CN109294382A - A kind of extra-weather-proof acid rain resistant stain resistant aqueous inorganic ceramic coating and preparation method thereof - Google Patents
A kind of extra-weather-proof acid rain resistant stain resistant aqueous inorganic ceramic coating and preparation method thereof Download PDFInfo
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- CN109294382A CN109294382A CN201811072985.3A CN201811072985A CN109294382A CN 109294382 A CN109294382 A CN 109294382A CN 201811072985 A CN201811072985 A CN 201811072985A CN 109294382 A CN109294382 A CN 109294382A
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- 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
- C09D143/00—Coating compositions based on homopolymers or copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and containing boron, silicon, phosphorus, selenium, tellurium, or a metal; Coating compositions based on derivatives of such polymers
- C09D143/04—Homopolymers or copolymers of monomers containing silicon
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- 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
- C09D5/00—Coating compositions, e.g. paints, varnishes or lacquers, characterised by their physical nature or the effects produced; Filling pastes
- C09D5/08—Anti-corrosive paints
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- 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
- C09D5/00—Coating compositions, e.g. paints, varnishes or lacquers, characterised by their physical nature or the effects produced; Filling pastes
- C09D5/16—Antifouling paints; Underwater paints
- C09D5/1656—Antifouling paints; Underwater paints characterised by the film-forming substance
- C09D5/1662—Synthetic film-forming substance
- C09D5/1668—Vinyl-type polymers
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- 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
- C09D5/00—Coating compositions, e.g. paints, varnishes or lacquers, characterised by their physical nature or the effects produced; Filling pastes
- C09D5/16—Antifouling paints; Underwater paints
- C09D5/1687—Use of special additives
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- 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
- C09D5/00—Coating compositions, e.g. paints, varnishes or lacquers, characterised by their physical nature or the effects produced; Filling pastes
- C09D5/18—Fireproof paints including high temperature resistant paints
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K3/00—Use of inorganic substances as compounding ingredients
- C08K3/18—Oxygen-containing compounds, e.g. metal carbonyls
- C08K3/24—Acids; Salts thereof
- C08K3/26—Carbonates; Bicarbonates
- C08K2003/265—Calcium, strontium or barium carbonate
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K3/00—Use of inorganic substances as compounding ingredients
- C08K3/30—Sulfur-, selenium- or tellurium-containing compounds
- C08K2003/3045—Sulfates
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K2201/00—Specific properties of additives
- C08K2201/014—Additives containing two or more different additives of the same subgroup in C08K
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L2201/00—Properties
- C08L2201/08—Stabilised against heat, light or radiation or oxydation
Abstract
The present invention relates to technical field of coatings, more particularly to a kind of extra-weather-proof acid rain resistant stain resistant aqueous inorganic ceramic coating and preparation method thereof, the inorganic nano ceramic coating is by silicone acrylic emulsion, silica solution, silane, active crosslinker, pigment, filler, wetting dispersing agent, defoaming agent, thickener and water composition, preparation method: first by by silicone acrylic emulsion, silica solution, silane, active crosslinker and water are prepared into the ceramic modified lotion of inorganic nano according to specific proportion and step, then the aqueous inorganic nano ceramics modified emulsion and pigment that will be prepared again, filler mixing, and dispersed, grinding, it is eventually adding auxiliary agent and water stirring, extra-weather-proof acid rain resistant stain resistant aqueous inorganic ceramic coating is made.Preparation method configuration of the invention is simple, and the coating products prepared have the characteristics that extra-weather-proof, acid rain resistant, stain resistant, height are hard wear-resisting and anti-scratch.
Description
Technical field
The present invention relates to technical field of coatings, make pottery more particularly, to a kind of extra-weather-proof acid rain resistant stain resistant aqueous inorganic nanometer
Porcelain coating and preparation method thereof.
Background technique
Currently, due to being chronically exposed in external environment, dust holds very much for exterior walls of buildings or automotive hub
Easily it is attached to coating surface layer or is drawn into coating internal layer, it is resistance to along with the influence of the various aspects factor such as exposing to the weather and acid rain
It is in shortening trend with year, after a period of time, the local film of superficies will be dirty or be destroyed by acid rain corrosion, special
It is not that coating surface after acid rain corrosion can occur dusting, fall off, blister and phenomena such as yellowing, influence the integrated beauty of appearance
It sees, and cleaning difficulty is big, costly, especially emphasizes that the high building of landscape consciousness emerges one after another now.
China's acid rain belongs to sulfate type acid rain, is primarily due to a large amount of high coals of combustion of sulfur amount and is formed, coating by
H into acid rain+Dissolved corrosion and SO4 2-Dilation erosion synergistic effect, leads to the painting of exterior walls of buildings and automobile wheel hub surface
Material is destroyed, and solves the problems, such as acid rain corrosion in prior art using high performance solvent based coating, but resistance to
Contamination capability difference is the generally existing disadvantage of traditional outdoor decoration protective coating, constrains its extensive use to a certain extent.
As people are increasingly enhanced environmental protection and own health consciousness, water paint is just organic with its low VOC(volatility
Compound) content and gradually replace solvent based coating, the stain resistance of existing emulsion paint is poor because its paint film be hydrophily,
The pigment of coating is excessively high to lead to paint film structure leakiness, if surface of the paint film speckles with dirt, dirt will be in capillary force
Under effect, entered in paint film using the vapor in air as medium.In order to improve the stain resistant ability of building coating, in the market
It is proposed a kind of fluorocarbon coating with overlength weatherability, resistance to soiling and anti-corrosive properties.Fluorocarbon coating is passed through on the basis of fluororesin
Cross a kind of new coating material of modified processing and formation.Contain a large amount of F-C key in the resin of fluorocarbon coating, shows excess of export
Long weatherability and resistant to chemical media corrosivity, thus its stability be it is best in all cold coatings, still, high valence
Lattice hinder the application of its large area.Also there is a large amount of patent literature report that polyfluorourethane can be used in water paint.
It for example, WO2005/07722 has synthesized a kind of novel polyfluorourethane, can be used in building or industrial paint, there is preferable reprimand
Water denounces oiliness.But it since binder usually accounts for about 1/3 in coating composition, is substituted with polyfluorourethane in original coating
Binder, just the auxiliary agent in formula must be reselected and be studied, this undoubtedly increases technical difficulty.
Therefore, urgent need is a kind of hard wear-resisting, anti-with excellent stain resistance and extra-weather-proof, acid rain resistant, height in the market
It scrapes and the coating of cost economy.
Summary of the invention
In order to solve the above-mentioned technical problem, the technical scheme adopted by the invention is as follows:
A kind of extra-weather-proof acid rain resistant stain resistant aqueous inorganic ceramic coating, which is characterized in that raw material composition and quality percentage
Than:
Aqueous inorganic nano ceramics modified emulsion 45~80%
Pigment 1~20%
Filler 1~30%
Wetting dispersing agent 0.1~0.5%
Defoaming agent 0.1~0.5%
Thickener 1~5%
Water surplus；
Wherein, the component of the aqueous inorganic nano ceramics modified emulsion and weight proportion are respectively as follows:
Silicone acrylic emulsion 10~40%
Silica solution 15~40%
Silane 15~40%
Active crosslinker 1~5%
Water surplus；
Preferably, the silicone acrylic emulsion is that the one or more of commercially available construction material silicone acrylic emulsion mix.
Preferably, the silica solution is made of the mixing of one or both of acidic silicasol, alkaline silica sol.
Preferably, the partial size of the silica solution is 1~160nm, and pH value is 2~10.
Preferably, the silane is mixed by one or more of alkoxy silanes.
Preferably, the alkoxy silane are as follows: methyltrimethoxysilane, methyltriethoxysilane, dimethylformamide dimethyl
Oxysilane, dimethyl diethoxysilane, vinyltrimethoxysilane, vinyltriethoxysilane, γ-metering system
One or more of acryloxypropylethoxysilane trimethoxy silane, 3- glycidyl ether oxypropyltrimethoxysilane.
Preferably, the active crosslinker is polycarbodiimide.
Preferably, the pigment is at least one of commercially available titanium dioxide, pearlescent pigment, fluorescent pigment, metallic pigments；
The filler is at least one of whisker powder, talcum powder, kaolin, mica powder, calcium carbonate, barium sulfate；
Preferably, the wetting dispersing agent is Silok-8008；The defoaming agent is BYK015；The thickener is BYK420.
A kind of extra-weather-proof acid rain resistant stain resistant aqueous inorganic ceramic coating, preparation method are as follows:
Step 1: first uniformly being mixed one or more of silane, active crosslinker is then added and is stirred dissolution, until
Active crosslinker is dissolved completely in silane mixture, forms transparent mixing liquid；
It is weighed in the silicone acrylic emulsion finished that feeds intake in advance step 2: silica solution and water are added to, stirring 5~30 minutes, then
The mixing liquid that slowly first step is prepared is added drop-wise in silicone acrylic emulsion and silica solution mixed liquor, and titration time is 30 minutes,
It after titration, starts to warm up, reaction temperature is maintained between 35~80 DEG C, and isothermal reaction 2~5 hours, metering is then added
Water, stop heating, cooling down, i.e., acquisition aqueous inorganic nano ceramics modified emulsion；
Step 3: the aqueous inorganic nano ceramics modified emulsion that second step prepares is mixed with pigment, filler, high speed dispersion is used
Machine carries out high speed dispersion, and jitter time is 10~30 minutes, is then ground using horizontal sand mill, and adjust cooling water
Material grinding temperature is set to be no more than 60 DEG C, milling time is 1~2 hour, is eventually adding auxiliary agent and water is stirred, stir evenly
Afterwards, that is, extra-weather-proof acid rain resistant stain resistant aqueous inorganic ceramic coating is obtained.
Technological innovation advantage of the invention is:
One, film forming matter uses aqueous inorganic nano ceramics resin, and the weather resistance with overlength, QUV degradation reaches
3000h can bear sunlight high temperature and be exposed to the sun, anti-aging；And it is high hard wear-resisting, pencil hardness may be up to 6H, and RCA paper tape is wear-resisting secondary
Number is 750 times, makes the film of inorganic nano ceramic coating prepared by the present invention that can bear to expose to wind and rain, sunlight is exposed to the sun, again
It is wear-resisting in strong wind and rain drop erosion that dust storm dust granules can be resisted；
Two, since inorganic nano ceramic coating water contact angle prepared by the present invention is up to 90 °, the arrangement of film coated surface molecular structure is non-
Chang Youxu makes its surface in strong hydrophobicity, is greatly lowered so as to cause the water absorption rate of film coated surface, glues to pollution sources
It echos sucking also to weaken significantly, along with gloss may be up to 90 °, therefore film coated surface easily washes with water, therefore has extremely strong
Contaminated resistance；
The three, present invention use polycarbodiimide as active crosslinker, and use system of the mixed silanes as crosslinking agent, silicon
Substance all has extremely strong acid-resistant property, and the silanol of inorganic nano silica and silane hydrolyzate is resistant to strong acid；And gather
Carbodiimides makes silanol have high crosslink density, further improves the ability that silanol acid rain resistant corrodes, therefore the present invention
The inorganic nano ceramic coating of preparation has splendid acid rain resistance energy.
Specific embodiment
Illustrate embodiments of the present invention below by way of specific specific example, those skilled in the art can be by this explanation
Other advantages and efficacy of the present invention can be easily understood for content disclosed by book.The present invention can also be by addition different specific
Embodiment is embodied or practiced, every details of this specification can also based on different viewpoints and application, without departing from
Various modifications or alterations are carried out under spirit of the invention.
Illustrate technical solution of the present invention below by way of specific specific example.It should be understood that these embodiments are only used for
The bright present invention, rather than limit the scope of the invention.
Embodiment 1 ~ 6
In order to express easily, the proportion and properties of product of 6 embodiments, respectively 1 ~ 6 reality are expressed with three tables below
Apply the material component and mass percent table of the extra-weather-proof acid rain resistant stain resistant aqueous inorganic ceramic coating of example；Aqueous inorganic
The component and mass percent table of nano ceramics modified emulsion；Extra-weather-proof acid rain resistant stain resistant aqueous inorganic ceramic coating produces
Product table of performance indicators.
Table 1: material component and the mass percent difference of extra-weather-proof acid rain resistant stain resistant aqueous inorganic ceramic coating
Are as follows:
Table 2: the component and mass percent of aqueous inorganic nano ceramics modified emulsion are respectively as follows:
Table 3: the extra-weather-proof acid rain resistant stain resistant aqueous inorganic ceramic coating product performance index that above-described embodiment 1 ~ 6 obtains
Table:
Embodiment 7: a kind of extra-weather-proof acid rain resistant stain resistant aqueous inorganic ceramic coating, preparation method are as follows:
Step 1: one or more of silane of Examples 1 to 6 in table 2 are uniformly mixed, be then added active crosslinker into
Row stirring and dissolving forms transparent mixing liquid until active crosslinker is dissolved completely in silane mixture；
Step 2: by table 2 silica solution and water be added to weigh in advance and feed intake in the silicone acrylic emulsion finished, stir 5~30 points
Clock, the mixing liquid for then slowly preparing the first step are added drop-wise in silicone acrylic emulsion and silica solution mixed liquor, and titration time is
30 minutes, after titration, start to warm up, reaction temperature is maintained between 35~80 DEG C, isothermal reaction 2~5 hours, then plus
Enter the water of metering, stops heating, cooling down, i.e. acquisition aqueous inorganic nano ceramics modified emulsion；
Step 3: the aqueous inorganic nano ceramics modified emulsion that second step prepares is mixed with pigment, the filler in table 1, use
High speed disperser carries out high speed dispersion, and jitter time is 10~30 minutes, is then ground using horizontal sand mill, and adjust
Section cooling water makes material grinding temperature be no more than 60 DEG C, and milling time is 1~2 hour, is eventually adding auxiliary agent and water is stirred,
After mixing evenly, that is, extra-weather-proof acid rain resistant stain resistant aqueous inorganic ceramic coating is obtained.
During preparing extra-weather-proof acid rain resistant stain resistant aqueous inorganic ceramic coating, not according to each material proportion
Together, respectively formula inorganic nano ceramic resin solid content should control between 30~50%, second step water obtained in embodiment 7
Property the ceramic modified emulsion appearance of inorganic nano be that milky is translucent or opaque low-viscosity (mobile) liquid.
Ceramic coating of the present invention effectively overcomes the number of drawbacks of the prior art.And preparation side of the invention
Method has configuration simple, and the stable feature of performance can be widely applied to exterior walls of buildings and automotive hub etc..Therefore, originally
Extra-weather-proof acid rain resistant stain resistant aqueous inorganic ceramic coating of invention and preparation method thereof has very high industry exploitation value
Value.
Above-described embodiment is only illustrative to illustrate the principle of the present invention and effect, and is not intended to limit the present invention.It is any ripe
Knowing those skilled in the art all can without violating the spirit and scope of the present invention, and changes may be made to the above embodiments or modification.
Therefore, institute is complete without departing from the spirit and technical ideas disclosed in the present invention by all those of ordinary skill in the art
At all equivalent modifications or change, still should be covered by the claims of the present invention.
Claims (10)
1. a kind of extra-weather-proof acid rain resistant stain resistant aqueous inorganic ceramic coating, which is characterized in that raw material composition and quality hundred
Divide ratio:
Aqueous inorganic nano ceramics modified emulsion 45~80%
Pigment 1~20%
Filler 1~30%
Wetting dispersing agent 0.1~0.5%
Defoaming agent 0.1~0.5%
Thickener 1~5%
Water surplus；
Wherein, the component of the aqueous inorganic nano ceramics modified emulsion and weight proportion are respectively as follows:
Silicone acrylic emulsion 10~40%
Silica solution 15~40%
Silane 15~40%
Active crosslinker 1~5%
Water surplus.
2. a kind of extra-weather-proof acid rain resistant stain resistant aqueous inorganic ceramic coating as described in claim 1, which is characterized in that
The silicone acrylic emulsion is that the one or more of commercially available construction material silicone acrylic emulsion mix.
3. a kind of extra-weather-proof acid rain resistant stain resistant aqueous inorganic ceramic coating as described in claim 1, which is characterized in that
The silica solution is made of the mixing of one or both of acidic silicasol, alkaline silica sol.
4. a kind of extra-weather-proof acid rain resistant stain resistant aqueous inorganic ceramic coating as claimed in claim 3, which is characterized in that
The partial size of the silica solution is 1~160nm, and pH value is 2~10.
5. a kind of extra-weather-proof acid rain resistant stain resistant aqueous inorganic ceramic coating as described in claim 1, which is characterized in that
The silane is mixed by one or more of alkoxy silanes.
6. a kind of extra-weather-proof acid rain resistant stain resistant aqueous inorganic ceramic coating as claimed in claim 5, which is characterized in that
The alkoxy silane are as follows: methyltrimethoxysilane, methyltriethoxysilane, dimethyldimethoxysil,ne, dimethyl
Diethoxy silane, vinyltrimethoxysilane, vinyltriethoxysilane, γ-methacryloxypropyl front three
One or more of oxysilane, 3- glycidyl ether oxypropyltrimethoxysilane.
7. a kind of extra-weather-proof acid rain resistant stain resistant aqueous inorganic ceramic coating as described in claim 1, which is characterized in that
The active crosslinker is polycarbodiimide.
8. a kind of extra-weather-proof acid rain resistant stain resistant aqueous inorganic ceramic coating as described in claim 1, which is characterized in that
The pigment is at least one of commercially available titanium dioxide, pearlescent pigment, fluorescent pigment, metallic pigments；The filler is whisker
At least one of powder, talcum powder, kaolin, mica powder, calcium carbonate, barium sulfate.
9. a kind of extra-weather-proof acid rain resistant stain resistant aqueous inorganic ceramic coating as described in claim 1, which is characterized in that
The wetting dispersing agent is Silok-8008；The defoaming agent is BYK015；The thickener is BYK420.
10. a kind of extra-weather-proof acid rain resistant stain resistant aqueous inorganic ceramic coating as described in claim 1, preparation method
Are as follows:
Step 1: first uniformly being mixed one or more of silane, active crosslinker is then added and is stirred dissolution, until
Active crosslinker is dissolved completely in silane mixture, forms transparent mixing liquid；
It is weighed in the silicone acrylic emulsion finished that feeds intake in advance step 2: silica solution and water are added to, stirring 5~30 minutes, then
The mixing liquid that slowly first step is prepared is added drop-wise in silicone acrylic emulsion and silica solution mixed liquor, and titration time is 30 minutes,
After titration, starting to warm up, reaction temperature is maintained at 35~80 DEG C, isothermal reaction 2~5 hours, the water of metering is then added,
Stop heating, cooling down, i.e. acquisition aqueous inorganic nano ceramics modified emulsion；
Step 3: the aqueous inorganic nano ceramics modified emulsion that second step prepares is mixed with pigment, filler, high speed dispersion is used
Machine carries out high speed dispersion, and jitter time is 10~30 minutes, is then ground using horizontal sand mill, and adjust cooling water
Material grinding temperature is set to be no more than 60 DEG C, milling time is 1~2 hour, is eventually adding auxiliary agent and water is stirred, stir evenly
Afterwards, that is, extra-weather-proof acid rain resistant stain resistant aqueous inorganic ceramic coating is obtained.
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Cited By (5)
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| CN111234571A (en) * | 2020-01-16 | 2020-06-05 | 上海宜瓷龙新材料股份有限公司 | Water-based ceramic coating for outer wall of stainless steel vacuum cup and preparation method thereof |
| CN111647329A (en) * | 2020-07-14 | 2020-09-11 | 上海保立佳新材料有限公司 | Single-component waterproof high-hardness water-based floor paint and preparation method thereof |
| CN114395318A (en) * | 2022-02-14 | 2022-04-26 | 青岛普泰纳米新材料科技有限公司 | Water-based nano ceramic coating for PET (polyethylene terephthalate) film and preparation method and coating method thereof |
| CN114634759A (en) * | 2022-04-20 | 2022-06-17 | 张卫星 | Water-based inorganic ceramic coating and spraying method thereof |
| CN115160919A (en) * | 2022-08-09 | 2022-10-11 | 南京长江涂料有限公司 | Outdoor super-weather-resistant aqueous photocuring woodenware coating and preparation method thereof |
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| CN115160919A (en) * | 2022-08-09 | 2022-10-11 | 南京长江涂料有限公司 | Outdoor super-weather-resistant aqueous photocuring woodenware coating and preparation method thereof |
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| CN109294382B (en) | 2020-12-22 |
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