceramic composite material.
2. The preparation method according to claim 1, wherein the mixing mode is roller ball milling, the rotating speed is 50-70 r/min, the ball-to-material ratio is 1.5-2:1, and the ball milling time is 1-1.5 h.
3. The method according to claim 1 or 2, wherein the composite powder has a bulk density of 1.01 to 1.15g/cm 3 Tap density of 1.50-1.61g/cm 3 The Calf index is 27.20-35.30, and the Haoshan ratio is 1.28-1.68.
4. A method of manufacturing according to any one of claims 1 to 3, wherein the parameters of the binder jet printing are: the powder scattering speed is 10-50 mm/s, the printing layer thickness is 20-50 mu m, the roller rotating speed is 300-400 rpm, the base layer for paving powder before printing is set to 15-20 layers, the heater sweeping speed is 15-30 mm/s, and the drainage oscillator speed is 2600-3000 rpm.
5. The method according to any one of claims 1 to 4, wherein the binder is an aqueous organic binder having a saturation of 70 to 75% and the binder is a spray-on binder comprising ethylene glycol, ethylene glycol monobutyl ether and a phenolic resin.
6. The method according to any one of claims 1 to 5, wherein the debonding temperature is 900 to 1000 ℃ and the debonding time is 9 to 10 hours; the porosity of the ceramic body after the debonding is controlled to be 50 to 70 percent and the density is controlled to be 0.98 to 1.22g/cm 3 。
7. The method according to any one of claims 1 to 6, wherein the mass ratio of silicon powder to ceramic greenware in the siliconizing sintering is 1 to 1.2:1.5-2; the siliconizing sintering temperature is 1500-1600 ℃, and the siliconizing sintering time is 4-5h.
8. The method of any one of claims 1-7, further comprising dip cracking the ceramic greenbody at least once between debinding and siliconizing sintering; the density of the ceramic biscuit after the dipping and cracking treatment is controlled to be 1.73-2.22 g/cm 3 The bending strength is 3.59-19.24 MPa.
9. A silicon carbide ceramic composite material obtainable by the process according to any one of claims 1 to 8, wherein the silicon carbide ceramic composite material has a flexural strength of 235 to 312MPa, an elastic modulus of 216 to 301GPa and a fracture toughness of 1.74 to 2.96 MPa-m 1/2 The density is 97-99%.
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