CN114381154A - Inorganic ceramic tile crack-beautifying coating and preparation method thereof - Google Patents
Inorganic ceramic tile crack-beautifying coating and preparation method thereof Download PDFInfo
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- 239000011248 coating agent Substances 0.000 title claims abstract description 79
- 238000000576 coating method Methods 0.000 title claims abstract description 79
- 238000002360 preparation method Methods 0.000 title claims abstract description 11
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims abstract description 70
- 229910021485 fumed silica Inorganic materials 0.000 claims abstract description 49
- 239000004111 Potassium silicate Substances 0.000 claims abstract description 47
- NNHHDJVEYQHLHG-UHFFFAOYSA-N potassium silicate Chemical compound [K+].[K+].[O-][Si]([O-])=O NNHHDJVEYQHLHG-UHFFFAOYSA-N 0.000 claims abstract description 47
- 229910052913 potassium silicate Inorganic materials 0.000 claims abstract description 47
- 235000019353 potassium silicate Nutrition 0.000 claims abstract description 47
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- 239000006087 Silane Coupling Agent Substances 0.000 claims abstract description 36
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 36
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- BPQQTUXANYXVAA-UHFFFAOYSA-N Orthosilicate Chemical compound [O-][Si]([O-])([O-])[O-] BPQQTUXANYXVAA-UHFFFAOYSA-N 0.000 description 2
- 150000001412 amines Chemical class 0.000 description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 2
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- GNEPOXWQWFSSOU-UHFFFAOYSA-N dichloro-methyl-phenylsilane Chemical compound C[Si](Cl)(Cl)C1=CC=CC=C1 GNEPOXWQWFSSOU-UHFFFAOYSA-N 0.000 description 1
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- JLUFWMXJHAVVNN-UHFFFAOYSA-N methyltrichlorosilane Chemical compound C[Si](Cl)(Cl)Cl JLUFWMXJHAVVNN-UHFFFAOYSA-N 0.000 description 1
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- ORVMIVQULIKXCP-UHFFFAOYSA-N trichloro(phenyl)silane Chemical compound Cl[Si](Cl)(Cl)C1=CC=CC=C1 ORVMIVQULIKXCP-UHFFFAOYSA-N 0.000 description 1
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Classifications
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09D—COATING COMPOSITIONS, e.g. PAINTS, VARNISHES OR LACQUERS; FILLING PASTES; CHEMICAL PAINT OR INK REMOVERS; INKS; CORRECTING FLUIDS; WOODSTAINS; PASTES OR SOLIDS FOR COLOURING OR PRINTING; USE OF MATERIALS THEREFOR
- C09D1/00—Coating compositions, e.g. paints, varnishes or lacquers, based on inorganic substances
- C09D1/02—Coating compositions, e.g. paints, varnishes or lacquers, based on inorganic substances alkali metal silicates
- C09D1/04—Coating compositions, e.g. paints, varnishes or lacquers, based on inorganic substances alkali metal silicates with organic additives
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09D—COATING COMPOSITIONS, e.g. PAINTS, VARNISHES OR LACQUERS; FILLING PASTES; CHEMICAL PAINT OR INK REMOVERS; INKS; CORRECTING FLUIDS; WOODSTAINS; PASTES OR SOLIDS FOR COLOURING OR PRINTING; USE OF MATERIALS THEREFOR
- C09D7/00—Features of coating compositions, not provided for in group C09D5/00; Processes for incorporating ingredients in coating compositions
- C09D7/40—Additives
- C09D7/60—Additives non-macromolecular
- C09D7/61—Additives non-macromolecular inorganic
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09D—COATING COMPOSITIONS, e.g. PAINTS, VARNISHES OR LACQUERS; FILLING PASTES; CHEMICAL PAINT OR INK REMOVERS; INKS; CORRECTING FLUIDS; WOODSTAINS; PASTES OR SOLIDS FOR COLOURING OR PRINTING; USE OF MATERIALS THEREFOR
- C09D7/00—Features of coating compositions, not provided for in group C09D5/00; Processes for incorporating ingredients in coating compositions
- C09D7/40—Additives
- C09D7/60—Additives non-macromolecular
- C09D7/63—Additives non-macromolecular organic
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09D—COATING COMPOSITIONS, e.g. PAINTS, VARNISHES OR LACQUERS; FILLING PASTES; CHEMICAL PAINT OR INK REMOVERS; INKS; CORRECTING FLUIDS; WOODSTAINS; PASTES OR SOLIDS FOR COLOURING OR PRINTING; USE OF MATERIALS THEREFOR
- C09D7/00—Features of coating compositions, not provided for in group C09D5/00; Processes for incorporating ingredients in coating compositions
- C09D7/40—Additives
- C09D7/65—Additives macromolecular
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09D—COATING COMPOSITIONS, e.g. PAINTS, VARNISHES OR LACQUERS; FILLING PASTES; CHEMICAL PAINT OR INK REMOVERS; INKS; CORRECTING FLUIDS; WOODSTAINS; PASTES OR SOLIDS FOR COLOURING OR PRINTING; USE OF MATERIALS THEREFOR
- C09D7/00—Features of coating compositions, not provided for in group C09D5/00; Processes for incorporating ingredients in coating compositions
- C09D7/40—Additives
- C09D7/70—Additives characterised by shape, e.g. fibres, flakes or microspheres
Abstract
The invention discloses an inorganic ceramic tile crack beautifying coating and a preparation method thereof, and aims to solve the technical problems of improving the environmental protection performance of the ceramic tile crack beautifying coating and reducing the cost. The inorganic ceramic tile crack beautifying coating comprises the following components: 305-320 parts of water, 150-200 parts of potassium silicate, 200-250 parts of organic silicon resin, 50-100 parts of fumed silica, 3-8 parts of an anionic stabilizer, 5-10 parts of a dispersing agent, 1-2 parts of cellulose, 30-50 parts of a silane coupling agent and 100-200 parts of a toner. The preparation method comprises the following steps: the slurry system is premixed, and the auxiliary agent, the gas phase dioxide, the toner and the film forming substance are added. Compared with the prior art, the inorganic ceramic tile crack beautifying coating has a petrochemical reaction with the original cement-based crack filling agent, combines the silicon material of the ceramic tile, and forms the ceramic tile, the original crack filling agent and the ceramic tile into an integrated structure, so that the ceramic tile and the waterproof layer are not damaged, the potential safety hazard is eliminated, no dust is generated in the construction process, no pollution is caused to home decoration or decorative surfaces, the environment is protected, and the cost is low.
Description
Technical Field
The invention relates to a building material and a preparation method thereof, in particular to a building decoration material and a preparation method thereof.
Background
In the modern home decoration case, people have higher and higher requirements on the home decoration effect, and gaps of floor tiles and wall tiles are mostly treated by using a white cement-based caulking agent. If the white cement-based joint compound is moved on the surface of the tile for a long time, the white cement-based joint compound is blackened, the color of the white cement-based joint compound is particularly prominent compared with that of the tile, and the vision and mood caused by the dirt are greatly influenced. Based on the situation, according to market demands, the water-based epoxy resin crack sealing agent is produced in the market and reaches a state of being used in large quantity at one time, but the water-based epoxy resin crack sealing agent is complex to construct, 1, the early cleaning work difficulty is high, the cement-based crack sealing agent in the original ceramic tile crack needs to be cleaned, the process difficulty is very high, the ceramic tile is damaged when the treatment is not good, and great time is spent on replacing the ceramic tile. 2. Dust is generated, the dust is easily generated in the cleaning process, the home decoration or the decorative surface is easily polluted, and the respiratory dust diseases are caused to workers. 3. The waterproof layer is damaged, the waterproof layer is easy to damage when the ceramic tiles are cleaned in kitchens and bathrooms, and the hidden danger of water leakage and water seepage is brought to later use. 4. The epoxy resin type seam beautifying agent in the prior art is a two-component composition, and along with the rising of the price of petroleum raw materials, the epoxy resin and auxiliary raw materials are also raised by water, so that the price of the epoxy resin type seam beautifying agent material is high. 5. The environment is polluted, and the epoxy resin type seam beautifying agent has volatile organic compound VOC release and can bring harm to the human body health. 6. The epoxy resin type crack beautifying agent is brittle after being cured, cracks can appear with ceramic tile faults along with expansion with heat and contraction with cold, the construction needs to be cleaned again, the epoxy resin type crack beautifying agent is high in hardness, secondary construction can be caused, the difficulty is increased, and the construction cost is greatly increased. Therefore, the market urgently needs environment-friendly, low-cost and beautiful tile crack-beautifying coating.
Disclosure of Invention
The invention aims to provide an inorganic ceramic tile crack beautifying coating and a preparation method thereof, and aims to solve the technical problems of improving the environmental protection performance of the ceramic tile crack beautifying coating and reducing the cost.
The invention adopts the following technical scheme: an inorganic ceramic tile crack beautifying coating comprises the following materials in parts by weight: 305-320 parts of water, 150-200 parts of potassium silicate, 200-250 parts of organic silicon resin, 50-100 parts of fumed silica, 3-8 parts of an anionic stabilizer, 5-10 parts of a dispersing agent, 1-2 parts of cellulose, 30-50 parts of a silane coupling agent and 100-200 parts of a toner.
The inorganic ceramic tile crack beautifying coating comprises the following materials in parts by weight: 1-3 parts of defoaming agent and 1-3 parts of thickening agent.
The inorganic ceramic tile crack beautifying coating disclosed by the invention is composed of the following materials in parts by weight: 320 parts of water, 150 parts of potassium silicate, 200 parts of organic silicon resin, 89.5 parts of fumed silica, 3 parts of an anionic stabilizer, 1 part of a defoaming agent, 5 parts of a dispersing agent, 1.5 parts of cellulose, 30 parts of a silane coupling agent, 1 part of a thickening agent and 200 parts of a toner.
The inorganic ceramic tile crack beautifying coating disclosed by the invention is composed of the following materials in parts by weight: 310 parts of water, 200 parts of potassium silicate, 230 parts of organic silicon resin, 50 parts of fumed silica, 6 parts of an anionic stabilizer, 2.3 parts of a defoaming agent, 7 parts of a dispersing agent, 1.7 parts of cellulose, 40 parts of a silane coupling agent, 3 parts of a thickening agent and 150 parts of a toner.
The inorganic ceramic tile crack beautifying coating disclosed by the invention is composed of the following materials in parts by weight: 3050 part of water, 170 parts of potassium silicate, 250 parts of organic silicon resin, 100 parts of fumed silica, 8 parts of an anionic stabilizer, 3 parts of a defoaming agent, 10 parts of a dispersing agent, 2 parts of cellulose, 50 parts of a silane coupling agent, 2 parts of a thickening agent and 100 parts of a toner.
A preparation method of an inorganic ceramic tile crack beautifying coating comprises the following steps:
step one, premixing a slurry system
At room temperature, adding 305-320 parts of water by mass into a dispersing container, adding 1-2 parts of cellulose at a speed of 0.1 part per second under a dispersing and stirring state at a rotating speed of 300-600 rpm, dispersing for 3-5 minutes until the mixture is uniform, adding 150-200 parts of potassium silicate at a speed of 1 part per second, and dispersing for 5 minutes at a rotating speed of 800rpm to obtain a colloidal transparent slurry system;
step two, adding an auxiliary agent
At the rotating speed of 300-600 rpm, sequentially adding 5-10 parts of dispersing agent, 3-8 parts of anionic stabilizer and 1-3 parts of defoaming agent into the slurry system in a dispersing container, and dispersing for 5 minutes at the rotating speed of 800-1000 rpm to obtain the slurry system added with the auxiliary agent;
step three, adding fumed silica
Adding 50-100 parts of fumed silica at the speed of 1 part per second at the rotating speed of 300-600 rpm, and stirring and dispersing for 10-15 minutes at the rotating speed of 800-1000 rpm to obtain a slurry system added with the fumed silica;
step four, adding toner
Adding 100-200 parts of toner into a slurry system added with fumed silica, and dispersing for 30 minutes at the rotating speed of 1200-1500 rpm to obtain slurry;
step five, adding a film forming substance
And (2) adding 30-50 parts of silane coupling agent at the speed of 1 part per second at the rotating speed of 800-1000 rpm, dispersing for 5 minutes, adding 200-250 parts of organic silicon resin at the speed of 1 part per second, and stirring for 5 minutes to obtain the inorganic tile seam beautifying coating.
Adjusting the viscosity after the fifth step of the method, adding 1-3 parts of thickening agent into the coating slurry, and stirring for 5 minutes at the rotating speed of 800-1000 rpm.
The method comprises the following steps of 320 parts of water, 150 parts of potassium silicate, 200 parts of organic silicon resin, 89.5 parts of fumed silica, 3 parts of an anionic stabilizer, 1 part of a defoaming agent, 5 parts of a dispersing agent, 1.5 parts of cellulose, 30 parts of a silane coupling agent, 1 part of a thickening agent and 200 parts of a toner.
The method comprises the following steps of 310 parts of water, 200 parts of potassium silicate, 230 parts of organic silicon resin, 50 parts of fumed silica, 6 parts of an anionic stabilizer, 2.3 parts of a defoaming agent, 7 parts of a dispersing agent, 1.7 parts of cellulose, 40 parts of a silane coupling agent, 3 parts of a thickening agent and 150 parts of a toner.
3050 part of water, 170 parts of potassium silicate, 250 parts of organic silicon resin, 100 parts of fumed silica, 8 parts of an anionic stabilizer, 3 parts of a defoaming agent, 10 parts of a dispersing agent, 2 parts of cellulose, 50 parts of a silane coupling agent, 2 parts of a thickening agent and 100 parts of a toner.
Compared with the prior art, the inorganic ceramic tile crack beautifying coating has a petrochemical reaction with the original cement-based gap filler, combines the silicon material of the ceramic tile, and forms an integrated structure of the ceramic tile, the original gap filler and the ceramic tile, so that the ceramic tile and the waterproof layer are not damaged, the potential safety hazard is eliminated, dust is not generated in the construction process, home decoration or decorative surfaces are not polluted, respiratory dust diseases of workers are not caused, VOC (volatile organic compounds) release is zero, the environment is protected, and the cost is low.
Detailed Description
The present invention will be described in further detail with reference to examples.
The inorganic ceramic tile crack beautifying coating disclosed by the invention is composed of the following materials in parts by weight: 305-320 parts of water, 150-200 parts of potassium silicate, 200-250 parts of organic silicon resin, 50-100 parts of fumed silica, 3-8 parts of an anionic stabilizer, 1-3 parts of a defoaming agent, 5-10 parts of a dispersing agent, 1-2 parts of cellulose, 30-50 parts of a silane coupling agent, 1-3 parts of a thickening agent and 100-200 parts of a toner.
The preparation method of the inorganic ceramic tile crack beautifying coating comprises the following steps:
step one, premixing a slurry system
Adding 305-320 parts of water into a dispersing container according to parts by weight at room temperature (20 ℃), slowly adding 1-2 parts of cellulose at the speed of 0.1 part per second under the condition of dispersing and stirring at the rotating speed of 300-600 rpm, dispersing for 3-5 minutes until the mixture is uniform, slowly adding 150-200 parts of potassium silicate at the speed of 1 part per second, and dispersing for 5 minutes at the rotating speed of 800rpm until the mixture is sufficiently and uniformly dispersed to obtain a colloidal transparent slurry system.
The method has the effects that the high alkalinity of the potassium silicate is utilized to rapidly dissolve the cellulose, so that the cellulose becomes transparent colloid in a potassium silicate system, the potassium silicate system is thickened, and a framework is provided for the stability of the inorganic ceramic tile crack beautifying coating by utilizing a three-dimensional network structure provided by the cellulose.
Step two, adding an auxiliary agent
And at the rotating speed of 300-600 rpm, sequentially adding 5-10 parts of dispersing agent, 3-8 parts of anionic stabilizer and 1-3 parts of defoaming agent into the slurry system in a dispersing container, dispersing for 5 minutes at the rotating speed of 800-1000 rpm, and mixing uniformly to obtain the slurry system added with the auxiliary agent.
The defoaming agent is added in the step to solve the problem of bubbles caused by high-speed dispersion so as to increase the mass of a unit volume, the dispersing agent is added to wet the dispersing agent of the toner powder after the fumed silica is added in the step three and the toner is added in the step four, so that the molecular tension is reduced, the toner powder in the unit volume is easier to disperse, and the anionic stabilizer is added to stabilize the stability of the free metal toner powder in a colloidal transparent slurry system, so that the whole inorganic tile seam beautifying coating system is stabilized.
Step three, adding fumed silica
Slowly adding 50-100 parts of fumed silica at the speed of 1 part per second at the rotating speed of 300-600 rpm, and stirring and dispersing for 10-15 minutes at the rotating speed of 800-1000 rpm to obtain a transparent and uniform slurry system added with the fumed silica.
The fumed silica is used as a thixotropic agent and a thickening agent of a liquid slurry system to prevent precipitation and sagging. The step is used for improving the viscoelastic property of the inorganic ceramic tile seam beautifying coating elastomer, reinforcing and improving the adhesive force and flexibility of the inorganic ceramic tile seam beautifying coating film.
Step four, adding toner
And adding 100-200 parts of toner into the slurry system added with the fumed silica, and dispersing for 30 minutes at the rotating speed of 1200-1500 rpm to a uniform state to obtain slurry.
The inorganic ceramic tile crack beautifying coating can obtain color diversity by adding the toner, and the requirements of different customers on the appearance are met.
Step five, adding a film forming substance
Slowly adding 30-50 parts of silane coupling agent at the speed of 1 part per second at the rotating speed of 800-1000 rpm, dispersing for 5 minutes until the mixture is uniformly stirred, slowly adding 200-250 parts of organic silicon resin at the speed of 1 part per second, and stirring for 5 minutes until the mixture is uniform, thereby obtaining the coating slurry.
The silane coupling agent is used for connecting the organic silicon resin and the inorganic material potassium silicate into a whole through the chain end of the silane coupling agent, and modifying the film forming substance to obtain the hybrid reaction of the film forming substance organic silicon resin, so that the functional diversity and the stability of the film forming substance are maintained.
Step six, adjusting the viscosity
And adding 1-3 parts of thickening agent into the coating slurry, and stirring at the rotating speed of 800-1000 rpm for 5 minutes to ensure that the viscosity of the coating slurry is 88-92 KU, thereby obtaining the inorganic ceramic tile crack beautifying coating.
The viscosity is controlled in the step, the later anti-settling and construction rheological property is acted, and the construction is convenient.
The inorganic ceramic tile crack beautifying coating prepared by the method can be packaged by a glass cement packaging bottle, the packaging bottle is hard or soft, the packaging bottle is stored in a cool and dry place, the quality guarantee period is 6 months at 25 ℃, and the inorganic ceramic tile crack beautifying coating is directly packaged and bottled in use and is extruded for construction.
In the inorganic ceramic tile crack beautifying coating and the preparation method thereof,
the water is used as a carrier and a solvent when used for manufacturing the inorganic ceramic tile crack beautifying coating, and is used for maintaining a cement base surface during ceramic tile crack beautifying construction.
In the embodiment, tap water is used as water.
The silicic acid ions in the potassium silicate exchange with the silicic acid ions in the cement matrix to generate fusion reaction, namely the potassium silicate is fused with the ceramic tile and the silicate in the cement-based joint filling. The potassium silicate is used as a film forming substance to enhance and improve the adhesive force and water resistance of the inorganic ceramic tile crack beautifying coating, and the molar ratio of silicon dioxide to potassium oxide in the potassium silicate is 3.8.
The potassium silicate is an inorganic material, and is easy to be brittle, and is combined with the fumed silica, so that the problems of poor coating hardness, easiness in falling, porosity, incompactness, poor stain resistance and easiness in thickening during storage are solved. Penetration of silicone resinThe ceramic tile and cement-based joint mixture has strong capacity, the molecular structure of the ceramic tile and cement-based joint mixture is in a nanometer level, and the ceramic tile and cement-based joint mixture can be easily permeated into gaps of the ceramic tile and cement-based joint mixture, namely, the ceramic tile and cement-based joint mixture can be reinforced by one-time surrounding after the cross-linking reaction of inorganic potassium silicate and the ceramic tile and cement-based joint mixture. Potassium silicate K2SiO3The inorganic ceramic tile crack beautifying coating has strong basicity and pH value of more than 11, inhibits the generation of microorganisms, has natural mould-proof performance, and can generate a soft-hard combined structure through chemical reaction after forming a film in a crack.
In the examples, the potassium silicate is AH-K2 inorganic potassium silicate of Ohan chemical Co., Ltd, Beijing, the Baume Be of the potassium silicate is 28.0-31.0 at 20 ℃, and the potassium oxide K2O% is not less than 7.5, silicon dioxide SiO2The viscosity is more than or equal to 18.0, the modulus is 3.75-4.15, the pH value is 11-12, and the appearance is colorless to yellowish, tasteless and slightly grayish transparent or semitransparent viscous liquid.
The organic silicon resin has strong permeability, the molecular structure of the organic silicon resin is in a nanometer level, the organic silicon resin can easily permeate into gaps of the ceramic tiles and the cement-based joint mixture, namely, the organic silicon resin is used for one-time surrounding reinforcement after the cross-linking reaction of the inorganic potassium silicate and the ceramic tiles and the cement joint mixture, and has strong hydrophobicity and dirt resistance. The organic silicon resin is polyorganosiloxane with a highly cross-linked network structure, is methyl trichlorosilane, dimethyl dichlorosilane, phenyl trichlorosilane, diphenyl dichlorosilane or a mixture of methyl phenyl dichlorosilane, an organic solvent and water, and is hydrolyzed by adding water at a lower temperature in the presence of organic solvent toluene to obtain an acidic hydrolysate. The initial product of hydrolysis is a mixture of cyclic, linear and crosslinked polymers, which usually also contain considerable hydroxyl groups. Washing the hydrolysate with water to remove acid, thermally oxidizing the neutral initial polymer in air or further polycondensing in the presence of catalyst to form a highly crosslinked stereo network structure.
In the embodiment, the organic silicon resin is LOONGRUN WR1932 organic silicon resin of Shenzhen Shanghan Runji chemical Limited, is water-diluted organic silicon resin emulsion, is milky white liquid in appearance, and has a density of 103-1.11 g/cm at 25 DEG C3。
The fumed silica is used for improving the viscoelastic property of the inorganic ceramic tile seam beautifying coating elastomerThe coating film has the advantages of strong adhesion and flexibility, capability of improving the adhesion and flexibility of an inorganic ceramic tile crack-beautifying coating film, capability of being used as a liquid thixotropic agent and a thickening agent, and precipitation and sagging prevention. The fumed silica is a porous material, and the composition thereof can be SiO2·nH2O represents, wherein nH2O is in the form of surface hydroxyl groups, and is soluble in caustic and hydrofluoric acid.
In the examples, the fumed silica used was degussa fumed silica R972, which was won from the industrial group.
The anionic stabilizer is a mild surfactant and has a stabilizing effect on a system to which potassium silicate is added.
In the examples, LOPON827 from Aohan chemical Co., Ltd, Beijing was used as the anionic stabilizer, the anionic stabilizer was an amine derivative, the solid content was 45%, the pH was 7.5, the viscosity was 450mpa.s at 5 ℃ and 60rpm, and the ionic property: an anion.
The defoaming agent is used for eliminating various bubbles generated in the production, packaging, transportation and construction processes.
In the examples, the antifoam used was a BYK-024 antifoam from Bike chemical, Germany, which is a mixture of hydrophobic solids in polyethylene glycol with a defoaming polysiloxane with a nonvolatile content of > 95%.
The dispersant plays a role in wetting and dispersing the fumed silica and the toner.
In the examples, 5040 dispersant is adopted as the dispersant, and the dispersant is a sodium polycarboxylate dispersant.
The cellulose is used for providing the inorganic ceramic tile crack beautifying coating system with the guarantee of good thickening, suspension, dispersion, emulsification, adhesion, film formation, moisture protection and protective colloid through the hydrophilicity of hydroxyethyl cellulose groups and a three-dimensional grid structure of the hydroxyethyl cellulose groups.
In the examples, 250HBR hydroxyethyl cellulose available from Xiamen Suanqianlong technologies, Inc. was used as the cellulose. The hydroxyethyl cellulose has a molar substitution degree of 1.8-2.0 and a viscosity range of 1500-2500 cps.
The silane coupling agent is N- (beta-aminoethyl-gamma-aminopropyl) trimethoxy silane which is bifunctional silane with active amino group and hydrolyzable inorganic methoxy silicon group, organic materials and inorganic materials are bonded and connected into a whole through the chain end of the silane coupling agent, and the organic materials and the inorganic materials are modified to form hybrid reaction of a film forming substance, so that the functional diversity of the film forming substance is maintained, the stability of the organic materials and the inorganic materials is also maintained, and the color phase of gaps is finally changed, namely the aesthetic diversity is maintained.
In the examples, KH792 silane coupling agent of Dewar chemical (Shanghai) Co., Ltd was used as the silane coupling agent, and the purity was 98% and the density was 1.03g/ml at 25 ℃.
The thickener is used as a rheological additive, can thicken the inorganic ceramic tile crack beautifying coating, prevents the sagging phenomenon in construction, and can endow the inorganic ceramic tile crack beautifying coating with excellent mechanical performance and storage stability.
In the embodiment, the thickener is ACRYSOL RM-8W thickener of Lohmere Haslen Asia Leshun company in America, which is nonionic polyurethane associative thickener with mass solid content: 20.8-21.8%, specific gravity: 1.04 kg/l, Brookfield viscosity: 0-99999 centipoise, chemical type: non-ionic.
The toner is used for keeping the diversity of the hue of the inorganic tile seam beautifying coating, so that the inorganic tile seam beautifying coating is compact after construction, and floating dust is prevented from entering.
In the embodiment, the toner is inorganic toner or glitter powder.
The inorganic ceramic tile crack beautifying coating is directly extruded and coated in ceramic tile cracks at the opening.
Example 1
Step one, premixing a slurry system
320kg of water was added to a dispersion vessel, 1.5kg of cellulose was slowly added at a rate of 0.1 part per second under dispersion stirring at a rotation speed of 600rpm, and dispersed for 5 minutes to uniformity, and 150kg of potassium silicate was slowly added at a rate of 1 part per second, and dispersed for 5 minutes at a rotation speed of 800rpm to be sufficiently and uniformly dispersed, to obtain a gelatinous and transparent slurry system.
Step two, adding an auxiliary agent
At the rotating speed of 600rpm, 5kg of dispersing agent, 3kg of anionic stabilizer and 1kg of defoaming agent are sequentially added into a dispersing container, and at the rotating speed of 800rpm, the materials are dispersed for 5 minutes until the materials are uniformly mixed, so that a slurry system added with the auxiliary agent is obtained.
Step three, adding fumed silica
89.5kg of fumed silica was slowly added at a rate of 1 part per second at 600rpm, and the mixture was dispersed with stirring at 800rpm for 10 minutes to obtain a transparent and uniform fumed silica-added slurry system.
Step four, adding toner
200kg of toner was added to the slurry system to which fumed silica was added, and dispersed at 1500rpm for 30 minutes to a uniform state to obtain a slurry.
Step five, adding a film forming substance
Under the condition of the rotating speed of 800rpm, slowly adding 30kg of silane coupling agent at the speed of 1 part per second, dispersing for 5 minutes until stirring uniformly, then slowly adding 200kg of organic silicon resin at the speed of 1 part per second, and stirring for 5 minutes until the uniform state is obtained, thus obtaining the coating slurry.
Step six, adjusting the viscosity
And adding 1kg of thickening agent into the coating slurry, and stirring for 5 minutes at the rotating speed of 1000rpm to ensure that the viscosity of the coating slurry is 88-92 KU, thereby obtaining the inorganic ceramic tile crack beautifying coating.
Example 2
Step one, premixing a slurry system
310kg of water was added to the dispersion vessel, and under a dispersion stirring condition at a rotation speed of 600 rpm), 1.7kg of cellulose was slowly added at a rate of 0.1 part per second, and dispersed for 5 minutes to be uniform, and 200 parts of potassium silicate was slowly added at a rate of 1 part per second, and dispersed at a rotation speed of 800rpm for 5 minutes to be sufficiently and uniformly dispersed, to obtain a paste system in a gelatinous and transparent state.
Step two, adding an auxiliary agent
7kg of dispersing agent, 6kg of anionic stabilizer and 2.3kg of defoaming agent are sequentially added into a dispersing container at the rotating speed of 600rpm, and the mixture is dispersed for 5 minutes at the rotating speed of 800rpm until the mixture is uniformly mixed to obtain a slurry system added with the auxiliary agent.
Step three, adding fumed silica
At the rotation speed of 600rpm, 50kg of fumed silica is slowly added at the speed of 1 part per second, and at the rotation speed of 800rpm, the mixture is stirred and dispersed for 10 minutes, so that a transparent and uniform fumed silica-added slurry system is obtained.
Step four, adding toner
150kg of toner was added to the slurry system to which fumed silica was added, and dispersed at 1500rpm for 30 minutes to a uniform state to obtain a slurry.
Step five, adding a film forming substance
Under the condition of the rotating speed of 800rpm, slowly adding 40kg of silane coupling agent at the speed of 1 part per second, dispersing for 5 minutes until stirring uniformly, then slowly adding 230kg of organic silicon resin at the speed of 1 part per second, and stirring for 5 minutes until the uniform state is obtained, thus obtaining the coating slurry.
Step six, adjusting the viscosity
Adding 3kg of thickening agent into the coating slurry, and stirring for 5 minutes at the rotating speed of 1000rpm to ensure that the viscosity is 88-92 KU, thereby obtaining the inorganic ceramic tile crack beautifying coating.
Example 3
Step one, premixing a slurry system
305kg of water was charged into a dispersion vessel, 2kg of cellulose was slowly charged at a rate of 0.1 part per second under dispersion stirring at a rotation speed of 600rpm, and dispersed for 5 minutes to be uniform, and 170 parts of potassium silicate was slowly charged at a rate of 1 part per second, and dispersed for 5 minutes at a rotation speed of 800rpm to be sufficiently and uniformly dispersed, thereby obtaining a gelatinous and transparent slurry system.
Step two, adding an auxiliary agent
At the rotating speed of 600rpm, 10kg of dispersing agent, 8kg of anionic stabilizer and 3kg of defoaming agent are sequentially added into a dispersing container, and the mixture is dispersed for 5 minutes at the rotating speed of 800rpm until the mixture is uniformly mixed to obtain a slurry system added with the auxiliary agent.
Step three, adding fumed silica
100kg of fumed silica was slowly added at a rate of 1 part per second at 600rpm, and the mixture was dispersed for 10 minutes under stirring at 800rpm to obtain a transparent and uniform fumed silica-added slurry system.
Step four, adding toner
100kg of toner was added to the slurry system to which fumed silica was added, and dispersed at 1500rpm for 30 minutes to a uniform state to obtain a slurry.
Step five, adding a film forming substance
Under the condition of the rotating speed of 800rpm, slowly adding 50kg of silane coupling agent at the speed of 1 part per second, dispersing for 5 minutes until stirring uniformly, then slowly adding 250kg of organic silicon resin at the speed of 1 part per second, and stirring for 5 minutes until the uniform state is obtained, thus obtaining the coating slurry.
Step six, adjusting the viscosity
Adding 2kg of thickening agent into the coating slurry, and stirring for 5 minutes at the rotating speed of 1000rpm to ensure that the viscosity is 88-92 KU, thereby obtaining the inorganic ceramic tile crack beautifying coating.
The difference between the comparative example 1 and the examples 1-3 is that the system is different, the comparative example 1 is an epoxy and amine two-component crosslinking curing system, and the examples 1-3 are single-component water moisture curing systems. The conditions from production, packaging to construction of the comparative example 1 are higher than those of the examples 1 to 3, the comparative example 1 is a two-component crosslinking curing reaction, the construction time is limited, and the construction time of the examples 1 to 3 can be greatly prolonged compared with that of the comparative example 1.
Taking 500g of the inorganic tile seam beautifying coating of the examples 1-3 and the coating of the comparative example 1, respectively constructing 5 square meters in the original tile seam of 60 x 60mm, and constructing according to the tile seam construction method of the inorganic tile seam beautifying coating and the coating. Testing and observing:
comparative example 1, need to clear up the cement base gap filler in original ceramic tile gap, this process probably can destroy the ceramic tile, and the cleaning work degree in earlier stage is big. Dust is easily generated in the cleaning process, the home decoration or the decorative surface is easily polluted, and respiratory dust diseases are caused to workers. The waterproof layer is easy to damage when the ceramic tiles are cleaned in the kitchen and the bathroom, and the hidden danger of water leakage and water seepage is brought to later use. The original epoxy resin type seam beautifying agent has VOC release and can bring harm to the body health of human bodies. Because the epoxy resin type crack beautifying agent is brittle after being cured, the crack can be broken with the ceramic tile along with expansion with heat and contraction with cold, the new construction needs to be cleaned, the hardness of the epoxy resin type crack beautifying agent is high, the difficulty of secondary construction is increased, and the construction cost is greatly increased.
In embodiments 1 to 3, the cement-based gap filler in the gap of the original ceramic tile does not need to be cleaned, the original cement-based gap filler can generate a petrochemical reaction with the inorganic ceramic tile seam beautifying coating, the ceramic tile, the original gap filler and the ceramic tile are integrated into a whole through the chemical reaction of the inorganic ceramic tile seam beautifying coating in combination with the silicon material of the ceramic tile, the labor cost is reduced, the risk of damaging the ceramic tile is avoided, the risk of damaging the waterproof layer is also avoided, and the potential safety hazard in the tile is eliminated. Dust can not be generated in the construction process, home decoration or decorative surfaces can not be polluted, and respiratory dust diseases can not be caused to workers. The inorganic ceramic tile crack beautifying coating disclosed by the invention has zero VOC (volatile organic compounds) release, and cannot cause pollution to the environment.
As can be seen from the comparison results, the inorganic tile crack beautifying coating of the embodiments 1-3 is environment-friendly and low in construction cost.
TABLE 1 Components and amounts of examples 1-3 and comparative example 1
The silane coupling agent is added, the silicon alkoxide group has hydrolysis reactivity, and the hydrolysis forms bonding between the inorganic material interface and the organic material interface to promote interface fusion.
Thus, the silane coupling agent is interposed between the inorganic and organic interfaces and forms a bonding layer of organic matrix-silane coupling agent-inorganic matrix, i.e. the silane coupling agent interacts both with the hydroxyl groups in the inorganic and with the long molecular chains in the organic polymer. The function of the composite material is to couple two materials with different properties, thereby improving the performance of the combination of the potassium silicate and the organic silicon resin. The silane coupling agent is added, so that the performance of combining organic and inorganic materials among inorganic potassium silicate, fumed silica and organic silicon resin is well improved, the petrochemical reaction of the inorganic potassium silicate, ceramic tiles and cement is kept, and the characteristics of the fumed silica are also kept: the inorganic ceramic tile crack beautifying coating is used as a thixotropic agent and a thickening agent of liquid, prevents precipitation and sagging, improves the suspension property and the dispersibility of a toner pigment filler in an inorganic ceramic tile crack beautifying coating liquid system, and improves the scratch resistance, the adhesive force and the flexibility of a paint film of the inorganic ceramic tile crack beautifying coating. Because of this, it is possible to reduce the number of the,
1. the structural general formula of the silane coupling agent is YRSiX3, and R is alkyl; y is an organic reactive group that reacts with the polymer; and X is a hydrophilic group which forms a firm chemical bond with the inorganic filler. These two materials, which differ greatly in their properties, are "coupled" by chemical bonds, giving good adhesion. In the general formula: x is different from Y in reaction characteristics, X is a group which can be hydrolyzed to generate a silicon hydroxyl group (Si-OH), X has the bonding capability with glass, silica, potassium silicate and pottery clay, and Y is an organic group which is reacted with the polymer to improve the reactivity and compatibility of silane and polymer, such as vinyl, amino, epoxy and mercapto. R has a carbon chain of saturated or unsaturated bonds, by which Y and Si atoms are linked, and such compounds are known as coupling agents.
2. The wetting effect and the surface energy effect are important in the production of inorganic composite materials for good wetting of the material with an adherend. If complete wetting is obtained, the bonding strength of the base material to the high-energy surface physical adsorption is far higher than the cohesive strength of the organic base material, and the surface tension of the inorganic material is improved by treating the surface of the inorganic material with the silane coupling agent, so that the organic material is promoted to be on the surface of the inorganic material, and the surface tension of the organic material is promoted to be wetted and spread on the surface of the inorganic material.
3. And (4) morphological theory. The silane coupling agent on the inorganic filler will modify the morphology of the adjacent organic polymer in some way, thereby improving the bonding effect. The deformable layer theory suggests that a flexible resin layer may be created to relieve the interfacial stress; while constrained layer theory holds that the silane can "tie" the polymer structure in the interphase region.
The gas phase silicon dioxide adopted by the invention has the characteristics of serious coordination insufficiency, huge specific surface area and insufficient surface oxygen, so that the gas phase silicon dioxide has extremely strong activity, can easily perform bonding action with the oxygen of epoxy cyclic molecules, improves the bonding force among molecules, and simultaneously has a part of gas phase silicon dioxide particles still distributed in the gaps of the silane coupling agent and the macromolecular chains of the organic silicon resin, shows very high flow ripple property, thereby greatly improving the strength, toughness and ductility of inorganic materials added into the gas phase silicon dioxide, and having the hydrophobicity and dirt resistance of the organic silicon resin.
When the ceramic tile is in seam beautifying construction, silicic acid ions in the potassium silicate exchange with silicic acid ions in the cement matrix to generate fusion reaction, so that the potassium silicate, the ceramic tile and the silicate in the cement-based seam filling matrix are fused into a whole. The potassium silicate is an inorganic material, and the problem that the inorganic ceramic tile crack beautifying coating is poor in hardness, easy to fall off, porous, not compact, poor in stain resistance and easy to thicken during storage due to the fact that the potassium silicate is fragile and added with fumed silica is solved. The organic silicon resin has strong permeability, the molecular structure of the organic silicon resin is in a nanometer level, the organic silicon resin can easily permeate into gaps of the ceramic tiles and the cement-based joint mixture, and the fumed silica reinforces the inorganic potassium silicate, the ceramic tiles and the cement joint mixture in a surrounding way after the crosslinking reaction.
When the inorganic ceramic tile seam beautifying coating is used, the cement-based gap filler in the gap of the original ceramic tile does not need to be cleaned, the original cement-based gap filler can generate petrochemical reaction with the inorganic ceramic tile seam beautifying coating, and the ceramic tile, the original gap filler and the ceramic tile form an integrated structure by combining with silicon materials of the ceramic tile and through the chemical reaction of the inorganic ceramic tile seam beautifying coating, so that the labor cost is saved, the risk of damaging the ceramic tile does not exist, the risk of damaging a waterproof layer made by the original building does not exist, and the potential safety hazard of building decoration is eliminated.
When the inorganic ceramic tile crack beautifying coating is used, no cement-based joint mixture in the ceramic tile crack is required to be cleaned, so that no dust is generated in the construction process, no pollution is caused to home decoration or decorative surfaces, and no respiratory dust pollution disease is caused to workers.
The inorganic ceramic tile crack beautifying coating disclosed by the invention adopts inorganic materials, VOC (volatile organic compounds) release is zero, and no pollution is caused to the environment.
The invention is single-component liquid coating, can be used after opening the tank, and has simple construction.
The invention adds micro-elastomer gas-like silicon dioxide, and can not cause the problem of shrinkage crack caused by thermal expansion and cold contraction. Even if the problem of small gaps occurs due to large thermal expansion and cold contraction. The repair is carried out by directly coating again, which brings great convenience to the construction.
The inorganic ceramic tile crack beautifying coating has the following advantages:
1. the cement-based joint mixture in the original ceramic tile gap does not need to be cleaned, the original cement-based joint mixture can generate petrochemical reaction with the inorganic ceramic tile joint beautifying coating, the ceramic tile, the original joint mixture and the ceramic tile are integrated into a whole through the chemical reaction of the inorganic ceramic tile joint beautifying coating by combining with the silicon material of the ceramic tile, the ceramic tile is not damaged, the waterproof layer is not damaged, and the potential safety hazard is eliminated.
2. Dust can not be generated in the construction process, home decoration or decorative surfaces can not be polluted, and respiratory dust diseases can not be caused to workers.
3. Zero VOC release and no pollution to the environment.
4. The paint is a single-component liquid paint, can be used after opening a tank, and is simple to construct.
5. The micro-elastomer gas-like silicon dioxide is added, so that the problem of shrinkage cracks caused by thermal expansion and cold contraction is avoided. Even if the problem of small gaps occurs due to large thermal expansion and cold contraction. The repair is carried out by directly coating again, which brings great convenience to the construction.
Claims (10)
1. An inorganic ceramic tile crack beautifying coating is characterized in that: the inorganic ceramic tile crack beautifying coating comprises the following materials in parts by weight: 305-320 parts of water, 150-200 parts of potassium silicate, 200-250 parts of organic silicon resin, 50-100 parts of fumed silica, 3-8 parts of an anionic stabilizer, 5-10 parts of a dispersing agent, 1-2 parts of cellulose, 30-50 parts of a silane coupling agent and 100-200 parts of a toner.
2. The inorganic tile crack sealer according to claim 1, wherein: the inorganic ceramic tile crack beautifying coating comprises the following materials in parts by weight: 1-3 parts of defoaming agent and 1-3 parts of thickening agent.
3. The inorganic tile crack sealer according to claim 2, wherein: the inorganic ceramic tile crack beautifying coating is prepared from the following materials in parts by weight: 320 parts of water, 150 parts of potassium silicate, 200 parts of organic silicon resin, 89.5 parts of fumed silica, 3 parts of an anionic stabilizer, 1 part of a defoaming agent, 5 parts of a dispersing agent, 1.5 parts of cellulose, 30 parts of a silane coupling agent, 1 part of a thickening agent and 200 parts of a toner.
4. The inorganic tile crack sealer according to claim 2, wherein: the inorganic ceramic tile crack beautifying coating is prepared from the following materials in parts by weight: 310 parts of water, 200 parts of potassium silicate, 230 parts of organic silicon resin, 50 parts of fumed silica, 6 parts of an anionic stabilizer, 2.3 parts of a defoaming agent, 7 parts of a dispersing agent, 1.7 parts of cellulose, 40 parts of a silane coupling agent, 3 parts of a thickening agent and 150 parts of a toner.
5. The inorganic tile crack sealer according to claim 2, wherein: the inorganic ceramic tile crack beautifying coating is prepared from the following materials in parts by weight: 3050 part of water, 170 parts of potassium silicate, 250 parts of organic silicon resin, 100 parts of fumed silica, 8 parts of an anionic stabilizer, 3 parts of a defoaming agent, 10 parts of a dispersing agent, 2 parts of cellulose, 50 parts of a silane coupling agent, 2 parts of a thickening agent and 100 parts of a toner.
6. A preparation method of an inorganic ceramic tile crack beautifying coating comprises the following steps:
step one, premixing a slurry system
At room temperature, adding 305-320 parts of water by mass into a dispersing container, adding 1-2 parts of cellulose at a speed of 0.1 part per second under a dispersing and stirring state at a rotating speed of 300-600 rpm, dispersing for 3-5 minutes until the mixture is uniform, adding 150-200 parts of potassium silicate at a speed of 1 part per second, and dispersing for 5 minutes at a rotating speed of 800rpm to obtain a colloidal transparent slurry system;
step two, adding an auxiliary agent
At the rotating speed of 300-600 rpm, sequentially adding 5-10 parts of dispersing agent, 3-8 parts of anionic stabilizer and 1-3 parts of defoaming agent into the slurry system in a dispersing container, and dispersing for 5 minutes at the rotating speed of 800-1000 rpm to obtain the slurry system added with the auxiliary agent;
step three, adding fumed silica
Adding 50-100 parts of fumed silica at the speed of 1 part per second at the rotating speed of 300-600 rpm, and stirring and dispersing for 10-15 minutes at the rotating speed of 800-1000 rpm to obtain a slurry system added with the fumed silica;
step four, adding toner
Adding 100-200 parts of toner into a slurry system added with fumed silica, and dispersing for 30 minutes at the rotating speed of 1200-1500 rpm to obtain slurry;
step five, adding a film forming substance
And (2) adding 30-50 parts of silane coupling agent at the speed of 1 part per second at the rotating speed of 800-1000 rpm, dispersing for 5 minutes, adding 200-250 parts of organic silicon resin at the speed of 1 part per second, and stirring for 5 minutes to obtain the inorganic tile seam beautifying coating.
7. The method for preparing the inorganic tile crack beautifying coating according to claim 6, characterized in that: and fifthly, adjusting the viscosity, adding 1-3 parts of thickening agent into the coating slurry, and stirring for 5 minutes at the rotating speed of 800-1000 rpm.
8. The method for preparing the inorganic tile crack beautifying coating according to claim 7, characterized in that: 320 parts of water, 150 parts of potassium silicate, 200 parts of organic silicon resin, 89.5 parts of fumed silica, 3 parts of an anionic stabilizer, 1 part of a defoaming agent, 5 parts of a dispersing agent, 1.5 parts of cellulose, 30 parts of a silane coupling agent, 1 part of a thickening agent and 200 parts of a toner.
9. The method for preparing the inorganic tile crack beautifying coating according to claim 7, characterized in that: 310 parts of water, 200 parts of potassium silicate, 230 parts of organic silicon resin, 50 parts of fumed silica, 6 parts of an anionic stabilizer, 2.3 parts of a defoaming agent, 7 parts of a dispersing agent, 1.7 parts of cellulose, 40 parts of a silane coupling agent, 3 parts of a thickening agent and 150 parts of a toner.
10. The method for preparing the inorganic tile crack beautifying coating according to claim 7, characterized in that: 3050 part of water, 170 parts of potassium silicate, 250 parts of organic silicon resin, 100 parts of fumed silica, 8 parts of an anionic stabilizer, 3 parts of a defoaming agent, 10 parts of a dispersing agent, 2 parts of cellulose, 50 parts of a silane coupling agent, 2 parts of a thickening agent and 100 parts of a toner.
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| JP2007277480A (en) * | 2006-04-11 | 2007-10-25 | Cemedine Co Ltd | Joint filler composition, joint-forming method, and joint structure |
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| CN110015864A (en) * | 2018-01-09 | 2019-07-16 | 广州芬得利建筑材料有限公司 | A kind of water-base resin base gap filler |
-
2022
- 2022-01-20 CN CN202210063478.3A patent/CN114381154A/en active Pending
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US4535109A (en) * | 1983-10-31 | 1985-08-13 | Toray Silicone Company, Ltd. | Method for producing silicone aqueous emulsion compositions |
| US4677160A (en) * | 1985-04-24 | 1987-06-30 | Toray Silicone Co., Ltd. | Method for producing an aqueous silicone emulsion composition |
| JP2007277480A (en) * | 2006-04-11 | 2007-10-25 | Cemedine Co Ltd | Joint filler composition, joint-forming method, and joint structure |
| US20170275479A1 (en) * | 2016-03-23 | 2017-09-28 | Henry Company, Llc | Low Dust Additives Comprising Emulsified Powder For Joint Compounds And Joint Compounds Thereof |
| CN110015864A (en) * | 2018-01-09 | 2019-07-16 | 广州芬得利建筑材料有限公司 | A kind of water-base resin base gap filler |
Non-Patent Citations (1)
| Title |
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| 兰永强 * |
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