CN105126637A - Gas-solid separation ceramic film and preparation method thereof - Google Patents

Abstract

The invention belongs to the technical field of high-temperature dust removal, and relates to a gas-solid separation ceramic membrane and a preparation method thereof. Under extremely harsh working conditions such as high temperature and high pressure, the ceramic membrane support body and membrane layer will suffer from brittle fracture due to the poor toughness of the material. Adopt gas-solid separation ceramic membrane modification method, add a small amount of micron-scale toughening additives such as zirconia powder, aluminum silicate fiber, mullite, etc. to the raw material of the ceramic membrane support body, and add oxidation A small amount of nano-scale toughening additives such as zirconium can effectively improve the toughness of silicon carbide ceramic membranes for gas-solid separation. Using these two modification methods, the gas-solid separation ceramic membranes can be improved without reducing the excellent performance of the gas-solid separation ceramic membranes. The toughness of the solid separation ceramic membrane prevents brittle fracture of the gas-solid separation ceramic membrane under harsh working conditions.

Description

A kind of gas-solid separation ceramic membrane and preparation method thereof

technical field

The invention discloses a gas-solid separation ceramic membrane and a preparation method thereof, belonging to the technical field of inorganic separation materials.

Background technique

At present, my country's atmospheric environment situation is very severe, with frequent occurrence of large-scale smog and severe PM2.5 in some cities. The problem of air pollution characterized by fine particles has become increasingly prominent, causing great harm to human health and environmental quality, and seriously restricting society sustainable economic development. The treatment of high-temperature flue gas discharged from industrial kilns such as steel, cement, electric power, and coal chemical industry has become one of the primary problems to be solved.

To solve the problem of excessive dust emission in high-temperature flue gas, gas-solid separation equipment is required. Traditional gas-solid separation processes, such as electrostatic precipitators, bag dust collectors, and cyclone dust collectors, generally have disadvantages such as low operating temperature and low separation efficiency, which cannot meet industrialization requirements. Requirements, with the emergence of high-performance gas-solid separation ceramic membranes, a feasible new technical route is provided to solve this problem.

Gas-solid separation ceramic membranes generally use silicon carbide materials as the substrate. They are obtained by adding pore-forming agents to silicon carbide raw materials, using isostatic pressing, extrusion molding and other molding processes, and are obtained through coating and high-temperature sintering with certain air permeability. High temperature filter fittings.

Silicon carbide ceramic membrane material is a composite ceramic material, which is composed of a filter layer and a support layer, and is a microporous material with an asymmetric structure. Among them, the supporting layer plays the role of rigid skeleton, and the filter layer plays the main role of filtering, which belongs to the category of surface filtering. Compared with other materials, silicon carbide-based ceramic membrane materials have excellent properties such as high temperature resistance, high strength, good thermal conductivity, small linear expansion coefficient, strong thermal shock resistance, good air permeability, and low pressure drop. It is the preferred high-temperature ceramic filter material. However, in the process of flue gas filtration under some extremely harsh working conditions, the silicon carbide ceramic membrane support and membrane layer will suffer from brittle fracture due to the poor toughness of the material.

Contents of the invention

The purpose of the present invention is to solve the problem that the film layer breaks due to the high toughness between the support body and the film layer during the gas-solid separation process of the silicon carbide ceramic film.

The main solution of the present invention is to improve the toughness of the gas-solid separation ceramic membrane without reducing the excellent properties of the gas-solid separation ceramic membrane by adding a toughening agent to the support layer or the membrane layer, so that the gas-solid separation The separation ceramic membrane will not undergo brittle fracture under particularly harsh working conditions such as high temperature and high pressure.

The technical solution is:

A ceramic membrane for gas-solid separation, including a support layer and a membrane layer, any one or both of the support layer or the membrane layer contains toughening aid particles; the support layer is based on silicon carbide.

The toughening particles are selected from zirconia powder, aluminum silicate fiber or mullite powder.

The average particle diameter of the toughening aid particles added in the support layer belongs to micron order.

The average particle size of the toughening aid particles added in the film layer belongs to the nanoscale.

The average pore diameter of the ceramic membrane is in the range of 0.01-5.0 μm, preferably 0.1-3.0 μm, more preferably 0.5-3.0 μm.

In the support layer, the mass percentage of silicon carbide is more than 60wt%, and the mass percentage of the toughening additive is preferably 0.5-40%, more preferably 2-35%, or 5-30% , 8-20%, 10-15%.

In the film layer, the matrix material is ceramic powder, and the ceramic powder is selected from one or more of alumina, silicon carbide, mullite, cordierite or aluminum titanate.

The mass percentage of the ceramic powder in the film layer can be more than 60wt%; the mass percentage of the toughening additive is preferably 0.5-40%, more preferably 2-35%, or 5-30% %, 8-20%, 10-15%.

According to another object of the present invention, the preparation method of the above-mentioned gas-solid separation ceramic membrane comprises the following steps:

(i), get silicon carbide powder, mix with pore-forming agent to prepare wet billet, after extrusion molding, then through sintering, obtain support body;

(ii), take the ceramic powder, mix it with a dispersion medium to prepare a coating liquid slurry, and then apply the slurry to the surface of the support to obtain a wet film;

(iii), after the wet membrane is dried and sintered, a gas-solid separation membrane is obtained;

Wherein, in step (i) or step (ii), toughening aid particles need to be added in the mixing step.

In step (i), the average particle size of the silicon carbide support body aggregate is 20-600 μm.

In the step (ii), the average particle size of the ceramic powder is 0.5-50 μm.

In step (i), a pore forming agent needs to be added during the mixing process.

In the step (ii), one or more of a pore enhancer, a thickener, a binder or a dispersant needs to be added during the mixing process.

Beneficial effect

The main advantages of the present invention are:

1. The modification method of gas-solid separation ceramic membrane is simple

Just add a small amount of micron-scale toughening additives such as zirconia powder aluminum silicate fiber and mullite to the raw material of the ceramic membrane support body, and add nano-scale toughening additives such as zirconia to the raw material of the ceramic membrane layer. , mixed evenly with the raw materials.

2. Prolong the service life of the gas-solid separation ceramic membrane

In the process of flue gas filtration under some extremely harsh working conditions, the silicon carbide ceramic membrane support and membrane layer will suffer from brittle fracture due to the poor toughness of the material. The gas-solid separation ceramic membrane prepared by the modification process has reduced brittleness, significantly improved toughness, and extended service life.

3. Reduce the operation and maintenance cost of gas-solid separation ceramic membrane dust collector

The toughening agent is easy to purchase, low in cost, prolongs the service life, prolongs the replacement time, and significantly reduces the operation and maintenance costs.

Detailed ways

The present invention will be further described in detail through specific embodiments below. However, those skilled in the art will understand that the following examples are only used to illustrate the present invention, and should not be considered as limiting the scope of the present invention. Those who do not indicate specific technology or conditions in the embodiments, according to the technology or conditions described in the literature in this field (for example, with reference to "Inorganic Membrane Separation Technology and Application" written by Xu Nanping, Chemical Industry Press, 2003) or according to product manual. The reagents or instruments used were not indicated by the manufacturer, and they were all commercially available conventional products.

Approximate terms used herein may be used throughout the specification and claims to modify any number of expressions, which permissible changes would result in a change in the basic function to which it is related. Accordingly, a value modified by a term such as "about" is not to be limited to the precise value specified. In at least some cases, the approximation may correspond to the precision of the instrument used to measure the value. Unless context or language dictates otherwise, range limitations may be combined and/or interchanged, and such ranges are identified to include all the subranges included herein. Except where indicated in the working examples or elsewhere, all numbers or expressions indicating amounts of ingredients, reaction conditions, etc. used in the specification and claims are to be understood in all cases as being protected by the word "about " Modification.

Values expressed in range format should be understood in a flexible manner to include not only the values explicitly recited as the limits of the range, but also all individual values or subranges encompassed within that range, as if each value and subrange were expressly List out. For example, a concentration range of "about 0.1% to about 5%" should be understood to include not only the explicitly recited concentrations of about 0.1% to about 5%, but also individual concentrations within the indicated range (e.g., 1%, 2%, %, 3% and 4%) and subranges (for example, 0.1% to 0.5%, 1% to 2.2%, 3.3% to 4.4%).

In the present invention, the terms "micron-level" and "nano-level" are commonly used understandings in the field of ultrafine powder technology, "micron-level" generally refers to the average particle size range of 1 μm to 5 μm; and "nano-level" is It means that the average particle size of the particles is in the range of 0.1nm to 100nm.

In the present invention, the term "toughening particles" refers to additive particles added to raw materials in order to improve the toughness of sintered ceramics in the technical field of ceramics. It can be understood that toughening particles are particles or powders, which can generally be selected from oxidation Ceramic particles such as zirconium powder, aluminum silicate fiber or mullite powder.

The gas-solid separation ceramic membrane prepared in the present invention refers to an asymmetric membrane, the bottom of which is a support layer, and the upper part of the support layer is a membrane layer. In some cases, it can also be between the support layer and the membrane layer. Set up the middle layer.

support layer

The main material of the support layer is silicon carbide, and the mass percentage of silicon carbide in it is more than 60wt%, and it can also be 70wt%, more than 80wt%, more than 90wt%, or more than 95wt%. During the preparation process, the silicon carbide support The average particle size of the body aggregate is preferably 20 to 600 μm. As the particles other than silicon carbide constituting the support layer, at least one element selected from Group 3 to Group 14 elements such as silicon, aluminum, zirconium, and titanium or their oxides, carbides, nitrides. These are used as sintering aids when sintering silicon carbide particles, which are the main component of the support layer.

In addition, the silicon carbide particles forming the support layer are not necessarily particles composed of silicon carbide alone, and may be particles containing silicon carbide. For example, it may be composite particles composed of silicon carbide and at least one element selected from the group 3 to 14 elements, or their oxides, carbides, and nitrides. In addition, boron can also be used as a sintering aid.

In the present invention, in order to improve the strength of the gas-solid separation membrane, a toughening aid can be added to the support layer, and the toughening aid can be selected from zirconia powder, aluminum silicate fiber or mullite powder, The particle size of these toughening aids is preferably micron-sized powder. In the support layer, the mass percentage of these toughening aids is preferably 0.5-40%, more preferably 2-35%, and can also be 5-30%, 8-20%, 10-15%.

film layer

The material constituting the membrane layer can be appropriately selected from conventionally known ceramic materials. For example, alumina, silicon carbide, mullite, cordierite, aluminum titanate can be used. The average particle size of the above ceramic powder material constituting the film layer is 0.5-50 μm. In the film layer, the mass percentage of the above-mentioned ceramic powder can be more than 60wt%, and can also be more than 70wt%, more than 80wt%, more than 90wt%, or more than 95wt%.

In the present invention, in order to improve the strength of the gas-solid separation membrane, a toughening aid can be added in the film layer, and the toughening aid can be selected from zirconia powder, aluminum silicate fiber or mullite powder, these The particle size of the toughening aid is preferably nanoscale powder. In the film layer, the mass percentage of these toughening aids is preferably 0.5-40%, more preferably 2-35%, and can also be 5-30%, 8-20%, 10-15%.

For the film layer and the support layer, the toughening aid contained therein does not necessarily have to be present in the film layer and the support layer at the same time, as long as it is contained in any one of them. In a preferred embodiment, the most It is better to have both in the film layer and the support layer, which can better improve the strength of the film layer.

Preparation of gas-solid separation membrane

The gas-solid separation membrane of this embodiment can be produced by the following steps: coating the surface of the porous support constituting the separation membrane with a membrane-forming liquid; and sintering the particles of the membrane-forming liquid by heat treatment to form a film layer on the surface of the support. process.

Among them, the preparation of the porous support can be carried out by mixing silicon carbide powder with a small amount of pore-forming agent (such as carbon powder, graphite, starch, wood chips), and adding other aggregate particles and extenders when necessary. toughening agent. The final percentage of silicon carbide or toughening agent in the support is calculated by the amount of these raw materials when added, and the porogen will disappear during the sintering process. Therefore, when calculating the particle weight content, it can be Not counted. After mixing the various powders, some water, solvent, binder, dispersant, etc. can be added if necessary, and the billet can be obtained through stirring or ball milling, and then extrusion molding and sintering to finally obtain the support body; among them, If the isostatic pressing molding process is adopted, solvents such as water may not be added.

Before the preparation of the film layer, it is necessary to disperse ceramic particles (alumina, silicon carbide, mullite, cordierite, aluminum titanate) into the dispersion medium to form a dispersion of ceramic particles. When adding toughening additives to the dispersion, toughening additive particles can also be added to the dispersion; the dispersion process can be carried out by conventional stirring, high-speed stirring, etc., and if necessary, the step of ball milling can also be added.

Basically, it is preferable to use water or an organic solvent as the dispersion medium, but in addition, a polymer monomer or an oligomer monomer or a mixture thereof may be used.

As the organic solvent mentioned above, for example, alcohols such as methanol, ethanol, propanol, diacetone alcohol, furfuryl alcohol, ethylene glycol, hexylene glycol, esters such as methyl acetate and ethyl acetate, diethyl ether, ethyl acetate, etc. Glycol monomethyl ether (methyl cellosolve), ethylene glycol monoethyl ether (ethyl cellosolve), ethylene glycol monobutyl ether (butyl cellosolve), diethylene glycol monomethyl ether, ethylene glycol monoethyl ether One or two or more solvents may be used such as ether alcohols, aromatic hydrocarbons such as dioxane, tetrahydrofuran, and xylene.

As the above-mentioned polymer monomer, acrylic or methacrylic monomers such as methyl acrylate and methyl methacrylate, epoxy-based monomers, and the like can be used. Moreover, as said oligomer, a urethane acrylate oligomer, an epoxy acrylate oligomer, an acrylate oligomer, etc. can be used.

In addition, a pore enhancer, a thickener, a binder, a dispersant, and deionized water may be added to the above-mentioned film-forming dispersion liquid. As a dispersant or a binder, organic polymers such as polyammonium carbonate, polyethylene glycol, polyvinyl alcohol, and polyvinylpyrrolidone can be used, for example.

When coating the film-making solution on the surface of the support layer, conventional film-coating methods can be used, such as bar coating, grouting, dipping, spraying, etc., as long as the film-making solution can be uniformly It only needs to be coated on the surface of the support, and there is no particular limitation.

For the membrane layer, the average pore diameter may be in the range of 0.01-5.0 μm, preferably 0.1-3.0 μm, more preferably 0.5-3.0 μm.

The sintering heat treatment temperature of the coating film is preferably 900°C to 2000°C, more preferably 1000°C to 1800°C. In addition, the sintering time is preferably not less than 0.5 hours and not more than 20 hours, more preferably not less than 1.0 hours and not more than 8 hours. The sintering atmosphere is not particularly limited, and may be performed in a reducing atmosphere such as hydrogen, oxygen or carbon monoxide, in an inert atmosphere such as nitrogen, argon, neon, or xenon, or in an oxidizing atmosphere such as oxygen or air.

Performance Testing

1. Bending strength test method: Use a bending strength tester to measure the average value of the bending strength at three points, with a span of 40mm and a loading speed of 0.5mm/min. For specific test steps, refer to the national standard GB/T1965-1996.

2. The pore size test method adopts the gas bubble pressure method, using deionized water as the wetting agent, and the specific test steps refer to relevant materials (references: Xu Nanping, Xing Weihong, Zhao Yijiang, Inorganic Membrane Separation Technology and Application, Chemical Industry Press, 2003, 21-22).

3. Membrane strength test

Use GB/T6739-1996 "Coating Film Hardness Pencil Determination Method" to characterize the film strength, use a Φ2mm stainless steel rod instead of a pencil, scrape the surface of the porous film, visually observe the damage of the porous film, and from the appearance Change judgment intensity. During the test, the load applied to the stainless steel rod was set to 500g, the testing machine was slid once on the porous membrane, the separation membrane without peeling off was judged as good, the separation membrane with a little peeling was judged as normal, and the separation membrane with a little peeling off was judged as normal. A separation membrane whose film layer was deeply cut was judged as poor.

Example 1

To prepare silicon carbide gas-solid separation ceramic membrane, the raw material slurry composition of the support body is as follows: 80g support body raw material silicon carbide powder particle size 100μm, toughening additive is zirconia particles, particle size is 5μm, 10g; the rest is pore increasing Agent graphite 10g, sintering aid MgO3g. After going through the isostatic pressing molding process again, a green body is obtained, and after sintering at 1400° C. for 6 hours, a support body is obtained.

The raw material of the film-making liquid is 80g of alumina powder with a particle size of 20μm, and the rest is 5g of polyvinyl alcohol, 2g of polyvinylpyrrolidone, and 160g of deionized water. membrane. After the wet film is obtained, it is dried and sintered at 1200°C for 5 hours to obtain the gas-solid separation film.

Example 2

To prepare silicon carbide gas-solid separation ceramic membrane, the raw material slurry composition of the support body is as follows: 85g support body raw material silicon carbide powder particle size 200μm, toughening additive is aluminum silicate fiber, average particle size is 3μm, 5g; the rest is Pore enhancer starch 10g, sintering aid MgO5g. After going through the isostatic pressing molding process again, a green body is obtained, and after sintering at 1500° C. for 4 hours, a support body is obtained.

The raw material of the film-making liquid is 80g of alumina powder with a particle size of 15μm, the toughening agent is 15g of zirconia particles with a particle size of 20nm, and the rest are 2g of polyvinyl alcohol, 4g of polyvinylpyrrolidone, and 140g of deionized water. The film-making solution is prepared by ball milling, and then the film is coated by the dipping method. After the wet film is obtained, it is dried and sintered at 1100° C. for 4 hours to obtain a gas-solid separation film.

Example 3

To prepare silicon carbide gas-solid separation ceramic membrane, the raw material slurry composition of the support body is as follows: 100g support body raw material silicon carbide powder particle size 300μm, toughening additive is mullite particles, particle size is 2μm, 20g; Pore agent graphite 10g, sintering aid MgO6g. After going through the isostatic pressing molding process again, a green body is obtained, and after sintering at 1300° C. for 4 hours, a support body is obtained.

The film-making liquid raw material is 90g of aluminum titanate powder with a particle size of 15 μm, the toughening agent is 8g of zirconia particles with a particle size of 20nm, and the rest are 4g of polyvinyl alcohol, 4g of polyvinylpyrrolidone, and 150g of deionized water. The film-making solution is prepared by mixing and ball milling, and then the film is coated by the dipping method. After the wet film is obtained, it is dried and sintered at 1200°C for 6 hours to obtain the gas-solid separation film.

Example 4

The difference from Example 1 is that a toughening aid is also added to the composition of the film-forming solution.

To prepare silicon carbide gas-solid separation ceramic membrane, the raw material slurry composition of the support body is as follows: 80g support body raw material silicon carbide powder particle size 100μm, toughening additive is zirconia particles, particle size is 5μm, 10g; the rest is pore increasing Agent graphite 10g, sintering aid MgO3g. After going through the isostatic pressing molding process again, a green body is obtained, and after sintering at 1400° C. for 6 hours, a support body is obtained.

The raw material of the film-making liquid is 80g of alumina powder with a particle size of 20μm, the toughening agent is 10g of zirconia particles with a particle size of 50nm, and the rest are 5g of polyvinyl alcohol, 2g of polyvinylpyrrolidone, and 160g of deionized water. The film-making solution is prepared by ball milling, and then the film is coated by the dipping method. After the wet film is obtained, it is dried and sintered at 1200°C for 5 hours to obtain the gas-solid separation film.

Example 5

To prepare silicon carbide gas-solid separation ceramic membrane, the raw material slurry composition of the support body is as follows: 80g support body raw material silicon carbide powder particle size 100μm, toughening additive is zirconia particles, particle size is 5μm, 10g; the rest is pore increasing Agent graphite 10g, sintering aid MgO3g. After going through the isostatic pressing molding process again, a green body is obtained, and after sintering at 1400° C. for 6 hours, a support body is obtained.

The raw material of the film-making solution is 80g of alumina powder (before preparation, the alumina powder is placed in an ethanol solution containing 20wt% silane coupling agent KH550 and soaked for 10 hours), the particle size is 20μm, and the rest is polyvinyl alcohol 5g, 2g of polyvinylpyrrolidone, and 160g of deionized water were used to prepare the film-making solution by mixing and ball milling, and then the film was coated by the dipping method. After the wet film is obtained, it is dried and sintered at 1200°C for 5 hours to obtain the gas-solid separation film.

Example 6

The difference from Example 2 is that no toughening aid is added to the raw materials of the support body.

To prepare silicon carbide gas-solid separation ceramic membrane, the raw material slurry composition of the support body is as follows: 85g support body raw material silicon carbide powder particle size 200μm; the rest is 10g pore enhancer starch and 5g sintering aid MgO. After going through the isostatic pressing molding process again, a green body is obtained, and after sintering at 1500° C. for 4 hours, a support body is obtained.

The raw material of the film-making liquid is 80g of alumina powder with a particle size of 15μm, the toughening agent is 15g of zirconia particles with a particle size of 20nm, and the rest are 2g of polyvinyl alcohol, 4g of polyvinylpyrrolidone, and 140g of deionized water. The film-making solution is prepared by ball milling, and then the film is coated by the dipping method. After the wet film is obtained, it is dried and sintered at 1100° C. for 4 hours to obtain a gas-solid separation film.

Comparative example 1

The difference from Example 1 is that no toughening aid is added to the raw materials for the preparation of the support layer and the film layer.

To prepare silicon carbide gas-solid separation ceramic membrane, the raw material slurry composition of the support body is as follows: 80g of support body raw material silicon carbide powder particle size 100μm, the rest is 10g of pore enhancer graphite, and 3g of sintering aid MgO. After going through the isostatic pressing molding process again, a green body is obtained, and after sintering at 1400° C. for 6 hours, a support body is obtained.

The raw material of the film-making liquid is 80g of alumina powder with a particle size of 20μm, and the rest is 5g of polyvinyl alcohol, 2g of polyvinylpyrrolidone, and 160g of deionized water. membrane. After the wet film is obtained, it is dried and sintered at 1200°C for 5 hours to obtain the gas-solid separation film.

As can be seen from the table, compared with comparative example 1, embodiment 1 can improve the strength between the film layers due to the addition of toughening aids in the raw material of the support layer; embodiment 1 is similar to embodiment 4. It can be seen that adding toughening aids to the support layer and the film layer can further improve the strength of the film layer; it can be seen from the comparison between Example 1 and Example 5 that the powder is pre-prepared with a silane coupling agent. After the treatment, the dispersibility of the powder can be improved, and then the strength after sintering can be improved; as can be seen from Example 2 compared with Example 6, it is also possible to add toughening aids only in the raw materials of the film layer, but compared to At the same time, the addition of the raw materials of the support body layer will cause the film layer strength to be slightly lower.

Claims (10)

1. A gas-solid separation ceramic membrane, comprising a support layer and a film layer, is characterized in that: in any one or both of the support layer or the film layer, toughening aid particles are included; the support layer is Based on silicon carbide. 2. The ceramic membrane for gas-solid separation according to claim 1, characterized in that: the toughening particles are selected from zirconia powder, aluminum silicate fiber or mullite powder. 3. The gas-solid separation ceramic membrane according to claim 1, characterized in that: the average particle diameter of the toughening aid particles added in the support layer belongs to micron order; the toughening aid particles added in the film layer The average particle size belongs to the nanoscale. 4. The ceramic membrane for gas-solid separation according to claim 1, characterized in that: the average pore size range of the ceramic membrane is 0.01-5.0 μm, preferably 0.1-3.0 μm, more preferably 0.5-3.0 μm μm. 5. The gas-solid separation ceramic membrane according to claim 1, characterized in that: in the support layer, the mass percentage of silicon carbide is more than 60wt%, and the mass percentage of the toughening additive is preferably 0.5-40%, more preferably 2-35%, may also be 5-30%, 8-20%, 10-15%. 6. The gas-solid separation ceramic membrane according to claim 1, characterized in that: in the membrane layer, the matrix material is ceramic powder, and the ceramic powder is selected from alumina, silicon carbide, mullite , cordierite or aluminum titanate or one or more. 7. The gas-solid separation ceramic membrane according to claim 1, characterized in that: the mass percentage of the ceramic powder in the film layer can be more than 60wt%; the mass percentage of the toughening aid is preferably It is 0.5 to 40%, more preferably 2 to 35%, and may be 5 to 30%, 8 to 20%, or 10 to 15%. 8. The preparation method of the gas-solid separation ceramic membrane described in any one of claims 1 to 7, comprising the steps of: (i), getting silicon carbide powder, mixing with a pore-forming agent to prepare a wet billet, after extrusion molding, After sintering, the support body is obtained; (ii), the ceramic powder is taken, mixed with the dispersion medium to prepare a coating liquid slurry, and then the slurry is applied to the surface of the support body to obtain a wet film; (iii) . After the wet film is dried and sintered, the gas-solid separation film is prepared, which is characterized in that: in step (i) or (ii), it is necessary to add toughening aid particles in the mixing step. 9. The method for preparing a ceramic membrane for gas-solid separation according to claim 8, characterized in that: in the step (i), the silicon carbide support aggregate has an average particle diameter of 20 to 600 μm; in the step (ii), The average particle size of the ceramic powder is 0.5-50 μm. 10. the preparation method of gas-solid separation ceramic membrane according to claim 8 is characterized in that: in (i) step, also need to add porogen in mixing process; It is necessary to add one or more of pore enhancers, thickeners, binders or dispersants.