CN103045153A - Acid liquor corrosion resistant dual-component polyurethane adhesive as well as preparation method and application thereof - Google Patents
Acid liquor corrosion resistant dual-component polyurethane adhesive as well as preparation method and application thereof Download PDFInfo
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- CN103045153A CN103045153A CN2012104685954A CN201210468595A CN103045153A CN 103045153 A CN103045153 A CN 103045153A CN 2012104685954 A CN2012104685954 A CN 2012104685954A CN 201210468595 A CN201210468595 A CN 201210468595A CN 103045153 A CN103045153 A CN 103045153A
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Abstract
The invention discloses an acid liquor corrosion resistant dual-component polyurethane adhesive as well as a preparation method and an application thereof. The acid liquor corrosion resistant dual-component polyurethane adhesive is characterized by being prepared by mixing a component A with a component B at a weight ratio of (0.8-20): 1, wherein the component A consists of the following components in parts by weight: 30-90 parts of polyether polyol, 1-20 parts of a chain expander, 10-50 parts of an acid resistant filling material, 10-50 parts of a plasticizer, 0.5-5 parts of a hydrolysis stabilizing agent, 0.5-2 parts of a water absorbent, 0.5-5 parts of an adhesion promoter, 1-10 parts of a thixotropic agent and 0.01-0.2 part of a catalyst; and the component B comprises the following components in parts by weight: 10-82 parts of polyisocyanate resin or the component B comprises the following components in parts by weight: 10-80 parts of polyisocyanate resin and 0.1-20 parts of a plasticizer. The dual-component polyurethane adhesive is prepared by respectively preparing the component A and the component B and then mixing. The acid liquor corrosion resistant dual-component polyurethane adhesive disclosed by the invention is comparatively high in intensity and hardness, excellent in acid liquid corrosion resistance and high in binding intensity, and is suitable for binding in an acid liquid environment and can be used in the fields of desulfurization chimney and acid liquid treatment pond.
Description
Technical field
The present invention relates to a kind of chemical adhesive, relate in particular to bi-component polyurethane adhesive of a kind of acidproof corrosion and its preparation method and application.
Background technology
The application of polyurethane adhesive is familiar with gradually.Urethane can be regarded a kind of segmented copolymer that contains soft chain segment and hard segment as.Hard section is comprised of with small molecule chain extender polyisocyanates or its, and segment molecule provides shearing, stripping strength and resistance toheat firmly, and soft section is provided by oligomer polyol, and normally polyethers and polyester polyol have the characteristics such as shock-resistant, antifatigue.Hard, soft section structure can make the satisfactory various structures polyurethane adhesive of intensity in the adjusting polyurethane molecular.
Current, polyurethane adhesive since its uniqueness mechanical property and processing performance, all obtained fast development in a lot of fields, especially be widely used in some waterproof fields.But because polyurethane adhesive, common polyurethane adhesive does not tolerate the corrosion of acid solution, has limited polyurethane adhesive under acid environment, such as the use in the fields such as desulfuration chimney, acid solution treating pond.
Summary of the invention
Technical problem to be solved by this invention provides a kind of bi-component polyurethane adhesive and its preparation method and application, has higher intensity and hardness, and acidproof corrosion performance can be excellent, and bonding strength is high, is suitable for the bonding use of acid solution environment.
Technical problem to be solved by this invention is achieved through the following technical solutions:
A kind of bi-component polyurethane adhesive of acidproof corrosion is characterized in that: being mixed by component A and B component, is 0.8-20 according to weight ratio A: B: 1;
Wherein said component A is composed of the following components by weight: polyether glycol 30-90, chainextender 1-20, acid resistance filler 10-50, softening agent 10-50, hydrolysis stabilizer 0.5-5, water-retaining agent 0.5-2 part, adhesion promoter 0.5-5, thixotropic agent 1-10 part, catalyzer 0.01-0.2;
Described B component is that polyisocyanate resin 10-82 or described B component are composed of the following components by weight: polyisocyanate resin 10-80, softening agent 0.1-20.
Be 1-10 according to weight ratio A: B preferably: 1.
Polyether glycol described in the component A comprises that functionality is that 2-4 and molecular weight are a kind of in the polyoxypropylene polyol of 300-20000;
Described chainextender is di-alcohols;
Described acid resistance filler is silicon powder, mica powder or barium sulfate;
Described softening agent is phthalate;
Described hydrolysis stabilizer is the Carbodiimides material;
Described adhesive power promotor is silane coupling agent;
Described water-retaining agent is p-Methyl benzenesulfonyl isocyanate or oxazole alkanes moisture scavenger;
Described thixotropic agent is aerosil or organobentonite;
Described catalyzer is the organic tin catalyzer.
Polyisocyanate resin described in the B component is polyisocyanates and derivative thereof; Described softening agent is phthalate.
Described di-alcohols is a kind of among Isosorbide-5-Nitrae butyleneglycol, ethylene glycol, Diethylene Glycol, 1,6 hexylene glycol, the HQEE (quinhydrones-two (B-hydroxyethyl) ether) or its mixture between arbitrarily;
Described phthalate is dibutyl phthalate, dioctyl phthalate (DOP), diisononyl phthalate or Di Iso Decyl Phthalate; Preferred dibutyl phthalate or diisononyl phthalate;
Described silane coupling agent is N-(β one an aminoethyl) γ one aminopropyl trimethoxysilane, γ one glycidyl ether oxygen propyl trimethoxy silicane, γ one aminopropyl trimethoxysilane, γ one aminopropyl triethoxysilane or γ monomethyl propylene phthalein oxygen propyl trimethoxy silicane;
Described organic tin catalyzer is dibutyl tin laurate, stannous octoate or mercaptan dibutyl tin.
Described polyisocyanates and derivative thereof are tolylene diisocyanate, diphenylmethanediisocyanate, hexamethylene diisocyanate, isophorone diisocyanate, polymethylene multi-phenenyl isocyanate, liquefied mdi (diphenylmethanediisocyanate), TDI (tolylene diisocyanate) tripolymer, HDI (hexamethylene diisocyanate) biuret or HDI (hexamethylene diisocyanate) tripolymer; Preferred polymethylene multi-phenenyl isocyanate or liquefied mdi (diphenylmethanediisocyanate);
Described phthalate is dibutyl phthalate, dioctyl phthalate (DOP), diisononyl phthalate or Di Iso Decyl Phthalate, preferred dibutyl phthalate or diisononyl phthalate.
The granularity of silicon powder, mica powder or barium sulfate is 100 orders-15000 orders.
The preparation method of the bi-component polyurethane adhesive of described acidproof corrosion is characterized in that: prepare respectively A component and B component, wherein the A component is prepared from by following steps:
(a) at room temperature in the stirring tank order add polyether glycol, chainextender, softening agent under vacuum protection blend 10-90 minute;
(b) add acid resistance filler, thixotropic agent, hydrolysis stabilizer, adhesion promoter, water-retaining agent, vacuum stirring 30 minutes;
(c) add catalyzer, vacuum stirring 10-90 minute;
(d) carry out degassed after, can obtain the A component product of paste;
Be prepared as follows when wherein the B component is mixture and form:
(a) at room temperature in the stirring tank order add polyisocyanate resin, softening agent, under vacuum protection blend 15-60 minute, obtain finely dispersed B component product;
A component and B component are proportionally mixed use.
The stirring tank of preparation A component is twin shaft planet stirring still, the enamel reaction stirring tank that preparation B component is.
The bi-component polyurethane adhesive of described acidproof corrosion is in the application in desulfuration chimney, acid solution treating pond field.
The present invention has following advantage:
The bonding system of the application's two component polyurethane, mainly improve cementability and hydrolytic resistance from the following aspects:
(1) adopts anti-hydrolytic performance and the good polyol component of acid corrosion-resistant performance, polyol component is polyoxypropylene polyol in the described two component adhesive of the application, it has preferably hydrophobic performance, and its ehter bond has preferably acidproof corrosion performance simultaneously;
(2) adopt the dibasic alcohol chainextender, improve the crystal property of system, reach the purpose that improves the acid corrosion-resistant performance;
(3) adopt acidproof filler, acid resistance filler itself has very high acid corrosion-resistant ability, after the adding system, can improve modulus and the degree of compactness of system, has improved equally the acid corrosion-resistant performance of system;
(4) introduce hydrolysis stabilizer, the present invention adopts the Carbodiimides material.The process of the hydrolysis of acid solution Promotion system is followed in the corrosion in acid solution of urethane, add hydrolysis stabilizer after, can slow down or lower the hydrolytic process of system, thereby reach the purpose of raising system acid corrosion-resistant ability;
(5) add adhesive power promotor.Adhesive power promotor used in the present invention is organo-silicon coupling agent, has formed hydrophobic chemical adhesive layer, when improving adhesiveproperties, also can improve the acid corrosion-resistant ability of glue-line;
(6) in formulating of recipe, all are selected materials and all adopt hydrophobic raw material, have reduced the perviousness of acid solution in system, thereby reach the purpose of raising system acid corrosion-resistant ability.
Embodiment
Embodiment 1
Accurate raw materials weighing (Kg):
The A component: the polyether glycol 2028 of molecular-weight average 4000 is 90, Isosorbide-5-Nitrae butyleneglycol 4, silicon powder (400 order) 15, dibutyl phthalate 30, N, N '-two (2,6-diisopropyl phenyl) carbodiimide) 1, oxazolidine water-retaining agent 1, γ one glycidyl ether oxygen propyl trimethoxy silicane 2, white carbon black 5, dibutyl tin laurate 0.1;
B component: polyisocyanate resin 80, dibutyl phthalate 20.
The present embodiment preparation:
The A component: during preparation, at room temperature in twin shaft planet stirring still, sequentially add polyether glycol 2028, butyleneglycol, dibutyl phthalate, blend is 10 minutes under vacuum protection; Add silicon powder (400 order), N, N '-two (2,6-diisopropyl phenyl) carbodiimide, white carbon black, oxazolidine water-retaining agent, γ one glycidyl ether oxygen propyl trimethoxy silicane, vacuum stirring 30 minutes; Add dibutyltin dilaurate catalyst, vacuum stirring 10 minutes; Carry out degassed after, can obtain the A component product of paste;
The B component: during preparation, order adds polyisocyanate resin and dibutyl phthalate in the at room temperature enamel reaction stirring tank, and blend is 15 minutes under vacuum protection, obtains B component product.
A component and B component are mixed use according to 6: 1 ratio of weight ratio.
The bi-component polyurethane adhesive of above-mentioned acidproof corrosion is applied in desulfuration chimney, acid solution treating pond field.
Embodiment 2
Accurate raw materials weighing (Kg):
The A component: the polyether glycol 3050 of molecular-weight average 3000 is 80,1,6 hexylene glycols 10, barium sulfate (2000 order) 50, diisononyl phthalate 20, polycarbodiimide 2, oxazolidine water-retaining agent 2, γ monomethyl propylene phthalein oxygen propyl trimethoxy silicane 3, white carbon black 4, stannous octoate 0.05
B component: polyisocyanate resin 75, dibutyl phthalate 15;
The present embodiment preparation:
The A component: during preparation, at room temperature in twin shaft planet stirring still, sequentially add polyether glycol 3050,1,6 hexylene glycol, diisononyl phthalate, blend is 10 minutes under vacuum protection; Add barium sulfate (2000 order), diisononyl phthalate, polycarbodiimide, white carbon black, oxazolidine water-retaining agent, γ monomethyl propylene phthalein oxygen propyl trimethoxy silicane, vacuum stirring 30 minutes; Add stannous octoate catalyst, vacuum stirring 10 minutes, carry out degassed after, can obtain the A component product of paste.
The B component: during preparation, order adds polyisocyanate resin, dibutyl phthalate in the at room temperature enamel reaction stirring tank, and blend is 15 minutes under vacuum protection, obtains B component product.
A component and B component are mixed use according to 4: 1 ratio of weight ratio.
Performance comparison was as shown in the table after embodiment and currently available products solidified:
Comparative Examples wherein: market product is similar dual-component polyurethane adhesive.
From the result of reality test, embodiment 1 and embodiment 2 are through behind 90 days 10% sulfuric acid corrosions, and tensile strength and retention rate thereof are still higher, obviously are better than the market like product.
Hardness: press GB/T531.1-2008 " vulcanized rubber and thermoplastic elastomer penetration hardness test method first part: the clear young that hardness of Shore durometer method " evaluation hardness.
Tensile strength: press GB/T528-1998 " mensuration of vulcanized rubber and thermoplastic elastomer tensile stress-strain performance " and estimate tensile strength.
Shearing resistance: press GB-T7124-2008 " mensuration of tackiness agent tensile shear strength (rigid material is to rigid material) " and estimate shearing resistance, the sandblast grinding process is made on the steel substrate surface.
The bi-component polyurethane adhesive of above-mentioned acidproof corrosion is applied in desulfuration chimney, acid solution treating pond field.
Embodiment 3
Accurate raw materials weighing (Kg):
Component A is composed of the following components by weight: polyether glycol 30, chainextender 1, acid resistance filler 10, softening agent 10, hydrolysis stabilizer 0.5, water-retaining agent 0.5, adhesion promoter 0.5, thixotropic agent 1, catalyzer 0.01; B component is polyisocyanate resin 10, softening agent 0.1.
Wherein polyether glycol is polyoxypropylene polyol, chainextender is Diethylene Glycol, acid resistance filler is mica powder, softening agent is diisononyl phthalate, and hydrolysis stabilizer is polycarbodiimide, and water-retaining agent is p-Methyl benzenesulfonyl isocyanate, adhesion promoter is N-(β one an aminoethyl) γ one aminopropyl trimethoxysilane, thixotropic agent is organobentonite, and catalyzer is stannous octoate, and polyisocyanate resin is polymethylene multi-phenenyl isocyanate.
The preparation method is with embodiment 1, and wherein A component and B component are mixed use according to 0.8: 1 ratio of weight ratio.
The bi-component polyurethane adhesive of above-mentioned acidproof corrosion is applied in desulfuration chimney, acid solution treating pond field.
Embodiment 4
Accurate raw materials weighing (Kg):
Component A is composed of the following components by weight: polyether glycol 90, chainextender 20, acid resistance filler 50, softening agent 50, hydrolysis stabilizer 5, water-retaining agent 2, adhesion promoter 5, thixotropic agent 10, catalyzer 0.2;
B component is composed of the following components by weight: polyisocyanate resin 80, softening agent 20.
Wherein polyether glycol is polyoxypropylene polyol, chainextender is HQEE, acid resistance filler is mica powder, softening agent is dibutyl phthalate, and hydrolysis stabilizer is polycarbodiimide, and water-retaining agent is the oxazolidine water-retaining agent, adhesion promoter is γ one glycidyl ether oxygen propyl trimethoxy silicane, thixotropic agent is organobentonite, and catalyzer is the mercaptan dibutyl tin, and polyisocyanate resin is liquefied mdi.
The preparation method is with embodiment 1, and wherein A component and B component are mixed use according to 20: 1 ratio of weight ratio.
The bi-component polyurethane adhesive of above-mentioned acidproof corrosion is applied in desulfuration chimney, acid solution treating pond field.
Embodiment 5
Accurate raw materials weighing (Kg):
Component A is composed of the following components by weight: polyether glycol 60, chainextender 10, acid resistance filler 30, softening agent 25, hydrolysis stabilizer 2, water-retaining agent 1.2, adhesion promoter 3, thixotropic agent 5, catalyzer 0.1; B component is polyisocyanate resin 82.
Wherein polyether glycol is polyoxypropylene polyol, chainextender is HQEE, acid resistance filler is mica powder, softening agent is dibutyl phthalate, and hydrolysis stabilizer is polycarbodiimide, and water-retaining agent is the oxazolidine water-retaining agent, adhesion promoter is γ monomethyl propylene phthalein oxygen propyl trimethoxy silicane, thixotropic agent is organobentonite, and catalyzer is the mercaptan dibutyl tin, and polyisocyanate resin is diphenylmethanediisocyanate.
The preparation method is with embodiment 1, and wherein A component and B component are mixed use according to 10: 1 ratio of weight ratio.
The bi-component polyurethane adhesive of above-mentioned acidproof corrosion is applied in desulfuration chimney, acid solution treating pond field.
Claims (10)
1. the bi-component polyurethane adhesive of an acidproof corrosion, it is characterized in that: being mixed by component A and B component, is 0.8-20 according to weight ratio A: B: 1;
Wherein said component A is composed of the following components by weight: polyether glycol 30-90, chainextender 1-20, acid resistance filler 10-50, softening agent 10-50, hydrolysis stabilizer 0.5-5, water-retaining agent 0.5-2, adhesion promoter 0.5-5, thixotropic agent 1-10, catalyzer 0.01-0.2;
Described B component is that polyisocyanate resin 10-82 or described B component are composed of the following components by weight: polyisocyanate resin 10-80, softening agent 0.1-20.
2. the bi-component polyurethane adhesive of acidproof corrosion as claimed in claim 1 is characterized in that: be 1-10 according to weight ratio A: B: 1.
3. the bi-component polyurethane adhesive of acidproof corrosion as claimed in claim 1 or 2 is characterized in that: polyether glycol described in the component A comprises that functionality is that 2-4 and molecular weight are a kind of in the polyoxypropylene polyol of 300-20000;
Described chainextender is di-alcohols;
Described acid resistance filler is silicon powder, mica powder or barium sulfate;
Described softening agent is phthalate;
Described hydrolysis stabilizer is the Carbodiimides material;
Described adhesive power promotor is silane coupling agent;
Described water-retaining agent is p-Methyl benzenesulfonyl isocyanate or oxazole alkanes moisture scavenger;
Described thixotropic agent is aerosil or organobentonite;
Described catalyzer is the organic tin catalyzer.
4. the bi-component polyurethane adhesive of acidproof corrosion as claimed in claim 1 or 2, it is characterized in that: polyisocyanate resin described in the B component is polyisocyanates and derivative thereof; Described softening agent is phthalate.
5. the bi-component polyurethane adhesive of acidproof corrosion as claimed in claim 3 is characterized in that: described di-alcohols is a kind of among Isosorbide-5-Nitrae butyleneglycol, ethylene glycol, Diethylene Glycol, 1,6 hexylene glycol, the HQEE or its mixture between arbitrarily;
Described phthalate is dibutyl phthalate, dioctyl phthalate (DOP), diisononyl phthalate or Di Iso Decyl Phthalate; Preferred dibutyl phthalate or diisononyl phthalate;
Described silane coupling agent is N-(β-aminoethyl)-γ-aminopropyltrimethoxysilane, γ-glycidyl ether oxygen propyl trimethoxy silicane, γ-aminopropyltrimethoxysilane, γ-aminopropyl triethoxysilane or γ-methacrylic phthalein oxygen propyl trimethoxy silicane;
Described organic tin catalyzer is dibutyl tin laurate, stannous octoate or mercaptan dibutyl tin.
6. the bi-component polyurethane adhesive of acidproof corrosion as claimed in claim 3, it is characterized in that: described polyisocyanates and derivative thereof are tolylene diisocyanate, diphenylmethanediisocyanate, hexamethylene diisocyanate, isophorone diisocyanate, polymethylene multi-phenenyl isocyanate, liquefied mdi, TDI tripolymer, HDI biuret or HDI tripolymer; Preferred polymethylene multi-phenenyl isocyanate or liquefied mdi;
Described phthalate is dibutyl phthalate, dioctyl phthalate (DOP), diisononyl phthalate or Di Iso Decyl Phthalate, preferred dibutyl phthalate or diisononyl phthalate.
7. the bi-component polyurethane adhesive of acidproof corrosion as claimed in claim 3, it is characterized in that: the granularity of silicon powder, mica powder or barium sulfate is 100 orders-15000 orders.
8. such as the preparation method of the bi-component polyurethane adhesive of the described acidproof corrosion of one of claim 1 to 7, it is characterized in that: prepare respectively A component and B component, wherein the A component is prepared from by following steps:
(a) at room temperature in the stirring tank order add polyether glycol, chainextender, softening agent under vacuum protection blend 10-90 minute;
(b) add acid resistance filler, thixotropic agent, hydrolysis stabilizer, adhesion promoter, water-retaining agent, vacuum stirring 30 minutes;
(c) add catalyzer, vacuum stirring 10-90 minute;
(d) carry out degassed after, can obtain the A component product of paste;
Be prepared as follows when wherein the B component is mixture and form:
(a) at room temperature in the stirring tank order add polyisocyanate resin, softening agent, under vacuum protection blend 15-60 minute, obtain finely dispersed B component product;
A component and B component are proportionally mixed use.
9. the preparation method of the bi-component polyurethane adhesive of acidproof corrosion as claimed in claim 8 is characterized in that: the stirring tank of preparation A component is twin shaft planet stirring still, the enamel reaction stirring tank that preparation B component is.
10. such as the application in desulfuration chimney, acid solution treating pond field of the bi-component polyurethane adhesive of the described acidproof corrosion of one of claim 1 to 7.
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| Application Number | Priority Date | Filing Date | Title |
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| CN201210468595.4A CN103045153B (en) | 2012-11-20 | 2012-11-20 | Bi-component polyurethane adhesive of a kind of resistance to acid liquid corrosion and its preparation method and application |
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| CN201210468595.4A CN103045153B (en) | 2012-11-20 | 2012-11-20 | Bi-component polyurethane adhesive of a kind of resistance to acid liquid corrosion and its preparation method and application |
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| CN103554410A (en) * | 2013-10-19 | 2014-02-05 | 泉州源利鞋材有限公司 | Shoe pad warm in winter and cool in summer as well as preparation method thereof |
| CN104559901A (en) * | 2014-12-26 | 2015-04-29 | 东莞市腾威电子材料技术有限公司 | Two-component adhesion agent, as well as preparation method and application thereof |
| CN107652934A (en) * | 2017-09-30 | 2018-02-02 | 温州生物材料与工程研究所 | A kind of room temperature super fast curing double component solvent-free polyurethane structure glue and its preparation and application |
| CN109206569A (en) * | 2017-07-03 | 2019-01-15 | 比亚迪股份有限公司 | A kind of aqueous polyurethane and Aqueous Polyurethane Adhesives and preparation method thereof |
| CN110343502A (en) * | 2019-06-13 | 2019-10-18 | 南京威邦新材料有限公司 | A kind of rubber-plastic composite floor board solvent-free polyurethane adhesive and preparation method thereof |
| CN111909348A (en) * | 2019-05-08 | 2020-11-10 | H.B.富乐公司 | Reactive polyurethane hot melt adhesive composition and preparation and application thereof |
| CN112126400A (en) * | 2020-09-07 | 2020-12-25 | 深圳市安品有机硅材料有限公司 | Polyurethane corrosion-resistant material and preparation method thereof |
| CN115477913A (en) * | 2022-09-19 | 2022-12-16 | 华南理工大学 | Oil gel-based underwater adhesive material and preparation method and application thereof |
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Cited By (11)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN103554410A (en) * | 2013-10-19 | 2014-02-05 | 泉州源利鞋材有限公司 | Shoe pad warm in winter and cool in summer as well as preparation method thereof |
| CN104559901A (en) * | 2014-12-26 | 2015-04-29 | 东莞市腾威电子材料技术有限公司 | Two-component adhesion agent, as well as preparation method and application thereof |
| CN109206569A (en) * | 2017-07-03 | 2019-01-15 | 比亚迪股份有限公司 | A kind of aqueous polyurethane and Aqueous Polyurethane Adhesives and preparation method thereof |
| CN109206569B (en) * | 2017-07-03 | 2021-01-19 | 比亚迪股份有限公司 | Waterborne polyurethane, waterborne polyurethane adhesive and preparation method thereof |
| CN107652934A (en) * | 2017-09-30 | 2018-02-02 | 温州生物材料与工程研究所 | A kind of room temperature super fast curing double component solvent-free polyurethane structure glue and its preparation and application |
| CN111909348A (en) * | 2019-05-08 | 2020-11-10 | H.B.富乐公司 | Reactive polyurethane hot melt adhesive composition and preparation and application thereof |
| CN111909348B (en) * | 2019-05-08 | 2022-10-28 | H.B.富乐公司 | Reactive polyurethane hot melt adhesive composition and preparation and application thereof |
| CN110343502A (en) * | 2019-06-13 | 2019-10-18 | 南京威邦新材料有限公司 | A kind of rubber-plastic composite floor board solvent-free polyurethane adhesive and preparation method thereof |
| CN112126400A (en) * | 2020-09-07 | 2020-12-25 | 深圳市安品有机硅材料有限公司 | Polyurethane corrosion-resistant material and preparation method thereof |
| CN115477913A (en) * | 2022-09-19 | 2022-12-16 | 华南理工大学 | Oil gel-based underwater adhesive material and preparation method and application thereof |
| CN115477913B (en) * | 2022-09-19 | 2023-08-18 | 华南理工大学 | Oil gel-based underwater adhesive material and preparation method and application thereof |
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