High-toughness high-temperature-resistant ceramic material and preparation method thereof

Abstract

The application relates to the technical field of ceramics, and discloses a high-toughness high-temperature-resistant ceramic material and a preparation method thereof.The high-toughness high-temperature-resistant ceramic material comprises 100 parts by weight of quartz powder, 15-32 parts by weight of potassium feldspar, 3-6 parts by weight of boric acid and 0.8-2 parts by weight of modified polysiloxane.The side chain of the modified polysiloxane contains a large amount of carboxyl groups, forms an interface interaction with the surfaces of the quartz and the potassium feldspar, plays a role of a dispersant, and is favorable for improving the mechanical strength of the ceramic material after calcination.The modified polysiloxane contains a naphthalene ring structure with high carbon content, after high-temperature calcination, the polysiloxane is used as a silicon source, the naphthalene ring is carbonized, high-temperature pyrolysis is easier to form a large amount of silicon carbide reinforcing phase, the silicon carbide reinforcing phase is uniformly dispersed in the quartz ceramic matrix, the mechanical strength and the toughness of the ceramic material are remarkably improved, and the high-temperature-resistant performance is excellent, and the ceramic material has good practical application in heat-resistant ceramic lampshades and heat-resistant ceramic bases.

Description

Technical Field

[0001] This invention relates to the field of ceramic technology, specifically to a high-toughness, high-temperature resistant ceramic material and its preparation method. Background Technology

[0002] Quartz ceramic materials possess advantages such as excellent high-temperature resistance, high thermal shock stability, and low thermal conductivity and coefficient of thermal expansion, making them widely used in lighting fixtures, building materials, photovoltaic panels, and refractory components. However, quartz ceramic materials currently suffer from issues such as relatively low mechanical strength, and their strength and toughness deteriorate after high-temperature calcination. Adding dispersants to ceramic slurries can improve the viscosity and rheological properties of the slurry, thereby enhancing the mechanical properties of the ceramic.

[0003] Silicone oil is an inexpensive and readily available polysiloxane substance. High-temperature pyrolysis in an inert or ammonia atmosphere can produce high-performance Si-OC ceramics, Si-NC ceramics, etc. Chinese patent application CN115557797A describes a method for preparing polyimide-modified interfaces and quartz / quartz composite materials. It uses polysiloxane as a silica precursor and polyimide as an interface material, blending it with quartz fibers, boron nitride nanopowder, etc., and then treating the mixture at high temperatures. The resulting ceramic material exhibits advantages such as high density and high flexural strength. However, this patent does not improve the toughness and high-temperature resistance of quartz ceramics. Summary of the Invention

[0004] (a) Technical problems to be solved:

[0005] To address the shortcomings of existing technologies, this invention provides a high-toughness and high-temperature resistant ceramic material and its preparation method, solving the problems of poor toughness and high-temperature resistance of quartz ceramics.

[0006] (II) Technical solution: A high-toughness and high-temperature resistant ceramic material, comprising the following raw materials: 100 parts by weight of quartz powder, 15-32 parts by weight of potassium feldspar, 0.8-2.2 parts by weight of nano zinc oxide, 3-6 parts by weight of boric acid, and 0.8-2 parts by weight of modified polysiloxane.

[0007] Furthermore, the preparation method of modified polysiloxane is as follows:

[0008] N,N-dimethylformamide, 100 parts by weight of 1,8-naphthalenedicarboxylic anhydride, and 66-72 parts by weight of 2-aminopentan-4-enoic acid were added to a flask. The mixture was stirred at 20-30°C for 3-4 hours. N,N-dimethylformamide was removed by vacuum distillation. The product was recrystallized in dichloromethane to give 2-(8-amido-1-naphthoic acid)pentan-4-enoic acid. The preparation reaction formula is as follows:

[0009]

[0010] Toluene, hydrogen-containing silicone oil, and 2-(8-amido-1-naphthoic acid)pent-4-enoic acid were added to a flask. Nitrogen gas was introduced, and the mixture was heated to the reaction temperature. An isopropanol solution containing chloroplatinic acid was added, and the mixture was stirred and distilled under reduced pressure to obtain the modified polysiloxane. The preparation reaction formula is as follows:

[0011]

[0012] Furthermore, the reaction temperature is 80-90℃, and the reaction time is 5-8 hours.

[0013] Furthermore, the amount of hydrogen-containing silicone oil is 100 parts by weight, the amount of 2-(8-amido-1-naphthoic acid)pent-4-enoic acid is 40-72 parts by weight, and the amount of chloroplatinic acid is 0.0018-0.0025 parts by weight.

[0014] Furthermore, the preparation method of the high-toughness and high-temperature resistant ceramic material is as follows: Quartz powder, potassium feldspar, nano zinc oxide, boric acid, modified polysiloxane, and water are added to a ball mill jar and ball-milled for 15-30 minutes. The mixture is then passed through a 100-300 mesh sieve, poured into a mold, and pressed into a blank at a pressure of 30-50 MPa. The blank is then dried in an oven at 80-110℃ for 6-12 hours. Finally, the blank is placed in a tube furnace and first heated to 1000-1200℃ in a nitrogen atmosphere at a heating rate of 2-5℃ / min, and calcined at that temperature for 1-2 hours. Then, the blank is heated to 1100-1400℃ in an air atmosphere, held at that temperature for 1-1.5 hours, and then cooled to obtain the high-toughness and high-temperature resistant ceramic material.

[0015] (III) Beneficial Technical Effects: This invention involves the addition reaction of 2-(8-amido-1-naphthoic acid)pent-4-enoic acid with hydrogen-containing silicone oil to obtain modified polysiloxane. This modified polysiloxane is then blended and calcined with quartz powder, potassium feldspar, boric acid, etc., to obtain quartz ceramic material. The side chains of this modified polysiloxane contain a large number of carboxyl groups, which form an interfacial interaction with the surfaces of quartz and potassium feldspar. This allows the polysiloxane segments to be adsorbed and coated on the surfaces of quartz and potassium feldspar, preventing particle agglomeration and acting as a dispersant. This makes the ceramic slurry form a more stable dispersion system, improves rheology, and is beneficial to improving the mechanical strength of the calcined ceramic material.

[0016] The modified polysiloxane of this invention contains a naphthalene ring structure with a high carbon content. After high-temperature calcination, using the polysiloxane as the silicon source and the naphthalene ring as the carbonization agent, high-temperature pyrolysis more easily forms a large amount of silicon carbide reinforcing phase, which is uniformly dispersed in the quartz ceramic matrix. This significantly improves the mechanical strength and toughness of the ceramic material, exhibiting higher flexural strength and fracture toughness. Even after high-temperature calcination at 1100-1400℃, this ceramic material still possesses high mechanical properties and excellent high-temperature resistance, making it well-suited for practical applications in heat-resistant ceramic lampshades and heat-resistant ceramic bases. Detailed Implementation

[0017] The embodiments described are provided to better illustrate the present invention, but are not intended to limit the scope of the invention to the embodiments described. Therefore, non-essential improvements and adjustments made to the embodiments by those skilled in the art based on the above description are still within the scope of protection of the present invention.

[0018] The following hydrogen-containing silicone oil is methyl hydrogen-containing silicone oil with a content of 99%, purchased from Jinan Jinshengyuan Chemical Technology Co., Ltd.

[0019] Example 1

[0020] (1) Add 60 mL of N,N-dimethylformamide, 5 g of 1,8-naphthalenedicarboxylic anhydride and 3.6 g of 2-aminopent-4-enoic acid to a flask, stir the reaction at 20 °C for 4 h, remove N,N-dimethylformamide by vacuum distillation, and recrystallize the product in dichloromethane to obtain 2-(8-amido-1-naphthoic acid)pent-4-enoic acid.

[0021] (2) Add 100 mL of toluene, 20 g of hydrogen-containing silicone oil, and 8 g (25.56 mmol) of 2-(8-amido-1-naphthoic acid)pent-4-enoic acid to a flask, purge with nitrogen, heat to 85 °C, add 40 μL of isopropanol solution containing 0.36 mg of chloroplatinic acid, stir and react for 5 h, remove low-boiling substances by vacuum distillation, and obtain modified polysiloxane.

[0022] (3) Add 1kg of quartz powder, 220g of potassium feldspar, 13g of nano zinc oxide, 30g of boric acid, 12g of modified polysiloxane, and 300mL of water to a ball mill jar and ball mill for 30min. Pass the mixture through a 100-mesh sieve, pour it into a mold, and press it into a blank with a pressure of 30MPa. Place it in an oven and dry it at 110℃ for 6h. Finally, place it in a tube furnace and heat it to 1200℃ in a nitrogen atmosphere at a heating rate of 2℃ / min. Hold it at this temperature for 1h. Then, heat it to 1400℃ in an air atmosphere and hold it for 1h. Cool it to obtain a high-toughness and high-temperature resistant ceramic material.

[0023] Example 2

[0024] (1) Add 50 mL of N,N-dimethylformamide, 5 g of 1,8-naphthalenedicarboxylic anhydride and 3.3 g of 2-aminopent-4-enoic acid to a flask, stir the reaction at 30 °C for 3 h, remove N,N-dimethylformamide by vacuum distillation, and recrystallize the product in dichloromethane to obtain 2-(8-amido-1-naphthoic acid)pent-4-enoic acid.

[0025] (2) Add 120 mL of toluene, 20 g of hydrogen-containing silicone oil, and 12.3 g of 2-(8-amido-1-naphthoic acid)pent-4-enoic acid to a flask, purge with nitrogen, heat to 80 °C, add 50 μL of isopropanol solution containing 0.45 mg of chloroplatinic acid, stir and react for 8 h, remove low-boiling substances by vacuum distillation, and obtain modified polysiloxane.

[0026] (3) Add 1kg of quartz powder, 320g of potassium feldspar, 8g of nano zinc oxide, 46g of boric acid, 20g of modified polysiloxane, and 300mL of water to a ball mill jar and ball mill for 30min. Then, pass the mixture through a 200-mesh sieve, pour it into a mold, and press it into a blank at a pressure of 30MPa. Place it in an oven and dry it at 100℃ for 8h. Finally, place it in a tube furnace and heat it to 1100℃ in a nitrogen atmosphere at a heating rate of 2℃ / min. Then, keep it at that temperature for 1h. Then, heat it to 1200℃ in an air atmosphere and keep it at that temperature for 1.5h. Cool it to obtain a high-toughness and high-temperature resistant ceramic material.

[0027] Example 3

[0028] (1) Add 150 mL of toluene, 20 g of hydrogen-containing silicone oil, and 14.4 g of 2-(8-amido-1-naphthoic acid)pent-4-enoic acid (prepared from Example 1) to a flask, purge with nitrogen, heat to 85 °C, add 50 μL of isopropanol solution containing 0.5 mg of chloroplatinic acid, stir and react for 8 h, remove low-boiling substances by vacuum distillation, and obtain modified polysiloxane.

[0029] (2) Add 1kg of quartz powder, 180g of potassium feldspar, 22g of nano zinc oxide, 60g of boric acid, 8g of modified polysiloxane, and 400mL of water to a ball mill jar and ball mill for 20min. Pass the mixture through a 100-mesh sieve, pour it into a mold, and press it into a blank with a pressure of 50MPa. Place it in an oven and dry it at 8℃ for 12h. Finally, place it in a tube furnace and heat it to 1000℃ in a nitrogen atmosphere at a heating rate of 2℃ / min. Hold it at this temperature for 2h. Then, heat it to 1100℃ in an air atmosphere and hold it for 1.5h. Cool it to obtain a high-toughness and high-temperature resistant ceramic material.

[0030] Example 4

[0031] (1) Add 100 mL of toluene, 20 g of hydrogen-containing silicone oil, and 10.3 g of 2-(8-amido-1-naphthoic acid)pent-4-enoic acid (prepared from Example 1) to a flask, purge with nitrogen, heat to 90 °C, add 40 μL of isopropanol solution containing 0.4 mg of chloroplatinic acid, stir and react for 6 h, remove low-boiling substances by vacuum distillation, and obtain modified polysiloxane.

[0032] (2) Add 1kg of quartz powder, 150g of potassium feldspar, 17g of nano zinc oxide, 53g of boric acid, 14g of modified polysiloxane, and 400mL of water to a ball mill jar and ball mill for 15min. Then, pass the mixture through a 300-mesh sieve, pour it into a mold, and press it into a blank with a pressure of 40MPa. Place it in an oven and dry it at 110℃ for 6h. Finally, place it in a tube furnace and heat it to 1000℃ in a nitrogen atmosphere at a heating rate of 5℃ / min. Then, keep it at that temperature for 2h. Then, heat it to 1300℃ in an air atmosphere and keep it at that temperature for 1h. Cool it to obtain a high-toughness and high-temperature resistant ceramic material.

[0033] Comparative Example 1

[0034] (1) Add 1kg of quartz powder, 220g of potassium feldspar, 13g of nano zinc oxide, 30g of boric acid and 300mL of water to a ball mill jar and ball mill for 30min. Then, pass the mixture through a 100-mesh sieve, pour it into a mold, and press it into a blank with a pressure of 30MPa. Place it in an oven and dry it at 110℃ for 6h. Finally, place it in a tube furnace and heat it to 1200℃ in a nitrogen atmosphere at a heating rate of 2℃ / min. Then, keep it at that temperature for 1h. Then, heat it to 1400℃ in an air atmosphere and keep it at that temperature for 1h. Cool it to obtain the ceramic material.

[0035] Comparative Example 2

[0036] (1) Add 1kg of quartz powder, 220g of potassium feldspar, 13g of nano zinc oxide, 30g of boric acid, 12g of hydrogen-containing silicone oil and 300mL of water to a ball mill jar and ball mill for 30min. Pass the mixture through a 100-mesh sieve, pour it into a mold, and press it into a blank with a pressure of 30MPa. Place it in an oven and dry it at 110℃ for 6h. Finally, place it in a tube furnace and heat it to 1200℃ in a nitrogen atmosphere at a heating rate of 2℃ / min. Hold it at this temperature for 1h. Then heat it to 1400℃ in an air atmosphere and hold it for 1h. Cool it to obtain the ceramic material.

[0037] Comparative Example 3

[0038] (1) Add 100 mL of toluene, 20 g of hydrogen-containing silicone oil and 2.2 g (25.56 mmol) of methacrylic acid to a flask, purge with nitrogen, heat to 85 °C, add 40 μL of isopropanol solution containing 0.36 mg of chloroplatinic acid, stir and react for 5 h, remove low-boiling substances by vacuum distillation to obtain modified polysiloxane.

[0039] (2) Add 1kg of quartz powder, 220g of potassium feldspar, 13g of nano zinc oxide, 30g of boric acid, 12g of modified polysiloxane, and 300mL of water to a ball mill jar and ball mill for 30min. Pass the mixture through a 100-mesh sieve, pour it into a mold, and press it into a blank at a pressure of 30MPa. Place it in an oven and dry it at 110℃ for 6h. Finally, place it in a tube furnace and heat it to 1200℃ in a nitrogen atmosphere at a heating rate of 2℃ / min. Hold it at this temperature for 1h. Then, heat it to 1400℃ in an air atmosphere and hold it for 1h. Cool it to obtain the ceramic material.

[0040] Comparative Example 4

[0041] (1) Add 60 mL of N,N-dimethylformamide, 3.74 g of phthalic anhydride, and 3.6 g of 2-aminopentan-4-enoic acid to a flask. Stir the mixture at 20 °C for 4 h. Remove the N,N-dimethylformamide by vacuum distillation. Recrystallize the product in dichloromethane to obtain 2-(2-amidobenzoic acid)pentan-4-enoic acid, with the structural formula:

[0042]

[0043] (2) Add 100 mL of toluene, 20 g of hydrogen-containing silicone oil, and 6.72 g (25.56 mmol) of 2-(2-amidobenzoic acid)pent-4-enoic acid to a flask, purge with nitrogen, heat to 85 °C, add 40 μL of isopropanol solution containing 0.36 mg of chloroplatinic acid, stir and react for 5 h, remove low-boiling substances by vacuum distillation, and obtain modified polysiloxane.

[0044] (3) Add 1kg of quartz powder, 220g of potassium feldspar, 13g of nano zinc oxide, 30g of boric acid, 12g of modified polysiloxane, and 300mL of water to a ball mill jar and ball mill for 30min. Pass the mixture through a 100-mesh sieve, pour it into a mold, and press it into a blank with a pressure of 30MPa. Place it in an oven and dry it at 110℃ for 6h. Finally, place it in a tube furnace and heat it to 1200℃ in a nitrogen atmosphere at a heating rate of 2℃ / min. Hold it at this temperature for 1h. Then, heat it to 1400℃ in an air atmosphere and hold it for 1h. Cool it to obtain the ceramic material.

[0045] The fracture toughness of ceramic materials was tested using the three-point bending method and a strength testing machine. Bending strength was tested according to the method specified in GB / T6569-2006.

[0046] Table 1 Properties of Ceramic Materials

[0047]

[0048] Compared with Comparative Example 1, the quartz ceramic materials of Examples 1-4 contain modified polysiloxanes. The side chains of these polysiloxanes contain a large number of carboxyl groups, which form an interfacial interaction with the surfaces of quartz and potassium feldspar. This allows the polysiloxane segments to be adsorbed and coated on the surfaces of quartz and potassium feldspar, preventing particle agglomeration and acting as a dispersant. This results in a more stable dispersion system for the ceramic slurry, improves rheology, and enhances the mechanical strength of the calcined ceramic material. Furthermore, the modified polysiloxanes contain a high-carbon naphthalene ring structure. After high-temperature calcination, with polysiloxanes as the silicon source and naphthalene rings as the carbonization, high-temperature pyrolysis more easily forms a large amount of silicon carbide reinforcing phase, which is uniformly dispersed in the quartz ceramic matrix. This significantly improves the mechanical strength and toughness of the ceramic material, exhibiting higher flexural strength and fracture toughness.

[0049] Comparative Example 2 only added hydrogen-containing silicone oil, which does not contain carboxyl groups and therefore cannot act as a dispersant. It also does not contain a high-carbon naphthalene ring structure, resulting in less silicon carbide reinforcing phase generated by high-temperature pyrolysis. This leads to poor mechanical strength and toughness of the ceramic material, as well as low flexural strength and fracture toughness.

[0050] Comparative Example 3 involved reacting methacrylic acid with hydrogen-containing silicone oil to obtain a modified polysiloxane with low carboxyl content and no high-carbon naphthalene ring structure, resulting in poor mechanical strength and toughness of the ceramic material, as well as low bending strength and fracture toughness.

[0051] Comparative Example 4 utilizes 2-(2-amidobenzoic acid)pent-4-enoic acid without naphthalene rings to react with hydrogen-containing silicone oil. The resulting modified polysiloxane has a lower carbon content than Example 1, and the silicon carbide reinforcing phase generated by high-temperature pyrolysis is less than that in Example 1. This results in poor mechanical strength and toughness of the ceramic material, as well as lower bending strength and fracture toughness.

[0052] Finally, it should be noted that the above embodiments are only used to illustrate the technical solutions of the present invention and not to limit it. Although the present invention has been described in detail with reference to preferred embodiments, those skilled in the art should understand that modifications or equivalent substitutions can be made to the technical solutions of the present invention without departing from the spirit and scope of the technical solutions of the present invention, and all such modifications or substitutions should be covered within the scope of the claims of the present invention.

Claims

1. A high-toughness, high-temperature resistant ceramic material, characterized in that, The high-toughness and high-temperature resistant ceramic material comprises the following raw materials: 100 parts by weight of quartz powder, 15-32 parts by weight of potassium feldspar, 0.8-2.2 parts by weight of nano zinc oxide, 3-6 parts by weight of boric acid, and 0.8-2 parts by weight of modified polysiloxane. The modified polysiloxane is prepared by adding toluene, hydrogen-containing silicone oil, and 2-(8-amido-1-naphthoic acid)pent-4-enoic acid to a flask, introducing nitrogen gas, heating to the reaction temperature, adding isopropanol solution containing chloroplatinic acid, stirring the reaction, and then distilling under reduced pressure to obtain the modified polysiloxane.

2. The high-toughness and high-temperature resistant ceramic material according to claim 1, characterized in that, The reaction temperature is 80-90℃, and the reaction time is 5-8 hours.

3. The high-toughness and high-temperature resistant ceramic material according to claim 1, characterized in that, The amount of the hydrogen-containing silicone oil is 100 parts by weight, the amount of 2-(8-amido-1-naphthoic acid)pent-4-enoic acid is 40-72 parts by weight, and the amount of chloroplatinic acid is 0.0018-0.0025 parts by weight.

4. The high-toughness and high-temperature resistant ceramic material according to claim 3, characterized in that, The preparation method of 2-(8-amido-1-naphthoic acid)pent-4-enoic acid is as follows: N,N-dimethylformamide, 100 parts by weight of 1,8-naphthalenedicarboxylic anhydride, and 66-72 parts by weight of 2-aminopent-4-enoic acid are added to a flask, and the mixture is stirred at 20-30°C for 3-4 hours. The mixture is then distilled under reduced pressure, and the product is recrystallized to obtain 2-(8-amido-1-naphthoic acid)pent-4-enoic acid.

5. A method for preparing a high-toughness, high-temperature resistant ceramic material as described in any one of claims 1-4, characterized in that, The preparation method is as follows: Quartz powder, potassium feldspar, nano zinc oxide, boric acid, modified polysiloxane, and water are added to a ball mill jar for ball milling, sieved, poured into a mold, pressed into a blank, dried, placed in a tube furnace, kept warm and calcined, and cooled to obtain a high-toughness and high-temperature resistant ceramic material.

6. The method for preparing the high-toughness and high-temperature resistant ceramic material according to claim 5, characterized in that, The ball milling time is 15-30 minutes, and the ball is passed through a 100-300 mesh sieve.

7. The method for preparing the high-toughness and high-temperature resistant ceramic material according to claim 5, characterized in that, The pressure for pressing the blank is 30-50 MPa; the drying temperature is 80-110℃, and the drying time is 6-12 hours.

8. The method for preparing the high-toughness and high-temperature resistant ceramic material according to claim 5, characterized in that, The heat preservation and calcination process is as follows: first, in a nitrogen atmosphere, the temperature is raised to 1000-1200℃ at a heating rate of 2-5℃ / min and held for 1-2 hours; then, in an air atmosphere, the temperature is raised to 1100-1400℃ and held for 1-1.5 hours.

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