Building wall thermal insulation integrated structure and preparation method thereof

Abstract

The invention discloses a building wall thermal insulation integrated structure and a preparation method thereof, and belongs to the technical field of building wall preparation. The building wall heat preservation integrated structure comprises a wall base layer, a heat preservation layer, a decoration layer and a durable layer which are sequentially arranged from inside to outside, and the heat preservation layer is made of myricetin, 1, 2-propylene glycol, 1, 2-propylene glycol, 1, 2-propylene glycol, 1, 2-propylene glycol and 1, 2-propylene glycol. The material of the durable layer is prepared from 1, 3-dibromopropane, 1-t-butyloxycarbonyl piperazine, 5-methyl-2-aminothiazole, polyether polyol and toluene diisocyanate, and the material of the durable layer is prepared from diphenyl sulfone, diphenol propane, 2, 4 '-difluorobenzophenone, 4, 4'-dihydroxybenzophenone and epoxy resin. The integrated structure prepared by the method has excellent thermal insulation property, flame retardant property and durability.

Description

Technical Field

[0001] This invention belongs to the field of building wall preparation technology, specifically relating to an integrated building wall insulation structure and its preparation method. Background Technology

[0002] Traditional building insulation systems, such as external insulation panels and embedded insulation layers, while providing insulation to some extent, also have increasingly prominent problems. On the one hand, these systems often require secondary construction after the main building structure is completed, increasing construction difficulty and cost, and potentially leading to weak adhesion between the insulation layer and the main wall structure, resulting in safety hazards such as detachment and cracking. On the other hand, traditional insulation materials, especially organic insulation materials, while possessing good insulation performance, are highly flammable. In the event of a fire, the flames will spread rapidly, posing a serious threat to life and property. Furthermore, these materials may produce harmful gases during use, polluting the environment. Therefore, finding a new type of building insulation structure that meets insulation requirements, possesses good fire resistance, and is environmentally friendly and safe has become an urgent problem to be solved by the construction industry.

[0003] Patent CN114163194B discloses a moisture-proof and heat-insulating structure for building walls, comprising several interconnected insulation boards. The insulation boards are made from a homogeneous mixture, which includes cement, corundum, an antioxidant, modified polystyrene particles, and water. The preparation method of the insulation boards is as follows: Step 1, preparing modified polystyrene particles: S1, preparing primary modified polystyrene particles; S2, preparing a secondary modification liquid; S3, adding the primary modified polystyrene particles to the secondary modification liquid, stirring evenly, cooling and pelletizing to obtain secondary modified polystyrene particles; Step 2, mixing cement, corundum, antioxidant, modified polystyrene particles, and water, heating and stirring evenly to obtain a homogeneous mixture; Step 3, pouring the homogeneous mixture into a mold, allowing it to cure, and then obtaining the insulation board. The insulation board obtained by this invention has a moisture-proof effect; however, there is still room for improvement in the heat insulation, flame retardancy, and durability of the integrated structure prepared by this method. Summary of the Invention

[0004] The purpose of this invention is to provide an integrated thermal insulation structure for building walls and its preparation method, which solves the technical problems of poor thermal insulation, flame retardancy and durability of integrated structures in the prior art.

[0005] To achieve the above objectives, the present invention adopts the following technical solution: This invention provides an integrated thermal insulation structure for building walls, comprising a wall base, an insulation layer, a decorative layer, and a durable layer, wherein the wall base, insulation layer, decorative layer, and durable layer are arranged sequentially from the inside out. The insulation layer material is prepared from myricetin, 1,3-dibromopropane, 1-tert-butyloxycarbonylpiperazine, 5-methyl-2-aminothiazole, polyether polyol, and toluene diisocyanate. The durable layer material is prepared from diphenyl sulfone, bisphenol A, 2,4'-difluorobenzophenone, 4,4'-dihydroxybenzophenone, and epoxy resin.

[0006] Preferably, the method for preparing the insulation layer material includes the following steps: Q1: Myricetin and potassium carbonate were added to a container containing N,N-dimethylformamide. After stirring and dissolving, iodomethane was added, and the reaction continued. After the reaction was completed, the mixture was filtered, washed, dried, and added to anhydrous ethanol. After heating and reflux, hydrochloric acid was added, and the reaction continued under reflux. After the reaction was completed, the mixture was cooled, filtered, washed, and dried to obtain compound 1. Compound 1 and potassium carbonate were added to a container containing N,N-dimethylformamide. After stirring at low temperature, 1,3-dibromopropane was slowly added dropwise to continue the reaction. After the reaction was completed, ice water was added, the mixture was stirred continuously, allowed to stand, filtered, dried, and purified to obtain compound 2. Q2: Potassium carbonate, acetonitrile, and 1-tert-butyloxycarbonylpiperazine were added to a container, heated to reflux, and then compound 2 was added. The reaction was continued to be heated. After the reaction was completed, the mixture was cooled, poured into ice water, stirred, precipitated, filtered, washed, and dried to obtain compound 3. Compound 3 and methanol were added to a container, stirred at room temperature, and then hydrochloric acid was added. The mixture was heated to reflux and reacted. After the reaction was completed, the mixture was stirred, filtered under reduced pressure, washed, and dried to obtain compound 4. 5-methyl-2-aminothiazole, pyridine, and acetonitrile were mixed and stirred. Chloroacetyl chloride was added under ice bath conditions, stirred, concentrated, poured into water, precipitated, filtered, washed, and dried to obtain compound 5. Q3: Add compound 4 and potassium carbonate to N,N-dimethylformamide, stir at room temperature, then add compound 5, heat under reflux to react, after the reaction is complete, cool, pour into cold water, extract, concentrate under reduced pressure, purify, and obtain compound 6; add polyether polyol, catalyst A33, foaming agent, distilled water, silicone oil and compound 6 to a container, mix and stir, then add phase change microcapsule emulsion and toluene diisocyanate, continue stirring, and mature to obtain the thermal insulation layer material.

[0007] In the above process, myricetin was used as the reactant. Iodomethane was added to the container to methylate and protect the hydroxyl groups in the structure. Then hydrochloric acid was added, and compound 1 was prepared by deglycosylation. 1,3-Dibromopropane and compound 1 underwent nucleophilic substitution at low temperature to synthesize compound 2. Then, using potassium carbonate as an acid-binding agent and acetonitrile as a solvent, compound 2 and 1-tert-butoxycarbonylpiperazine were heated under reflux to prepare compound 3. Then, compound 3 underwent a substitution reaction in a methanol and hydrochloric acid system to give compound 4. Subsequently, 5-methyl-2-aminothiazole and chloroacetyl chloride were reacted under low temperature to prepare compound 5. Compound 4 and compound 5 were heated under reflux in potassium carbonate and N,N-dimethylformamide to give compound 6. The synthesis reaction formula of compound 6 is as follows: ; The mass spectrometry analysis results of compound 1 were: m / z: 388.12 (100.0%), 389.12 (22.2%), 390.12 (3.9%); the mass spectrometry analysis results of compound 2 were: m / z: 508.07 (100.0%), 510.07 (97.3%), 509.08 (25.5%), 511.07 (24.2%), 510.08 (4.8%), 512.08 (4.7%), 511.08 (1.2%); the mass spectrometry analysis results of compound 3 were: m / z: 614.28 (100.0%), 615.29 (35.5%), 616.29 (8.2%), 617.29 (1.4%); the mass spectrometry analysis results of compound 4 were: m / z: Compound 5 was analyzed by mass spectrometry and its m / z values ​​were: 514.23 (100.0%), 515.23 (29.9%), 516.24 (6.0%). The m / z values ​​of compound 5 were: 190.00 (100.0%), 191.99 (36.5%), 191.00 (7.4%), 193.00 (2.4%), 193.99 (1.5%). The m / z values ​​of compound 6 were: 668.25 (100.0%), 669.25 (38.0%), 670.26 (8.3%), 670.25 (5.4%), 671.25 (1.7%), 671.26 (1.6%).

[0008] Preferably, in Q1, the ratio of myricetin, potassium carbonate, N,N-dimethylformamide, iodomethane, anhydrous ethanol, and hydrochloric acid is (5-10) g : (23-36) g : (115-120) mL : (6.68-7.12) mL : (60-75) mL : (9.87-10.12) mL, the reaction time is 48-60 h, the reflux temperature is 100-110 °C, the reaction time is 1-2 h, and the reflux reaction time is 3-5 h; the ratio of compound 1, potassium carbonate, N,N-dimethylformamide, and 1,3-dibromopropane is (2-3) g : (2.1-2.5) g : (40-50) mL : (1.2-1.8) mL, the low-temperature stirring temperature is 0-1 °C, and the stirring reaction time is 1-1.5 h.

[0009] Preferably, in Q2, the ratio of potassium carbonate, acetonitrile, 1-tert-butyloxycarbonylpiperazine, and compound 2 is (2.12-2.68) g : (20-25) mL : (2.58-2.93) g : (2.8-3.6) g, the reflux temperature is 80-85℃, the reflux time is 30-45 min, and the reaction is continued at a temperature of 6-8 h; the ratio of compound 3, methanol, and hydrochloric acid is (2-2.5). g: (18-24) mL: (1.11-1.32) mL, reflux temperature is 80-90℃, reaction time is 2-3h; the ratio of 5-methyl-2-aminothiazole, pyridine, acetonitrile and chloroacetyl chloride is (1-1.2) g: (0.9-0.95) g: (20-22) mL: (0.82-0.88) mL, mixing and stirring time is 30-45 min, stirring reaction time is 2-4h.

[0010] Preferably, in Q3, the ratio of compound 4, potassium carbonate, N,N-dimethylformamide, and compound 5 is (0.5-0.7) g : (0.46-0.52) g : (9.5-10.2) mL : (0.27-0.34) g, the stirring time at room temperature is 30-60 min, the reflux reaction temperature is 80-90℃, and the reaction time is 8-10 h; polyether polyol, catalyst A33, and foaming agent are also present. The ratio of distilled water, silicone oil, compound 6, phase change microcapsule emulsion and toluene diisocyanate is (50-60) g : (0.4-0.5) g : (10-15) g : (0.5-0.8) mL : (1.2-1.5) g : (8.12-10.12) g : (2.1-4.5) g : (62-65) g. The mixing and stirring time is 3-6 min, and the stirring time is continued for 20-25 min.

[0011] Preferably, the method for preparing the durable layer material includes the following steps: S1: Diphenyl sulfone was added to a container equipped with a thermometer, a mechanical stirrer and a nitrogen inlet. The mixture was heated and stirred under a nitrogen atmosphere. Then sodium carbonate, bisphenol propane, 2,4'-difluorobenzophenone and 4,4'-dihydroxybenzophenone were added and the mixture was heated and stirred. After the reaction was completed, the mixture was added to a container containing deionized water. A precipitate was formed. The precipitate was crushed and washed to obtain the polymer. S2: Add the polymer and sulfuric acid to a container, heat and stir, then pour into ice water, crush, wash, soak in sodium hydroxide, wash, and dry to obtain sulfonated polymer; S3: Add sulfonated polymer to epoxy resin and mix to obtain durable layer material.

[0012] The synthesis reaction formula for the sulfonated polymer in the above process is as follows: ; Preferably, in S1, the ratio of diphenyl sulfone, sodium carbonate, bisphenol propane, 2,4'-difluorobenzophenone, and 4,4'-dihydroxybenzophenone is (400-480) g : (0.03-0.082) g : (30-35) g : (75-88) g : (20-23.68) g. The temperature for stirring and heating is 120-140℃, the reaction time is 10-14 h, and the temperature is increased sequentially to 220℃, 250℃, 290℃, and 310℃, and maintained at each temperature for 2 h.

[0013] Preferably, in step S2, the ratio of polymer to sulfuric acid is (10-12) g: (150-180) mL, the heating and stirring temperature is 80-90℃, the time is 10-12 h, the sodium hydroxide concentration is 1 mol / L, and the soaking time is 10-12 h; in step S3, the ratio of sulfonated polymer to epoxy resin is (2-5) g: (12-18) g.

[0014] Preferably, the method for preparing an integrated building wall insulation structure includes the following steps: Step 1: Tie the reinforcing bars, then pour concrete, cure, remove the formwork to obtain the wall base, clean the base, evenly apply the insulation material, and then apply crack-resistant mortar to obtain a wall with an insulation layer structure. Step 2: Clean the insulation layer, then apply primer, attach the stone, fill the joints, then apply an interface agent to the stone surface, then apply a layer of durable material, and polish to obtain an integrated building wall insulation structure.

[0015] In summary, due to the adoption of the above technical solution, the beneficial effects of the present invention are: 1. This invention first uses myricetin, 1,3-dibromopropane, 1-tert-butoxycarbonylpiperazine, 5-methyl-2-aminothiazole, polyether polyol and toluene diisocyanate as raw materials to prepare a thermal insulation layer material. Subsequently, using diphenyl sulfone, bisphenol propane, 2,4'-difluorobenzophenone, 4,4'-dihydroxybenzophenone and epoxy resin as raw materials, a durability layer material is prepared. Adding both to the preparation process of building walls can effectively improve the flame retardant performance, thermal insulation performance and durability of building walls.

[0016] 2. This invention applies the prepared thermal insulation layer material to an integrated thermal insulation structure for building walls, which can effectively improve its thermal insulation and flame retardant effects. The thiazopiperazine structure contained in compound 6 has rigid aromatic rings and polar groups, which can enhance the intermolecular forces of polyurethane materials and form a dense microstructure, thereby reducing heat conduction. At the same time, the phase change microcapsules can undergo phase change within a specific temperature range, absorbing or releasing a large amount of latent heat, regulating temperature fluctuations, and further improving the thermal insulation effect. The synergistic effect of the two forms a multi-layered thermal resistance structure, which significantly reduces the thermal conductivity of the wall and effectively regulates the indoor temperature in environments with large day-night temperature differences, reducing energy consumption. In terms of flame retardant properties, the thiazole ring in Compound 6 contains sulfur and nitrogen elements, which decompose at high temperatures to produce non-combustible gases, dilute the concentration of combustible gases, and form a char layer, blocking heat and oxygen. The piperazine structure promotes the formation of the char layer during combustion, further enhancing the flame retardant effect. The combination of Compound 6 and the polyurethane matrix forms a highly efficient flame retardant system, significantly improving the flame retardant rating of the insulation layer, reducing the risk of fire, making the material less prone to combustion in high-temperature environments, and improving the safety of building walls.

[0017] 3. This invention applies the prepared durable layer material to an integrated thermal insulation structure for building walls, effectively improving its durability. The aromatic ring structure and sulfonic acid groups of the sulfonated polymer backbone in the durable layer material provide stability against the corrosion of acids, alkalis, solvents, and salts. Simultaneously, the dense protective layer formed by the epoxy resin further blocks corrosive media, ensuring the material maintains stable performance in harsh environments such as acid rain and salt spray, extending the service life of the building walls. Furthermore, the material's high glass transition temperature and the thermal stability of the sulfonic acid groups allow it to maintain stable mechanical properties and appearance even at high temperatures. The UV resistance and antioxidant properties of the epoxy resin effectively delay material aging, preventing yellowing, embrittlement, or cracking. Moreover, the aromatic ring structure and sulfonic acid groups of the sulfonated polymer form a char layer and release non-flammable gases during combustion, synergistically enhancing the flame-retardant properties of the epoxy resin and significantly reducing the risk of fire. Detailed Implementation

[0018] The technical solutions in the embodiments of the present invention will be clearly and completely described below. Obviously, the described embodiments are only some embodiments of the present invention, and not all embodiments. Based on the embodiments of the present invention, all other embodiments obtained by those skilled in the art without creative effort are within the scope of protection of the present invention.

[0019] Example 1: This example discloses a method for preparing a thermal insulation layer material, including the following steps: Q1: 7.5g of myricetin and 29.5g of potassium carbonate were added to a container containing 117mL of N,N-dimethylformamide. After stirring and dissolving, 6.83mL of iodomethane was added, and the reaction was continued for 48h. After the reaction was completed, the mixture was filtered, washed, dried, and added to 67.5mL of anhydrous ethanol. The mixture was heated to reflux at 100℃ for 1h, and then 9.93mL of hydrochloric acid was added. The mixture was refluxed for another 4h. After the reaction was completed, the mixture was cooled, filtered, washed, and dried to obtain compound 1. 2.5g of compound 1 and 2.3g of potassium carbonate were added to a container containing 45mL of N,N-dimethylformamide. The mixture was stirred at 0℃ for 1h, and then 1.5mL of 1,3-dibromopropane was slowly added dropwise to continue the reaction. After the reaction was completed, ice water was added, the mixture was stirred continuously, allowed to stand, filtered, dried, and purified to obtain compound 2. Q2: 2.4 g potassium carbonate, 22.5 mL acetonitrile, and 2.73 g 1-tert-butyloxycarbonylpiperazine were added to a container and heated to reflux at 85 °C for 30 min. Then, 3.2 g of compound 2 was added, and the reaction was continued for 8 h. After the reaction was completed, the mixture was cooled, poured into ice water, stirred, precipitated, filtered, washed, and dried to obtain compound 3. 2.25 g of compound 3 and 21 mL methanol were added to a container and stirred at room temperature. Then, 1.21 mL hydrochloric acid was added, and the mixture was heated to reflux at 85 °C for 3 h. After the reaction was completed, the mixture was stirred, filtered under reduced pressure, washed, and dried to obtain compound 4. 1.1 g 5-methyl-2-aminothiazole, 0.92 g pyridine, and 21 mL acetonitrile were mixed and stirred for 45 min. 0.85 mL chloroacetyl chloride was added under ice bath conditions, and the mixture was stirred for 4 h. The mixture was concentrated, poured into water, precipitated, filtered, washed, and dried to obtain compound 5. Q3: Add 0.6g of compound 4 and 0.49g of potassium carbonate to 9.7mL of N,N-dimethylformamide, stir at room temperature for 30min, then add 0.31g of compound 5, heat to reflux at 85℃ for 10h. After the reaction is complete, cool, pour into cold water, extract, concentrate under reduced pressure, and purify to obtain compound 6. Add 55g of polyether polyol, 0.45g of catalyst A33, 12.5g of foaming agent, 0.65mL of distilled water, 1.35g of silicone oil and 9.12g of compound 6 to a container, mix and stir for 6min, then add 3.3g of phase change microcapsule emulsion and 63.5g of toluene diisocyanate, continue stirring for 25min, and mature to obtain the thermal insulation layer material.

[0020] This embodiment discloses a method for preparing a durable layer material, including the following steps: S1: 440g of diphenyl sulfone was added to a container equipped with a thermometer, a mechanical stirrer, and a nitrogen inlet. Under a nitrogen atmosphere, the mixture was heated to 140℃ and stirred for 12h. Then, 0.051g of sodium carbonate, 32.5g of bisphenol propane, 82g of 2,4'-difluorobenzophenone, and 21.84g of 4,4'-dihydroxybenzophenone were added, and the temperature was increased to 220℃, 250℃, 290℃, and 310℃, and maintained at each temperature for 2h. After the reaction was completed, the mixture was added to a container containing deionized water. A precipitate was formed. The precipitate was crushed, washed, and the polymer was obtained. S2: Add 11g of polymer and 165mL of sulfuric acid to a container, heat and stir at 85℃ for 12h, then pour into ice water, crush, wash, soak in 1mol / L sodium hydroxide solution for 12h, wash, and dry to obtain sulfonated polymer; S3: Add 3.5g of sulfonated polymer to 15g of epoxy resin and mix to obtain a durable layer material.

[0021] This embodiment discloses a method for preparing an integrated thermal insulation structure for building walls, including the following steps: Step 1: Tie the reinforcing bars, then pour concrete, cure, remove the formwork to obtain the wall base, clean the base, evenly apply the insulation material, and then apply crack-resistant mortar to obtain a wall with an insulation layer structure. Step 2: Clean the insulation layer, then apply primer, attach the stone, fill the joints, then apply an interface agent to the stone surface, then apply a layer of durable material, and polish to obtain an integrated building wall insulation structure.

[0022] Example 2: This example discloses a method for preparing a thermal insulation layer material, including the following steps: Q1: 5g of myricetin and 23g of potassium carbonate were added to a container containing 115mL of N,N-dimethylformamide. After stirring and dissolving, 6.68mL of iodomethane was added, and the reaction was continued for 48h. After the reaction was completed, the mixture was filtered, washed, dried, and added to 60mL of anhydrous ethanol. The mixture was heated to 100℃ and refluxed for 1h, and then 9.87mL of hydrochloric acid was added. The mixture was refluxed for another 4h. After the reaction was completed, the mixture was cooled, filtered, washed, and dried to obtain compound 1. 2g of compound 1 and 2.1g of potassium carbonate were added to a container containing 40mL of N,N-dimethylformamide. The mixture was stirred at 0℃ for 1h, and then 1.2mL of 1,3-dibromopropane was slowly added dropwise to continue the reaction. After the reaction was completed, ice water was added, the mixture was stirred continuously, allowed to stand, filtered, dried, and purified to obtain compound 2. Q2: 2.12 g potassium carbonate, 20 mL acetonitrile, and 2.58 g 1-tert-butyloxycarbonylpiperazine were added to a container and heated to reflux at 85 °C for 30 min. Then 2.8 g compound 2 was added, and the reaction was continued for 8 h. After the reaction was completed, the mixture was cooled, poured into ice water, stirred, precipitated, filtered, washed, and dried to obtain compound 3. 2.5 g compound 3 and 18 mL methanol were added to a container and stirred at room temperature. Then 1.11 mL hydrochloric acid was added, and the mixture was heated to reflux at 85 °C for 3 h. After the reaction was completed, the mixture was stirred, filtered under reduced pressure, washed, and dried to obtain compound 4. 1 g 5-methyl-2-aminothiazole, 0.9 g pyridine, and 20 mL acetonitrile were mixed and stirred for 45 min. 0.82 mL chloroacetyl chloride was added under ice bath conditions, and the mixture was stirred for 4 h. The mixture was concentrated, poured into water, precipitated, filtered, washed, and dried to obtain compound 5. Q3: Add 0.5g of compound 4 and 0.46g of potassium carbonate to 9.5mL of N,N-dimethylformamide, stir at room temperature for 30min, then add 0.27g of compound 5, heat to reflux at 85℃ for 10h. After the reaction is complete, cool, pour into cold water, extract, concentrate under reduced pressure, and purify to obtain compound 6; add 50g of polyether polyol, 0.4g of catalyst A33, 10g of foaming agent, 0.5mL of distilled water, 1.2g of silicone oil and 8.12g of compound 6 to a container, mix and stir for 6min, then add 2.1g of phase change microcapsule emulsion and 62g of toluene diisocyanate, continue stirring for 25min, and mature to obtain the thermal insulation layer material.

[0023] This embodiment discloses a method for preparing a durable layer material, including the following steps: S1: 400g of diphenyl sulfone was added to a container equipped with a thermometer, a mechanical stirrer and a nitrogen inlet. The mixture was heated to 140℃ and stirred for 12h under a nitrogen atmosphere. Then, 0.03g of sodium carbonate, 30g of bisphenol propane, 75g of 2,4'-difluorobenzophenone and 20g of 4,4'-dihydroxybenzophenone were added and the temperature was raised to 220℃, 250℃, 290℃ and 310℃ respectively, and maintained at each temperature for 2h. After the reaction was completed, the mixture was added to a container containing deionized water. A precipitate was formed. The precipitate was crushed and washed to obtain the polymer. S2: Add 12g of polymer and 150mL of sulfuric acid to a container, heat and stir at 85℃ for 12h, then pour into ice water, crush, wash, soak in 1mol / L sodium hydroxide solution for 12h, wash, and dry to obtain sulfonated polymer; S3: Add 2g of sulfonated polymer to 12g of epoxy resin and mix to obtain a durable layer material.

[0024] This embodiment discloses a method for preparing an integrated thermal insulation structure for building walls, including the following steps: Step 1: Tie the reinforcing bars, then pour concrete, cure, remove the formwork to obtain the wall base, clean the base, evenly apply the insulation material, and then apply crack-resistant mortar to obtain a wall with an insulation layer structure. Step 2: Clean the insulation layer, then apply primer, attach the stone, fill the joints, then apply an interface agent to the stone surface, then apply a layer of durable material, and polish to obtain an integrated building wall insulation structure.

[0025] Example 3: This example discloses a method for preparing a thermal insulation layer material, including the following steps: Q1: 10g of myricetin and 36g of potassium carbonate were added to a container containing 120mL of N,N-dimethylformamide. After stirring and dissolving, 7.12mL of iodomethane was added, and the reaction was continued for 48h. After the reaction was completed, the mixture was filtered, washed, dried, and added to 75mL of anhydrous ethanol. The mixture was heated to reflux at 100℃ for 1h, and then 10.12mL of hydrochloric acid was added. The mixture was refluxed for another 4h. After the reaction was completed, the mixture was cooled, filtered, washed, and dried to obtain compound 1. 3g of compound 1 and 2.5g of potassium carbonate were added to a container containing 50mL of N,N-dimethylformamide. The mixture was stirred at 0℃ for 1h, and then 1.8mL of 1,3-dibromopropane was slowly added dropwise to continue the reaction. After the reaction was completed, ice water was added, the mixture was stirred continuously, allowed to stand, filtered, dried, and purified to obtain compound 2. Q2: 2.68 g potassium carbonate, 25 mL acetonitrile, and 2.93 g 1-tert-butyloxycarbonylpiperazine were added to a container and heated to reflux at 85 °C for 30 min. Then, 3.6 g of compound 2 was added, and the reaction was continued for 8 h. After the reaction was completed, the mixture was cooled, poured into ice water, stirred, precipitated, filtered, washed, and dried to obtain compound 3. 2 g of compound 3 and 24 mL methanol were added to a container and stirred at room temperature. Then, 1.32 mL hydrochloric acid was added, and the mixture was heated to reflux at 85 °C for 3 h. After the reaction was completed, the mixture was stirred, filtered under reduced pressure, washed, and dried to obtain compound 4. 1.2 g 5-methyl-2-aminothiazole, 0.95 g pyridine, and 22 mL acetonitrile were mixed and stirred for 45 min. 0.88 mL chloroacetyl chloride was added under ice bath conditions, and the mixture was stirred for 4 h. The mixture was concentrated, poured into water, precipitated, filtered, washed, and dried to obtain compound 5. Q3: Add 0.7g of compound 4 and 0.52g of potassium carbonate to 10.2mL of N,N-dimethylformamide, stir at room temperature for 30min, then add 0.34g of compound 5, heat to reflux at 85℃ for 10h. After the reaction is complete, cool, pour into cold water, extract, concentrate under reduced pressure, and purify to obtain compound 6. Add 60g of polyether polyol, 0.5g of catalyst A33, 15g of foaming agent, 0.8mL of distilled water, 1.5g of silicone oil and 10.12g of compound 6 to a container, mix and stir for 6min, then add 4.5g of phase change microcapsule emulsion and 65g of toluene diisocyanate, continue stirring for 25min, and mature to obtain the thermal insulation layer material.

[0026] This embodiment discloses a method for preparing a durable layer material, including the following steps: S1: 480g of diphenyl sulfone was added to a container equipped with a thermometer, a mechanical stirrer, and a nitrogen inlet. Under a nitrogen atmosphere, the mixture was heated to 140℃ and stirred for 12h. Then, 0.082g of sodium carbonate, 35g of bisphenol propane, 88g of 2,4'-difluorobenzophenone, and 23.68g of 4,4'-dihydroxybenzophenone were added, and the temperature was increased to 220℃, 250℃, 290℃, and 310℃, and maintained at each temperature for 2h. After the reaction was completed, the mixture was added to a container containing deionized water. A precipitate was formed. The precipitate was crushed, washed, and the polymer was obtained. S2: Add 10g of polymer and 180mL of sulfuric acid to a container, heat and stir at 85℃ for 12h, then pour into ice water, crush, wash, soak in 1mol / L sodium hydroxide solution for 12h, wash, and dry to obtain sulfonated polymer; S3: Add 5g of sulfonated polymer to 18g of epoxy resin and mix to obtain a durable layer material.

[0027] This embodiment discloses a method for preparing an integrated thermal insulation structure for building walls, including the following steps: Step 1: Tie the reinforcing bars, then pour concrete, cure, remove the formwork to obtain the wall base, clean the base, evenly apply the insulation material, and then apply crack-resistant mortar to obtain a wall with an insulation layer structure. Step 2: Clean the insulation layer, then apply primer, attach the stone, fill the joints, then apply an interface agent to the stone surface, then apply a layer of durable material, and polish to obtain an integrated building wall insulation structure.

[0028] Example 4: This example discloses a method for preparing a thermal insulation layer material, including the following steps: Q1: 8g of myricetin and 25g of potassium carbonate were added to a container containing 116mL of N,N-dimethylformamide. After stirring and dissolving, 6.71mL of iodomethane was added, and the reaction was continued for 48h. After the reaction was completed, the mixture was filtered, washed, dried, and added to 62mL of anhydrous ethanol. The mixture was heated to 100℃ and refluxed for 1h, and then 9.89mL of hydrochloric acid was added. The mixture was refluxed for another 4h. After the reaction was completed, the mixture was cooled, filtered, washed, and dried to obtain compound 1. 2.2g of compound 1 and 2.2g of potassium carbonate were added to a container containing 42mL of N,N-dimethylformamide. The mixture was stirred at 0℃ for 1h, and then 1.4mL of 1,3-dibromopropane was slowly added dropwise to continue the reaction. After the reaction was completed, ice water was added, the mixture was stirred continuously, allowed to stand, filtered, dried, and purified to obtain compound 2. Q2: 2.26 g potassium carbonate, 21 mL acetonitrile, and 2.61 g 1-tert-butyloxycarbonylpiperazine were added to a container and heated to reflux at 85 °C for 30 min. Then 2.9 g compound 2 was added, and the reaction was continued for 8 h. After the reaction was completed, the mixture was cooled, poured into ice water, stirred, precipitated, filtered, washed, and dried to obtain compound 3. 2.1 g compound 3 and 20 mL methanol were added to a container and stirred at room temperature. Then 1.18 mL hydrochloric acid was added, and the mixture was heated to reflux at 85 °C for 3 h. After the reaction was completed, the mixture was stirred, filtered under reduced pressure, washed, and dried to obtain compound 4. 1.05 g 5-methyl-2-aminothiazole, 0.91 g pyridine, and 20.5 mL acetonitrile were mixed and stirred for 45 min. 0.83 mL chloroacetyl chloride was added under ice bath conditions, and the mixture was stirred for 4 h. The mixture was concentrated, poured into water, precipitated, filtered, washed, and dried to obtain compound 5. Q3: Add 0.55g of compound 4 and 0.47g of potassium carbonate to 9.6mL of N,N-dimethylformamide, stir at room temperature for 30min, then add 0.29g of compound 5, heat to reflux at 85℃ for 10h. After the reaction is complete, cool, pour into cold water, extract, concentrate under reduced pressure, and purify to obtain compound 6. Add 52g of polyether polyol, 0.41g of catalyst A33, 11g of foaming agent, 0.6mL of distilled water, 1.3g of silicone oil and 8.62g of compound 6 to a container, mix and stir for 6min, then add 2.5g of phase change microcapsule emulsion and 63g of toluene diisocyanate, continue stirring for 25min, and mature to obtain the thermal insulation layer material.

[0029] This embodiment discloses a method for preparing a durable layer material, including the following steps: S1: 420g of diphenyl sulfone was added to a container equipped with a thermometer, a mechanical stirrer and a nitrogen inlet. The mixture was heated to 140℃ and stirred for 12h under a nitrogen atmosphere. Then, 0.04g of sodium carbonate, 31g of bisphenol propane, 79g of 2,4'-difluorobenzophenone and 20.57g of 4,4'-dihydroxybenzophenone were added and the temperature was raised to 220℃, 250℃, 290℃ and 310℃ in sequence, and maintained at each temperature for 2h. After the reaction was completed, the mixture was added to a container containing deionized water. A precipitate was formed. The precipitate was crushed and washed to obtain the polymer. S2: Add 10.5g of polymer and 160mL of sulfuric acid to a container, heat and stir at 85℃ for 12h, then pour into ice water, crush, wash, soak in 1mol / L sodium hydroxide solution for 12h, wash, and dry to obtain sulfonated polymer. S3: Add 3g of sulfonated polymer to 14g of epoxy resin and mix to obtain a durable layer material.

[0030] This embodiment discloses a method for preparing an integrated thermal insulation structure for building walls, including the following steps: Step 1: Tie the reinforcing bars, then pour concrete, cure, remove the formwork to obtain the wall base, clean the base, evenly apply the insulation material, and then apply crack-resistant mortar to obtain a wall with an insulation layer structure. Step 2: Clean the insulation layer, then apply primer, attach the stone, fill the joints, then apply an interface agent to the stone surface, then apply a layer of durable material, and polish to obtain an integrated building wall insulation structure.

[0031] Example 5: This example discloses a method for preparing a thermal insulation layer material, including the following steps: Q1: 6g of myricetin and 32g of potassium carbonate were added to a container containing 118mL of N,N-dimethylformamide. After stirring and dissolving, 7.05mL of iodomethane was added, and the reaction was continued for 48h. After the reaction was completed, the mixture was filtered, washed, dried, and added to 73mL of anhydrous ethanol. The mixture was heated to reflux at 100℃ for 1h, and then 10.07mL of hydrochloric acid was added. The mixture was refluxed for another 4h. After the reaction was completed, the mixture was cooled, filtered, washed, and dried to obtain compound 1. 2.8g of compound 1 and 2.4g of potassium carbonate were added to a container containing 48mL of N,N-dimethylformamide. The mixture was stirred at 0℃ for 1h, and then 1.6mL of 1,3-dibromopropane was slowly added dropwise to continue the reaction. After the reaction was completed, ice water was added, the mixture was stirred continuously, allowed to stand, filtered, dried, and purified to obtain compound 2. Q2: 2.53 g potassium carbonate, 24 mL acetonitrile, and 2.83 g 1-tert-butyloxycarbonylpiperazine were added to a container and heated to reflux at 85 °C for 30 min. Then 3.4 g compound 2 was added, and the reaction was continued for 8 h. After the reaction was completed, the mixture was cooled, poured into ice water, stirred, precipitated, filtered, washed, and dried to obtain compound 3. 2.4 g compound 3 and 23 mL methanol were added to a container and stirred at room temperature. Then 1.29 mL hydrochloric acid was added, and the mixture was heated to reflux at 85 °C for 3 h. After the reaction was completed, the mixture was stirred, filtered under reduced pressure, washed, and dried to obtain compound 4. 1.15 g 5-methyl-2-aminothiazole, 0.94 g pyridine, and 21.5 mL acetonitrile were mixed and stirred for 45 min. 0.86 mL chloroacetyl chloride was added under ice bath conditions, and the mixture was stirred for 4 h. The mixture was concentrated, poured into water, precipitated, filtered, washed, and dried to obtain compound 5. Q3: Add 0.65g of compound 4 and 0.51g of potassium carbonate to 10.1mL of N,N-dimethylformamide, stir at room temperature for 30min, then add 0.33g of compound 5, heat to reflux at 85℃ for 10h. After the reaction is complete, cool, pour into cold water, extract, concentrate under reduced pressure, and purify to obtain compound 6. Add 57g of polyether polyol, 0.48g of catalyst A33, 14g of foaming agent, 0.7mL of distilled water, 1.4g of silicone oil and 9.62g of compound 6 to a container, mix and stir for 6min, then add 4g of phase change microcapsule emulsion and 64g of toluene diisocyanate, continue stirring for 25min, and mature to obtain the thermal insulation layer material.

[0032] This embodiment discloses a method for preparing a durable layer material, including the following steps: S1: 460g of diphenyl sulfone was added to a container equipped with a thermometer, a mechanical stirrer, and a nitrogen inlet. Under a nitrogen atmosphere, the mixture was heated to 140℃ and stirred for 12h. Then, 0.061g of sodium carbonate, 34g of bisphenol propane, 85g of 2,4'-difluorobenzophenone, and 22.83g of 4,4'-dihydroxybenzophenone were added, and the temperature was increased to 220℃, 250℃, 290℃, and 310℃, and maintained at each temperature for 2h. After the reaction was completed, the mixture was added to a container containing deionized water. A precipitate was formed. The precipitate was crushed, washed, and the polymer was obtained. S2: Add 11.5g of polymer and 170mL of sulfuric acid to a container, heat and stir at 85℃ for 12h, then pour into ice water, crush, wash, soak in 1mol / L sodium hydroxide solution for 12h, wash, and dry to obtain sulfonated polymer. S3: Add 4g of sulfonated polymer to 16g of epoxy resin and mix to obtain a durable layer material.

[0033] This embodiment discloses a method for preparing an integrated thermal insulation structure for building walls, including the following steps: Step 1: Tie the reinforcing bars, then pour concrete, cure, remove the formwork to obtain the wall base, clean the base, evenly apply the insulation material, and then apply crack-resistant mortar to obtain a wall with an insulation layer structure. Step 2: Clean the insulation layer, then apply primer, attach the stone, fill the joints, then apply an interface agent to the stone surface, then apply a layer of durable material, and polish to obtain an integrated building wall insulation structure.

[0034] Comparative Example 1: Compared with Example 1, Comparative Example 1 did not add myricetin during the preparation of the integrated thermal insulation structure of building walls, and all other conditions remained unchanged.

[0035] Comparative Example 2: Compared with Example 1, Comparative Example 2 did not add bisphenol A propane during the preparation of the integrated thermal insulation structure of building walls, and all other conditions remained unchanged.

[0036] Experimental Example: The building walls prepared in Examples 1-5 and Comparative Examples 1-2 were subjected to performance tests. The thermal insulation performance of the samples was tested according to GB / T10294-2008, the combustion performance was tested according to GB 8624-2012, and the durability was tested according to JG / T 158-2013. The test results are shown in Table 1. Table 1 ; As shown in Table 1, the integrated building wall insulation structure prepared in Examples 1-5 of this invention exhibits excellent flame retardant, thermal insulation, and durability properties. A comparison between Comparative Example 1 and Examples 1-5 shows that adding myricetin can effectively improve the flame retardant and durability properties of the integrated building wall insulation structure; a comparison between Comparative Example 2 and Examples 1-5 shows that adding bisphenol A can effectively improve the flame retardant and thermal insulation properties of the integrated building wall insulation structure.

[0037] The above description is only a preferred embodiment of the present invention, but the scope of protection of the present invention is not limited thereto. Any equivalent substitutions or modifications made by those skilled in the art within the scope of the technology disclosed in the present invention, based on the technical solution and inventive concept of the present invention, should be covered within the scope of protection of the present invention.

[0038] The preferred embodiments of the present invention disclosed above are merely illustrative of the invention. These preferred embodiments do not exhaustively describe all details, nor do they limit the invention to specific implementations. Clearly, many modifications and variations can be made based on the content of this specification. This specification selects and specifically describes these embodiments to better explain the principles and practical applications of the invention, thereby enabling those skilled in the art to better understand and utilize the invention. The invention is limited only by the claims and their full scope and equivalents.

Claims

1. An integrated thermal insulation structure for building walls, characterized in that, The wall includes a base layer, an insulation layer, a decorative layer, and a durability layer, which are arranged sequentially from the inside out. The insulation layer material is prepared from myricetin, 1,3-dibromopropane, 1-tert-butyloxycarbonylpiperazine, 5-methyl-2-aminothiazole, polyether polyol, and toluene diisocyanate. The durability layer material is prepared from diphenyl sulfone, bisphenol A, 2,4'-difluorobenzophenone, 4,4'-dihydroxybenzophenone, and epoxy resin.

2. The integrated thermal insulation structure for building walls according to claim 1, characterized in that, The method for preparing the insulation layer material includes the following steps: Q1: Myricetin and potassium carbonate were added to a container containing N,N-dimethylformamide. After stirring and dissolving, iodomethane was added, and the reaction continued. After the reaction was completed, the mixture was filtered, washed, dried, and added to anhydrous ethanol. After heating and reflux, hydrochloric acid was added, and the reaction continued under reflux. After the reaction was completed, the mixture was cooled, filtered, washed, and dried to obtain compound 1. Compound 1 and potassium carbonate were added to a container containing N,N-dimethylformamide. After stirring at low temperature, 1,3-dibromopropane was slowly added dropwise to continue the reaction. After the reaction was completed, ice water was added, the mixture was stirred continuously, allowed to stand, filtered, dried, and purified to obtain compound 2. Q2: Potassium carbonate, acetonitrile, and 1-tert-butyloxycarbonylpiperazine were added to a container, heated to reflux, and then compound 2 was added. The reaction was continued to be heated. After the reaction was completed, the mixture was cooled, poured into ice water, stirred, precipitated, filtered, washed, and dried to obtain compound 3. Compound 3 and methanol were added to a container, stirred at room temperature, and then hydrochloric acid was added. The mixture was heated to reflux and reacted. After the reaction was completed, the mixture was stirred, filtered under reduced pressure, washed, and dried to obtain compound 4. 5-methyl-2-aminothiazole, pyridine, and acetonitrile were mixed and stirred. Chloroacetyl chloride was added under ice bath conditions, stirred, concentrated, poured into water, precipitated, filtered, washed, and dried to obtain compound 5. Q3: Add compound 4 and potassium carbonate to N,N-dimethylformamide, stir at room temperature, then add compound 5, heat under reflux to react, after the reaction is complete, cool, pour into cold water, extract, concentrate under reduced pressure, purify, and obtain compound 6; add polyether polyol, catalyst A33, foaming agent, distilled water, silicone oil and compound 6 to a container, mix and stir, then add phase change microcapsule emulsion and toluene diisocyanate, continue stirring, and mature to obtain the thermal insulation layer material.

3. The integrated thermal insulation structure for building walls according to claim 2, characterized in that, In Q1, the ratio of myricetin, potassium carbonate, N,N-dimethylformamide, iodomethane, anhydrous ethanol, and hydrochloric acid is (5-10) g : (23-36) g : (115-120) mL : (6.68-7.12) mL : (60-75) mL : (9.87-10.12) mL, the reaction time is 48-60 h, the reflux temperature is 100-110 °C, the reaction time is 1-2 h, and the reflux reaction time is 3-5 h; the ratio of compound 1, potassium carbonate, N,N-dimethylformamide, and 1,3-dibromopropane is (2-3) g : (2.1-2.5) g : (40-50) mL : (1.2-1.8) mL, the low-temperature stirring temperature is 0-1 °C, and the stirring reaction time is 1-1.5 h.

4. The integrated thermal insulation structure for building walls according to claim 2, characterized in that, In Q2, the ratio of potassium carbonate, acetonitrile, 1-tert-butyloxycarbonylpiperazine, and compound 2 is (2.12-2.68) g : (20-25) mL : (2.58-2.93) g : (2.8-3.6) g; the reflux temperature is 80-85℃; the reflux time is 30-45 min; and the reaction is continued at a temperature of 6-8 h. The ratio of compound 3, methanol, and hydrochloric acid is (2-2.5) g: The ratio of 5-methyl-2-aminothiazole, pyridine, acetonitrile and chloroacetyl chloride is (1-1.2) g: (0.9-0.95) g: (20-22) mL: (0.82-0.88) mL. The mixing and stirring time is 30-45 min, and the stirring reaction time is 2-4 h.

5. The integrated thermal insulation structure for building walls according to claim 2, characterized in that, In Q3, the ratio of compound 4, potassium carbonate, N,N-dimethylformamide, and compound 5 is (0.5-0.7) g : (0.46-0.52) g : (9.5-10.2) mL : (0.27-0.34) g. The stirring time at room temperature is 30-60 min, the reflux reaction temperature is 80-90℃, and the reaction time is 8-10 h. Polyether polyol, catalyst A33, foaming agent, and steam... The ratio of distilled water, silicone oil, compound 6, phase change microcapsule emulsion, and toluene diisocyanate is (50-60) g : (0.4-0.5) g : (10-15) g : (0.5-0.8) mL : (1.2-1.5) g : (8.12-10.12) g : (2.1-4.5) g : (62-65) g. The mixing and stirring time is 3-6 min, and the stirring time is continued for 20-25 min.

6. The integrated thermal insulation structure for building walls according to claim 1, characterized in that, The method for preparing the durable layer material includes the following steps: S1: Diphenyl sulfone was added to a container equipped with a thermometer, a mechanical stirrer and a nitrogen inlet. The mixture was heated and stirred under a nitrogen atmosphere. Then sodium carbonate, bisphenol propane, 2,4'-difluorobenzophenone and 4,4'-dihydroxybenzophenone were added and the mixture was heated and stirred. After the reaction was completed, the mixture was added to a container containing deionized water. A precipitate was formed. The precipitate was crushed and washed to obtain the polymer. S2: Add the polymer and sulfuric acid to a container, heat and stir, then pour into ice water, crush, wash, soak in sodium hydroxide, wash, and dry to obtain sulfonated polymer; S3: Add sulfonated polymer to epoxy resin and mix to obtain durable layer material.

7. The integrated thermal insulation structure for building walls according to claim 6, characterized in that, In S1, the ratio of diphenyl sulfone, sodium carbonate, bisphenol propane, 2,4'-difluorobenzophenone and 4,4'-dihydroxybenzophenone is (400-480) g : (0.03-0.082) g : (30-35) g : (75-88) g : (20-23.68) g. The temperature for stirring and heating is 120-140℃, and the reaction time is 10-14 h. The temperature increase process is as follows: the temperature is increased to 220℃, 250℃, 290℃ and 310℃ in sequence, and each temperature is maintained for 2 h.

8. The integrated thermal insulation structure for building walls according to claim 6, characterized in that, In S2, the ratio of polymer to sulfuric acid is (10-12) g: (150-180) mL, the heating and stirring temperature is 80-90℃, the time is 10-12 h, the sodium hydroxide concentration is 1 mol / L, and the soaking time is 10-12 h; in S3, the ratio of sulfonated polymer to epoxy resin is (2-5) g: (12-18) g.

9. A method for preparing an integrated building wall insulation structure as described in any one of claims 1-8, characterized in that, Includes the following steps: Step 1: Tie the reinforcing bars, then pour concrete, cure, remove the formwork to obtain the wall base, clean the base, evenly apply the insulation material, and then apply crack-resistant mortar to obtain a wall with an insulation layer structure. Step 2: Clean the insulation layer, then apply primer, attach the stone, fill the joints, then apply an interface agent to the stone surface, then apply a layer of durable material, and polish to obtain an integrated building wall insulation structure.