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

Abstract

The invention 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, by weight, 100 parts of quartz powder, 15-32 parts of potassium feldspar, 3-6 parts of boric acid, 0.8-2 parts of modified polysiloxane and the like. And the side chain of the modified polysiloxane contains a large amount of carboxyl, and forms interfacial interaction with the surfaces of the quartz and the potassium feldspar, so that the effect of a dispersing agent is achieved, and the mechanical strength of the calcined ceramic material is favorably improved. Modified polysiloxane contains a naphthalene ring structure with high carbon content, after high-temperature calcination, polysiloxane is taken as a silicon source, naphthalene rings are carbonized, high-temperature pyrolysis is carried out, a large number of silicon carbide reinforced phases are more easily formed, the silicon carbide reinforced phases are uniformly dispersed in a quartz ceramic matrix, the mechanical strength and toughness of the ceramic material are remarkably improved, the high-temperature resistance is excellent, and the modified polysiloxane has good application prospects in heat-resistant ceramic lampshades, heat-resistant ceramic lampshades, heat-resistant ceramic lampshades and heat-resistant ceramic lampshades. The heat-resistant ceramic base has good practical application.

Description

Technical Field

[0001] The present invention relates to the technical field of ceramics, in particular to a high-toughness and high-temperature-resistant ceramic material and a preparation method thereof. Background Art

[0002] Quartz ceramics offer advantages such as excellent high-temperature resistance, high thermal shock stability, and low thermal conductivity and thermal expansion coefficient. They are widely used in lighting, building materials, photovoltaic panels, and refractory components. However, quartz ceramics currently suffer from low mechanical strength, and their strength and toughness deteriorate after high-temperature calcination. Adding a dispersant to the ceramic slurry can improve the slurry's viscosity and rheological properties, thereby enhancing the mechanical properties of the ceramic.

[0003] Silicone oil is a readily available, inexpensive polysiloxane-based material that can be pyrolyzed at high temperatures in an inert or ammonia atmosphere to produce high-performance Si-OC ceramics and Si-NC ceramics. Chinese patent application CN115557797A discloses a method for preparing a polyimide-modified interface and quartz / quartz composite material. The method uses polysiloxane as a silica precursor and polyimide as an interface material, blended with quartz fiber and boron nitride nanopowder, and then subjected to high-temperature treatment. The resulting ceramic material exhibits high density and flexural strength, but the patent fails to improve the toughness and high-temperature resistance of the quartz ceramic. Summary of the Invention

[0004] (1) Technical problems to be solved:

[0005] In view of the shortcomings of the existing technology, the present invention provides a high-toughness and high-temperature resistant ceramic material and a preparation method thereof, which solves the problems of poor toughness and high-temperature resistance of quartz ceramics.

[0006] (2) 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 the modified polysiloxane is:

[0008] Add N,N-dimethylformamide, 100 parts by weight of 1,8-naphthalene dicarboxylic anhydride, and 66-72 parts by weight of 2-aminopent-4-enoic acid to a flask, stir and react at 20-30°C for 3-4 hours, remove N,N-dimethylformamide by distillation under reduced pressure, and recrystallize the product from dichloromethane to obtain 2-(8-amido-1-naphthoic acid)pent-4-enoic acid. The preparation reaction formula is:

[0009]

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

[0011]

[0012] Furthermore, the reaction temperature is 80-90° C., and the reaction time is 5-8 h.

[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 and ball milled for 15-30 minutes, passed through a 100-300 mesh sieve, poured into a mold, and pressed into a blank at a pressure of 30-50 MPa; placed in an oven at 80-110°C and dried for 6-12 hours; finally placed in a tubular furnace, first in a nitrogen atmosphere, at a heating rate of 2-5°C / min, heated to 1000-1200°C, and kept warm for calcining for 1-2 hours; then in an air atmosphere, heated to 1100-1400°C, kept warm for 1-1.5 hours, and cooled to obtain a high-toughness and high-temperature resistant ceramic material.

[0015] (3) Beneficial technical effects: The present invention conducts an addition reaction between 2-(8-amido-1-naphthoic acid)pent-4-enoic acid and hydrogenated silicone oil to obtain a modified polysiloxane, which is then blended and calcined with quartz powder, potassium feldspar, boric acid, etc. to obtain a quartz ceramic material. The side chain of the modified polysiloxane contains a large number of carboxyl groups, which form an interfacial interaction with the surface of quartz and potassium feldspar, so that the polysiloxane chain segments are adsorbed and coated on the surface of quartz and potassium feldspar, preventing the agglomeration of particles and acting as a dispersant, so that the ceramic slurry forms a more stable dispersion system, improves the rheological properties, and is beneficial to improving the mechanical strength of the ceramic material after calcination.

[0016] The modified polysiloxane of the present invention contains a naphthalene ring structure with a high carbon content. After high-temperature calcination, the polysiloxane serves as a silicon source, and the naphthalene rings are carbonized. High-temperature pyrolysis easily forms a large amount of silicon carbide reinforcement phase, which is evenly 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. This ceramic material, even after high-temperature calcination at 1100-1400°C, still maintains high mechanical properties and excellent high-temperature resistance, and has good practical applications in heat-resistant ceramic lampshades and heat-resistant ceramic bases. DETAILED DESCRIPTION

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

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

[0019] Example 1

[0020] (1) 60 mL of N,N-dimethylformamide, 5 g of 1,8-naphthalene dicarboxylic anhydride, and 3.6 g of 2-aminopent-4-enoic acid were added to a flask and stirred at 20°C for 4 h. N,N-dimethylformamide was removed by distillation under reduced pressure, and the product was recrystallized from dichloromethane to obtain 2-(8-amido-1-naphthoic acid)pent-4-enoic acid.

[0021] (2) To a flask, 100 mL of toluene, 20 g of hydrogenated silicone oil, and 8 g (25.56 mmol) of 2-(8-amido-1-naphthoic acid)pent-4-enoic acid were added, nitrogen was introduced, and the mixture was heated to 85°C. 40 μL of an isopropanol solution containing 0.36 mg of chloroplatinic acid was added, and the mixture was stirred for 5 h. Low-boiling substances were removed by distillation under reduced pressure to obtain a modified polysiloxane.

[0022] (3) 1 kg of quartz powder, 220 g of potassium feldspar, 13 g of nano zinc oxide, 30 g of boric acid, 12 g of modified polysiloxane, and 300 mL of water were added to a ball mill and ball milled for 30 min. The mixture was passed through a 100-mesh sieve, poured into a mold, and pressed into a blank at a pressure of 30 MPa. The blank was placed in an oven at 110 °C for 6 h. Finally, the blank was placed in a tubular furnace and heated to 1200 °C at a heating rate of 2 °C / min in a nitrogen atmosphere and calcined for 1 h. The blank was then heated to 1400 °C in an air atmosphere, kept warm for 1 h, and cooled to obtain a high-toughness and high-temperature resistant ceramic material.

[0023] Example 2

[0024] (1) 50 mL of N,N-dimethylformamide, 5 g of 1,8-naphthalene dicarboxylic anhydride, and 3.3 g of 2-aminopent-4-enoic acid were added to a flask and stirred at 30°C for 3 h. N,N-dimethylformamide was removed by distillation under reduced pressure, and the product was recrystallized from dichloromethane to obtain 2-(8-amido-1-naphthoic acid)pent-4-enoic acid.

[0025] (2) 120 mL of toluene, 20 g of hydrogenated silicone oil, and 12.3 g of 2-(8-amido-1-naphthoic acid)pent-4-enoic acid were added to a flask, nitrogen was introduced, and the mixture was heated to 80°C. 50 μL of an isopropanol solution containing 0.45 mg of chloroplatinic acid was added, and the mixture was stirred for 8 h. Low-boiling substances were removed by distillation under reduced pressure to obtain a modified polysiloxane.

[0026] (3) 1 kg of quartz powder, 320 g of potassium feldspar, 8 g of nano zinc oxide, 46 g of boric acid, 20 g of modified polysiloxane, and 300 mL of water were added to a ball mill and ball milled for 30 min. The mixture was passed through a 200-mesh sieve, poured into a mold, and pressed into a blank at a pressure of 30 MPa. The blank was placed in an oven at 100 °C for 8 h. Finally, the blank was placed in a tubular furnace and heated to 1100 °C at a heating rate of 2 °C / min in a nitrogen atmosphere and calcined for 1 h. The blank was then heated to 1200 °C in an air atmosphere, kept warm for 1.5 h, and cooled to obtain a high-toughness and high-temperature resistant ceramic material.

[0027] Example 3

[0028] (1) To a flask, 150 mL of toluene, 20 g of hydrogenated silicone oil, and 14.4 g of 2-(8-amido-1-naphthoic acid)pent-4-enoic acid (prepared in Example 1) were added, nitrogen was introduced, and the mixture was heated to 85° C. 50 μL of an isopropanol solution containing 0.5 mg of chloroplatinic acid was added. The mixture was stirred for 8 h, and low-boiling substances were removed by distillation under reduced pressure to obtain a modified polysiloxane.

[0029] (2) 1 kg of quartz powder, 180 g of potassium feldspar, 22 g of nano zinc oxide, 60 g of boric acid, 8 g of modified polysiloxane, and 400 mL of water were added to a ball mill and ball milled for 20 min. The mixture was passed through a 100-mesh sieve, poured into a mold, and pressed into a blank at a pressure of 50 MPa. The blank was placed in an oven at 8 ° C for 12 h. Finally, the blank was placed in a tubular furnace and heated to 1000 ° C at a heating rate of 2 ° C / min in a nitrogen atmosphere and calcined for 2 h. The blank was then heated to 1100 ° C in an air atmosphere, kept warm for 1.5 h, and cooled to obtain a high-toughness and high-temperature resistant ceramic material.

[0030] Example 4

[0031] (1) To a flask, 100 mL of toluene, 20 g of hydrogenated silicone oil, and 10.3 g of 2-(8-amido-1-naphthoic acid)pent-4-enoic acid (prepared in Example 1) were added, nitrogen was introduced, and the mixture was heated to 90° C. 40 μL of an isopropanol solution containing 0.4 mg of chloroplatinic acid was added. The mixture was stirred for 6 h, and low-boiling substances were removed by distillation under reduced pressure to obtain a modified polysiloxane.

[0032] (2) 1 kg of quartz powder, 150 g of potassium feldspar, 17 g of nano zinc oxide, 53 g of boric acid, 14 g of modified polysiloxane, and 400 mL of water were added to a ball mill and ball milled for 15 min. The mixture was sieved through a 300-mesh sieve, poured into a mold, and pressed into a blank at a pressure of 40 MPa. The blank was placed in an oven at 110 °C for 6 h. Finally, the blank was placed in a tubular furnace and heated to 1000 °C at a heating rate of 5 °C / min in a nitrogen atmosphere and calcined for 2 h. The blank was then heated to 1300 °C in an air atmosphere, kept warm for 1 h, and cooled to obtain a high-toughness and high-temperature resistant ceramic material.

[0033] Comparative Example 1

[0034] (1) 1 kg of quartz powder, 220 g of potassium feldspar, 13 g of nano zinc oxide, 30 g of boric acid, and 300 mL of water were added to a ball mill and ball milled for 30 min. The mixture was passed through a 100-mesh sieve, poured into a mold, and pressed into a blank at a pressure of 30 MPa. The blank was placed in an oven and dried at 110 °C for 6 h. Finally, the blank was placed in a tubular furnace and heated to 1200 °C at a heating rate of 2 °C / min in a nitrogen atmosphere and calcined for 1 h. The blank was then heated to 1400 °C in an air atmosphere, kept at this temperature for 1 h, and cooled to obtain a ceramic material.

[0035] Comparative Example 2

[0036] (1) 1 kg of quartz powder, 220 g of potassium feldspar, 13 g of nano zinc oxide, 30 g of boric acid, 12 g of hydrogenated silicone oil, and 300 mL of water were added to a ball mill and ball milled for 30 min. The mixture was passed through a 100-mesh sieve, poured into a mold, and pressed into a blank at a pressure of 30 MPa. The blank was placed in an oven and dried at 110 °C for 6 h. Finally, the blank was placed in a tubular furnace and heated to 1200 °C at a heating rate of 2 °C / min in a nitrogen atmosphere and calcined for 1 h. The blank was then heated to 1400 °C in an air atmosphere, kept warm for 1 h, and cooled to obtain a ceramic material.

[0037] Comparative Example 3

[0038] (1) To a flask, 100 mL of toluene, 20 g of hydrogenated silicone oil, and 2.2 g (25.56 mmol) of methacrylic acid were added, nitrogen was introduced, and the mixture was heated to 85°C. 40 μL of an isopropanol solution containing 0.36 mg of chloroplatinic acid was added, and the mixture was stirred for 5 h. Low-boiling substances were removed by distillation under reduced pressure to obtain a modified polysiloxane.

[0039] (2) 1 kg of quartz powder, 220 g of potassium feldspar, 13 g of nano zinc oxide, 30 g of boric acid, 12 g of modified polysiloxane, and 300 mL of water were added to a ball mill and ball milled for 30 min. The mixture was passed through a 100-mesh sieve, poured into a mold, and pressed into a blank at a pressure of 30 MPa. The blank was placed in an oven and dried at 110 °C for 6 h. Finally, the blank was placed in a tubular furnace and heated to 1200 °C at a heating rate of 2 °C / min in a nitrogen atmosphere and calcined for 1 h. The blank was then heated to 1400 °C in an air atmosphere, kept warm for 1 h, and cooled to obtain a ceramic material.

[0040] Comparative Example 4

[0041] (1) 60 mL of N,N-dimethylformamide, 3.74 g of phthalic anhydride, and 3.6 g of 2-aminopent-4-enoic acid were added to a flask, and the mixture was stirred at 20°C for 4 h. N,N-dimethylformamide was removed by distillation under reduced pressure, and the product was recrystallized from dichloromethane to obtain 2-(2-amidobenzoic acid)pent-4-enoic acid, with the structural formula:

[0042]

[0043] (2) To a flask, 100 mL of toluene, 20 g of hydrogenated silicone oil, and 6.72 g (25.56 mmol) of 2-(2-amidobenzoic acid)pent-4-enoic acid were added, nitrogen was introduced, and the mixture was heated to 85°C. 40 μL of an isopropanol solution containing 0.36 mg of chloroplatinic acid was added, and the mixture was stirred for 5 h. Low-boiling substances were removed by distillation under reduced pressure to obtain a modified polysiloxane.

[0044] (3) 1 kg of quartz powder, 220 g of potassium feldspar, 13 g of nano zinc oxide, 30 g of boric acid, 12 g of modified polysiloxane, and 300 mL of water were added to a ball mill and ball milled for 30 min. The mixture was passed through a 100-mesh sieve, poured into a mold, and pressed into a blank at a pressure of 30 MPa. The blank was placed in an oven and dried at 110 °C for 6 h. Finally, the blank was placed in a tubular furnace and heated to 1200 °C at a heating rate of 2 °C / min in a nitrogen atmosphere and calcined for 1 h. The blank was then heated to 1400 °C in an air atmosphere, kept warm for 1 h, and cooled to obtain a ceramic material.

[0045] The fracture toughness of ceramic materials was tested using a three-point bending method and a strength testing machine. The 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, modified polysiloxane is added to the quartz ceramic materials of Examples 1 to 4, and its side chains contain a large number of carboxyl groups, which form interfacial interactions with the surfaces of quartz and potassium feldspar, so that the polysiloxane chain segments are adsorbed and coated on the surfaces of quartz and potassium feldspar, preventing the agglomeration of particles, and can act as a dispersant, so that the ceramic slurry forms a more stable dispersion system, improves the rheological properties, and is beneficial to improving the mechanical strength of the ceramic material after calcination. In addition, the modified polysiloxane contains a naphthalene ring structure with a high carbon content. After high-temperature calcination, with polysiloxane as the silicon source and the naphthalene ring as carbonized, high-temperature pyrolysis makes it easier to form a large amount of silicon carbide reinforcement phase, which is evenly dispersed in the quartz ceramic matrix, significantly improving the mechanical strength and toughness of the ceramic material, and exhibiting higher bending strength and fracture toughness.

[0049] In Comparative Example 2, only hydrogenated silicone oil is added, which does not contain carboxyl groups and cannot act as a dispersant. It also does not contain a naphthalene ring structure with a high carbon content. The silicon carbide reinforcing phase generated by high-temperature pyrolysis is small, resulting in poor mechanical strength and toughness of the ceramic material, and low bending strength and fracture toughness.

[0050] Comparative Example 3 uses methacrylic acid to react with hydrogenated silicone oil, and the resulting modified polysiloxane has a low carboxyl content and does not contain a naphthalene ring structure with a high carbon content, resulting in poor mechanical strength and toughness of the ceramic material, and low bending strength and fracture toughness.

[0051] In Comparative Example 4, 2-(2-amidobenzoic acid)pent-4-enoic acid without a naphthalene ring is reacted with hydrogenated silicone oil. The carbon content of the obtained modified polysiloxane is lower than that of Example 1, and the silicon carbide reinforcing phase generated by high-temperature pyrolysis is less than that of Example 1, resulting in poor mechanical strength and toughness of the ceramic material, and low 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 are not limiting. Although the present invention has been described in detail with reference to the preferred embodiments, those skilled in the art should understand that the technical solutions of the present invention may be modified or replaced by equivalents without departing from the purpose and scope of the technical solutions of the present invention, which should all be covered by the scope of the claims of the present invention.

Claims

1. A high-toughness and 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 preparation method comprises the following steps: adding toluene, hydrogenated silicone oil, and 2-(8-amido-1-naphthoic acid)pent-4-enoic acid into a flask, introducing nitrogen, heating to a reaction temperature, adding an isopropanol solution containing chloroplatinic acid, stirring for reaction, and then performing reduced pressure distillation 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° C., and the reaction time is 5-8 h.

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 comprises: adding N,N-dimethylformamide, 100 parts by weight of 1,8-naphthalic anhydride, and 66-72 parts by weight of 2-aminopent-4-enoic acid into a flask, stirring and reacting at 20-30° C. for 3-4 hours, performing distillation under reduced pressure, and recrystallizing the product 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 according to any one of claims 1 to 4, characterized in that: The preparation method comprises the following steps: adding quartz powder, potassium feldspar, nano zinc oxide, boric acid, modified polysiloxane and water into a ball mill, performing ball milling, sieving, pouring into a mold, pressing into a blank, drying, placing in a tube furnace, calcining at a heat preservation temperature, and cooling to obtain a high-toughness and high-temperature resistant ceramic material.

6. The method for preparing a 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 product is passed through a 100-300 mesh sieve.

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

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

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