CN111548557A - Low-dielectric high-thermal-conductivity polypropylene alloy and preparation method thereof - Google Patents
Low-dielectric high-thermal-conductivity polypropylene alloy and preparation method thereof Download PDFInfo
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- CN111548557A CN111548557A CN202010405413.3A CN202010405413A CN111548557A CN 111548557 A CN111548557 A CN 111548557A CN 202010405413 A CN202010405413 A CN 202010405413A CN 111548557 A CN111548557 A CN 111548557A
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- 239000004743 Polypropylene Substances 0.000 title claims abstract description 75
- 229920001155 polypropylene Polymers 0.000 title claims abstract description 70
- -1 polypropylene Polymers 0.000 title claims abstract description 58
- 239000000956 alloy Substances 0.000 title claims abstract description 44
- 229910045601 alloy Inorganic materials 0.000 title claims abstract description 42
- 238000002360 preparation method Methods 0.000 title abstract description 10
- 229920000106 Liquid crystal polymer Polymers 0.000 claims abstract description 35
- 239000004977 Liquid-crystal polymers (LCPs) Substances 0.000 claims abstract description 35
- 229920000642 polymer Polymers 0.000 claims abstract description 21
- 239000004611 light stabiliser Substances 0.000 claims abstract description 14
- 239000011347 resin Substances 0.000 claims abstract description 11
- 229920005989 resin Polymers 0.000 claims abstract description 11
- 239000003963 antioxidant agent Substances 0.000 claims abstract description 9
- 230000003078 antioxidant effect Effects 0.000 claims abstract description 9
- 239000000314 lubricant Substances 0.000 claims abstract description 7
- 150000004767 nitrides Chemical class 0.000 claims abstract description 7
- 125000001997 phenyl group Chemical group [H]C1=C([H])C([H])=C(*)C([H])=C1[H] 0.000 claims abstract description 7
- 238000000034 method Methods 0.000 claims description 17
- 239000000463 material Substances 0.000 claims description 15
- 238000002156 mixing Methods 0.000 claims description 11
- PLIKAWJENQZMHA-UHFFFAOYSA-N 4-aminophenol Chemical compound NC1=CC=C(O)C=C1 PLIKAWJENQZMHA-UHFFFAOYSA-N 0.000 claims description 10
- IAZDPXIOMUYVGZ-UHFFFAOYSA-N Dimethylsulphoxide Chemical compound CS(C)=O IAZDPXIOMUYVGZ-UHFFFAOYSA-N 0.000 claims description 10
- ADCOVFLJGNWWNZ-UHFFFAOYSA-N antimony trioxide Chemical compound O=[Sb]O[Sb]=O ADCOVFLJGNWWNZ-UHFFFAOYSA-N 0.000 claims description 10
- MVPPADPHJFYWMZ-UHFFFAOYSA-N chlorobenzene Chemical compound ClC1=CC=CC=C1 MVPPADPHJFYWMZ-UHFFFAOYSA-N 0.000 claims description 10
- BWHMMNNQKKPAPP-UHFFFAOYSA-L potassium carbonate Chemical compound [K+].[K+].[O-]C([O-])=O BWHMMNNQKKPAPP-UHFFFAOYSA-L 0.000 claims description 10
- WFDIJRYMOXRFFG-UHFFFAOYSA-N Acetic anhydride Chemical compound CC(=O)OC(C)=O WFDIJRYMOXRFFG-UHFFFAOYSA-N 0.000 claims description 9
- CDAWCLOXVUBKRW-UHFFFAOYSA-N 2-aminophenol Chemical compound NC1=CC=CC=C1O CDAWCLOXVUBKRW-UHFFFAOYSA-N 0.000 claims description 8
- 238000001125 extrusion Methods 0.000 claims description 7
- KKEYFWRCBNTPAC-UHFFFAOYSA-N Terephthalic acid Chemical compound OC(=O)C1=CC=C(C(O)=O)C=C1 KKEYFWRCBNTPAC-UHFFFAOYSA-N 0.000 claims description 6
- RUVINXPYWBROJD-UHFFFAOYSA-N para-methoxyphenyl Natural products COC1=CC=C(C=CC)C=C1 RUVINXPYWBROJD-UHFFFAOYSA-N 0.000 claims description 6
- SCVFZCLFOSHCOH-UHFFFAOYSA-M potassium acetate Chemical compound [K+].CC([O-])=O SCVFZCLFOSHCOH-UHFFFAOYSA-M 0.000 claims description 6
- RUVINXPYWBROJD-ONEGZZNKSA-N trans-anethole Chemical compound COC1=CC=C(\C=C\C)C=C1 RUVINXPYWBROJD-ONEGZZNKSA-N 0.000 claims description 6
- KAUQJMHLAFIZDU-UHFFFAOYSA-N 6-Hydroxy-2-naphthoic acid Chemical compound C1=C(O)C=CC2=CC(C(=O)O)=CC=C21 KAUQJMHLAFIZDU-UHFFFAOYSA-N 0.000 claims description 5
- 238000006243 chemical reaction Methods 0.000 claims description 5
- 229910000027 potassium carbonate Inorganic materials 0.000 claims description 5
- LNETULKMXZVUST-UHFFFAOYSA-N 1-naphthoic acid Chemical compound C1=CC=C2C(C(=O)O)=CC=CC2=C1 LNETULKMXZVUST-UHFFFAOYSA-N 0.000 claims description 4
- CWLKGDAVCFYWJK-UHFFFAOYSA-N 3-aminophenol Chemical compound NC1=CC=CC(O)=C1 CWLKGDAVCFYWJK-UHFFFAOYSA-N 0.000 claims description 4
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 claims description 4
- 239000003054 catalyst Substances 0.000 claims description 4
- 150000002148 esters Chemical group 0.000 claims description 4
- 238000010438 heat treatment Methods 0.000 claims description 4
- HQKMJHAJHXVSDF-UHFFFAOYSA-L magnesium stearate Chemical compound [Mg+2].CCCCCCCCCCCCCCCCCC([O-])=O.CCCCCCCCCCCCCCCCCC([O-])=O HQKMJHAJHXVSDF-UHFFFAOYSA-L 0.000 claims description 4
- UHOVQNZJYSORNB-UHFFFAOYSA-N monobenzene Natural products C1=CC=CC=C1 UHOVQNZJYSORNB-UHFFFAOYSA-N 0.000 claims description 4
- YKSSSKBJDZDZTD-XVNBXDOJSA-N (E)-isoeugenyl benzyl ether Chemical compound COC1=CC(\C=C\C)=CC=C1OCC1=CC=CC=C1 YKSSSKBJDZDZTD-XVNBXDOJSA-N 0.000 claims description 3
- PMZBHPUNQNKBOA-UHFFFAOYSA-N 5-methylbenzene-1,3-dicarboxylic acid Chemical compound CC1=CC(C(O)=O)=CC(C(O)=O)=C1 PMZBHPUNQNKBOA-UHFFFAOYSA-N 0.000 claims description 3
- 235000011056 potassium acetate Nutrition 0.000 claims description 3
- PJISLFCKHOHLLP-UHFFFAOYSA-N 2-diethoxyphosphorylsulfanyl-n,n-diethylethanamine Chemical compound CCOP(=O)(OCC)SCCN(CC)CC PJISLFCKHOHLLP-UHFFFAOYSA-N 0.000 claims description 2
- 229940018563 3-aminophenol Drugs 0.000 claims description 2
- YLKCHWCYYNKADS-UHFFFAOYSA-N 5-hydroxynaphthalene-1-sulfonic acid Chemical compound C1=CC=C2C(O)=CC=CC2=C1S(O)(=O)=O YLKCHWCYYNKADS-UHFFFAOYSA-N 0.000 claims description 2
- 229910052582 BN Inorganic materials 0.000 claims description 2
- PZNSFCLAULLKQX-UHFFFAOYSA-N Boron nitride Chemical compound N#B PZNSFCLAULLKQX-UHFFFAOYSA-N 0.000 claims description 2
- ZFMSMUAANRJZFM-UHFFFAOYSA-N Estragole Chemical compound COC1=CC=C(CC=C)C=C1 ZFMSMUAANRJZFM-UHFFFAOYSA-N 0.000 claims description 2
- 239000005662 Paraffin oil Substances 0.000 claims description 2
- JKIJEFPNVSHHEI-UHFFFAOYSA-N Phenol, 2,4-bis(1,1-dimethylethyl)-, phosphite (3:1) Chemical compound CC(C)(C)C1=CC(C(C)(C)C)=CC=C1OP(OC=1C(=CC(=CC=1)C(C)(C)C)C(C)(C)C)OC1=CC=C(C(C)(C)C)C=C1C(C)(C)C JKIJEFPNVSHHEI-UHFFFAOYSA-N 0.000 claims description 2
- BGYHLZZASRKEJE-UHFFFAOYSA-N [3-[3-(3,5-ditert-butyl-4-hydroxyphenyl)propanoyloxy]-2,2-bis[3-(3,5-ditert-butyl-4-hydroxyphenyl)propanoyloxymethyl]propyl] 3-(3,5-ditert-butyl-4-hydroxyphenyl)propanoate Chemical compound CC(C)(C)C1=C(O)C(C(C)(C)C)=CC(CCC(=O)OCC(COC(=O)CCC=2C=C(C(O)=C(C=2)C(C)(C)C)C(C)(C)C)(COC(=O)CCC=2C=C(C(O)=C(C=2)C(C)(C)C)C(C)(C)C)COC(=O)CCC=2C=C(C(O)=C(C=2)C(C)(C)C)C(C)(C)C)=C1 BGYHLZZASRKEJE-UHFFFAOYSA-N 0.000 claims description 2
- CJZGTCYPCWQAJB-UHFFFAOYSA-L calcium stearate Chemical compound [Ca+2].CCCCCCCCCCCCCCCCCC([O-])=O.CCCCCCCCCCCCCCCCCC([O-])=O CJZGTCYPCWQAJB-UHFFFAOYSA-L 0.000 claims description 2
- 235000013539 calcium stearate Nutrition 0.000 claims description 2
- 239000008116 calcium stearate Substances 0.000 claims description 2
- 238000001816 cooling Methods 0.000 claims description 2
- PMHQVHHXPFUNSP-UHFFFAOYSA-M copper(1+);methylsulfanylmethane;bromide Chemical compound Br[Cu].CSC PMHQVHHXPFUNSP-UHFFFAOYSA-M 0.000 claims description 2
- 238000001035 drying Methods 0.000 claims description 2
- BDAGIHXWWSANSR-UHFFFAOYSA-N formic acid Substances OC=O BDAGIHXWWSANSR-UHFFFAOYSA-N 0.000 claims description 2
- IUSBVFZKQJGVEP-SNAWJCMRSA-N isoeugenol acetate Chemical compound COC1=CC(\C=C\C)=CC=C1OC(C)=O IUSBVFZKQJGVEP-SNAWJCMRSA-N 0.000 claims description 2
- 239000011777 magnesium Substances 0.000 claims description 2
- 229910052749 magnesium Inorganic materials 0.000 claims description 2
- 235000019359 magnesium stearate Nutrition 0.000 claims description 2
- 239000000155 melt Substances 0.000 claims description 2
- SSDSCDGVMJFTEQ-UHFFFAOYSA-N octadecyl 3-(3,5-ditert-butyl-4-hydroxyphenyl)propanoate Chemical compound CCCCCCCCCCCCCCCCCCOC(=O)CCC1=CC(C(C)(C)C)=C(O)C(C(C)(C)C)=C1 SSDSCDGVMJFTEQ-UHFFFAOYSA-N 0.000 claims description 2
- 239000003921 oil Substances 0.000 claims description 2
- IAAKNVCARVEIFS-UHFFFAOYSA-M sodium;4-hydroxynaphthalene-1-sulfonate Chemical compound [Na+].C1=CC=C2C(O)=CC=C(S([O-])(=O)=O)C2=C1 IAAKNVCARVEIFS-UHFFFAOYSA-M 0.000 claims description 2
- 239000002904 solvent Substances 0.000 claims description 2
- XOLBLPGZBRYERU-UHFFFAOYSA-N tin dioxide Chemical compound O=[Sn]=O XOLBLPGZBRYERU-UHFFFAOYSA-N 0.000 claims description 2
- 229910001887 tin oxide Inorganic materials 0.000 claims description 2
- IUSBVFZKQJGVEP-UHFFFAOYSA-N trans-isoeugenol acetate Natural products COC1=CC(C=CC)=CC=C1OC(C)=O IUSBVFZKQJGVEP-UHFFFAOYSA-N 0.000 claims description 2
- 239000011787 zinc oxide Substances 0.000 claims description 2
- XOOUIPVCVHRTMJ-UHFFFAOYSA-L zinc stearate Chemical compound [Zn+2].CCCCCCCCCCCCCCCCCC([O-])=O.CCCCCCCCCCCCCCCCCC([O-])=O XOOUIPVCVHRTMJ-UHFFFAOYSA-L 0.000 claims description 2
- 239000011159 matrix material Substances 0.000 abstract description 5
- 239000002994 raw material Substances 0.000 description 17
- 239000000203 mixture Substances 0.000 description 8
- 230000000052 comparative effect Effects 0.000 description 7
- 238000007792 addition Methods 0.000 description 6
- 238000009472 formulation Methods 0.000 description 6
- 102100035182 Plastin-2 Human genes 0.000 description 5
- 101710081231 Plastin-2 Proteins 0.000 description 5
- 239000003365 glass fiber Substances 0.000 description 5
- 230000004048 modification Effects 0.000 description 5
- 238000012986 modification Methods 0.000 description 5
- 239000000047 product Substances 0.000 description 4
- 238000010998 test method Methods 0.000 description 4
- 239000012752 auxiliary agent Substances 0.000 description 3
- 238000004891 communication Methods 0.000 description 3
- 239000008367 deionised water Substances 0.000 description 3
- 229910021641 deionized water Inorganic materials 0.000 description 3
- 238000003756 stirring Methods 0.000 description 3
- 238000012360 testing method Methods 0.000 description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 2
- 239000002131 composite material Substances 0.000 description 2
- 239000003989 dielectric material Substances 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- VTHJTEIRLNZDEV-UHFFFAOYSA-L magnesium dihydroxide Chemical class [OH-].[OH-].[Mg+2] VTHJTEIRLNZDEV-UHFFFAOYSA-L 0.000 description 2
- 238000011056 performance test Methods 0.000 description 2
- 230000008569 process Effects 0.000 description 2
- 230000009467 reduction Effects 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- VYRBHKNXUFOBGW-UHFFFAOYSA-N 1-(methoxymethoxy)-4-prop-2-enylbenzene Chemical compound COCOC1=CC=C(CC=C)C=C1 VYRBHKNXUFOBGW-UHFFFAOYSA-N 0.000 description 1
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 1
- 239000006087 Silane Coupling Agent Substances 0.000 description 1
- 238000006640 acetylation reaction Methods 0.000 description 1
- 230000002411 adverse Effects 0.000 description 1
- 125000003342 alkenyl group Chemical group 0.000 description 1
- 125000003118 aryl group Chemical group 0.000 description 1
- 239000012298 atmosphere Substances 0.000 description 1
- 238000005452 bending Methods 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000006227 byproduct Substances 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 238000003889 chemical engineering Methods 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 239000011231 conductive filler Substances 0.000 description 1
- 229920001577 copolymer Polymers 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000004821 distillation Methods 0.000 description 1
- 229920006351 engineering plastic Polymers 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 230000002349 favourable effect Effects 0.000 description 1
- 238000011049 filling Methods 0.000 description 1
- 238000001914 filtration Methods 0.000 description 1
- 230000036541 health Effects 0.000 description 1
- 230000017525 heat dissipation Effects 0.000 description 1
- 230000009878 intermolecular interaction Effects 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 239000004973 liquid crystal related substance Substances 0.000 description 1
- 239000000347 magnesium hydroxide Substances 0.000 description 1
- 229910001862 magnesium hydroxide Inorganic materials 0.000 description 1
- 125000000956 methoxy group Chemical group [H]C([H])([H])O* 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 239000012299 nitrogen atmosphere Substances 0.000 description 1
- 238000005580 one pot reaction Methods 0.000 description 1
- 238000004806 packaging method and process Methods 0.000 description 1
- 238000005191 phase separation Methods 0.000 description 1
- 238000012545 processing Methods 0.000 description 1
- 239000012744 reinforcing agent Substances 0.000 description 1
- 230000003014 reinforcing effect Effects 0.000 description 1
- 239000000377 silicon dioxide Substances 0.000 description 1
- 235000012239 silicon dioxide Nutrition 0.000 description 1
- 229920002994 synthetic fiber Polymers 0.000 description 1
- 229920001169 thermoplastic Polymers 0.000 description 1
- 239000004416 thermosoftening plastic Substances 0.000 description 1
- 239000012745 toughening agent Substances 0.000 description 1
- 238000001291 vacuum drying Methods 0.000 description 1
- 238000005406 washing Methods 0.000 description 1
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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
- C08L23/00—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers
- C08L23/02—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers not modified by chemical after-treatment
- C08L23/10—Homopolymers or copolymers of propene
- C08L23/14—Copolymers of propene
-
- 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
- C08G69/00—Macromolecular compounds obtained by reactions forming a carboxylic amide link in the main chain of the macromolecule
- C08G69/44—Polyester-amides
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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
- C08L23/00—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers
- C08L23/02—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers not modified by chemical after-treatment
- C08L23/10—Homopolymers or copolymers of propene
- C08L23/12—Polypropene
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- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
- C09K5/00—Heat-transfer, heat-exchange or heat-storage materials, e.g. refrigerants; Materials for the production of heat or cold by chemical reactions other than by combustion
- C09K5/08—Materials not undergoing a change of physical state when used
- C09K5/14—Solid materials, e.g. powdery or granular
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K3/00—Use of inorganic substances as compounding ingredients
- C08K3/28—Nitrogen-containing compounds
- C08K2003/282—Binary compounds of nitrogen with aluminium
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- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K3/00—Use of inorganic substances as compounding ingredients
- C08K3/38—Boron-containing compounds
- C08K2003/382—Boron-containing compounds and nitrogen
- C08K2003/385—Binary compounds of nitrogen with boron
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- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K2201/00—Specific properties of additives
- C08K2201/011—Nanostructured additives
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- 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
- C08L2205/02—Polymer mixtures characterised by other features containing two or more polymers of the same C08L -group
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- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
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- C08L2205/00—Polymer mixtures characterised by other features
- C08L2205/02—Polymer mixtures characterised by other features containing two or more polymers of the same C08L -group
- C08L2205/025—Polymer mixtures characterised by other features containing two or more polymers of the same C08L -group containing two or more polymers of the same hierarchy C08L, and differing only in parameters such as density, comonomer content, molecular weight, structure
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- 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
Abstract
The invention provides a low-dielectric high-thermal-conductivity polypropylene alloy and a preparation method thereof, wherein the polypropylene alloy is prepared from the following components in parts by mass: 54-84 parts of polypropylene resin, preferably 59-74 parts, 10-30 parts of liquid crystal polymer, preferably 10-20 parts, 5-20 parts of nano nitride, preferably 5-10 parts, 0-1 part of antioxidant, preferably 0.2-0.6 part, 0-1 part of light stabilizer, preferably 0.2-0.4 part, and 0-1 part of lubricant, preferably 0.2-0.4 part; the liquid crystal polymer is a modified LCP with double bonds and benzene rings on a polymer branched chain, and the repeating unit of the branched chain is more than or equal to 1. The compatibility of the modified LCP with PP is enhanced, the molecular chain spacing is increased by utilizing the large benzene ring structure on the LCP branched chain, and the molecular free volume is improved, so that the dielectric constant and the dielectric loss of a matrix are reduced, and the alloy has excellent dielectric property and mechanical strength.
Description
Technical Field
The invention relates to a polypropylene alloy, in particular to a low-dielectric high-thermal conductivity polypropylene alloy and a preparation method thereof.
Background
Polypropylene (PP) is a thermoplastic synthetic material with excellent performance, and has wide application in the fields of automobiles, household electrical appliances, food packaging and medical treatment and health care. In order to enhance the mechanical strength of PP, the prior art often modifies the PP by adding polar substances to generate PP alloy with wider application range, but the modification of the polar substances can cause the dielectric constant of the alloy material to be obviously increased, and the industrial requirement of the low dielectric material can not be met, such as the 5G communication industry. The liquid crystal polymer is a novel special engineering plastic, and the molecules in the liquid crystal phase have a high-degree orientation structure under specific conditions, so that the material is endowed with excellent mechanical property and heat resistance, and therefore, the addition of the liquid crystal polymer to modify a PP material is a new idea for preparing a novel modified PP alloy. However, the liquid crystal polymer and PP are incompatible systems, phase separation is easy to occur in the processing process, and the problem that the dielectric constant of PP alloy is obviously increased cannot be solved by conventional addition; in addition, with the application of low dielectric materials in the field of high-frequency communication, the good heat dissipation capacity of the PP alloy plays a key role in the normal operation of equipment.
Patent CN106543554A discloses a glass fiber reinforced polypropylene material with low dielectric constant and a preparation method thereof, wherein the polypropylene composite material has a low dielectric constant by using low dielectric glass fiber as a reinforcing agent and doping a certain amount of silicon dioxide. However, the reinforcing effect of the low dielectric glass fiber on polypropylene is far inferior to that of the common glass fiber, and the polypropylene reinforced by the low dielectric glass fiber cannot simultaneously meet the use requirements of low dielectric and high strength.
The patent CN109251419A discloses a high-thermal-conductivity-coefficient polypropylene modified material and a preparation method thereof, the high-thermal-conductivity-coefficient polypropylene modified material is composed of polypropylene, a toughening agent, a compatilizer, modified magnesium hydroxide, a lubricant and an antioxidant, and silane coupling agent is used for carrying out surface modification on the magnesium hydroxide, so that the thermal conductivity of the polypropylene is improved. However, the dielectric property and the heat conductivity are two factors that are mutually restricted, and the introduction of the heat conductive filler with high filling content tends to increase the dielectric constant of the material, thereby bringing adverse effects.
The prior art can not well solve the requirements of low dielectric and high thermal conductivity of the PP material, and related reports about the low dielectric and high thermal conductivity PP composite material at home and abroad are few, so that a new process and technology are urgently needed to be developed to make up for the defects of the prior art.
Disclosure of Invention
The invention provides a low-dielectric high-thermal-conductivity polypropylene alloy and a preparation method thereof. The compatibility of the modified LCP with PP is enhanced, the molecular chain spacing is increased by utilizing the large benzene ring structure on the LCP branched chain, and the molecular free volume is improved, so that the dielectric constant and the dielectric loss of a matrix are reduced, and the alloy has excellent dielectric property and mechanical strength.
In order to achieve the purpose, the technical scheme adopted by the invention is as follows:
the low-dielectric high-thermal-conductivity polypropylene alloy is characterized by being prepared from the following components in parts by mass:
the liquid crystal polymer is a modified LCP with double bonds and benzene rings on polymer branched chains, and the repeating unit of the branched chains is more than or equal to 1, preferably the mesh number is 800-3000. The interface compatibility of LCP and PP can be improved by double bond modification, the benzene ring structure is favorable for increasing the molecular chain distance, reducing the dielectric constant and dielectric loss of a matrix, and meeting the use requirements of the dielectric property and mechanical strength of the alloy.
Further, the polypropylene resin is one or more of high-flow homopolymerized PP, high-flow copolymerized PP and high-flow high-impact PP, and the high-flow copolymerized PP is preferred.
Further, the melt index of the polypropylene resin is 30-1800g/10 min. The high-fluidity polypropylene resin is adopted, so that the wrapping property of the resin on the surface of a liquid crystal polymer can be improved, the dispersity of the resin in a matrix is further improved, and the polypropylene alloy has excellent mechanical properties.
Further, the preparation method of the liquid crystal polymer comprises the following steps:
1) under the atmosphere of nitrogen, mixing and heating naphthoic acid, aminophenol, acetic anhydride, potassium acetate, 5-methyl isophthalic acid and terephthalic acid, firstly carrying out acetylation reaction, and then adding an ester exchange catalyst for continuous reaction to generate a polymer LCP; the preparation of the polymer can be carried out by reference to the method in One-pot synthesis of soluble porous aromatic liquid copolymers (ester amides) with high thermal and dimensional stability [ Chemical Engineering Communications,2019:1-10 ]. Taking the reaction raw materials in the following formula as an example, the reaction expression of the step is as follows:
2) blending and heating the polymer LCP, methoxy alkenyl benzene compounds, dimethyl sulfoxide and potassium carbonate in a chlorobenzene solvent to prepare the liquid crystal polymer; taking the methoxy alkenylbenzene compound as 1-methoxy-4- (1-propenyl) benzene as an example, the reaction expression is shown as the following formula:
preferably, the methoxy alkenyl benzene compound is one or more of 1-methoxy-4- (1-propenyl) benzene, 1-benzyloxy-2-methoxy-4-propenyl benzene, 1- (methoxy) -4- (2-propen-1-yl) benzene and acetyl isoeugenol, and preferably 1-methoxy-4- (1-propenyl) benzene.
Further, the naphthoic acid is one or more of 6-hydroxy-2-naphthoic acid, 1-naphthol-2-formic acid, 1-naphthol-4-sulfonic acid and 1-naphthol-5-sulfonic acid, preferably 6-hydroxy-2-naphthoic acid;
preferably, the aminophenol is one or more of o-aminophenol, m-aminophenol, p-aminophenol, preferably p-aminophenol;
preferably, the ester exchange catalyst is one or more of antimony trioxide, tin oxide and zinc oxide, and antimony trioxide is preferred.
Further, the nano nitride has a rod-like structure, preferably one or more of boron nitride, aluminum nitride and magnesium nitride having a rod-like structure. The nano nitride with the rod-shaped structure has higher length-diameter ratio, can form a heat conduction channel with liquid crystal polymers, and can play a better heat conduction effect under the condition of low addition amount, thereby reducing the influence of the auxiliary agent on the dielectric property of the alloy and overcoming the problem that the dielectric property and the heat conduction property are mutually restricted due to the addition of a large amount of the auxiliary agent in the prior art.
Further, the antioxidant is one or more of antioxidant 1010, antioxidant 168, antioxidant 1076 and antioxidant DSDP.
Further, the light stabilizer is one or more of light stabilizer 5585, light stabilizer 5589, light stabilizer 234 and light stabilizer 770.
Further, the lubricant is one or more of zinc stearate, calcium stearate, magnesium stearate, white oil and paraffin oil.
A preparation method of a low-dielectric high-thermal-conductivity polypropylene alloy comprises the following steps:
a. mixing polypropylene resin, nano nitride, antioxidant, light stabilizer and lubricant in a high-speed mixer for 10-30 minutes to uniformly disperse the components;
b. adding the mixed material into a main feed of a double-screw extruder, adding liquid crystal polymer into a side feed, performing melt extrusion at the temperature of 140-;
c. and cooling, granulating and drying the extruded material to obtain the polypropylene alloy.
Compared with the prior art, the invention has the following technical advantages:
1) according to the invention, the PP alloy is prepared by taking the rodlike nano nitride as an auxiliary agent, and can form a heat conduction path with liquid crystal polymers, so that the heat conduction performance of the material is obviously improved;
2) the liquid crystal polymer is modified by methoxy alkenyl benzene compounds, so that the liquid crystal polymer has an end alkenyl structure to improve the compatibility with a PP material, and the introduced benzene ring structure has larger steric hindrance to increase the distance between molecular chains, thereby improving the free volume of a matrix and further reducing the dielectric constant of the material;
3) the polypropylene alloy disclosed by the invention not only has lower dielectric property and good heat-conducting property, but also has lighter mass and good mechanical property, and is beneficial to popularization and application of the alloy material in a wider market environment.
Drawings
FIG. 1 is a graph of the shear viscosity trend of the polymers prepared in the examples as a function of frequency.
Detailed Description
The invention is further illustrated by the accompanying drawings and specific examples, which are given by way of illustration only and do not limit the scope of the invention.
In each of the examples and comparative examples, the main raw material sources were as follows:
other raw materials and reagents were obtained from commercial sources unless otherwise specified.
In each example and comparative example, the performance test parameters and corresponding test methods for PP alloys were as follows:
| content of test | Unit of | Test method |
| Tensile strength | MPa | ISO 527 |
| Bending strength | MPa | ISO 178 |
| Flexural modulus | MPa | ISO 178 |
| Notched impact strength | KJ/m2 | ISO 180 |
| Heat distortion temperature (0.45N/mm)2) | ℃ | ISO 75/B |
| Dielectric constant | 2.5GHz | Resonant cavity method single point test |
| Dielectric loss | 2.5GHz | Resonant cavity method single point test |
| Coefficient of thermal conductivity | w/m.k | GB/T 3399-1982 |
Polymer viscosity test method: the polymer was dissolved in N-methylpyrrolidone at a mass concentration of 30%, and the shear viscosity of the polymer as a function of frequency was measured by means of a rotational rheometer (TA Instruments AR2000) and plotted to give a viscosity trend graph.
[ example 1 ]
(1) Preparing liquid crystal polymer:
putting 188g of 6-hydroxy-2-naphthoic acid, 109g of p-aminophenol, 176g of 5-methyl isophthalic acid and 166g of terephthalic acid into a three-neck flask, adding 0.5g of acetic anhydride and 0.5g of potassium acetate, and reacting for 1h at 150 ℃ in a nitrogen atmosphere; then adding 1g of antimony trioxide, gradually raising the temperature to 300 ℃, reacting for 2 hours, continuously removing by-products by a distillation method, filtering and washing to obtain a polymer A; 2) 100g of polymer A, 10g of 1-methoxy-4- (1-propenyl) benzene, 1g of potassium carbonate and 1g of dimethyl sulfoxide are put into a three-neck flask, 50g of chlorobenzene is added, stirring is continuously carried out at 80 ℃ for 20 hours, the product is repeatedly washed by deionized water, and vacuum drying is carried out, so as to obtain the liquid crystal polymer LCP-1. The viscosity change trend of the polymer A and the LCP-1 is shown in figure 1, after rigid short-chain groups are introduced into LCP branched chains, the intermolecular distance is increased, the intermolecular interaction force is weakened, and the shear viscosity is obviously reduced.
(2) LCP-1 and the formula components in the table 1 are used as raw materials, and the polypropylene alloy is prepared according to the following method by referring to the raw material dosage in the table 1:
uniformly mixing polypropylene resin, nano nitride, an antioxidant, a light stabilizer and a lubricant in a high-speed mixer to obtain a blend, wherein the mixing speed is set to be 60rpm, the mixing time is set to be 10 minutes, and the mixing temperature is set to be 50 ℃;
secondly, adding the blend through a main feeding port of a double-screw extruder, adding liquid crystal polymer through a side feeding port of the double screw extruder, and fully mixing two materials in the double-screw extruder, wherein the extrusion conditions are as follows: the rotating speed of the screw is 600rpm, and the temperature of the screw is set from the feed opening to the machine head in a segmented mode as follows: 140 ℃, 155 ℃, 180 ℃, 210 ℃, 220 ℃, 225 ℃, 220 ℃ and 210 ℃ to obtain the polypropylene alloy.
[ example 2 ]
(1) Preparing liquid crystal polymer:
polymer A was prepared according to the method of example 1. Then, 100g of polymer A, 10g of 1-benzyloxy-2-methoxy-4-propenyl benzene, 1g of potassium carbonate and 1g of dimethyl sulfoxide are put into a three-neck flask, 100g of chlorobenzene is added, stirring is continuously carried out at 80 ℃ for 20 hours, and the product is repeatedly washed by deionized water and dried in vacuum, so that liquid crystal polymer which is recorded as LCP-2 is obtained. The viscosity of LCP-2 showed a trend as shown in FIG. 1, with a significant reduction in shear viscosity compared to Polymer A.
(2) The polypropylene alloy was prepared according to the method of example 1 using LCP-2 and the formulation components in table 1 as raw materials and referring to the amounts of the raw materials in table 1, except that the extrusion conditions of the twin-screw extruder were: the screw rotation speed is 750rpm, and the screw temperature is set from the feed opening to the machine head in a segmented mode as follows: 140 deg.C, 155 deg.C, 180 deg.C, 210 deg.C, 230 deg.C, 235 deg.C, 230 deg.C.
[ example 3 ]
(1) Preparing liquid crystal polymer:
polymer A was prepared according to the method of example 1. Then, 100g of polymer A, 10g of 1- (methoxymethoxy) -4- (2-propen-1-yl) benzene, 1g of potassium carbonate and 1g of dimethyl sulfoxide were taken and placed in a three-necked flask, 50g of chlorobenzene was added, stirring was continued at 80 ℃ for 20 hours, and the product was repeatedly washed with deionized water and vacuum-dried to obtain a liquid crystal polymer, which was designated as LCP-3. The viscosity of LCP-3 shows a trend as shown in FIG. 1, with a significant reduction in shear viscosity compared to Polymer A.
(2) The polypropylene alloy was prepared according to the method of example 1 using LCP-3 and the formulation components in table 1 as raw materials and referring to the amounts of the raw materials in table 1, except that the extrusion conditions of the twin-screw extruder were: the screw rotating speed is 900rpm, and the screw temperature is set from the feed opening to the machine head in a segmented mode as follows: 140 deg.C, 155 deg.C, 180 deg.C, 220 deg.C, 240 deg.C, 245 deg.C, 240 deg.C.
[ example 4 ]
The LCP-1 prepared in example 1 was used as a raw material, and a polypropylene alloy was prepared according to the method in example 1, except that the formulation and the amount of the raw material in table 1 were different, and the extrusion conditions of the twin-screw extruder were: the screw rotation speed is 750rpm, and the screw temperature is set from the feed opening to the machine head in a segmented mode as follows: 140 deg.C, 155 deg.C, 180 deg.C, 210 deg.C, 230 deg.C, 235 deg.C, 230 deg.C.
[ example 5 ]
The LCP-1 prepared in example 1 was used as a raw material, and a polypropylene alloy was prepared according to the method in example 1, except that the formulation and the amount of the raw material in table 1 were different, and the extrusion conditions of the twin-screw extruder were: the screw rotating speed is 900rpm, and the screw temperature is set from the feed opening to the machine head in a segmented mode as follows: 140 deg.C, 155 deg.C, 180 deg.C, 220 deg.C, 240 deg.C, 245 deg.C, 240 deg.C.
Comparative example 1
A polypropylene alloy was prepared from a commercially available liquid crystal polymer E6008 as a raw material by the method of example 1, except for the formulation and the amounts of the raw materials shown in Table 1.
Comparative example 2
The polypropylene alloy was prepared according to the method and formulation of example 1, except that the liquid crystal polymer and the nano-nitride were not added to the raw materials.
TABLE 1 raw materials and amounts used in examples 1-5(S1-S5) and comparative examples 1-2(D1-D2)
The mechanical properties, dielectric properties and thermal conductivity of the polypropylene alloys prepared in the examples and comparative examples were measured, and the results are shown in table 2.
TABLE 2 product Performance test results for examples 1-5(S1-S5) and comparative examples 1-2(D1-D2)
| Test method | S1 | S2 | S3 | S4 | S5 | D1 | D2 |
| Tensile Strength (MPa) | 48 | 77 | 103 | 96 | 118 | 36 | 24 |
| Flexural Strength (MPa) | 52 | 75 | 127 | 116 | 134 | 45 | 35 |
| Flexural modulus (MPa) | 4800 | 6700 | 8500 | 7300 | 9300 | 2600 | 1500 |
| Notched impact strength at ambient temperature (KJ/m)2) | 21.3 | 35.1 | 42.7 | 32.6 | 58.5 | 11.5 | 5.6 |
| Dielectric constant | 2.25 | 2.28 | 2.32 | 2.41 | 2.34 | 2.69 | 2.30 |
| Dielectric loss (10)-3) | 1.12 | 1.18 | 1.23 | 1.35 | 1.22 | 4.31 | 1.21 |
| Thermal conductivity/lambda | 2.3 | 2.5 | 2.9 | 2.7 | 2.1 | 0.9 | 0.3 |
| HDT(℃) | 130 | 147 | 150 | 150 | 155 | 130 | 90 |
The above description is only a preferred embodiment of the present invention, and it should be noted that, for those skilled in the art, several modifications and additions can be made without departing from the method of the present invention, and these modifications and additions should also be regarded as the protection scope of the present invention.
Claims (10)
1. The low-dielectric high-thermal-conductivity polypropylene alloy is characterized by being prepared from the following components in parts by mass:
the liquid crystal polymer is a modified LCP with double bonds and benzene rings on a polymer branched chain, and the repeating unit of the branched chain is more than or equal to 1.
2. The polypropylene alloy with low dielectric constant and high thermal conductivity as claimed in claim 1, wherein the polypropylene resin is one or more of high flow homopolymerized PP, high flow copolymerized PP and high flow high impact PP, preferably high flow copolymerized PP.
3. The polypropylene alloy with low dielectric constant and high thermal conductivity as claimed in claim 2, wherein the polypropylene resin has a melt index of 30-1800g/10 min.
4. The polypropylene alloy with low dielectric constant and high thermal conductivity as claimed in any one of claims 1 to 3, wherein the liquid crystal polymer is prepared by the following steps:
1) mixing and heating naphthoic acid, aminophenol, acetic anhydride, potassium acetate, 5-methyl isophthalic acid and terephthalic acid, and adding an ester exchange catalyst for continuous reaction to generate a polymer LCP;
2) blending and heating the polymer LCP, methoxy alkenyl benzene compounds, dimethyl sulfoxide and potassium carbonate in a chlorobenzene solvent to prepare the liquid crystal polymer;
preferably, the methoxy alkenyl benzene compound is one or more of 1-methoxy-4- (1-propenyl) benzene, 1-benzyloxy-2-methoxy-4-propenyl benzene, 1- (methoxy) -4- (2-propen-1-yl) benzene and acetyl isoeugenol, and preferably 1-methoxy-4- (1-propenyl) benzene.
5. The polypropylene alloy with low dielectric constant and high thermal conductivity as claimed in claim 4, wherein the naphthoic acid is one or more of 6-hydroxy-2-naphthoic acid, 1-naphthol-2-formic acid, 1-naphthol-4-sulfonic acid and 1-naphthol-5-sulfonic acid, preferably 6-hydroxy-2-naphthoic acid;
preferably, the aminophenol is one or more of o-aminophenol, m-aminophenol, p-aminophenol, preferably p-aminophenol;
preferably, the ester exchange catalyst is one or more of antimony trioxide, tin oxide and zinc oxide, and antimony trioxide is preferred.
6. The polypropylene alloy with low dielectric and high thermal conductivity according to any one of claims 1 to 5, wherein the nano-nitride has a rod-like structure, preferably one or more of boron nitride, aluminum nitride and magnesium nitride having a rod-like structure.
7. The polypropylene alloy with low dielectric constant and high thermal conductivity of any one of claims 1 to 6, wherein the antioxidant is one or more of antioxidant 1010, antioxidant 168, antioxidant 1076, and antioxidant DSDP.
8. The polypropylene alloy with low dielectric constant and high thermal conductivity as claimed in any one of claims 1 to 7, wherein the light stabilizer is one or more of light stabilizer 5585, light stabilizer 5589, light stabilizer 234 and light stabilizer 770.
9. The polypropylene alloy of any one of claims 1 to 8, wherein the lubricant is one or more of zinc stearate, calcium stearate, magnesium stearate, white oil, and paraffin oil.
10. A method for preparing the polypropylene alloy with low dielectric constant and high thermal conductivity as defined in any one of claims 1 to 9, comprising the steps of:
a. mixing polypropylene resin, nano nitride, antioxidant, light stabilizer and lubricant in a high-speed mixer, and uniformly dispersing;
b. adding the mixed material into a main feed of a double-screw extruder, adding liquid crystal polymer into a side feed, performing melt extrusion at the temperature of 140-;
c. and cooling, granulating and drying the extruded material to obtain the polypropylene alloy.
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| CN113717465A (en) * | 2021-08-19 | 2021-11-30 | 金旸（厦门）新材料科技有限公司 | Low-dielectric-constant high-weather-resistance polypropylene composite material and preparation method thereof |
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