阅读说明：本技术 一种高性能硼化锆-碳化硅复相陶瓷电极制备方法 (Preparation method of high-performance zirconium boride-silicon carbide composite ceramic electrode ) 是由 巩鹏程 王前 任学美 巩长生 于 2021-10-15 设计创作，主要内容包括：本发明公开的属于超高温陶瓷材料技术领域,具体为一种高性能硼化锆-碳化硅复相陶瓷电极制备方法,该高性能硼化锆-碳化硅复相陶瓷电极制备方法的具体步骤流程图如下：取料：称取一定重量的碳化硅粉末和硼化锆粉末,将两种粉末倒入研磨装置的内部,使用研磨装置对两种粉末进行不断粉碎,当完全粉碎后,使用搅拌装置对其进行充分搅拌8-10分钟,直至完全混合后,向其中加入过量的乙醇溶液,继续充分搅拌5-7分钟；恒温球磨：将两种混合物倒入研磨装置的内部,保持温度控制在30-40摄氏度,对其进行持续恒温球磨2-4小时,恒温球磨之后,生产的硼化锆-碳化硅复相陶瓷电极的韧性有效提高,在后期使用的过程中不容易发生断裂,从而提高陶瓷电极质量。(The invention belongs to the technical field of ultra-high temperature ceramic materials, and particularly relates to a preparation method of a high-performance zirconium boride-silicon carbide complex phase ceramic electrode, which comprises the following specific steps: taking materials: weighing silicon carbide powder and zirconium boride powder in certain weight, pouring the two kinds of powder into a grinding device, continuously grinding the two kinds of powder by using the grinding device, fully stirring the powder for 8-10 minutes by using a stirring device after the powder is completely ground, adding excessive ethanol solution into the powder until the powder is completely mixed, and continuously and fully stirring the powder for 5-7 minutes; constant temperature ball milling: pouring the two mixtures into a grinding device, keeping the temperature at 30-40 ℃, continuously ball-milling the mixture at constant temperature for 2-4 hours, and after ball-milling at constant temperature, effectively improving the toughness of the produced zirconium boride-silicon carbide complex phase ceramic electrode, and being not easy to break in the later use process, thereby improving the quality of the ceramic electrode.)

1. A preparation method of a high-performance zirconium boride-silicon carbide complex phase ceramic electrode is characterized by comprising the following steps: the preparation method of the high-performance zirconium boride-silicon carbide complex phase ceramic electrode comprises the following specific steps of:

taking materials: weighing silicon carbide powder and zirconium boride powder in certain weight, pouring the two kinds of powder into a grinding device, continuously grinding the two kinds of powder by using the grinding device, fully stirring the powder for 8-10 minutes by using a stirring device after the powder is completely ground, adding excessive ethanol solution into the powder until the powder is completely mixed, and continuously and fully stirring the powder for 5-7 minutes;

constant temperature ball milling: pouring the two mixtures into a grinding device, keeping the temperature at 30-40 ℃, carrying out continuous constant-temperature ball milling on the mixture for 2-4 hours, and after the ball milling at the constant temperature, placing the mixture at the rotating speed of 30-60r/min and continuously drying the mixture for 30-40 minutes;

spark plasma sintering: and (2) putting the powder obtained in the step into a graphite die, placing the graphite die in a vacuum environment, uniformly pressurizing to perform discharge plasma sintering, stably and uniformly increasing the environmental pressure to 30-40 MPa in the process of increasing the temperature from room temperature to 1600-1700℃, then keeping the temperature for 8-10min under the conditions of 1700 ℃ and 40MPa, and then cutting off the power and naturally cooling to the room temperature to obtain the high-performance zirconium boride-silicon carbide complex phase ceramic electrode.

2. The preparation method of the high-performance zirconium boride-silicon carbide complex phase ceramic electrode according to claim 1, characterized in that: in the material taking and constant-temperature ball milling steps, the grinding devices required to be used are agate ball milling tanks.

3. The preparation method of the high-performance zirconium boride-silicon carbide complex phase ceramic electrode according to claim 1, characterized in that: in the step of constant temperature ball milling, the ball milling method is wet planetary ball milling.

4. The preparation method of the high-performance zirconium boride-silicon carbide complex phase ceramic electrode according to claim 1, characterized in that: in the step of constant-temperature ball milling, a binder and a plasticizer are required to be added, the ratio of the binder to the plasticizer is 1: 2, the binder adopts polyvinyl butyral, and the plasticizer adopts polyethylene glycol.

5. The preparation method of the high-performance zirconium boride-silicon carbide complex phase ceramic electrode according to claim 1, characterized in that: in the material taking step, the particles obtained by grinding the silicon carbide powder and the zirconium boride powder need to be sieved by a 200-mesh sieve.

Technical Field

The invention relates to the technical field of ultra-high temperature ceramic materials, in particular to a preparation method of a high-performance zirconium boride-silicon carbide complex phase ceramic electrode.

Background

The ZrB2-SiC composite material has the characteristics of melting point, good electrical conductivity, good neutron control capability and the like, and is generally used in various fields such as high-temperature structural ceramic materials, refractory materials, electrode materials, aerospace and the like. Particularly, the demand of ZrB2-SiC is more urgent due to the high-speed development of the existing rocket and missile technologies, the performance requirements of the fields on ZrB2-SiC composite materials are high, and the ultrahigh-temperature ceramic material is a special ceramic material capable of keeping physical and chemical stability in a high-temperature environment and a reaction atmosphere. Such materials include mainly transition metal borides, carbides and nitrides, all with melting points in excess of 3000 ℃. The transition metal boride is a most advantageous high-temperature structural ceramic material by virtue of high melting point, high thermal conductivity, high electrical conductivity, good chemical stability and thermal shock resistance, and has wide application prospects in extreme environments such as hypersonic flight, atmosphere reentry, cross-atmosphere flight, rocket propulsion systems and the like.

However, the existing preparation method of the zirconium boride-silicon carbide complex phase ceramic electrode is relatively backward, and the prepared zirconium boride-silicon carbide complex phase ceramic electrode has relatively poor toughness, so that the zirconium boride-silicon carbide complex phase ceramic electrode is easy to break in the later use process, thereby influencing the use.

Disclosure of Invention

The invention aims to provide a preparation method of a high-performance zirconium boride-silicon carbide complex phase ceramic electrode, and aims to solve the problem that the zirconium boride-silicon carbide complex phase ceramic electrode prepared by the existing preparation method in the background technology has poor toughness, so that the zirconium boride-silicon carbide complex phase ceramic electrode is easy to break in the later use process, and the use is influenced.

In order to achieve the purpose, the invention provides the following technical scheme: a preparation method of a high-performance zirconium boride-silicon carbide complex phase ceramic electrode comprises the following specific steps of:

taking materials: weighing silicon carbide powder and zirconium boride powder in certain weight, pouring the two kinds of powder into a grinding device, continuously grinding the two kinds of powder by using the grinding device, fully stirring the powder for 8-10 minutes by using a stirring device after the powder is completely ground, adding excessive ethanol solution into the powder until the powder is completely mixed, and continuously and fully stirring the powder for 5-7 minutes;

constant temperature ball milling: pouring the two mixtures into a grinding device, keeping the temperature at 30-40 ℃, carrying out continuous constant-temperature ball milling on the mixture for 2-4 hours, and after the ball milling at the constant temperature, placing the mixture at the rotating speed of 30-60r/min and continuously drying the mixture for 30-40 minutes;

spark plasma sintering: and (2) putting the powder obtained in the step into a graphite die, placing the graphite die in a vacuum environment, uniformly pressurizing to perform discharge plasma sintering, stably and uniformly increasing the environmental pressure to 30-40 MPa in the process of increasing the temperature from room temperature to 1600-1700℃, then keeping the temperature for 8-10min under the conditions of 1700 ℃ and 40MPa, and then cutting off the power and naturally cooling to the room temperature to obtain the high-performance zirconium boride-silicon carbide complex phase ceramic electrode.

Preferably, in the material taking and constant-temperature ball milling steps, all grinding devices required are agate ball milling tanks.

Preferably, in the constant-temperature ball milling step, the ball milling method is wet planetary ball milling.

Preferably, in the step of constant-temperature ball milling, a binder and a plasticizer are required to be added, the ratio of the binder to the plasticizer is 1: 2, the binder is polyvinyl butyral, and the plasticizer is polyethylene glycol.

Preferably, in the material taking step, the particles obtained by grinding the silicon carbide powder and the zirconium boride powder need to be sieved by a 200-mesh sieve.

Compared with the prior art, the invention has the beneficial effects that:

through the common cooperation of material taking, constant-temperature ball milling and discharge plasma sintering, the toughness of the produced zirconium boride-silicon carbide complex phase ceramic electrode is effectively improved, and the zirconium boride-silicon carbide complex phase ceramic electrode is not easy to break in the later use process, so that the quality of the ceramic electrode is improved.

Drawings

FIG. 1 is a flow chart of the steps of the preparation method of the present invention.

Detailed Description

The technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the drawings in the embodiments of the present invention, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all of the embodiments. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.

In the description of the present invention, it is to be understood that the terms "upper", "lower", "front", "rear", "left", "right", "top", "bottom", "inner", "outer", and the like, indicate orientations or positional relationships based on the orientations or positional relationships shown in the drawings, are merely for convenience in describing the present invention and simplifying the description, and do not indicate or imply that the device or element being referred to must have a particular orientation, be constructed and operated in a particular orientation, and thus, should not be construed as limiting the present invention.

Referring to fig. 1, the present invention provides a technical solution: a preparation method of a high-performance zirconium boride-silicon carbide complex phase ceramic electrode comprises the following specific steps of:

taking materials: weighing silicon carbide powder and zirconium boride powder in certain weight, pouring the two kinds of powder into a grinding device, continuously grinding the two kinds of powder by using the grinding device, fully stirring the powder for 8-10 minutes by using a stirring device after the powder is completely ground, adding excessive ethanol solution into the powder until the powder is completely mixed, and continuously and fully stirring the powder for 5-7 minutes;

constant temperature ball milling: pouring the two mixtures into a grinding device, keeping the temperature at 30-40 ℃, carrying out continuous constant-temperature ball milling on the mixture for 2-4 hours, and after the ball milling at the constant temperature, placing the mixture at the rotating speed of 30-60r/min and continuously drying the mixture for 30-40 minutes;

spark plasma sintering: and (2) putting the powder obtained in the step into a graphite die, placing the graphite die in a vacuum environment, uniformly pressurizing to perform discharge plasma sintering, stably and uniformly increasing the environmental pressure to 30-40 MPa in the process of increasing the temperature from room temperature to 1600-1700℃, then keeping the temperature for 8-10min under the conditions of 1700 ℃ and 40MPa, and then cutting off the power and naturally cooling to the room temperature to obtain the high-performance zirconium boride-silicon carbide complex phase ceramic electrode.

In the material taking and constant-temperature ball milling steps, the grinding devices required to be used are agate ball milling tanks.

In the step of constant temperature ball milling, the ball milling method is wet planetary ball milling.

In the step of constant-temperature ball milling, a binder and a plasticizer are required to be added, the ratio of the binder to the plasticizer is 1: 2, the binder adopts polyvinyl butyral, and the plasticizer adopts polyethylene glycol.

In the material taking step, the particles obtained by grinding the silicon carbide powder and the zirconium boride powder need to be sieved by a 200-mesh sieve.

ZrB2 is a hexagonal C32 metalloid structure compound, has high melting point, high hardness, high stability, and good electrical conductivity, thermal conductivity and chemical corrosion resistance, so that the ZrB2 has a great development prospect in the industries of refractory materials, nozzles, cutting tools and bearings, and ZrB2 has good neutron control capability and can be used in the nuclear industry.

SiC can form different crystal structures under different physical and chemical environments, the crystals with the same components, different shapes, different structures and different physical characteristics are called homogeneous multi-image variants, the toughening application of SiC in engineering mainly comprises SiCp and SiCw, the SiCp toughening ceramic composite base material belongs to a dispersed particle reinforced composite material, the composite material is isotropic, and the preparation and processing method is simple; the SiCp toughening mechanism comprises residual stress field toughening, microcrack toughening, crack deflection, crack bifurcation, crack bridging, crack pinning and the like; the toughening mechanism of SiCp is mainly that an inner crystal structure is formed in the composite material, the grain refinement of nano composite ceramic with the inner crystal structure generates a secondary crystal boundary at the same time, so that the number of the crystal boundaries is greatly increased, the strength and the toughness of the material are also greatly improved, some ceramics even show super toughness, and the nano composite ceramic material with the inner crystal structure is mainly used for enhancing the ceramic material through the following effects: firstly, the introduction of disperse phase effectively inhibits the growth of matrix grains and lightens the abnormal growth of the grains; local stress exists around the dispersed phase or the dispersed phase, the stress is generated by thermal expansion mismatch between the matrix and the dispersed phase, dislocation is generated in the cooling stage, and nano particles are pinned or enter a dislocation region to generate a latent crystal boundary in basic crystal grains, so that the crystal grains are refined to weaken the action of the main crystal boundary; inducing transgranular fracture by local tensile stress around the nano particles, and toughening the hard particles due to the reflection effect of the hard particles on the crack tips; fourthly, the dislocation motion is controlled by the nano particles at high temperature, so that the high-temperature mechanical properties such as hardness, strength and creep resistance are improved.

Example 1:

the preparation method of the high-performance zirconium boride-silicon carbide complex phase ceramic electrode comprises the following specific steps of:

taking materials: weighing silicon carbide powder and zirconium boride powder in certain weight, pouring the two kinds of powder into a grinding device, continuously grinding the two kinds of powder by using the grinding device, fully stirring the powder for 8 minutes by using a stirring device after the powder is completely ground, adding excessive ethanol solution into the powder after the powder is completely mixed, and continuously and fully stirring the powder for 5 minutes;

constant temperature ball milling: pouring the two mixtures into a grinding device, keeping the temperature at 30 ℃, carrying out continuous constant-temperature ball milling on the mixture for 2 hours, and after carrying out constant-temperature ball milling, placing the mixture at a rotating speed of 30-60r/min and continuously drying the mixture for 30 minutes;

spark plasma sintering: putting the powder obtained in the step into a graphite die, placing the graphite die in a vacuum environment, uniformly pressurizing to perform discharge plasma sintering, wherein during sintering, in the process of rising from room temperature to 1600 ℃, the environmental pressure is stably and uniformly increased to 30MPa, then, the temperature is kept for 8min under the conditions that the temperature is 1700 ℃ and the pressure is 40MPa, and then, the power is cut off and the ceramic electrode is naturally cooled to the room temperature to obtain the high-performance zirconium boride-silicon carbide complex phase ceramic electrode;

example 2:

the preparation method of the high-performance zirconium boride-silicon carbide complex phase ceramic electrode comprises the following specific steps of:

taking materials: weighing silicon carbide powder and zirconium boride powder in certain weight, pouring the two kinds of powder into a grinding device, continuously grinding the two kinds of powder by using the grinding device, fully stirring the powder for 9 minutes by using a stirring device after the powder is completely ground, adding excessive ethanol solution into the powder after the powder is completely mixed, and continuously and fully stirring the powder for 6 minutes;

constant temperature ball milling: pouring the two mixtures into a grinding device, keeping the temperature at 35 ℃, carrying out continuous constant-temperature ball milling on the mixture for 3 hours, and after carrying out constant-temperature ball milling, placing the mixture at a rotating speed of 45r/min and continuously drying the mixture for 35 minutes;

spark plasma sintering: putting the powder obtained in the step into a graphite die, placing the graphite die in a vacuum environment, uniformly pressurizing to perform discharge plasma sintering, stably and uniformly increasing the environmental pressure to 35MPa in the process of increasing the room temperature to 1650 ℃, then keeping the temperature for 9min under the conditions that the temperature is 1700 ℃ and the pressure is 40MPa, and then naturally cooling to the room temperature after power failure to obtain the high-performance zirconium boride-silicon carbide complex phase ceramic electrode;

example 3:

the preparation method of the high-performance zirconium boride-silicon carbide complex phase ceramic electrode comprises the following specific steps of:

taking materials: weighing silicon carbide powder and zirconium boride powder in certain weight, pouring the two kinds of powder into a grinding device, continuously grinding the two kinds of powder by using the grinding device, fully stirring the powder for 10 minutes by using a stirring device after the powder is completely ground, adding excessive ethanol solution into the powder after the powder is completely mixed, and continuously fully stirring the powder for 7 minutes;

constant temperature ball milling: pouring the two mixtures into a grinding device, keeping the temperature at 40 ℃, carrying out continuous constant-temperature ball milling on the mixture for 4 hours, and after carrying out constant-temperature ball milling, placing the mixture at a rotating speed of 30-60r/min and continuously drying the mixture for 40 minutes;

spark plasma sintering: and (2) putting the powder obtained in the step into a graphite die, placing the graphite die in a vacuum environment, uniformly pressurizing to perform discharge plasma sintering, stably and uniformly increasing the environmental pressure to 40MPa in the process of increasing the temperature from room temperature to 1700 ℃, then preserving the temperature for 10min under the conditions of 1700 ℃ and 40MPa, and then powering off and naturally cooling to room temperature to obtain the high-performance zirconium boride-silicon carbide complex phase ceramic electrode.

While there have been shown and described the fundamental principles and essential features of the invention and advantages thereof, it will be apparent to those skilled in the art that the invention is not limited to the details of the foregoing exemplary embodiments, but is capable of other specific forms without departing from the spirit or essential characteristics thereof; the present embodiments are therefore to be considered in all respects as illustrative and not restrictive, the scope of the invention being indicated by the appended claims rather than by the foregoing description, and all changes which come within the meaning and range of equivalency of the claims are therefore intended to be embraced therein, and any reference signs in the claims are not intended to be construed as limiting the claim concerned.

Although embodiments of the present invention have been shown and described, it will be appreciated by those skilled in the art that changes, modifications, substitutions and alterations can be made in these embodiments without departing from the principles and spirit of the invention, the scope of which is defined in the appended claims and their equivalents.