CN110527273B - Polypropylene-polyphenylene oxide-polystyrene ternary alloy and preparation method thereof - Google Patents
Polypropylene-polyphenylene oxide-polystyrene ternary alloy and preparation method thereof Download PDFInfo
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- CN110527273B CN110527273B CN201910808158.4A CN201910808158A CN110527273B CN 110527273 B CN110527273 B CN 110527273B CN 201910808158 A CN201910808158 A CN 201910808158A CN 110527273 B CN110527273 B CN 110527273B
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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
- C08L71/00—Compositions of polyethers obtained by reactions forming an ether link in the main chain; Compositions of derivatives of such polymers
- C08L71/08—Polyethers derived from hydroxy compounds or from their metallic derivatives
- C08L71/10—Polyethers derived from hydroxy compounds or from their metallic derivatives from phenols
- C08L71/12—Polyphenylene oxides
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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
- 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
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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
- C08L2205/00—Polymer mixtures characterised by other features
- C08L2205/08—Polymer mixtures characterised by other features containing additives to improve the compatibility between two polymers
Abstract
The invention provides a polypropylene polyphenyl ether-polystyrene ternary alloy which is characterized by comprising the following components in parts by weight: 100 parts of polypropylene, polyphenyl ether and polystyrene, and 5-25 parts of A-B-A type block copolymer; wherein, in the A-B-A type block copolymer, the A block is a copolymer of styrene and vinyl C4-C12 alkyl aromatic compounds, the B block is a selective hydrogenated polymer of a conjugated diene compound, and the molecular weight is 5-30 ten thousand. The polypropylene polyphenyl ether polystyrene ternary alloy has the advantages of good compatibility and high toughness.
Description
Technical Field
The invention relates to the technical field of high polymer materials, in particular to a polypropylene polyphenyl ether-polystyrene ternary alloy and a preparation method thereof.
Background
Polyphenylene Ether (PPE) has high heat resistance, good mechanical property and electrical property, high price and poor solvent resistance; polypropylene (PP) is inexpensive and excellent in solvent resistance, but low in heat resistance. The general Polystyrene (PS) is an amorphous random polymer, has excellent heat insulation, insulation and transparency, is 0-70 ℃ in long-term use, but is brittle and easy to crack at low temperature. The three components are combined to prepare the alloy material with moderate price and balanced heat resistance and solvent resistance.
However, ternary alloys are not compatible with each other, and therefore it is often necessary to add a compatibilizing agent to improve compatibility with each other. Chinese patent CN102719014A discloses a polypropylene polyphenylene oxide polystyrene ternary alloy, which has excellent balance among rigidity, toughness and processability, and can be applied in various fields. Mainly, the compatilizer is a selectively hydrogenated A-B-A type triblock copolymer of an alkenyl aromatic compound and conjugated diene, a block B is a conjugated diene compound, and a block A is a vinyl aromatic compound; the vinyl aromatic compound is styrene, alkyl styrene, ethyl vinyl benzene or divinyl benzene, and the conjugated diene compound is butadiene or isoprene. However, in this formulation, the toughening effect of the compatibilizer is limited, and in most applications additional toughening agents are required to improve toughness.
Disclosure of Invention
The invention aims to provide a polypropylene polyphenyl ether-polystyrene ternary alloy which has the advantages of good compatibility and high toughness.
The invention also aims to provide a preparation method of the polypropylene polyphenylene oxide polystyrene ternary alloy.
The invention is realized by the following technical scheme:
the polypropylene polyphenyl ether polystyrene ternary alloy comprises the following components in parts by weight:
100 parts of polypropylene, polyphenyl ether and polystyrene,
5-25 parts of A-B-A type block copolymer;
wherein, in the A-B-A type block copolymer, the A block is a copolymer of styrene and vinyl C4-C12 alkyl aromatic compounds, the B block is a selective hydrogenated polymer of a conjugated diene compound, and the molecular weight is 5-30 ten thousand.
Preferably, the composition comprises the following components in parts by weight:
100 parts of polypropylene, polyphenyl ether and polystyrene,
10-18 parts of A-B-A type block copolymer;
wherein, in the A-B-A type block copolymer, the A block is a copolymer of styrene and vinyl C4-C12 alkyl aromatic compounds, the B block is a selective hydrogenated polymer of a conjugated diene compound, and the molecular weight is 5-30 ten thousand.
In the prior polystyrene-poly-conjugated diene compound-polystyrene block copolymer, the compatibility of a polystyrene chain segment and polyphenyl ether is better, but the polystyrene chain segment does not provide addition of toughness; the B block of the poly-conjugated diene compound provides the desired toughness.
The A block of the A-B-A block copolymer used in the present invention contains a long chain alkyl group of a vinyl C4-C12 alkyl aromatic compound, and the long chain alkyl group can provide a certain toughness addition. Therefore, the toughness of the alloy can be improved more by adding the A-B-A type block copolymer, and meanwhile, the A-B-A type block copolymer has good compatibility.
The polystyrene in the A-B-A type block copolymer accounts for 60-99% of the molecular weight of the A block.
In the A block, the vinyl C4-C12 alkyl aromatic compound is less in content because the steric effect of the long-chain alkyl group thereof hinders the progress of polymerization, and the excessively long-chain alkyl chain segment hinders the compatibility of the polystyrene segment with polyphenylene ether, lowering processability. Moreover, the existence of the propylene long-chain alkyl can prevent the aryl from contacting with the styrene to reduce the compatibility, so that the compatibility can be effectively ensured by keeping most of the styrene content.
The conjugated diene compound in the A-B-A type block copolymer of the present invention may be a conjugated diene compound commonly used in polymer synthesis, and the conjugated diene compound is selected from at least one of butadiene and isoprene commonly used in the market, and the B block accounts for 45 to 80% of the molecular weight of the A-B-A type block copolymer in view of cost.
Preferably, in the vinyl C4-C12 alkyl aromatic compound, the C4-C12 alkyl is positioned at the para position of the aromatic ring.
Preferably, in the vinyl C4-C12 alkyl aromatic compound, the C4-C12 alkyl is linear. The linear alkyl has the function of extending long alkyl chain segments, and can improve the toughness. If C6 is hexyl, the addition to toughness is better than that of cyclohexane. However, during the synthesis, it is possible that some C4-C12 alkyl groups may undergo isomerization reactions to form other nonlinear C4-C12 alkyl groups, typically such reactions will not exceed 1% of the total C4-C12 alkyl groups.
In the vinyl C4-C12 alkyl aromatic compound, the aromatic compound is at least one selected from phenyl, naphthyl and phenanthryl. The aromatic compound may contain a halogen or an alkyl group having not more than C3, and does not significantly affect the vinyl C4-C12 alkyl group.
In the ternary alloy, 10-60% of polypropylene, 10-60% of polyphenyl ether and 5-30% of polystyrene are used;
the polyphenylene ether used in the present invention may be poly (2, 6-dimethylphenol), poly (2, 6-dimethyl-1, 4-phenylene) ether, poly (2-methyl-6-ethyl-1, 4-phenylene) ether, poly (2, 6-diethyl-1, 4-phenylene) ether, poly (2-ethyl-6-n-propyl-1, 4-phenylene) ether, poly (2, 6-di-n-propyl-1, 4-phenylene) ether, poly (2-methyl-6-n-butyl-1, 4-phenylene) ether, poly (2-ethyl-6-isopropyl-1, 4-phenylene) ether, poly (2-methyl-6-chloroethyl-1, at least one of 4-phenylene ether, poly (2-methyl-6-hydroxyethyl-1, 4-phenylene) ether, and poly (2-methyl-6-chloroethyl-1, 4-phenylene) ether; preferably at least one of poly (2, 6-dimethyl-1, 4-phenylene) ether, poly (2-methyl-6-ethyl-1, 4-phenylene) ether, poly (2, 6-diethyl-1, 4-phenylene) ether and poly (2, 6-dimethylphenol).
The polypropylene used in the invention can be homo-polypropylene and co-polypropylene, and the co-polypropylene can be ethylene/propylene copolymer. There is no particular requirement for the melt index of the polypropylene.
0-100 parts of reinforcing fiber is also included according to the parts by weight; the reinforcing fiber is at least one selected from glass fiber, carbon fiber, metal fiber and whisker.
0-10 parts of auxiliary agent is also included according to the parts by weight; the auxiliary agent is at least one selected from antioxidant, lubricant, flame retardant, heat stabilizer, light stabilizer and ultraviolet light absorption additive.
Antioxidants include primary antioxidants or stabilizers (such as hindered phenols and/or secondary arylamines) and optional secondary antioxidants (such as phosphates and/or thioesters). Suitable antioxidants include, for example, organophosphates such as tris (nonylphenyl) phosphite, tris (2, 4-di-tert-butylphenyl) phosphite, bis (2, 4-di-tert-butylphenyl) pentaerythritol diphosphite, distearyl pentaerythritol diphosphite or the like, alkylated monophenols or polyphenols; alkylation reaction products of polyhydric phenols with dienes such as tetrakis [ methylene (3, 5-di-tert-butyl-4-hydroxyhydrocinnamate) ] methane and the like; butylated reaction products of p-cresol or dicyclopentadiene; alkylated hydroquinones; hydroxylated thiodiphenyl ether; alkylidene bisphenols; a benzyl compound; esters of beta- (3, 5-di-tert-butyl-4-hydroxyphenyl) -propionic acid with mono-or polyhydric alcohols; esters of beta- (5-tert-butyl-4-hydroxy-3-methylphenyl) -propionic acid with mono-or polyhydric alcohols; esters of thioalkyl or thioaryl compounds such as distearylthiopropionate, dilaurylthiopropionate, ditridecylthiopropionate, octadecyl-3- (3, 5-di-t-butyl-4-hydroxyphenyl) propionate, pentaerythritol-tetrakis [3- (3, 5-di-t-butyl-4-hydroxyphenyl) ] propionate and the like; amides of beta- (3, 5-di-tert-butyl-4-hydroxyphenyl) -propionic acid and the like; or combinations comprising at least one of the foregoing antioxidants.
Suitable heat stabilizers include, for example, organophosphites such as triphenyl phosphite, tris (2, 6-dimethylphenyl) phosphite, tris (mixed mono-and dinonylphenyl) phosphite, and the like; phosphonates such as dimethylbenzene phosphonate or the like; phosphate esters such as trimethyl phosphate and the like; or combinations comprising at least one of the foregoing heat stabilizers.
Light stabilizers and/or ultraviolet light (UV) absorbing additives may be added. Suitable light stabilizers include, for example, benzotriazoles such as 2- (2-hydroxy-5-methylphenyl) benzotriazole, 2- (2-hydroxy-5-tert-octylphenyl) -benzotriazole, and 2-hydroxy-4-n-octyloxybenzophenone, and the like, as well as triazine based ultraviolet light absorbers or combinations comprising at least one of the foregoing light stabilizers.
Suitable UV absorbing additives include, for example, hydroxybenzophenones; hydroxybenzotriazoles; hydroxybenzotriazines; cyanoacrylate esters; oxalyldiphenylamines; benzoxazinones; 2- (2H-benzotriazol-2-yl) -4- (1,1,3, 3-tetramethylbutyl) phenol (CYASORM 5411); 2-hydroxy-4-n-octoxy benzophenone (CYASORM 531); 2- [4, 6-bis (2, 4-dimethylphenyl) -1,3, 5-triazin-2-yl ] -5- (octyloxy) phenol (1164); 2, 2' - (1, 4-phenylene) bis (4H-3, 1-benzoxazin-4-one) (CYASORM UV-3638); 1, 3-bis [ (2-cyano-3, 3-diphenylacryloyl) oxy ] -2, 2-bis [ [ (2-cyano-3, 3-diphenylacryloyl) oxy ] methyl ] propane (uvinlu 3030); nano-sized inorganic materials such as titanium oxide, cerium oxide and zinc oxide, all of which have a particle size of less than 100nm, or the like; or combinations comprising at least one of the foregoing UV absorbers.
The lubricant is at least one selected from stearate lubricants, fatty acid lubricants, stearate lubricants and organic silicon lubricants; the stearate lubricant is at least one selected from calcium stearate, magnesium stearate and zinc stearate; the fatty acid lubricant is at least one selected from fatty acid, fatty acid derivative and fatty acid ester; the stearate lubricant is at least one selected from pentaerythritol stearate; preferably, the lubricant is at least one selected from fatty acid lubricants and stearate lubricants.
The flame retardant can be polyphosphate compounds (ammonium polyphosphate, melamine phosphate, melamine pyrophosphate, melamine polyphosphate and the like), and can also be a bromine-antimony flame retardant system (octabromoether, decabromodiphenylethane, brominated epoxy, brominated polystyrene, antimony-containing compounds and the like).
The preparation method of the polypropylene polyphenylene oxide polystyrene ternary alloy comprises the following steps: adding polypropylene, polyphenyl ether, polystyrene, A-B-A type block copolymer and an auxiliary agent into a high-speed mixer according to the proportion, uniformly mixing, putting into a double-screw extruder, feeding reinforcing fibers laterally, and performing extrusion granulation to obtain the polypropylene, polyphenyl ether and polystyrene ternary alloy, wherein the temperature of each section of the screw is 180-DEG C in the first section and 240-DEG C in the second to ninth sections.
Compared with the prior art, the invention has the following beneficial effects
According to the invention, the polypropylene polyphenylene oxide polystyrene ternary alloy is added with the copolymer of which the A block is styrene and vinyl C4-C12 alkyl aromatic compound and the A-B-A type block copolymer of which the B block is a selective hydrogenated polymer of a conjugated diene compound as the compatible toughening agent, so that compared with the existing A-B-A type toughening agent, the toughness of the alloy can be further improved while good compatibility is ensured. The application range of the polypropylene polyphenyl ether polystyrene ternary alloy is expanded, and the addition of other toughening agents can be reduced.
Detailed Description
The present invention is further illustrated by the following specific examples, which are, however, not intended to limit the scope of the invention.
The preparation methods of the polypropylene polyphenylene oxide polystyrene ternary alloys of the examples and the comparative examples are as follows: adding polypropylene, polyphenyl ether, polystyrene, A-B-A type block copolymer and an auxiliary agent into a high-speed mixer according to the proportion, uniformly mixing, putting into a double-screw extruder, and performing extrusion granulation to obtain the flame-retardant polypropylene polyphenyl ether-polystyrene ternary alloy, wherein the temperature of each section of the screw is 180-DEG C in one zone and 240-DEG C in two to nine zones.
The examples and comparative examples use the following starting materials, without limiting the invention:
polyphenylene ether: PPE LXR 040;
polypropylene: PP HP 550J;
polystyrene: PS 350K;
A-B-A type block copolymer A: the A block is a copolymer of styrene, vinyl C7 linear alkylphenyl, with styrene content of about 76% of the molecular weight of the A block, the B block is a selectively hydrogenated (fully hydrogenated) polyisoprene, the B block is 65% of the total molecular weight of the A-B-A block copolymer, the total molecular weight being about 20 ten thousand;
A-B-A type block copolymer B: the A block is a copolymer of styrene, vinyl C4 linear alkylnaphthyl, wherein the styrene content is about 76% of the molecular weight of the A block, the B block is selectively hydrogenated (fully hydrogenated) polyisoprene, and the B block is 65% of the total molecular weight of the A-B-A block copolymer, the total molecular weight being about 20 ten thousand;
A-B-A type block copolymer C: the A block is a copolymer of styrene, vinyl C4 linear alkylphenyl, with styrene content of about 76% of the molecular weight of the A block, the B block is a selectively hydrogenated (fully hydrogenated) polyisoprene, and the B block is 40% of the total molecular weight of the A-B-A block copolymer, with a total molecular weight of about 20 ten thousand;
A-B-A type block copolymer D: the A block is styrene and the B block is hydrogenated polyisoprene, having a total molecular weight of about 20 million.
A toughening agent: SEBS 6151;
lubricant: silicone lubricant, MB 50-002;
antioxidant: an antioxidant 168/1010;
the performance test method comprises the following steps:
(1) tensile strength: according to ISO 527 standard;
(2) notched impact strength: according to the ISO 180 standard.
Table 1: the proportion (parts by weight) of each component and the results of each performance test in examples and comparative examples
| Example 1 | Example 2 | Example 3 | Example 4 | Example 5 | Example 6 | Comparative example 1 | Comparative example 2 | |
| Polypropylene | 30 | 30 | 30 | 30 | 30 | 30 | 30 | 30 |
| Polyphenylene ether | 60 | 60 | 60 | 60 | 60 | 60 | 60 | 60 |
| Polystyrene | 10 | 10 | 10 | 10 | 10 | 10 | 10 | 10 |
| A-B-A type block copolymer A | 5 | 10 | 18 | 25 | - | - | - | - |
| A-B-A type block copolymer B | - | - | - | - | 10 | - | - | - |
| A-B-A type block copolymer C | - | - | - | - | - | 10 | - | - |
| A-B-A type block copolymer D | - | - | - | - | - | - | 10 | - |
| Toughening agent | - | - | - | - | - | - | - | 10 |
| Lubricant agent | 0.3 | 0.3 | 0.3 | 0.3 | 0.3 | 0.3 | 0.3 | 0.3 |
| Antioxidant agent | 0.4 | 0.4 | 0.4 | 0.4 | 0.4 | 0.4 | 0.4 | 0.4 |
| Tensile strength, MPa | 32 | 30 | 27 | 25 | 31 | 31 | 30 | 32 |
| Notched impact strength, kJ/m2 | 8 | 16 | 25 | 29 | 15 | 12 | 9 | 7 |
As can be seen from examples 1 to 4, the toughness of the product increased with the increase in the amount of the A-B-A type block copolymer.
As can be seen from example 2/5 and comparative examples 1 and 2, SEBS, polystyrene-hydrogenated polyisoprene-polystyrene triblock copolymer commonly used in polypropylene polyphenylene ether-polystyrene terpolymer alloys as toughening agent has a poorer toughening effect than the A-B-A type block copolymer used in the present invention.
Claims (9)
1. The polypropylene polyphenylene oxide-polystyrene ternary alloy is characterized by comprising the following components in parts by weight:
100 parts of polypropylene, polyphenyl ether and polystyrene,
5-25 parts of A-B-A type block copolymer;
in the A-B-A type block copolymer, an A block is a copolymer of styrene and vinyl C4-C12 linear alkyl aromatic compounds, wherein polystyrene accounts for 60-99% of the molecular weight of the A block;
the B block is a selective hydrogenated polymer of a conjugated diene compound, and accounts for 45-80% of the total molecular weight of the A-B-A type block copolymer;
the molecular weight of the A-B-A type block copolymer is 5-30 ten thousand.
2. The polypropylene polyphenylene ether-polystyrene ternary alloy as claimed in claim 1, which comprises the following components in parts by weight:
100 parts of polypropylene, polyphenyl ether and polystyrene,
10-18 parts of A-B-A type block copolymer.
3. The polypropylene polyphenylene ether-polystyrene ternary alloy as claimed in claim 1 or 2, wherein said conjugated diene compound is at least one selected from butadiene and isoprene.
4. The polypropylene polyphenylene ether-polystyrene ternary alloy as claimed in claim 1 or 2, wherein in the vinyl C4-C12 linear alkyl aromatic compound, the C4-C12 alkyl group and vinyl group are respectively positioned at para position of aromatic ring.
5. The polypropylene polyphenylene ether-polystyrene ternary alloy as claimed in claim 1 or 2, wherein in the vinyl C4-C12 alkyl aromatic compound, the aromatic compound is at least one selected from phenyl, naphthyl and phenanthryl.
6. The polypropylene polyphenylene ether-polystyrene ternary alloy as claimed in claim 1 or 2, wherein the polypropylene is 10-60%, the polyphenylene ether is 10-60%, and the polystyrene is 5-30%.
7. The polypropylene polyphenylene ether-polystyrene ternary alloy as claimed in claim 1 or 2, further comprising 0 to 100 parts by weight of a reinforcing fiber; the reinforcing fiber is at least one selected from glass fiber, carbon fiber, metal fiber and whisker.
8. The polypropylene polyphenylene ether-polystyrene ternary alloy as claimed in claim 1 or 2, further comprising 0 to 10 parts by weight of an auxiliary; the auxiliary agent is at least one selected from antioxidant, lubricant, flame retardant, heat stabilizer, light stabilizer and ultraviolet light absorption additive.
9. The method for preparing a polypropylene polyphenylene ether-polystyrene ternary alloy as claimed in claim 8, comprising the steps of: adding polypropylene, polyphenyl ether, polystyrene, A-B-A type block copolymer and an auxiliary agent into a high-speed mixer according to the proportion, uniformly mixing, putting into a double-screw extruder, and performing extrusion granulation to obtain the polypropylene, polyphenyl ether and polystyrene ternary alloy, wherein the temperature of each section of the screw is 180-DEG C in one zone and 240-DEG C in two to nine zones.
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| PCT/CN2020/103917 WO2021036615A1 (en) | 2019-08-29 | 2020-07-24 | Polypropylene-polyphenylene ether-polystyrene ternary alloy and preparation method therefor |
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| CN116178844A (en) * | 2023-03-24 | 2023-05-30 | 湖南恒屹新材料有限公司 | PPE/PP alloy material for compatibilization and toughening and preparation method thereof |
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| JP2004517999A (en) * | 2000-12-28 | 2004-06-17 | ゼネラル・エレクトリック・カンパニイ | Poly (arylene ether) -polyolefin compositions and articles obtained therefrom |
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| CN103788621A (en) * | 2014-01-27 | 2014-05-14 | 上海日之升新技术发展有限公司 | Ultrahigh-CTI (Comparative Tracking Index) halogen-free and flame-retardant polyphenyl ether alloy and preparation method thereof |
| CN104448666A (en) * | 2014-12-26 | 2015-03-25 | 金发科技股份有限公司 | High-toughness PPE/HIPS/PP (Polypheylene Ether/High Impact Polystyrene/Propene Polymer) ternary alloy and preparation as well as application |
| CN109825059B (en) * | 2019-01-11 | 2021-06-01 | 金发科技股份有限公司 | Polypropylene-polyphenylene oxide-polystyrene ternary alloy and preparation method and application thereof |
| CN110527273B (en) * | 2019-08-29 | 2021-11-12 | 金发科技股份有限公司 | Polypropylene-polyphenylene oxide-polystyrene ternary alloy and preparation method thereof |
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| CN1050881A (en) * | 1985-08-16 | 1991-04-24 | 国际壳牌研究有限公司 | Contain the modified block copolymer impact-resistant compositions |
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