CN102898885A - Cheap modified paint self-cleaning coating with super-hydrophobicity and preparation method and application thereof - Google Patents
Cheap modified paint self-cleaning coating with super-hydrophobicity and preparation method and application thereof Download PDFInfo
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- CN102898885A CN102898885A CN2012104074842A CN201210407484A CN102898885A CN 102898885 A CN102898885 A CN 102898885A CN 2012104074842 A CN2012104074842 A CN 2012104074842A CN 201210407484 A CN201210407484 A CN 201210407484A CN 102898885 A CN102898885 A CN 102898885A
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Abstract
The invention provides a cheap modified paint self-cleaning coating with super-hydrophobicity and a preparation method thereof, wherein the prepared cheap modified paint self-cleaning coating with the super-hydrophobicity has a nanometer rough surface structure with a coralline or coralline-like surface; the coating is 50-1000 nm in thickness; and a contact angle of water drop on the surface of the coating is 130-150 degrees. The method provided by the invention has the characteristics of simple technology, good repeatability, low cost and unnecessity of high-cost hydrophobic agent for reducing surface free energy. The modified coating, prepared according to the preparation method provided by the invention, can be used for forming films on various base surfaces consisting of construction outer surface, engineering material surface, mining machinery surface and the like, so that the hydrophobicity can be improved, therefore the outdoor service life is prolonged.
Description
Technical field
The present invention relates to the paint field, be specifically related to a kind of cheap modification paint automatic cleaning coating with super-hydrophobicity and its preparation method and application.
Adopt the method for adding inorganic particle to increase the roughness of paint coating, thereby increase the hydrophobic performance of paint coating, can increase waterproof and the self-cleaning performance of coating, and therefore prolong the life-span of coating.
Background technology
Because water droplet has not wetting property to super hydrophobic surface, water droplet can keep spherical on its surface and be very easy to tumble, and in tumbling process the pollutents such as dust is cleared up away.Because the automatically cleaning characteristic so that it has potential using value in fields such as corrosion-resistant coating, drag reduction surfaces, therefore has been subject to the extensive concern from industry member and scientific research circle scientific research personnel.Find by research, realize that surface super hydrophobic sexual needs satisfy two conditions: 1. this surface has higher surfaceness; 2. this surface has lower surface free energy.According to these two conditions, the scientific research personnel prepares multiple coating with good super-hydrophobicity.As: it is template that the people such as Zhang adopt anodised aluminium, waters the nanometer stick array that casts out tetrafluoroethylene and Sodium styrene sulfonate compositions of mixtures, and water droplet reaches as high as 171 ° at its surperficial contact angle, and roll angle is less than 5 °.The people such as Jin adopt silica dioxide granule to regulate the pattern of silicon rubber insulator, prepare the silicone rubber coating with micron and nanometer composite structure, so that the surface of insulator has had super-hydrophobic characteristic, contact angle can reach 152.5 °.The people such as Kwok adopt modified version plasma etching method that etching has been carried out on the surface of polytetrafluoroethylmaterial material, for increasing its surperficial roughness, so that after when smooth 107 ° of its surperficial contact angle are increased to coarse processing 153 ° of water droplet.Adopt the prepared surface out of these preparation methods all to have good super-hydrophobicity, but preparation process relative complex, cost high, be not suitable for large scale application, especially adopt various templates to prepare the method cost of super-hydrophobic coat very high.
Summary of the invention
In order to solve the problem that runs in the super-hydrophobic coat large-scale promotion application process,, high in cost of production shortcoming complicated such as preparation process.To realize the large-scale application of super-hydrophobic automatic cleaning coating: such as mining machinery, rainproof door and window, outdoor equipment, carrier vehicle etc.
The object of the present invention is to provide a kind of cheap modification paint automatic cleaning coating with super-hydrophobicity.
Another object of the present invention is to provide a kind of preparation method with cheap modification paint automatic cleaning coating of super-hydrophobicity.
An also purpose of the present invention is to provide the above-mentioned application of cheap modification paint automatic cleaning coating in spraying mining machinery, rainproof door and window, outdoor equipment or carrier vehicle top layer with super-hydrophobicity.
In order to realize purpose of the present invention, the invention provides a kind of cheap modification paint automatic cleaning coating with super-hydrophobicity, it has the nanometer rough surface structure on coralliform or class coralliform surface; The thickness of this coating is 50nm ~ 1000nm; Water droplet is 130 ° ~ 150 ° at its surperficial contact angle.
The present invention also provides a kind of preparation method with cheap modification paint automatic cleaning coating of super-hydrophobicity, and it comprises the steps:
(1) making ZnO micron and nanometer composite structure particle: in proportion with zinc nitrate hexahydrate solution (Zn(NO
3)
26H
2O) and vulkacit H solution (C
6H
12N
4, HMT) carry out ultrasonic agitation; Then take out after mixed solution being placed 50 ~ 95 ℃ water bath to react 0.5 ~ 4h; After the room temperature cooling, outwell supernatant liquid, take out the white ZnO particle that the bottom generates, again through the ethanol ultra-sonic dispersion, centrifugal, after ultrasonic procedure is cleaned, place loft drier dry, obtain the white solid powder and be ZnO micron and nanometer composite structure particle (described ZnO micron and nanometer composite structure particle is the ZnO particle of taraxacum shape, its block dimension about 5 microns, in the nanometer branch structure is arranged);
(2) in proportion step (1) gained ZnO micron and nanometer composite structure particle and paint are scattered in the middle of the organic solvent, under heating ultrasonic agitation condition, the mixing solutions reaction forms the precursor liquid of modification paint automatic cleaning coating;
(3) precursor liquid of the described modification of step (2) paint automatic cleaning coating is applied to the surface of workpiece, film-forming namely forms a kind of cheap modification paint automatic cleaning coating with super-hydrophobicity under field conditions (factors).
Preferably, zinc nitrate hexahydrate solution has identical concentration with hexamethylene tetramine solution described in the step (1), and concentration range is 0.1 ~ 1mol/L, and the volume ratio of the two is 0.5 ~ 2:1.
Preferably, the described ultrasonic power of step (1) is 40 ~ 100W, and ultrasonic time is 10 ~ 60min; The temperature of described stirring is room temperature, and the speed of stirring is 1000 ~ 2000rpm, and the time is 5 ~ 10min; Described centrifugal speed is 1000 ~ 8000rpm, and the centrifugal time is 5 ~ 10min.
Preferably, the mass ratio of micron and nanometer composite structure particle, organic solvent and paint is preferably 0.15 ~ 4.0:0.2 ~ 2.0:1 ~ 16 described in the step (2).Described organic solvent is preferably silane coupling agent, rosin, acetone, various alcohol, aldehyde, ether, benzene, alkane etc.; Wherein the silane coupling agent model has KH-550, KH-560, KH-570, KH-792.
Wherein, the ultrasonic power of the ultrasonic agitation of heating described in the step (2) is 40 ~ 100W, ultrasonic time 10 ~ 60min; The speed that stirs is 1000 ~ 2000rpm, and the stirring heating temperature is 20 ~ 80 ℃, and the time of stirring is 30min ~ 4h.
Wherein, be applied to described in the step (3) workpiece surface modification paint automatic cleaning coating precursor liquid can with lift, spin coating, curtain coating is coated with or spraying method.
Further, the present invention also provides the above-mentioned application of cheap modification paint automatic cleaning coating in spraying mining machinery, rainproof door and window, outdoor equipment or carrier vehicle top layer with super-hydrophobicity.
Beneficial effect of the present invention:
The present invention adopts ZnO micro-nano composite structure particle as the properties-correcting agent additive, join paint in the middle of mix fully with paint.In conjunction with the anchor of the film forming of ZnO particle own and the hydrophobicity of paint itself, so that the modified oil lacquering has possessed higher surfaceness and lower surface free energy simultaneously, thereby so that the more smooth painted surface of hydrophobicity on modified oil lacquering surface is greatly increased, water droplet can be become by about 90 ° of general paint at its surperficial contact angle and reaches about 150 °, has super-hydrophobic state.
The method technique that the present invention adopts is simple, good reproducibility, cost are low, need not to use the expensive hydrophobic agents (such as fluoride reagents) that reduces surface free energy.
The present invention gets final product making ZnO micro-nano composite particles with simple chemical liquid deposition, this particle can be realized modification to all paint, is used for different occasions: as being mixed for the glass vehicle window, being mixed for mechanical metal shell etc. with rust-inhibiting paint with the clear lacquer.
The modified coating that the present invention prepares can be in various substrate surface film forming, comprise that external surface of buildings, engineering materials surface, mining machinery are surperficial etc., can improve its hydrophobicity, increase its outdoor work-ing life.
Description of drawings
Fig. 1 is the surface topography that adopts the modified oil lacquering that the inventive method prepares;
Fig. 2 is the state that adopts the modified oil lacquering surface water contact that the inventive method prepares.
Embodiment
Below in conjunction with embodiment the present invention is described in further detail.
Adopt JSM6700LV surface sweeping electron microscope that the surface topography of modified coating is observed.
Adopt contact angle measurement (Soren, Shanghai Information technology company limited) that water droplet is measured at the contact condition on modified oil lacquering surface.
The paint that adopts among the present invention can have hydrophobic paint for various, such as iron red alcohol acid rust-inhibiting paint GB/T2525, and black prepared alkyd paint HG/T2455-93, alkyd varnish GB/T23995, epoxy resin-based paint etc.The paint that uses is domestic water chestnut lake board paint.
The power adjustable desktop heating of ultrasonic use Shanghai High Kudos Science Instrument Co., Ltd., the ultrasonic cleaner of model SK2210HP, stirring what uses is the Community of Jin Tan County city Jin Cheng state victory laboratory apparatus 78HW-1 of factory constant temperature blender with magnetic force.What spin-coating method used is the desk-top sol evenning machine of KW-4A type that Chinese Academy of Sciences Microelectronics Institute produces.
Embodiment 1
(1) making ZnO micron and nanometer composite structure particle: getting concentration is 0.5mol/L zinc nitrate hexahydrate solution (Zn(NO
3)
26H
2O) and 0.5mol/L vulkacit H solution (C
6H
12N
4, HMT) each 200ml carries out ultrasonicly, and ultrasonic power is 80W, and ultrasonic time 30min mixes, and stirs for some time; Then take out after mixed solution being placed 90 ℃ water bath reaction 2h; Outwell supernatant liquid after the cooling of cooling room temperature, take out the white ZnO particle that the bottom generates, again through the ethanol ultra-sonic dispersion, ultrasonic power is 80W, ultrasonic time 10min; The centrifugal 5min of 8000rpm, outwell supernatant liquid, after ultrasonic procedure is cleaned, place loft drier dry, obtaining the white solid powder is ZnO micron and nanometer composite structure particle (described ZnO micron and nanometer composite structure particle is the ZnO particle of taraxacum shape, its block dimension about 5 microns, in the nanometer branch structure is arranged);
(2) preparation of modification paint liquid:
Be scattered in respectively central (if a large amount of configuration of 100ml KH-550 silane coupling agent with the taraxacum shape ZnO micron and nanometer composite structure particle 5g of step (1) preparation with through water chestnut lake board iron oxide red anticorrosive paint (model GB/T2525) 10ml that once filters, constant according to the above ratio), then with the ultrasonic mixing of 80W 30min under two kinds of solution room temperatures, 50 ℃/1500rpm magnetic agitation 1h, the precursor liquid that forms the modified oil lacquering is for subsequent use;
(3) modified oil is painted film:
Precursor liquid is applied to matrix with method of pulling up surface is painted in modification, and pull rate is under field conditions (factors) film-forming of 10cm/min., forms a kind of modified oil lacquering with super-hydrophobicity.
As shown in Figure 1, paint can form on the surface of ZnO particle good coating, and simultaneously modification painted surface has higher surfaceness.
As shown in Figure 2, drop reaches 147 ° at the contact angle of common antirust modification painted surface, has super-hydrophobic state.
The paint that adopts among the present invention can have hydrophobic paint for various.
Embodiment 2
(1) making ZnO micron and nanometer composite structure particle:
Getting 100ml concentration is 0.1mol/L zinc nitrate hexahydrate solution (Zn(NO
3)
26H
2O) and 200ml concentration be 0.1mol/L vulkacit H solution (C
6H
12N
4, HMT) mixing ultrasonic (if a large amount of configuration is constant according to the above ratio), ultrasonic power is 40W, ultrasonic time 50min mixes, and stirs for some time; Then take out after mixed solution being placed 95 ℃ water bath reaction 1h; Outwell supernatant liquid after the cooling of cooling room temperature, take out the white ZnO particle that the bottom generates, again through the ethanol ultra-sonic dispersion, ultrasonic power is 50W, ultrasonic time 20min; The centrifugal 5min of 5000rpm outwells supernatant liquid, after ultrasonic procedure is cleaned, places loft drier dry, obtains the white solid powder and is ZnO micron and nanometer composite structure particle;
(2) preparation of modification paint liquid:
Be scattered in respectively (if a large amount of configuration in the middle of the 100ml KH-550 silane coupling agent with the taraxacum shape ZnO micro-nano composite structure particle 2g of embodiment 1 preparation with through the iron oxide red anticorrosive paint 5ml that once filters, constant according to the above ratio), then with the ultrasonic mixing of 40W 30min under two kinds of solution room temperatures, 50 ℃/2000rpm magnetic agitation 30min, the precursor liquid that forms the modified oil lacquering is for subsequent use;
(3) modified oil is painted film:
The surface that precursor liquid is sprayed at matrix is painted in modification, and film-forming forms a kind of modified oil lacquering with super-hydrophobicity under field conditions (factors).
The surface contact angle that records with contact angle measurement is 130 °-150 °
Embodiment 3
(1) making ZnO micron and nanometer composite structure particle:
Getting concentration is 0.1mol/L zinc nitrate hexahydrate solution (Zn(NO
3)
26H
2O) and 0.1mol/L vulkacit H solution (C
6H
12N
4, HMT) each 300ml carries out ultrasonic (if a large amount of configuration is constant according to the above ratio), and ultrasonic power is 40W, and ultrasonic time 60min mixes, and stirs for some time; Then take out after mixed solution being placed 50 ℃ water bath reaction 3h; Outwell supernatant liquid after the cooling of cooling room temperature, take out the white ZnO particle that the bottom generates, again through the ethanol ultra-sonic dispersion, ultrasonic power is 50W, ultrasonic time 60min; The centrifugal 5min of 6000rpm, outwell supernatant liquid, after ultrasonic procedure is cleaned, place loft drier dry, obtaining the white solid powder is ZnO micron and nanometer composite structure particle (described ZnO micron and nanometer composite structure particle is the ZnO particle of taraxacum shape, its block dimension about 5 microns, in the nanometer branch structure is arranged);
(2) preparation of modification paint liquid:
The taraxacum shape ZnO micro-nano composite structure particle 5g of embodiment 1 preparation and alkyd varnish 5ml are scattered in respectively (if a large amount of configuration in the middle of the 100ml KH-550 silane coupling agent, constant according to the above ratio), then with the ultrasonic mixing of 100W 60min under two kinds of solution room temperatures, 50 ℃/1500rpm magnetic agitation 30min, the precursor liquid that forms the modified oil lacquering is for subsequent use;
(3) modified oil is painted film:
Precursor liquid is painted in modification be coated with the surface that method is applied to matrix with curtain coating, film-forming forms a kind of modified oil lacquering with super-hydrophobicity under field conditions (factors).
The surface contact angle that records with contact angle measurement is 130 °-150 °
Embodiment 4
(1) making ZnO micron and nanometer composite structure particle:
Getting concentration is 0.2mol/L zinc nitrate hexahydrate solution (Zn(NO
3)
26H
2O) 200ml and 0.2mol/L vulkacit H solution (C
6H
12N
4, HMT) 100ml carries out ultrasonic (if a large amount of configuration is constant according to the above ratio), and ultrasonic power is 80W, and ultrasonic time 30min mixes, and stirs for some time; Then take out after mixed solution being placed 60 ℃ water bath reaction 0.5h; Outwell supernatant liquid after the cooling of cooling room temperature, take out the white ZnO particle that the bottom generates, again through the ethanol ultra-sonic dispersion, ultrasonic power is 60W, ultrasonic time 40min; The centrifugal 5min of 2000rpm, outwell supernatant liquid, after ultrasonic procedure is cleaned, place loft drier dry, obtaining the white solid powder is ZnO micron and nanometer composite structure particle (described ZnO micron and nanometer composite structure particle is the ZnO particle of taraxacum shape, its block dimension about 5 microns, in the nanometer branch structure is arranged);
(2) preparation of modification paint liquid:
Be scattered in respectively (if a large amount of configuration in the middle of the 100ml acetone soln with the taraxacum shape ZnO micro-nano composite structure particle 15g of embodiment 1 preparation with through the iron oxide red anticorrosive paint 20ml that once filters, constant according to the above ratio), then with the ultrasonic mixing of 60W 60min under two kinds of solution room temperatures, the room temperature lower magnetic force stirs (stir speed (S.S.) is 1200rpm) 2h, and the precursor liquid that forms the modified oil lacquering is for subsequent use;
(3) modified oil is painted film:
With sol evenning machine precursor liquid is spun on matrix with the rotating speed of 2000rpm surface is painted in modification, film-forming forms a kind of modified oil lacquering with super-hydrophobicity under field conditions (factors).
The surface contact angle that records with contact angle measurement is 130 °-150 °
Embodiment 5
(1) making ZnO micron and nanometer composite structure particle:
Getting concentration is 0.1mol/L zinc nitrate hexahydrate solution (Zn(NO
3)
26H
2O) 200ml and 0.1mol/L hexamethylene tetramine solution (C
6H
12N
4, HMT) 400ml carries out ultrasonicly, and ultrasonic power is 80W, and ultrasonic time 50min mixes, and stirs for some time; Then take out after mixed solution being placed 80 ℃ water bath reaction 4h; Outwell supernatant liquid after the cooling of cooling room temperature, take out the white ZnO particle that the bottom generates, again through the ethanol ultra-sonic dispersion, ultrasonic power is 75W, ultrasonic time 50min; The centrifugal 5min of 4000rpm outwells supernatant liquid, after ultrasonic procedure is cleaned, places loft drier dry, obtains the white solid powder and is ZnO micron and nanometer composite structure particle;
(2) preparation of modification paint liquid:
The taraxacum shape ZnO micro-nano composite structure particle of embodiment 1 preparation is respectively 2g, 5g, each 50ml of 10g and alkyd varnish is scattered in respectively central (if a large amount of configuration of 200ml rosin, constant according to the above ratio), then with ultrasonic mixing 10min under two kinds of solution room temperatures, the room temperature lower magnetic force stirs (stir speed (S.S.) is 1600rpm) 4h, and the precursor liquid that forms the modified oil lacquering is for subsequent use;
(3) modified oil is painted film:
With sol evenning machine precursor liquid is spun on matrix with the rotating speed of 2000rpm surface is painted in modification, film-forming forms a kind of modified oil lacquering with super-hydrophobicity under field conditions (factors).
The surface contact angle that records with contact angle measurement is 130 °-150 °
Although illustrated and described embodiments of the invention, for the ordinary skill in the art, be appreciated that without departing from the principles and spirit of the present invention and can carry out multiple variation, modification, replacement and modification to these embodiment, scope of the present invention is limited by claims and equivalent thereof.
Claims (9)
1. the cheap modification paint automatic cleaning coating with super-hydrophobicity is characterized in that, it has the nanometer rough surface structure on coralliform or class coralliform surface; The thickness of this coating is 50nm ~ 1000nm; Water droplet is 130 ° ~ 150 ° at its surperficial contact angle.
2. prepare the method with cheap modification paint automatic cleaning coating of super-hydrophobicity claimed in claim 1, it comprises the steps:
(1) making ZnO micron and nanometer composite structure particle: in proportion zinc nitrate hexahydrate solution and hexamethylene tetramine solution are carried out ultrasonic agitation; Then take out after mixed solution being placed 50 ~ 95 ℃ water bath to react 0.5 ~ 4h; After the room temperature cooling, outwell supernatant liquid, take out the white ZnO particle that the bottom generates, through the ethanol ultra-sonic dispersion, centrifugal again, after ultrasonic procedure is cleaned, place loft drier dry, obtain the white solid powder and be ZnO micron and nanometer composite structure particle;
(2) in proportion step (1) gained ZnO micron and nanometer composite structure particle and paint are scattered in the middle of the organic solvent, under heating ultrasonic agitation condition, the mixing solutions reaction forms the precursor liquid of modification paint automatic cleaning coating;
(3) precursor liquid of the described modification of step (2) paint automatic cleaning coating is applied to the surface of workpiece, film-forming namely forms a kind of cheap modification paint automatic cleaning coating with super-hydrophobicity under field conditions (factors).
3. method according to claim 2 is characterized in that, the concentration of zinc nitrate hexahydrate solution and vulkacit H solution is 0.1 ~ 1mol/L described in the step (1), and the volume ratio of the two is 0.5 ~ 2:1.
4. method according to claim 2 is characterized in that, the described ultrasonic power of step (1) is 40 ~ 100W, and ultrasonic time is 10 ~ 60min; Described stir speed (S.S.) is 1000 ~ 2000rpm; Described centrifugal speed is 1000 ~ 8000rpm.
5. method according to claim 2 is characterized in that, the mass ratio of micron and nanometer composite structure particle, organic solvent and paint is 0.15 ~ 4.0:0.2 ~ 2.0:1 ~ 16 described in the step (2).
6. method according to claim 5 is characterized in that, organic solvent is preferably silane coupling agent described in the step (2), rosin, acetone or various alcohol, aldehyde, ether, benzene, alkane.
7. method according to claim 2 is characterized in that, the ultrasonic power of the ultrasonic agitation of heating described in the step (2) is 40 ~ 100W, ultrasonic time 10 ~ 60min; The speed that stirs is 1000 ~ 2000rpm, and the stirring heating temperature is 20 ~ 80 ℃, and the time of stirring is 30min ~ 4h.
8. method according to claim 2 is characterized in that, be applied to described in the step (3) workpiece surface modification paint automatic cleaning coating precursor liquid can with lift, spin coating, curtain coating is coated with or spraying method.
9. the described application of cheap modification paint automatic cleaning coating in spraying mining machinery, rainproof door and window, outdoor equipment or carrier vehicle top layer with super-hydrophobicity of claim 1.
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| CN104017403A (en) * | 2014-05-28 | 2014-09-03 | 江苏巨珩新材料科技有限公司 | Solvent-free UV paint applied to aluminium plate surfaces and preparation method thereof |
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| CN105694732A (en) * | 2016-03-21 | 2016-06-22 | 苏州市湘园特种精细化工有限公司 | Water-proof antibacterial paint |
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| CN106590291A (en) * | 2016-12-13 | 2017-04-26 | 天长市银狐漆业有限公司 | Corrosion-resistant expandable graphite water-based ultrathin steel structure fireproof coating and preparation method thereof |
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| CN104017403A (en) * | 2014-05-28 | 2014-09-03 | 江苏巨珩新材料科技有限公司 | Solvent-free UV paint applied to aluminium plate surfaces and preparation method thereof |
| CN105694732A (en) * | 2016-03-21 | 2016-06-22 | 苏州市湘园特种精细化工有限公司 | Water-proof antibacterial paint |
| CN105670500B (en) * | 2016-04-15 | 2017-12-08 | 南京林业大学 | A kind of preparation method of zinc oxide/Cellulose nanocrystal bluk recombination super-hydrophobic coat |
| CN105670500A (en) * | 2016-04-15 | 2016-06-15 | 南京林业大学 | Preparation method of zinc oxide and cellulose nanocrystal composite super-hydrophobic coating |
| CN106046980B (en) * | 2016-06-28 | 2018-02-13 | 山东科技大学 | A kind of surface of stainless steel processing and anti-fouling method |
| CN106046980A (en) * | 2016-06-28 | 2016-10-26 | 山东科技大学 | Surface treatment and anti-fouling method for stainless steel material |
| CN106590299A (en) * | 2016-12-13 | 2017-04-26 | 天长市银狐漆业有限公司 | Heat-resistant expandable graphite water-based ultrathin steel structure fireproof coating and preparation method thereof |
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| CN106590291A (en) * | 2016-12-13 | 2017-04-26 | 天长市银狐漆业有限公司 | Corrosion-resistant expandable graphite water-based ultrathin steel structure fireproof coating and preparation method thereof |
| CN113174780A (en) * | 2021-04-26 | 2021-07-27 | 杭州西红柿环保科技有限公司 | Full-degradable dry-pressed aviation lunch box and preparation method thereof |
| CN113522931A (en) * | 2021-07-09 | 2021-10-22 | 浙江工业大学 | Mineral oxidation acid production inhibition method based on in-situ rapid film formation on surface of sulfurized mineral |
| CN113522931B (en) * | 2021-07-09 | 2023-03-24 | 浙江工业大学 | Mineral oxidation acid production inhibition method based on in-situ rapid film formation on surface of sulfurized mineral |
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