CN106046326A - Epoxy resin water-permeable material curing agent and preparation method and application thereof - Google Patents
Epoxy resin water-permeable material curing agent and preparation method and application thereof Download PDFInfo
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- CN106046326A CN106046326A CN201610605074.7A CN201610605074A CN106046326A CN 106046326 A CN106046326 A CN 106046326A CN 201610605074 A CN201610605074 A CN 201610605074A CN 106046326 A CN106046326 A CN 106046326A
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- curing agent
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- polyamine
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- 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
- C08G59/00—Polycondensates containing more than one epoxy group per molecule; Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups
- C08G59/18—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing
- C08G59/40—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing characterised by the curing agents used
- C08G59/50—Amines
- C08G59/56—Amines together with other curing agents
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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
- C08L63/00—Compositions of epoxy resins; Compositions of derivatives of epoxy resins
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- Health & Medical Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Medicinal Chemistry (AREA)
- Polymers & Plastics (AREA)
- Organic Chemistry (AREA)
- Epoxy Resins (AREA)
Abstract
The invention belongs to the technical field of preparation of curing agents, and discloses an epoxy resin water-permeable material curing agent and a preparation method and application thereof. The curing agent is prepared from the following components in percentage by mass: 50-80 percent of ricinoleic acid and/or a polymer thereof, and 20-50 percent of fatty polyamine, alicyclic polyamine or polyoxypropylene polyamine containing a polypropylene oxide chain segment. The curing agent provided by the invention is a waterborne curing agent, has superior curing performance, and can be cured at the room temperature; a cured product has superior water permeability and air permeability, and can be applied to curing of an epoxy water-permeable material to prepare an epoxy ceramic forming mold or an epoxy water-permeable material. A fatty polyamine, polyoxypropylene polyamine or alicyclic polyamine curing agent is modified, so that the curing agent contains hydrophobic long-chain alkyl, hydrophilic hydroxyl, an amino group, acylamino and an ester group, has self-emulsifying performance, and can also be taken as a curing agent; a gap and a channel are formed between the epoxy resin and inorganic filler through a hydrophobic group, so that the obtained epoxy material has superior water permeability and air permeability.
Description
Technical field
The invention belongs to firming agent preparing technical field, particularly to a kind of epoxy resin pervious materials curing agent and system thereof
Preparation Method and application.
Background technology
Along with ceramic industry is to mechanization and the development of automatization, traditional Gypsum Fibrosum as pottery molding mold materials because of
Its intensity is low, water absorption rate is low can not meet modern production requirement, and mould of plastics is increasingly becoming following pottery forming mould
The main flow of tool material.
Epoxy resin is a kind of common thermosetting resin, has excellent properties such as adhesive property, and adhesion property, heat are steady
Qualitative, mechanical property, resistance to chemical corrosion, electrical insulation capability, high mechanical properties, be widely used in coating, adhesive, electronics
The field such as insulating material, composite.
Epoxy resin has above-mentioned excellent performance, is prepared into being applied to pottery molding for the seepy material of perforate and uses
In mold materials, it is possible to be effectively improved intensity and the water permeable ability of material.
Owing to epoxy resin is oil-soluble, conventional epoxy resin polyamine curing agent is water miscible, at aqueous solution
In, the polyamine being dissolved in water can not well solidify liquid-state epoxy resin, needs to add emulsifying agent in advance and carries out emulsifying, Cai Neng
Aqueous inorganic filler solidifies.Therefore, firming agent is modified so that it is become the firming agent of aqueous, solid having
Autoemulsification can also be played while change effect, enable epoxy resin-firming agent aqueous inorganic filler heterogeneous system steady
Fixed exist, be one of modified main target of epoxy resin waterborne curing agent.But, existing epoxy resin waterborne curing agent,
Although having certain self emulsifying and solidification, but the reason of the aspects such as its molecular structure, molecular weight, HLB, with asphalt mixtures modified by epoxy resin
Fat and aqueous phase inorganic filler system mixing cured during, epoxy resin-firming agent-heterogeneous body of aqueous inorganic filler can not be made
System is steady in a long-term to be existed, and the separation of phase more or less occurs so that the material after solidification and moisture phase and produce defect, contraction or
Distribution of pores inequality and closed pore phenomenon, can not get the epoxy resin through hole type seepy material that water permeability is excellent.
Summary of the invention
In order to overcome the shortcoming of above-mentioned prior art with not enough, the primary and foremost purpose of the present invention is to provide a kind of epoxy resin
Seepy material firming agent.
Another object of the present invention is to provide the preparation method of a kind of above-mentioned epoxy resin pervious materials curing agent.
Still a further object of the present invention is to provide the application of above-mentioned epoxy resin pervious materials curing agent.
The purpose of the present invention is realized by following proposal:
A kind of epoxy resin pervious materials curing agent, is prepared by the component including following mass percent:
Castor oil acid and/or its polymer 50~80%;
Fat polyamine, alicyclic ring polyamines or the polyether polyamine 20~50% containing polyoxypropylene segment.
Wherein in an embodiment, described castor oil acid and/or its polymer are castor oil acid, dimerization Oleum Ricini
At least one in acid, four poly-castor oil acids and dehydrated castor oleic acid.
Wherein in an embodiment, described fat polyamine be diethylenetriamine, triethylene tetramine, TEPA and
At least one in polyethylene polyamine.
Wherein in an embodiment, described alicyclic ring polyamines is diphenylmethanediamiand (MDA), isophorone diamine
(IPDA) at least one and in N-aminoethyl piperazine.
Wherein in an embodiment, the described polyether polyamine containing polyoxypropylene segment is polyetheramine T403 and polyethers
At least one in amine D230.
The present invention also provides for the preparation method of a kind of above-mentioned epoxy resin pervious materials curing agent, including walking in detail below
Rapid: by castor oil acid and/or its polymer, fat polyamine, alicyclic ring polyamines or the polyether polyamine containing polyoxypropylene segment mix,
Reacting by heating, obtains epoxy resin pervious materials curing agent.
Wherein in an embodiment, described reacting by heating refers to be warming up to 110~200 DEG C of reactions 5~10h.
The epoxy resin pervious materials curing agent of the present invention is waterborne curing agent, and its curing performance is excellent, room-temperature-curable,
Solidfied material has the air-and water-permeable performance of excellence, can be applicable to the solidification of epoxy seepy material prepare epoxy ceramic mould or
Epoxy seepy material.
Fat polyamine, polyether polyamine or alicyclic ring polyamine curing agent are modified processing by the present invention, make modified solidification
Agent contains hydrophobic chain alkyl and hydrophilic hydroxyl, amido, amide groups and ester group, has good automatic emulsifying performance, can
Enough again can be as firming agent as emulsifying agent.The surface-active action of this waterborne curing agent, makes the water in aqueous inorganic filler
Drop in the emulsion droplet that in whole system, dispersed one-tenth is tiny, and be dispersed between epoxy resin and inorganic filler, and make epoxy
Resin-hardener-stable containing water packing heterogeneous system.Owing to the hydrophobic group on firming agent makes epoxy resin and inorganic filler
Between form certain space and passage, stable through-hole structure, this firming agent will be formed after epoxy resin is fully cured
The epoxy material of solidification is just provided with the water-permeable and air permeable performance of excellence.
Firming agent prepared by the present invention has good autoemulsification and heterogeneous Stabilization, it is possible at wider consumption
In the range of well mix with aqueous inorganic filler, it is thus achieved that having of even pore distribution, aperture and adjustable porosity is good saturating
Water, the seepy material of permeability.
The present invention, relative to prior art, has such advantages as and beneficial effect:
(1) without adding organic solvent in epoxy resin pervious materials curing agent preparation process prepared by the present invention, preparation
Method is simple, and raw material is easy to get environmental protection.
(2) epoxy resin pervious materials curing agent prepared by the present invention has good self emulsifying and Stabilization, solidification
Material has permeable, the permeability of excellence.
(3) the epoxy resin pervious materials curing agent curing materials hole that prepared by the present invention is adjustable.
(4) preparation method of the present invention is simple and environmentally-friendly pollution-free.
Accompanying drawing explanation
Fig. 1 is the infrared spectrogram of the firming agent 1 that embodiment 1 obtains.
Detailed description of the invention
Below in conjunction with embodiment and accompanying drawing, the present invention is described in further detail, but embodiments of the present invention do not limit
In this.
The reagent used in the following example all can obtain from commercial channel.
Embodiment 1: the preparation of firming agent
144g castor oil acid and 50g diethylenetriamine are added with stirring, thermometer there-necked flask in, the lower temperature of stirring
Degree is increased between 110~160 DEG C, reacts 5~10h, and is removed by the water constantly produced, has finally given firming agent 1.
Embodiment 2: the preparation of firming agent
280g dimerization castor oil acid and 50g diethylenetriamine are added with stirring, thermometer there-necked flask in, stirring
Lower temperature is increased between 130~200 DEG C, reacts 5~10h, and is removed by the water constantly produced, has finally given firming agent 2.
Embodiment 3: the preparation of firming agent
Poly-for 220.6g tetra-castor oil acid and 20g diethylenetriamine are added with stirring, thermometer there-necked flask in, stir
Mix lower temperature to be increased between 130~200 DEG C, react 5~10h, and the water constantly produced is removed, finally given firming agent
3。
Embodiment 4: the preparation of firming agent
87.6g castor oil acid and 50g isophorone diamine are added with stirring, thermometer there-necked flask in, stirring
Lower temperature is increased between 110~160 DEG C, reacts 5~10h, and is removed by the water constantly produced, has finally given firming agent 4.
Embodiment 5: the preparation of firming agent
170g dimerization castor oil acid and 50g isophorone diamine are added with stirring, thermometer there-necked flask in, stir
Mix lower temperature to be increased between 130~200 DEG C, react 5~10h, and the water constantly produced is removed, finally given firming agent
5。
Embodiment 6: the preparation of firming agent
Poly-for 334.7g tetra-castor oil acid and 50g isophorone diamine are added with stirring, thermometer there-necked flask in,
The lower temperature of stirring is increased between 130~200 DEG C, reacts 5~10h, and is removed by the water constantly produced, has finally given solidification
Agent 6.
Embodiment 7: firming agent 1 performance detects
50g E-51 epoxy resin and 33g firming agent 1 being mixed to join in plastic cup, stirring 3~5min makes it mix
Uniformly obtain epoxy resin-firming agent 1 mixed liquor, weigh 83g aqueous inorganic filler (water 40wt%, SiO260wt%), add
In epoxy resin-firming agent 1 mixed liquor, quickly stirring 2~3min makes epoxy resin-firming agent 1 mixed liquor and inorganic filler
Mix homogeneously, and transfer in mould in 2min, and in mixed liquor, it is previously inserted a plastic tube, inserting height is shaping mould
/ 3rd of height, at room temperature solidify 24h.After curing molding, plastic tube is extracted, will be formed one default little
Hole.It is inserted among duck eye with the pipeline being compressed air or pressure (hydraulic) water of 0.2MPa respectively with air compressor afterwards and does
The permeable inspection of gas, when Observation Blocks surface is immersed in water test, continuous bubbling or emit the situation of water around module, bubbling or emit
The expression air-and water-permeable performance that water is uniform and area is big is good.
Testing the air-and water-permeable performance of module under the conditions of 25 DEG C, test result is shown in Table 1.
Water absorption rate is the mass percent that dried curing materials is absorbed the water increased within a certain period of time, can be anti-
Reflect the perforate porosity status of seepy material.Experiment is that at 70 DEG C, module is dried under vacuum to constant weight m0After be cooled to room temperature submergence
Recording module quality in water after 24 hours is m1, then it is calculated as follows water absorption rate:
(m1-m0)/m0× 100%
Testing the water absorption rate of module under the conditions of 25 DEG C, test result is shown in Table 1.
Embodiment 8: firming agent 2 performance detects
40g E-51 epoxy resin and 50.8g firming agent 2 being mixed to join in plastic cup, stirring 3~5min makes it mix
Close and uniformly obtain epoxy resin-firming agent 2 mixed liquor, weigh 181.6g aqueous inorganic filler (water 40wt%, SiO2
60wt%), joining in epoxy resin-firming agent 2 mixed liquor, quickly stirring 2~3min makes epoxy resin-firming agent 2 mix
Liquid and inorganic filler mix homogeneously, and transfer in mould in 2min, and in mixed liquor, it is previously inserted a plastic tube, insert
It is highly 1/3rd of shaping mould height, at room temperature solidifies 24h.After curing molding, plastic tube is extracted, one will be formed
Individual default duck eye.It is inserted into little with the pipeline being compressed air or pressure (hydraulic) water of 0.2MPa respectively with air compressor afterwards
Air-and water-permeable inspection is done among hole, when Observation Blocks surface is immersed in water test, continuous bubbling or emit the feelings of water around module
Condition, bubbling or to emit the expression air-and water-permeable performance that water is uniform and area is big good.The air-and water-permeable of module youngster is tested under the conditions of 25 DEG C
Performance, test result is shown in Table 1.
Testing the water absorption rate of module under the conditions of 25 DEG C, test result is shown in Table 1.
Embodiment 9: firming agent 3 performance detects
40g E-51 epoxy resin and 88.96g firming agent 3 being mixed to join in plastic cup, stirring 3~5min makes it mix
Close and uniformly obtain epoxy resin-firming agent 3 mixed liquor, weigh 386.9g aqueous inorganic filler (water 40wt%, SiO2
60wt%), joining in epoxy resin-firming agent 3 mixed liquor, quickly stirring 2~3min makes epoxy resin-firming agent 3 mix
Liquid and inorganic filler mix homogeneously, and transfer in mould in 2min, and in mixed liquor, it is previously inserted a plastic tube, insert
It is highly 1/3rd of shaping mould height, at room temperature solidifies 24h.After curing molding, plastic tube is extracted, one will be formed
Individual default duck eye.It is inserted into little with the pipeline being compressed air or pressure (hydraulic) water of 0.2MPa respectively with air compressor afterwards
Air-and water-permeable inspection is done among hole, when Observation Blocks surface is immersed in water test, continuous bubbling or emit the feelings of water around module
Condition, bubbling or to emit the expression air-and water-permeable performance that water is uniform and area is big good.
Testing the air-and water-permeable performance of module youngster under the conditions of 25 DEG C, test result is shown in Table 1.
Testing the water absorption rate of module under the conditions of 25 DEG C, test result is shown in Table 1.
Embodiment 10: firming agent 4 performance detects
50g E-51 epoxy resin and 57g firming agent 4 being mixed to join in plastic cup, stirring 3~5min makes it mix
Uniformly obtain epoxy resin-firming agent 4 mixed liquor, weigh 107g aqueous inorganic filler (water 40wt%, SiO260wt%), add
Entering in epoxy resin-firming agent 4 mixed liquor, quickly stirring 2~3min makes epoxy resin-firming agent 4 mixed liquor and inorganic fills out
Material mix homogeneously, and transfer in mould in 2min, and in mixed liquor, it is previously inserted a plastic tube, insert height for molding
/ 3rd of mould height, at room temperature solidify 24h.After curing molding, plastic tube is extracted, will be formed one default little
Hole.It is inserted among duck eye with the pipeline being compressed air or pressure (hydraulic) water of 0.2MPa respectively with air compressor afterwards and does
The permeable inspection of gas, when Observation Blocks surface is immersed in water test, continuous bubbling or emit the situation of water around module, bubbling or emit
The expression air-and water-permeable performance that water is uniform and area is big is good.
Testing the air-and water-permeable performance of module youngster under the conditions of 25 DEG C, test result is shown in Table 1.
Testing the water absorption rate of module under the conditions of 25 DEG C, test result is shown in Table 1.
Embodiment 11: firming agent 5 performance detects
30g E-51 epoxy resin and 55.8g firming agent 5 being mixed to join in plastic cup, stirring 3~5min makes it mix
Close and uniformly obtain epoxy resin-firming agent 5 mixed liquor, weigh 171.6g aqueous inorganic filler (water 40wt%, SiO2
60wt%), joining in epoxy resin-firming agent 5 mixed liquor, quickly stirring 2~3min makes epoxy resin-firming agent 5 mix
Liquid and inorganic filler mix homogeneously, and transfer in mould in 2min, and in mixed liquor, it is previously inserted a plastic tube, insert
It is highly 1/3rd of shaping mould height, at room temperature solidifies 24h.After curing molding, plastic tube is extracted, one will be formed
Individual default duck eye.It is inserted into little with the pipeline being compressed air or pressure (hydraulic) water of 0.2MPa respectively with air compressor afterwards
Air-and water-permeable inspection is done among hole, when Observation Blocks surface is immersed in water test, continuous bubbling or emit the feelings of water around module
Condition, bubbling or to emit the expression air-and water-permeable performance that water is uniform and area is big good.
Testing the air-and water-permeable performance of module youngster under the conditions of 25 DEG C, test result is shown in Table 1.
Testing the water absorption rate of module under the conditions of 25 DEG C, test result is shown in Table 1.
Embodiment 12: firming agent 6 performance detects
30g E-51 epoxy resin and 98.7g firming agent 6 being mixed to join in plastic cup, stirring 3~5min makes it mix
Close and uniformly obtain epoxy resin-firming agent 6 mixed liquor, weigh 386.1g aqueous inorganic filler (water 40wt%, SiO2
60wt%), joining in epoxy resin-firming agent 6 mixed liquor, quickly stirring 2~3min makes epoxy resin-firming agent 6 mix
Liquid and inorganic filler mix homogeneously, and transfer in mould in 2min, and in mixed liquor, it is previously inserted a plastic tube, insert
It is highly 1/3rd of shaping mould height, at room temperature solidifies 24h.After curing molding, plastic tube is extracted, one will be formed
Individual default duck eye.It is inserted into little with the pipeline being compressed air or pressure (hydraulic) water of 0.2MPa respectively with air compressor afterwards
Air-and water-permeable inspection is done among hole, when Observation Blocks surface is immersed in water test, continuous bubbling or emit the feelings of water around module
Condition, bubbling or to emit the expression air-and water-permeable performance that water is uniform and area is big good.
Testing the air-and water-permeable performance of module youngster under the conditions of 25 DEG C, test result is shown in Table 1.
Testing the water absorption rate of module under the conditions of 25 DEG C, test result is shown in Table 1.
From table 1, its solidfied material of firming agent prepared by the present invention has the air-and water-permeable performance of excellence, and along with it
Water absorption rate, along with the change of water consumption percentage ratio and respective change in whole system, shows the firming agent system using the present invention to prepare
The solidfied material obtained has the adjustable characteristic of hole.
Fig. 1 is the infrared spectrogram of synthesized solidified dose 1 that embodiment 1 obtains, and spectrogram shows as can be seen from Figure
1675cm-1Occur in that the characteristic peak of carbonyl in amide group (C=O), at 3250cm-1~3400cm-1Between occur in that amide groups
Amido (N-H) absworption peak in group.
The test result of table 1 embodiment 7~12 firming agent performance
Embodiment | Air-and water-permeable performance | 24 hours water absorption rates (%) |
7 | Excellent | 23.95 |
8 | Excellent | 28.80 |
9 | Excellent | 32.63 |
10 | Excellent | 26.35 |
11 | Excellent | 30.50 |
12 | Excellent | 32.46 |
Above-described embodiment is the present invention preferably embodiment, but embodiments of the present invention are not by above-described embodiment
Limit, the change made under other any spirit without departing from the present invention and principle, modify, substitute, combine, simplify,
All should be the substitute mode of equivalence, within being included in protection scope of the present invention.
Claims (8)
1. an epoxy resin pervious materials curing agent, it is characterised in that be prepared into by the component including following mass percent
Arrive:
Castor oil acid and/or its polymer 50~80%;
Fat polyamine, alicyclic ring polyamines or the polyether polyamine 20~50% containing polyoxypropylene segment.
Epoxy resin pervious materials curing agent the most according to claim 1, it is characterised in that: described castor oil acid and/
Or its polymer is at least one in castor oil acid, dimerization castor oil acid, four poly-castor oil acids and dehydrated castor oleic acid.
Epoxy resin pervious materials curing agent the most according to claim 1, it is characterised in that: described fat polyamine is two
At least one in ethylene triamine, triethylene tetramine, TEPA and polyethylene polyamine.
Epoxy resin pervious materials curing agent the most according to claim 1, it is characterised in that: described alicyclic ring polyamines is two
At least one in phenylmethane diamidogen, isophorone diamine and N-aminoethyl piperazine.
Epoxy resin pervious materials curing agent the most according to claim 1, it is characterised in that: described containing polyoxypropylene
The polyether polyamine of segment is polyetheramine T403 and at least one in polyetheramine D230.
6. the preparation method of the epoxy resin pervious materials curing agent described in an any one of Claims 1 to 5, it is characterised in that
Including step in detail below:
By castor oil acid and/or its polymer, fat polyamine, alicyclic ring polyamines or the polyether polyamine containing polyoxypropylene segment mix
Close, reacting by heating, obtain epoxy resin pervious materials curing agent.
The preparation method of epoxy resin pervious materials curing agent the most according to claim 6, it is characterised in that: described adds
Thermal response refers to be warming up to 110~200 DEG C of reactions 5~10h.
8. the application in epoxy seepy material of the epoxy resin pervious materials curing agent described in any one of Claims 1 to 5.
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CN107805000A (en) * | 2017-10-30 | 2018-03-16 | 重庆亲禾建科建材有限公司 | A kind of epoxy water-permeable brick |
CN108676148A (en) * | 2018-06-07 | 2018-10-19 | 安徽匠星联创新材料科技有限公司 | A kind of epoxy curing agent and preparation method thereof applied to porous pavement material |
CN108997713A (en) * | 2018-06-28 | 2018-12-14 | 广州均实复合材料科技有限公司 | A kind of pressure resistance water penetration porous material and preparation method thereof |
CN109503849A (en) * | 2018-12-04 | 2019-03-22 | 中科院广州化学有限公司南雄材料生产基地 | A kind of response type epoxy resin emulsifing thickener and the preparation method and application thereof |
CN111253554A (en) * | 2020-02-25 | 2020-06-09 | 中科院广州化学有限公司 | Polyamide type self-emulsifying epoxy resin curing agent and preparation method and application thereof |
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CN107805000A (en) * | 2017-10-30 | 2018-03-16 | 重庆亲禾建科建材有限公司 | A kind of epoxy water-permeable brick |
CN107805000B (en) * | 2017-10-30 | 2021-03-26 | 重庆亲禾生态环境科技有限公司 | Epoxy brick that permeates water |
CN108676148A (en) * | 2018-06-07 | 2018-10-19 | 安徽匠星联创新材料科技有限公司 | A kind of epoxy curing agent and preparation method thereof applied to porous pavement material |
CN108997713A (en) * | 2018-06-28 | 2018-12-14 | 广州均实复合材料科技有限公司 | A kind of pressure resistance water penetration porous material and preparation method thereof |
CN108997713B (en) * | 2018-06-28 | 2020-12-11 | 广州均实复合材料科技有限公司 | Pressure-resistant water-permeable porous material and preparation method thereof |
CN109503849A (en) * | 2018-12-04 | 2019-03-22 | 中科院广州化学有限公司南雄材料生产基地 | A kind of response type epoxy resin emulsifing thickener and the preparation method and application thereof |
CN109503849B (en) * | 2018-12-04 | 2021-04-27 | 中科院广州化学有限公司南雄材料生产基地 | Reactive epoxy resin emulsifying thickener and preparation method and application thereof |
CN111253554A (en) * | 2020-02-25 | 2020-06-09 | 中科院广州化学有限公司 | Polyamide type self-emulsifying epoxy resin curing agent and preparation method and application thereof |
CN111253554B (en) * | 2020-02-25 | 2023-03-10 | 中科院广州化学有限公司 | Polyamide type self-emulsifying epoxy resin curing agent and preparation method and application thereof |
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