CN106189816A - A kind of environmental protection steel alloy anticorrosive paint and preparation method thereof - Google Patents
A kind of environmental protection steel alloy anticorrosive paint and preparation method thereof Download PDFInfo
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- CN106189816A CN106189816A CN201610545391.4A CN201610545391A CN106189816A CN 106189816 A CN106189816 A CN 106189816A CN 201610545391 A CN201610545391 A CN 201610545391A CN 106189816 A CN106189816 A CN 106189816A
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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
- C09D179/00—Coating compositions based on macromolecular compounds obtained by reactions forming in the main chain of the macromolecule a linkage containing nitrogen, with or without oxygen, or carbon only, not provided for in groups C09D161/00 - C09D177/00
- C09D179/02—Polyamines
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
- C08G73/00—Macromolecular compounds obtained by reactions forming a linkage containing nitrogen with or without oxygen or carbon in the main chain of the macromolecule, not provided for in groups C08G12/00 - C08G71/00
- C08G73/02—Polyamines
- C08G73/026—Wholly aromatic polyamines
- C08G73/0266—Polyanilines or derivatives thereof
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
- C08G73/00—Macromolecular compounds obtained by reactions forming a linkage containing nitrogen with or without oxygen or carbon in the main chain of the macromolecule, not provided for in groups C08G12/00 - C08G71/00
- C08G73/06—Polycondensates having nitrogen-containing heterocyclic rings in the main chain of the macromolecule
- C08G73/0605—Polycondensates containing five-membered rings, not condensed with other rings, with nitrogen atoms as the only ring hetero atoms
- C08G73/0611—Polycondensates containing five-membered rings, not condensed with other rings, with nitrogen atoms as the only ring hetero atoms with only one nitrogen atom in the ring, e.g. polypyrroles
-
- 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
-
- 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
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L2205/00—Polymer mixtures characterised by other features
- C08L2205/03—Polymer mixtures characterised by other features containing three or more polymers in a blend
- C08L2205/035—Polymer mixtures characterised by other features containing three or more polymers in a blend containing four or more polymers in a blend
Abstract
The invention discloses a kind of environmental protection steel alloy anticorrosive paint, it is made up of the raw material of following weight parts；Tetrahydrofurfuryl alcohol 0.1 0.2, aniline 50 60, pyrroles 30 40, sulfosalicylic acid 79, epoxy resin E513 4, Ammonium persulfate. 1.3 2, molybdic acid 46, polyamide 35, n-butyl alcohol 160 170, butyl glycol ether 20 30, polyacrylamide 0.8 2, casein 34, ammonium metaborate 0.7 1,2-Propenoic acid, 2-methyl-, isooctyl ester 0.2 0.3, polyamide wax micropowder 12, hydrolytic polymaleic anhydride 0.4 1, ureidopropyltriethoxysilane 0.1 0.2.The coating nontoxic pollution-free of the present invention, the feature of environmental protection is good, and safety is high.
Description
Technical field
The present invention relates to anticorrosive paint technical field, particularly relate to a kind of environmental protection steel alloy anticorrosive paint and preparation side thereof
Method.
Background technology
Polyaniline increasingly causes the attention of people as a kind of novel conducting polymer composite in recent years.It synthesizes work
Skill is simple, environmentally safe, low cost have the features such as stable thermodynamic property and chemical property and make it lead at each
Territory is all widely used.Particularly its excellent antiseptic property makes it the most extensive in the application of corrosion-resistant field.But its paint film
Fragile adhesive force and slightly solubility are applied to create the biggest restriction.If by chemical corrosion resistance excellent for polyaniline and ring
The adhesive force of epoxy resins excellence and mechanical property combine prepares blended coating, and this will be greatly improved epoxy coating
Antiseptic power, also overcomes the weakness of polyaniline paint simultaneously, thus is greatly improved its range of application and antiseptic property；
Polyaniline film can carry out protection in acid medium to ferrous materials makes its surface soul and the erosion medium resistance that is not corroded,
This discovery starts so that polyaniline is shown up prominently at corrosion-resistant field.Showed through the substantial amounts of experimental data of research worker later, poly-
Aniline has scratch resistance and the effect of anti-spot corrosion of uniqueness, and after it mixes with epoxy resin, Xu is overlying on the anticorrosion of metal surface
Having exceeded during performance-based only coated with resins and got well all times of even an order of magnitude, it is harsh that it also can be suitably used for ocean and Aero-Space etc.
Condition makes this material increasingly be taken seriously.Additionally also there is polyaniline in fields such as microelectronics packaging and electronic package
Figure；
Polyaniline bad dispersibility in polyaniline/cold coating and poor adhesive force etc. the most all greatly reduce the anti-of polyaniline
Rotten performance, the physics impermeabilisation ability of polyaniline does not reaches the most far away the use condition requirement of harshness simultaneously.So how improve
The insoluble energy of polyaniline, dispersive property and impermeabilisation ability are to improve the key of anticorrosive polyaniline ability, are also to promote it
Practical, the key of extensiveization；.
Summary of the invention
The object of the invention is contemplated to make up the defect of prior art, it is provided that a kind of environmental protection steel alloy anticorrosive paint and system thereof
Preparation Method.
The present invention is achieved by the following technical solutions:
A kind of environmental protection steel alloy anticorrosive paint, it is made up of the raw material of following weight parts；
Tetrahydrofurfuryl alcohol 0.1-0.2, aniline 50-60, pyrroles 30-40, sulfosalicylic acid 7-9, epoxy resin E513-4, Ammonium persulfate.
1.3-2, molybdic acid 4-6, polyamide 3-5, n-butyl alcohol 160-170, butyl glycol ether 20-30, polyacrylamide 0.8-2, dry
Casein 3-4, ammonium metaborate 0.7-1,2-Propenoic acid, 2-methyl-, isooctyl ester 0.2-0.3, polyamide wax micropowder 1-2, hydrolytic polymaleic anhydride
0.4-1, ureidopropyltriethoxysilane 0.1-0.2.
The preparation method of a kind of described environmental protection steel alloy anticorrosive paint, comprises the following steps:
(1) Ammonium persulfate. is joined in its weight 21-25 times deionized water, stir, obtain initiator solution；
(2) above-mentioned polyacrylamide is joined in the deionized water of its weight 10-15 times, add hydrolytic polymaleic anhydride, stir
Mixing uniformly, secure satisfactory grades sub-aqueous solution；
(3) by above-mentioned tetrahydrofurfuryl alcohol, polyamide wax micropowder mixing, insulated and stirred 10-14 minute at 80-90 DEG C, mixing is added
The dehydrated alcohol of material weight 7-10 times, stirring, to room temperature, adds above-mentioned ureidopropyltriethoxysilane, ultrasonic 2-3 minute, obtains
Silanol liquid；
(4) by above-mentioned sulfosalicylic acid, casein mixing, joining in the deionized water of compound weight 47-50 times, magnetic force stirs
Mix 20-30 minute, add aniline, stir, drip the 47-50% of above-mentioned initiator solution weight, regulation temperature after dropping
Degree, for 20-25 DEG C, adds the 30-40% of above-mentioned water-soluble polymers weight, stirring reaction 10-12 hour, filters, precipitation used
Acetone, distilled water wash 3-4 time successively, be dried 10-12 hour, obtain acid doped polyaniline at 60-65 DEG C；
(5) molybdic acid is joined in the deionized water of its weight 60-65 times, stir, add above-mentioned pyrroles, magnetic agitation
50-60 minute, drip remaining initiator solution, regulate temperature after dropping and be 0-5 DEG C, add remaining macromolecule water-soluble
Liquid, stirring reaction 6-7 hour, filter, the ethanol of precipitation 30-35% is washed 2-3 time, be dried 6-8 hour at 70-85 DEG C,
Acid doping polypyrrole；
(6) by above-mentioned n-butyl alcohol, butyl glycol ether mixing, stir, obtain mixed solvent；
(7) take the 50-60% of above-mentioned mixed solvent weight, add above-mentioned acid doped polyaniline, ultrasonic 10-15 minute, add above-mentioned
Epoxy resin, stirring reaction 40-50 minute, obtain epoxy emulsion；
(8) above-mentioned acid doping polypyrrole is joined in remaining mixed solvent, stir, add polyamide, ultrasonic
30-40 minute, obtain polyamide emulsion；
(9) by above-mentioned epoxy emulsion, polyamide emulsion, the mixing of silanol liquid, insulated and stirred in the water bath with thermostatic control of 60-70 DEG C
40-50 minute, add the dimethicone of compound weight 1-2%, stir, add and remain each raw material, be passed through 80-90 DEG C
Steam, heat aging 30-40 minute, cooling, obtain described coating.
A kind of environmental protection steel alloy anticorrosive paint and preparation method thereof, the using method of described coating is:
Be applied to paint brush of the present invention to clean up, dried alloy steel material working electrode surface, control coating thickness one
Cause, as in baking oven, be dried 20-25 hour at 60-70 DEG C,.
The invention have the advantage that the doped polypyrrole of the present invention is conduction, during as anti-corrosion material protection metal, always
Be first with surface metal generation partial reaction, make surface metal corrode purification, corrosion potential presents and generally reduces, molybdic acid official's energy
Group, as a kind of anti-corrosion function functional group, may depart from also faster when touching metal material from polypyrrole strand
React with metal, make metal surface protected and be passivated, and use being total to of the sulfosalisylic acid doping of bigger organic group
Polymers is embedded in copolymer molecule interchain because of large scale counter ion, it is possible to increases the extension degree of polymer chain and expands interchain
Away from, organic macromolecule sulfonic acid group has strong surface-active action, makes the dissolubility of subject polymer be improved, simultaneously
Have both good electrical conductivity, can be formed different electric field, the direction of the electric field of formation and corrosion when it acts on metal surface
When reaction occurs, electronics flowing is in opposite direction, and therefore this electric field is equal to being applied with a counteracting force to corrosion reaction, hinders
Electronics, to the movement of metal surface, makes corrosion reaction by a definite limitation, the polyphenyl that this sulfosalisylic acid doping is formed simultaneously
Amine is blended with polypyrrole so that the grain diameter of copolymer diminishes, and granule is uniform, careful, piles up more tight, agglomeration
Basic disappear, the coating of the present invention can effectively improve the ability of passive metal so that steel alloy Surface Creation one floor height
The oxide-film of consistency, preferably isolating metal base material and corrosive medium, enhance the ability of its suppression anode reaction, show
Preferably corrosion resistance；The coating nontoxic pollution-free of the present invention, the feature of environmental protection is good, and safety is high.
Detailed description of the invention
A kind of environmental protection steel alloy anticorrosive paint, it is made up of the raw material of following weight parts；
Tetrahydrofurfuryl alcohol 0.1, aniline 50, pyrroles 30, sulfosalicylic acid 7, epoxy resin E513, Ammonium persulfate. 1.3, molybdic acid 4, polyamides
Polyimide resin 3, n-butyl alcohol 160, butyl glycol ether 20, polyacrylamide 0.8, casein 3, ammonium metaborate 0.7, methacrylic acid are different
Monooctyl ester 0.2, polyamide wax micropowder 1, hydrolytic polymaleic anhydride 0.4, ureidopropyltriethoxysilane 0.1.
The preparation method of a kind of described environmental protection steel alloy anticorrosive paint, comprises the following steps:
(1) Ammonium persulfate. is joined in 21 times of deionized waters of its weight, stir, obtain initiator solution；
(2) being joined by above-mentioned polyacrylamide in the deionized water of its weight 10 times, add hydrolytic polymaleic anhydride, stirring is all
Even, secure satisfactory grades sub-aqueous solution；
(3) by above-mentioned tetrahydrofurfuryl alcohol, polyamide wax micropowder mixing, insulated and stirred 10 minutes at 80 DEG C, compound weight 7 is added
Dehydrated alcohol again, stirring, to room temperature, adds above-mentioned ureidopropyltriethoxysilane, ultrasonic 2 minutes, obtains silanol liquid；
(4) by above-mentioned sulfosalicylic acid, casein mixing, join in the deionized water of compound weight 47 times, magnetic agitation
20 minutes, adding aniline, stir, drip the 47% of above-mentioned initiator solution weight, regulating temperature after dropping is 20
DEG C, adding the 30% of above-mentioned water-soluble polymers weight, stirring is reacted 10 hours, filters, by precipitation acetone, distilled water successively
Wash 3 times, be dried 10 hours at 60 DEG C, obtain acid doped polyaniline；
(5) molybdic acid is joined in the deionized water of its weight 60 times, stir, add above-mentioned pyrroles, magnetic agitation 50 points
Clock, drips remaining initiator solution, and regulating temperature after dropping is 0 DEG C, adds remaining water-soluble polymers, and stirring is anti-
Answer 6 hours, filter, precipitation is washed 2 times with the ethanol of 30%, be dried 6 hours at 70 DEG C, obtain acid doping polypyrrole；
(6) by above-mentioned n-butyl alcohol, butyl glycol ether mixing, stir, obtain mixed solvent；
(7) take the 50% of above-mentioned mixed solvent weight, add above-mentioned acid doped polyaniline, ultrasonic 10 minutes, add above-mentioned asphalt mixtures modified by epoxy resin
Fat, stirring reaction 40 minutes, obtain epoxy emulsion；
(8) above-mentioned acid doping polypyrrole is joined in remaining mixed solvent, stir, add polyamide, ultrasonic
30 minutes, obtain polyamide emulsion；
(9) by above-mentioned epoxy emulsion, polyamide emulsion, the mixing of silanol liquid, insulated and stirred 40 points in the water bath with thermostatic control of 60 DEG C
Clock, adds the dimethicone of compound weight 1%, stirs, and adds and remains each raw material, is passed through the steam of 80 DEG C, heats ripe
Change 30 minutes, cooling, obtain described coating.
Described a kind of environmental protection steel alloy anticorrosive paint and preparation method thereof, the using method of described coating is:
Be applied to paint brush of the present invention to clean up, dried alloy steel material working electrode surface, control coating thickness one
Cause, as in baking oven, be dried 20 hours at 60 DEG C,.
Performance test with the coating formation film of the present invention:
Impact strength: 53kg.cm；
Hardness: 3H.
Claims (3)
1. an environmental protection steel alloy anticorrosive paint, it is characterised in that it is made up of the raw material of following weight parts；
Tetrahydrofurfuryl alcohol 0.1-0.2, aniline 50-60, pyrroles 30-40, sulfosalicylic acid 7-9, epoxy resin E513-4, Ammonium persulfate.
1.3-2, molybdic acid 4-6, polyamide 3-5, n-butyl alcohol 160-170, butyl glycol ether 20-30, polyacrylamide 0.8-2, dry
Casein 3-4, ammonium metaborate 0.7-1,2-Propenoic acid, 2-methyl-, isooctyl ester 0.2-0.3, polyamide wax micropowder 1-2, hydrolytic polymaleic anhydride
0.4-1, ureidopropyltriethoxysilane 0.1-0.2.
2. the preparation method of an environmental protection steel alloy anticorrosive paint as claimed in claim 1, it is characterised in that include following step
Rapid:
(1) Ammonium persulfate. is joined in its weight 21-25 times deionized water, stir, obtain initiator solution；
(2) above-mentioned polyacrylamide is joined in the deionized water of its weight 10-15 times, add hydrolytic polymaleic anhydride, stir
Mixing uniformly, secure satisfactory grades sub-aqueous solution；
(3) by above-mentioned tetrahydrofurfuryl alcohol, polyamide wax micropowder mixing, insulated and stirred 10-14 minute at 80-90 DEG C, mixing is added
The dehydrated alcohol of material weight 7-10 times, stirring, to room temperature, adds above-mentioned ureidopropyltriethoxysilane, ultrasonic 2-3 minute, obtains
Silanol liquid；
(4) by above-mentioned sulfosalicylic acid, casein mixing, joining in the deionized water of compound weight 47-50 times, magnetic force stirs
Mix 20-30 minute, add aniline, stir, drip the 47-50% of above-mentioned initiator solution weight, regulation temperature after dropping
Degree, for 20-25 DEG C, adds the 30-40% of above-mentioned water-soluble polymers weight, stirring reaction 10-12 hour, filters, precipitation used
Acetone, distilled water wash 3-4 time successively, be dried 10-12 hour, obtain acid doped polyaniline at 60-65 DEG C；
(5) molybdic acid is joined in the deionized water of its weight 60-65 times, stir, add above-mentioned pyrroles, magnetic agitation
50-60 minute, drip remaining initiator solution, regulate temperature after dropping and be 0-5 DEG C, add remaining macromolecule water-soluble
Liquid, stirring reaction 6-7 hour, filter, the ethanol of precipitation 30-35% is washed 2-3 time, be dried 6-8 hour at 70-85 DEG C,
Acid doping polypyrrole；
(6) by above-mentioned n-butyl alcohol, butyl glycol ether mixing, stir, obtain mixed solvent；
(7) take the 50-60% of above-mentioned mixed solvent weight, add above-mentioned acid doped polyaniline, ultrasonic 10-15 minute, add above-mentioned
Epoxy resin, stirring reaction 40-50 minute, obtain epoxy emulsion；
(8) above-mentioned acid doping polypyrrole is joined in remaining mixed solvent, stir, add polyamide, ultrasonic
30-40 minute, obtain polyamide emulsion；
(9) by above-mentioned epoxy emulsion, polyamide emulsion, the mixing of silanol liquid, insulated and stirred in the water bath with thermostatic control of 60-70 DEG C
40-50 minute, add the dimethicone of compound weight 1-2%, stir, add and remain each raw material, be passed through 80-90 DEG C
Steam, heat aging 30-40 minute, cooling, obtain described coating.
3. according to a kind of environmental protection steel alloy anticorrosive paint described in claim 1-2 and preparation method thereof, it is characterised in that described
The using method of coating be:
Be applied to paint brush of the present invention to clean up, dried alloy steel material working electrode surface, control coating thickness one
Cause, as in baking oven, be dried 20-25 hour at 60-70 DEG C,.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201610545391.4A CN106189816A (en) | 2016-07-12 | 2016-07-12 | A kind of environmental protection steel alloy anticorrosive paint and preparation method thereof |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201610545391.4A CN106189816A (en) | 2016-07-12 | 2016-07-12 | A kind of environmental protection steel alloy anticorrosive paint and preparation method thereof |
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| CN106189816A true CN106189816A (en) | 2016-12-07 |
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107043584A (en) * | 2016-12-20 | 2017-08-15 | 铜陵市经纬流体科技有限公司 | A kind of environmentally friendly mild steel valve anticorrosive paint and preparation method thereof |
| CN110156461A (en) * | 2019-04-29 | 2019-08-23 | 曹博海 | A kind of disappearance alloy for die casting steel coating and preparation method thereof |
Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105001759A (en) * | 2015-07-21 | 2015-10-28 | 中国科学院金属研究所 | Molybdate doped polypyrrole/epoxy resin self-healing coating, preparation method thereof and application thereof |
| CN105368304A (en) * | 2015-09-23 | 2016-03-02 | 航天科工防御技术研究试验中心 | Anticorrosive paint and preparation method thereof |
-
2016
- 2016-07-12 CN CN201610545391.4A patent/CN106189816A/en not_active Withdrawn
Patent Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105001759A (en) * | 2015-07-21 | 2015-10-28 | 中国科学院金属研究所 | Molybdate doped polypyrrole/epoxy resin self-healing coating, preparation method thereof and application thereof |
| CN105368304A (en) * | 2015-09-23 | 2016-03-02 | 航天科工防御技术研究试验中心 | Anticorrosive paint and preparation method thereof |
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107043584A (en) * | 2016-12-20 | 2017-08-15 | 铜陵市经纬流体科技有限公司 | A kind of environmentally friendly mild steel valve anticorrosive paint and preparation method thereof |
| CN110156461A (en) * | 2019-04-29 | 2019-08-23 | 曹博海 | A kind of disappearance alloy for die casting steel coating and preparation method thereof |
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Application publication date: 20161207 |