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CN113788683A - A kind of preparation method of SiC ceramic powder - Google Patents

A kind of preparation method of SiC ceramic powder Download PDF

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CN113788683A
CN113788683A CN202111155379.XA CN202111155379A CN113788683A CN 113788683 A CN113788683 A CN 113788683A CN 202111155379 A CN202111155379 A CN 202111155379A CN 113788683 A CN113788683 A CN 113788683A
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silicon carbide
sic
ceramic powder
polyethylene glycol
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刘世凯
宋志健
陈颖鑫
王嘉琳
张玥
杜晓双
顾磊磊
李芳润
孙亚光
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Henan University of Technology
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    • C04B35/622Forming processes; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
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    • C04B2235/02Composition of constituents of the starting material or of secondary phases of the final product
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Abstract

本发明提供了一种SiC陶瓷粉体的制备方法,属于无机非金属材料和纳米复合材料领域。具体制备方法的步骤为:将碳化硅微粉加入到乙醇水溶液中,超声搅拌1~2h;在上述混合溶液中配制SiO2溶胶,干燥后得到纳米包覆的碳化硅颗粒;将聚乙二醇10000加入到无水乙醇中,超声搅拌0.5~1h后,加入处理后的碳化硅颗粒,磁力搅拌1~2h,干燥后加入PVA混合均匀,密封静置后,进行制粒干燥,将这些SiC颗粒在1200~1500℃真空下进行热处理2~3h,冷却至室温后,在500~600℃进行无压热处理2~3h,得到粒度再造的SiC陶瓷粉体。本发明通过加入SiO2溶胶和聚乙二醇10000的方式,大大降低了烧结温度,并且粒度再造后的陶瓷粉体,纯度高、使用性能优良,很好的解决了废弃碳化硅粉体在陶瓷方面利用的问题。The invention provides a preparation method of SiC ceramic powder, which belongs to the field of inorganic non-metallic materials and nano-composite materials. The steps of the specific preparation method are as follows: adding silicon carbide micropowder into an aqueous ethanol solution, and ultrasonically stirring for 1-2 hours; preparing a SiO 2 sol in the above mixed solution, and drying to obtain nano-coated silicon carbide particles; adding polyethylene glycol 10000 Add to absolute ethanol, after ultrasonic stirring for 0.5~1h, add the treated silicon carbide particles, stir magnetically for 1~2h, add PVA after drying and mix evenly, seal and let stand, granulate and dry, and put these SiC particles in Heat treatment under vacuum at 1200~1500°C for 2~3h, and after cooling to room temperature, pressureless heat treatment at 500~600°C for 2~3h to obtain SiC ceramic powder with reconstituted particle size. The present invention greatly reduces the sintering temperature by adding SiO 2 sol and polyethylene glycol 10000, and the reconstituted ceramic powder has high purity and excellent performance. aspects of use.

Description

Preparation method of SiC ceramic powder
Technical Field
The invention belongs to the field of inorganic non-metallic materials and nano composite materials, and particularly relates to a preparation method of SiC ceramic powder.
Background
Silicon carbide ceramic as a novel structural ceramic material has properties incomparable with structural materials such as a plurality of metals and the like: the high-temperature-resistant high-strength wear-resistant high-temperature-resistant high-hardness high-wear-resistant high-corrosion-resistance high-hardness high-wear-resistant high-corrosion-resistance high-hardness high-creep-resistance high-wear-resistance high-corrosion-resistance high-hardness high-creep-resistance high-wear-resistance high-corrosion-resistance high-wear-resistance high-hardness high-wear-resistance high-corrosion-resistance high-hardness high-creep-resistance high-wear-resistance high-corrosion-resistance high-hardness high-creep-resistance high-toughness high-creep-resistance high-corrosion-resistance high-hardness high-resistance high-creep-resistance high-corrosion-resistance high-hardness high-resistance high-wear-resistance high-hardness high-resistance high-creep-resistance high-corrosion-resistance high-hardness high-creep-corrosion-resistance high-hardness high-corrosion-resistance high-wear-resistance high-hardness high-corrosion-resistance high-hardness high-resistance high-creep-resistance high-hardness high-creep-hardness high-resistance creep-wear-resistance high-hardness high-resistance high-hardness high-resistance creep-resistance high-creep-resistance high-hardness high-resistance high-hardness high-wear-resistance high-toughness high-resistance high-hardness high-resistance high-hardness high-.
The grain size of silicon carbide has a very important influence on its own applications. The application of silicon carbide in ceramics is common, the silicon carbide ceramics has good performance but is difficult to sinter and densify, and if the granularity of the silicon carbide micro powder used in the preparation of the ceramics is small, the silicon carbide micro powder is not beneficial to molding and the usability of the sintered product is not good. In the preparation process of silicon carbide, a plurality of superfine silicon carbide micro-powders are often generated, and the silicon carbide micro-powders cannot be effectively utilized due to the excessively fine particle size, so that the production cost is increased and certain environmental pollution is caused. The silicon carbide powder with ultra-fine granularity can meet the basic granularity requirement of the ceramic material through granularity reconstruction, thereby more effectively utilizing resources and reducing production cost.
Disclosure of Invention
In order to solve the problems in the production and application of silicon carbide, the invention uses SiO2The sol, the polyethylene glycol and the PVA are used as additives, and the preparation method of the SiC ceramic powder is provided.
Specifically, the preparation method of the SiC ceramic powder provided by the invention is implemented according to the following steps:
s1: weighing a certain amount of silicon carbide micro powder, adding the silicon carbide micro powder in S2 into an ethanol aqueous solution under the condition of ultrasonic stirring, continuously stirring for 1-2 hours until the silicon carbide micro powder is fully dispersed, wherein the volume ratio of absolute ethanol to water in the absolute ethanol aqueous solution is 1-3: 1, taking the mass ratio of the volume of the absolute ethyl alcohol to the silicon carbide micro powder as 0.2-1 ml: 1g of a compound;
s2: preparing nano-coated silicon carbide particles;
s21: adding tetraethoxysilane into the SiC mixed solution of S1 under the condition of ultrasonic stirring, wherein SiO contained in the tetraethoxysilane2The mass ratio of the amount of the silicon carbide to the silicon carbide in S1 is 3-10%, continuously stirring, adding glacial acetic acid to adjust the pH value to 1-3, fully reacting for 2-6 h, and drying at 80-120 ℃ for 4-8 h to obtain nano-coated silicon carbide particles;
s3: adding polyethylene glycol 10000 into 10-15 ml of absolute ethyl alcohol under the condition of ultrasonic stirring, wherein the molar ratio of the C content in the polyethylene glycol 10000 to the Si content in ethyl orthosilicate in S21 is 1.2-2, and continuously stirring for 0.5-1 h until the mixture is fully dispersed;
s4, adding the silicon carbide particles coated with the nano particles in the S21 into a mixed solution of S3 polyethylene glycol 10000 under the condition of magnetic stirring, continuously and magnetically stirring for 1-2 hours until the silicon carbide particles are fully dispersed, and drying the mixture for 3-5 hours at 100-150 ℃ to obtain silicon carbide mixed powder;
s5: adding PVA into the silicon carbide mixed powder of S4, wherein the mass percentage of the PVA to the silicon carbide mixed powder of S4 is 3-5%, mechanically stirring for 1-2 h, sealing and standing for 5-10 h after uniform mixing to obtain a SiC micropowder mixture;
s6: pouring the uniformly mixed powder in the S5 into a granulator for granulation to obtain SiC granules with uniform size and granularity ranging from 10 to 200 mu m, and drying the SiC granules at the temperature of 90 to 100 ℃ for 1 to 2 hours to obtain SiC granules with proper humidity;
s7: and (3) putting the silicon carbide particles treated in the step (S6) into a high-temperature vacuum atmosphere furnace for sintering, carrying out heat treatment for 2-3 h at 1300-1500 ℃, cooling to room temperature, putting into a muffle furnace for carrying out heat treatment for 2-3 h at 500-600 ℃, and then obtaining SiC ceramic powder with reconstructed particle size.
Preferably, the particle size of the SiC micropowder used in S1 is 0.5-3 μm.
Preferably, SiO contained in the tetraethoxysilane used in S212The mass ratio of the amount of the silicon carbide to the silicon carbide in the S1 is 3% -10%.
Preferably, the molar ratio of the content of C in polyethylene glycol 10000 used in S3 to the content of Si in tetraethoxysilane used in S21 is 1.2-2, and the organic carbon source polyethylene glycol 10000 can be replaced by polyethylene glycol 2000, polyethylene glycol 6000, polyethylene glycol 20000, glucose and the like.
Preferably, the sintering temperature of the SiC particles in S7 is 1300-1500 ℃, and the sintering atmosphere can be vacuum argon protection and vacuum nitrogen protection; the temperature of the secondary heat treatment is 500-600 ℃.
The silicon carbide ceramic powder with reconstructed granularity prepared by the method has high purity, low porosity and excellent use performance.
The silicon carbide ceramic powder with the reconstructed granularity prepared by the method is widely applied, in particular to the application in the fields of high-temperature corrosion resistance, national defense and military industry, special ceramics and the like.
The technical scheme of the invention has the following beneficial effects:
the invention firstly provides a preparation method of SiC ceramic powder, which utilizes polyethylene glycol 10000 and SiO2The sol and PVA are used as additives, and the problem that the silicon carbide micro powder cannot be utilized due to the excessively fine granularity is solved. Nano SiO2The addition of the sol and the polyethylene glycol 10000 reduces the sintering temperature, and the ceramic powder after particle size reconstruction has high purity, low porosity and excellent service performance, thereby well solving the problem of recycling the waste silicon carbide powder in the aspect of ceramics. The preparation method of the SiC ceramic powder provided by the invention can be well applied to other types of ceramic micro powder, and has good practicability.
Detailed Description
The present invention is further described with reference to the following specific examples, which should be construed by those skilled in the art as being illustrative and not limiting.
All technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art. In the following examples, unless otherwise specified, the methods used were all conventional methods, and the starting materials used were all commercially available analytical pure materials. Without limiting the invention thereto, one skilled in the art can, in light of the present disclosure and knowledge of the prior art, use similar methods, apparatus, materials to practice the invention repeatedly.
The following specifically exemplifies the technical solution of the present invention.
Example 1
A preparation method of SiC ceramic powder comprises the following specific steps:
s1: weighing 30g of silicon carbide micro powder, adding the silicon carbide micro powder in S2 into 30ml of ethanol aqueous solution under the condition of ultrasonic stirring, and continuously stirring for 2h until the silicon carbide micro powder is fully dispersed, wherein the volume ratio of absolute ethanol to water in the absolute ethanol aqueous solution is 1.5: 1, taking the mass ratio of the volume of the absolute ethyl alcohol to the silicon carbide micro powder as 1 ml: 1g of a compound;
s2: preparing nano-coated silicon carbide particles;
s21: adding tetraethoxysilane into the SiC mixed solution of S1 under the condition of ultrasonic stirring, wherein SiO contained in the tetraethoxysilane2The mass ratio of the amount of the silicon carbide to the silicon carbide in S1 is 5%, the stirring is continued, glacial acetic acid is added to adjust the PH value to 2, the mixture is fully reacted for 6 hours, and the mixture is dried for 8 hours at 80 ℃ to obtain nano-coated silicon carbide particles;
s3: adding polyethylene glycol 10000 into 15ml of absolute ethyl alcohol under the condition of ultrasonic stirring, wherein the molar ratio of the C content in the polyethylene glycol 10000 to the Si content in the tetraethoxysilane in S21 is 1.5, and continuously stirring for 1h until the mixture is fully dispersed;
s4, adding the silicon carbide particles coated with the nano particles in the S21 into a mixed solution of S3 polyethylene glycol 10000 under the condition of magnetic stirring, continuously and magnetically stirring for 2 hours until the silicon carbide particles are fully dispersed, and drying the mixture for 5 hours at 100 ℃ to obtain silicon carbide mixed powder;
s5: adding PVA into the silicon carbide mixed powder of S4, wherein the mass percentage of the PVA to the silicon carbide mixed powder of S4 is 5%, mechanically stirring for 1h, uniformly mixing, sealing and standing for 10h to obtain a SiC micro powder mixture;
s6: pouring the powder uniformly mixed in the S5 into a granulator for granulation to obtain SiC granules with uniform size and granularity of 15 mu m, and drying at 90 ℃ for 1h to obtain SiC granules with proper humidity;
s7: and (3) putting the silicon carbide particles treated in the step (S6) into a high-temperature vacuum atmosphere furnace for sintering, carrying out heat treatment for 3h at 1450 ℃, cooling to room temperature, putting into a muffle furnace for carrying out heat treatment for 2h at 500 ℃, and then obtaining SiC ceramic powder with reconstructed particle size.
Example 2
A preparation method of SiC ceramic powder comprises the following specific steps:
s1: weighing 30g of silicon carbide micro powder, adding the silicon carbide micro powder in S2 into 20ml of ethanol aqueous solution under the condition of ultrasonic stirring, and continuously stirring for 2h until the silicon carbide micro powder is fully dispersed, wherein the volume ratio of absolute ethanol to water in the absolute ethanol aqueous solution is 2: 1, taking the mass ratio of the volume of the absolute ethyl alcohol to the silicon carbide micro powder as 1 ml: 1g of a compound;
s2: preparing nano-coated silicon carbide particles;
s21: adding tetraethoxysilane into the SiC mixed solution of S1 under the condition of ultrasonic stirring, wherein SiO contained in the tetraethoxysilane2The mass ratio of the amount of the silicon carbide to the silicon carbide in S1 is 7%, the stirring is continued, glacial acetic acid is added to adjust the PH value to 3, the mixture is dried for 8 hours at 80 ℃ after the full reaction for 6 hours, and the nano-coated silicon carbide particles are obtained;
s3: adding polyethylene glycol 10000 into 15ml of absolute ethyl alcohol under the condition of ultrasonic stirring, wherein the molar ratio of the C content in the polyethylene glycol 10000 to the Si content in the tetraethoxysilane in S21 is 1.5, and continuously stirring for 1h until the mixture is fully dispersed;
s4, adding the silicon carbide particles coated with the nano particles in the S21 into a mixed solution of S3 polyethylene glycol 10000 under the condition of magnetic stirring, continuously and magnetically stirring for 1h until the silicon carbide particles are fully dispersed, and drying the mixture for 5h at 100 ℃ to obtain silicon carbide mixed powder;
s5: adding PVA into the silicon carbide mixed powder of S4, wherein the mass percentage of the PVA to the silicon carbide mixed powder of S4 is 5%, mechanically stirring for 1h, uniformly mixing, sealing and standing for 10h to obtain a SiC micro powder mixture;
s6: pouring the powder uniformly mixed in the S5 into a granulator for granulation to obtain SiC granules with uniform size and granularity of 20 mu m, and drying at 90 ℃ for 1h to obtain SiC granules with proper humidity;
s7: and (3) putting the silicon carbide particles treated in the step (S6) into a high-temperature vacuum atmosphere furnace for sintering, carrying out heat treatment for 3h at 1450 ℃, cooling to room temperature, putting into a muffle furnace for carrying out heat treatment for 2h at 500 ℃, and then obtaining SiC ceramic powder with reconstructed particle size.
The SiC ceramic powder prepared in the embodiment 1 and the embodiment 2 has the advantages of stable process, reliable quality and excellent performance. For example, SiC ceramic is prepared by selecting SiC particles with the particle sizes of 15 μm and 20 μm prepared in the example 1 and the example 2, and compared with SiC ceramic prepared by SiC powder with the same particle size in the market, the sintering temperature is low; the sintering temperature of the SiC ceramics prepared in the embodiment 1 and the embodiment 2 is respectively reduced by 50 ℃ and 40 ℃, and the strength is respectively improved by 2 percent and 3 percent; the ceramic powder prepared by the invention has good molding fluidity and higher density.
The above-mentioned embodiments are merely preferred embodiments for fully illustrating the present invention, and the scope of protection is not limited thereto. The equivalents and modifications of the present invention which may occur to those skilled in the art are within the scope of the present invention as defined by the appended claims.

Claims (7)

1.一种SiC陶瓷粉体的制备方法,其特征在于,具体实施步骤如下:1. a preparation method of SiC ceramic powder, is characterized in that, concrete steps are as follows: S1:称取一定量的碳化硅微粉,在超声搅拌的条件下将S2中的碳化硅微粉加入到乙醇的水溶液中,持续搅拌1~2h至充分分散,无水乙醇的水溶液中无水乙醇与水的体积比在1~3:1,取用无水乙醇的体积与碳化硅微粉的质量比为0.2~1ml:1g;S1: Weigh a certain amount of silicon carbide micropowder, add the silicon carbide micropowder in S2 to the aqueous solution of ethanol under the condition of ultrasonic stirring, continue to stir for 1~2h to fully disperse, and the anhydrous ethanol and the anhydrous ethanol in the aqueous solution of anhydrous ethanol are mixed with The volume ratio of water is 1~3:1, and the volume ratio of absolute ethanol to the mass ratio of silicon carbide micropowder is 0.2~1ml:1g; S2:制备纳米包覆的碳化硅颗粒;S2: prepare nano-coated silicon carbide particles; S21:将正硅酸乙酯在超声搅拌的条件下加入到S1的SiC混合液中,正硅酸乙酯中所含的SiO2量与S1中碳化硅的质量比在3%~10%,持续搅拌,加入冰醋酸调节PH值至1~3,充分反应2~6h后,在80~120℃下干燥4~8h,得到纳米包覆的碳化硅颗粒;S21: adding tetraethyl orthosilicate to the SiC mixed solution of S1 under the condition of ultrasonic stirring, the mass ratio of the amount of SiO2 contained in the ethyl orthosilicate to the silicon carbide in S1 is 3%~10%, Continue stirring, add glacial acetic acid to adjust the pH to 1~3, fully react for 2~6h, and then dry at 80~120°C for 4~8h to obtain nano-coated silicon carbide particles; S3:将聚乙二醇10000在超声搅拌的条件下加入到10~15ml无水乙醇中,聚乙二醇10000中的含C量与S21中正硅酸乙酯含Si量的摩尔比为1.2~2,持续搅拌0.5~1h至充分分散;S3: The polyethylene glycol 10000 is added to 10~15ml of absolute ethanol under the condition of ultrasonic stirring, and the molar ratio of the C content in the polyethylene glycol 10000 to the Si content of the ethyl orthosilicate in S21 is 1.2~ 2. Continue stirring for 0.5~1h until fully dispersed; S4:将S21中纳米包覆的碳化硅颗粒在磁力搅拌的条件下加入到S3聚乙二醇10000的混合溶液中,持续磁力搅拌1~2h至充分分散,在100~150℃干燥3~5h,得到碳化硅混合粉料;S4: Add the nano-coated silicon carbide particles in S21 to the mixed solution of S3 polyethylene glycol 10000 under the condition of magnetic stirring, continue magnetic stirring for 1~2h until fully dispersed, and dry at 100~150 ℃ for 3~5h , to obtain silicon carbide mixed powder; S5:将PVA加入到S4的碳化硅混合粉料中,PVA的质量与S4的碳化硅混合粉料的质量的百分比为3%~5%,机械搅拌1~2h,混合均匀后,密封静置5~10h后得到SiC微粉混合料;S5: Add PVA to the silicon carbide mixed powder of S4, the percentage of the mass of PVA to the mass of the silicon carbide mixed powder of S4 is 3%~5%, mechanically stir for 1~2h, after mixing evenly, seal and stand After 5~10h, the SiC micropowder mixture is obtained; S6:将S5中混合均匀后的粉料倒入制粒机中进行制粒,得到大小均匀,粒度范围为10~200μm的SiC颗粒,在90~100℃下干燥1~2h,得到湿度适当的SiC颗粒;S6: Pour the uniformly mixed powder in S5 into a granulator for granulation to obtain SiC particles with a uniform size and a particle size range of 10-200 μm, and dry at 90-100 ° C for 1-2 hours to obtain a suitable humidity. SiC particles; S7:将S6中处理后的碳化硅颗粒放入高温真空气氛炉中进行烧结,在1300~1500℃下进行热处理2~3h,冷却至室温后,放入马弗炉中在500~600℃进行热处理2~3h,然后得到粒度再造的SiC陶瓷粉体。S7: Put the silicon carbide particles treated in S6 into a high-temperature vacuum atmosphere furnace for sintering, heat treatment at 1300-1500 °C for 2-3 hours, cool to room temperature, and put them into a muffle furnace at 500-600 °C for sintering Heat treatment for 2 to 3 hours, and then obtain SiC ceramic powder with reconstituted particle size. 2.根据权利要求1所述的SiC陶瓷粉体的制备方法,其特征在于,S1中所用SiC微粉粒度为0.5~3μm。2. The preparation method of SiC ceramic powder according to claim 1, wherein the particle size of the SiC micropowder used in S1 is 0.5-3 μm. 3.根据权利要求1所述的SiC陶瓷粉体的制备方法,其特征在于,S21中所用正硅酸乙酯中所含的SiO2量与S1中碳化硅的质量比在3%~10%。3. the preparation method of SiC ceramic powder according to claim 1 is characterized in that, the SiO contained in the tetraethyl orthosilicate used in S21 Amount and the mass ratio of silicon carbide in S1 are 3%~10% . 4.根据权利要求1所述的SiC陶瓷粉体的制备方法,其特征在于,S3中所用聚乙二醇10000中的含C量与S21中正硅酸乙酯含Si量的摩尔比为1.2~2,有机碳源聚乙二醇10000可以被替换为聚乙二醇2000,聚乙二醇6000,聚乙二醇20000以及葡萄糖等。4. the preparation method of SiC ceramic powder according to claim 1, is characterized in that, the mol ratio of the C content in the polyethylene glycol 10000 used in S3 and the Si content of ethyl orthosilicate in S21 is 1.2~ 2. The organic carbon source polyethylene glycol 10000 can be replaced with polyethylene glycol 2000, polyethylene glycol 6000, polyethylene glycol 20000 and glucose, etc. 5.根据权利要求1所述的SiC陶瓷粉体的制备方法,其特征在于,S7中SiC颗粒的烧结温度为1300℃~1500℃,烧结气氛可以是真空氩气保护,真空氮气保护;二次热处理的温度是500~600℃。5. the preparation method of SiC ceramic powder according to claim 1 is characterized in that, the sintering temperature of SiC particles in S7 is 1300 ℃~1500 ℃, and the sintering atmosphere can be vacuum argon protection, vacuum nitrogen protection; secondary The temperature of the heat treatment is 500 to 600°C. 6.一种SiC陶瓷粉体,其特征在于,由权利要求1~5任一所述的方法制备获得。6. A SiC ceramic powder, characterized in that, prepared by the method described in any one of claims 1 to 5. 7.根据权利要求6所述的SiC陶瓷粉体,其特征在于,可应用在高温耐腐蚀、国防军工、特种陶瓷等领域。7. The SiC ceramic powder according to claim 6, characterized in that, it can be applied in fields such as high temperature corrosion resistance, national defense and military industry, special ceramics and the like.
CN202111155379.XA 2021-09-29 2021-09-29 A kind of preparation method of SiC ceramic powder Pending CN113788683A (en)

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN113912399A (en) * 2021-12-15 2022-01-11 山东金鸿新材料股份有限公司 Preparation method of high-density pressureless sintered silicon carbide ceramic

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN113912399A (en) * 2021-12-15 2022-01-11 山东金鸿新材料股份有限公司 Preparation method of high-density pressureless sintered silicon carbide ceramic
CN113912399B (en) * 2021-12-15 2022-02-25 山东金鸿新材料股份有限公司 Preparation method of high-density pressureless sintered silicon carbide ceramic

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