Heat-conducting and insulating packaging material and preparation method thereof

Abstract

The invention relates to the technical field of high polymer materials, and discloses a heat-conducting and insulating packaging material and a preparation method thereof. The preparation method comprises the following steps: compounding alkenyl carbon nanotubes and a nano aluminum nitride / ethylene propylene diene monomer composite material to obtain a heat-conducting additive; the preparation method comprises the following steps: uniformly mixing a polyolefin elastomer, ethylene propylene diene monomer, a tackifier gamma-methacryloxypropyltrimethoxysilane, styrene, an antioxidant, a light stabilizer, a heat-conducting additive and an initiator tert-butylperoxycarbonic acid-2-ethylhexyl ester, and vulcanizing to obtain the heat-conducting and insulating packaging material. The packaging material has excellent heat-conducting property and insulating property, and is good in adhesive property.

Description

Technical Field

[0001] The invention relates to the technical field of polymer materials, and in particular to a thermally conductive insulating packaging material and a preparation method thereof. Background Art

[0002] Packaging materials play a vital role in protecting components from environmental factors and ensuring stable operation of components. The main packaging materials currently include: ethylene-vinyl acetate copolymer, silicone resin, polyvinyl butyral, thermoplastic polyolefins and other materials. Among polyolefin materials, polyolefin elastomer is a thermoplastic elastomer obtained by copolymerizing α-hydrocarbons and polyolefins using metallocene as a catalyst. Since its molecular chain is a saturated olefin, it has excellent aging resistance; the main chain of EPDM rubber is composed of chemically stable saturated hydrocarbons, but contains unsaturated double bonds in the side chains. The molecules have no polar substituents, low intermolecular cohesive energy, extremely high chemical stability, good water resistance and aging resistance, and excellent electrical insulation and corona resistance.

[0003] Existing technologies such as Chinese patent CN102516674A disclose a thermally conductive EPDM rubber composite material and a preparation method thereof; the thermal conductivity of the composite material is improved by adding a thermally conductive additive to the EPDM rubber matrix; however, since the prepared composite material has low insulation properties and the EPDM rubber itself has poor bonding strength, the application of the material is limited. Summary of the invention

[0004] The purpose of the present invention is to overcome the deficiencies of the prior art and provide a thermally conductive insulating packaging material and a preparation method thereof, wherein the packaging material has excellent thermal conductivity and insulating properties and good bonding properties.

[0005] In order to achieve the above object, the technical solution adopted by the present invention is as follows:

[0006] A method for preparing a thermally conductive insulating packaging material comprises the following steps:

[0007] Step (1), mixing alkenyl carbon nanotubes and nano aluminum nitride / ethylene propylene diene monomer rubber composite material to obtain a thermal conductive additive;

[0008] Wherein, the olefin-based carbon nanotubes are prepared by the following steps:

[0009] S11, mixing carboxylated carbon nanotubes, dicyclohexylcarbodiimide, and ethylenediamine, ultrasonically dispersing, reacting, and after the reaction is completed, filtering, washing, and drying to obtain amino carbon nanotubes; mixing amino carbon nanotubes, 3,5-diaminobenzoic acid, pyridine, triphenyl phosphite, and N-methylpyrrolidone, reacting, and after the reaction is completed, filtering, washing, and drying to obtain hyperbranched polymer modified carbon nanotubes;

[0010] S12, mixing the hyperbranched polymer modified carbon nanotubes with dichloromethane and triethylamine in a nitrogen atmosphere, adding acryloyl chloride solution dropwise, reacting after the addition is complete, and after the reaction is complete, removing the solvent dichloromethane by rotary evaporation, washing, and drying to obtain olefinic carbon nanotubes;

[0011] The nano aluminum nitride / ethylene propylene diene monomer rubber composite material is prepared by the following steps:

[0012] S21, mixing amino nano-aluminum nitride with dichloromethane, ultrasonically dispersing, adding 2-bromoisobutyric acid and triethylamine, reacting, and after the reaction is completed, continuing the reaction, filtering, washing, and drying to obtain modified nano-aluminum nitride;

[0013] S22, mixing EPDM rubber, cyclohexane and modified nano-aluminum nitride, adding N,N,N',N",N"-pentamethyldiethylenetriamine and cuprous bromide in a nitrogen atmosphere, reacting, filtering, washing and drying after the reaction to obtain a nano-aluminum nitride / EPDM rubber composite material;

[0014] Step (2), mixing the polyolefin elastomer and EPDM rubber evenly, adding γ-methacryloxypropyl trimethoxysilane, styrene, antioxidant, light stabilizer, thermal conductive additive and tert-butyl peroxycarbonate-2-ethylhexyl ester and mixing evenly, discharging and vulcanizing to obtain a thermally conductive insulating packaging material.

[0015] Preferably, in step (1), the mass ratio of alkenyl carbon nanotubes to nano-aluminum nitride / ethylene propylene diene rubber composite material is 1:8-10.

[0016] Preferably, when preparing alkenyl carbon nanotubes in step (1), in S11: the mass ratio of carboxylated carbon nanotubes, dicyclohexylcarbodiimide and ethylenediamine is 0.15-0.2:1:170-250; when preparing amino carbon nanotubes, the reaction conditions are: reacting at a temperature of 100-120°C for 24-26h.

[0017] Preferably, when preparing alkenyl carbon nanotubes in step (1), in S11: the mass ratio of aminated carbon nanotubes, 3,5-diaminobenzoic acid, pyridine, triphenyl phosphite, and N-methylpyrrolidone is 5.5-6.5:0.55-0.65:6-8:6-8:60-80; when preparing hyperbranched polymer modified carbon nanotubes, the reaction conditions are: reacting in a nitrogen atmosphere at a temperature of 70-80°C for 5-6h.

[0018] Preferably, when preparing alkenyl carbon nanotubes in step (1), in S12: the mass ratio of hyperbranched polymer modified carbon nanotubes, dichloromethane, triethylamine, and acryloyl chloride solution is 1:23-35:0.15-0.3:4-5, the acryloyl chloride solution is prepared by mixing acryloyl chloride and dichloromethane in a mass ratio of 1:8-10, and the dropwise addition condition is dropwise addition at a temperature of 0-5°C for 15-30min; the reaction conditions are: reaction at a temperature of 0-5°C for 1-2h.

[0019] Preferably, when preparing the nano-aluminum nitride / ethylene propylene rubber composite material in step (1), in S21: the mass ratio of amino nano-aluminum nitride, dichloromethane, 2-bromoisobutyric acid, and triethylamine is 15:160-200:9-10:10-12; the reaction conditions are: react at a temperature of 0-5°C for 2-3h; and the continued reaction conditions are: continue the reaction at a temperature of 20-30°C for 10-12h.

[0020] Preferably, when preparing the nano-aluminum nitride / ethylene propylene rubber composite material in step (1), in S22: the mass ratio of ethylene propylene rubber, cyclohexane, modified nano-aluminum nitride, N,N,N',N",N"-pentamethyldiethylenetriamine, and cuprous bromide is 4-5:140-160:10:2-2.5:1.6-2; and the reaction conditions are: reacting in a nitrogen atmosphere at a temperature of 60-70°C for 20-24h.

[0021] Preferably, in step (2), the mass ratio of polyolefin elastomer, EPDM rubber, γ-methacryloxypropyl trimethoxysilane, styrene, antioxidant, light stabilizer, thermal conductive additive, and tert-butyl peroxycarbonate-2-ethylhexyl is: 30-40:60-70:0.1-0.2:1.5-2:0.2-0.3:0.15-0.2:25-30:0.8-1.5 ; The mixing conditions are: uniform mixing at a speed of 50-60r / min and a temperature of 50-60°C; the nano aluminum nitride / ethylene propylene diene monomer rubber composite material in the preparation of the thermal conductive additive is the same as the ethylene propylene diene monomer rubber used in the preparation of the thermal conductive insulating packaging material; the vulcanization conditions are: vulcanization at a temperature of 135-155°C for 8-12 minutes.

[0022] Preferably, a thermally conductive insulating packaging material is prepared using the method for preparing a thermally conductive insulating packaging material as described above.

[0023] Compared with the prior art, the present invention has the following beneficial effects:

[0024] The invention uses hyperbranched polymer to modify carbon nanotubes to obtain olefinic carbon nanotubes; obtains nano aluminum nitride / ethylene propylene diene monomer rubber composite material through atom transfer radical polymerization reaction; compound the two to obtain a thermal conductive additive; and uniformly mix polyolefin elastomer, ethylene propylene diene monomer rubber, additive, thermal conductive additive, and initiator and vulcanize to obtain a thermal conductive insulating packaging material, which has excellent thermal conductivity and insulation performance and good bonding performance.

[0025] The invention prepares amino carbon nanotubes by subjecting carboxylated carbon nanotubes to amidation reaction with ethylenediamine, and further subjecting the amino functional groups on the surface of the carbon nanotubes to amidation reaction with 3,5-diaminobenzoic acid, using the carbon nanotubes as carrier materials, polymerizing on the surface of the carbon nanotubes to generate hyperbranched polyaromatic amide polymers, and then capping the carbon nanotubes with acryloyl chloride. The obtained alkenyl carbon nanotubes not only have improved compatibility in a polymer matrix, but also form a polymer layer on the surface of the carbon nanotubes, thereby hindering contact between the carbon nanotubes and reducing the electrical conductivity of the carbon nanotubes. The carbon nanotubes can be used as a thermal conductive filler component to improve the thermal conductivity of the polymer matrix.

[0026] In addition, since olefinic carbon nanotubes contain carbon-carbon double bond functional groups, they can participate in the vulcanization reaction between the components in the polymer matrix to generate a network cross-linked structure, further improving their dispersibility in the matrix;

[0027] The invention uses an amidation reaction between the amino group of amino nano-aluminum nitride and the carboxyl group of 2-bromoisobutyric acid to prepare a modified nano-aluminum nitride containing a bromine-substituted group; N,N,N',N",N"-pentamethyldiethylenetriamine and cuprous bromide are used as a catalyst system, and an atom transfer free radical polymerization reaction occurs between the bromine-substituted group of the modified nano-aluminum nitride and the unsaturated double bonds of the side chain of ethylene propylene rubber to prepare a nano-aluminum nitride / ethylene propylene rubber composite material, and the nano-aluminum nitride / ethylene propylene rubber composite material is compounded with alkenyl carbon nanotubes to prepare a thermal conductive additive; wherein the nano-aluminum nitride / ethylene propylene rubber composite material has good compatibility with the ethylene propylene rubber component, can be uniformly dispersed in a polymer matrix, improves the insulation performance of the material, and cooperates with the alkenyl carbon nanotubes to form a thermal conductive path in the polymer matrix, thereby improving the thermal conductivity of the material;

[0028] The invention prepares a thermally conductive insulating packaging material by uniformly mixing polyolefin elastomer, ethylene propylene diene monomer rubber, tackifier gamma-methacryloxypropyl trimethoxysilane, styrene, an antioxidant, a light stabilizer, a thermally conductive additive and an initiator tert-butyl peroxycarbonate-2-ethylhexyl ester, and vulcanizing the mixture. The polyolefin elastomer and the ethylene propylene diene monomer rubber form a cross-linked network during the vulcanization process, and the aging resistance of the packaging material is improved. The tackifier gamma-methacryloxypropyl trimethoxysilane can improve the bonding performance of the packaging material. The styrene plays a role in stabilizing free radicals and preventing depolymerization during the vulcanization process. BRIEF DESCRIPTION OF THE DRAWINGS

[0029] Figure 1 is a process flow chart for preparing a thermally conductive insulating packaging material in the present invention;

[0030] Figure 2 1 is a histogram of thermal conductivity in performance tests of embodiments and comparative examples of the present invention. DETAILED DESCRIPTION

[0031] The technical solutions in the embodiments of the present invention will be clearly and completely described below in conjunction with the embodiments of the present invention. Obviously, the described embodiments are only part of the embodiments of the present invention, rather than all of the embodiments. Based on the embodiments of the present invention, all other embodiments obtained by ordinary technicians in this field without making creative work are within the scope of protection of the present invention.

[0032] Example 1

[0033] This embodiment discloses a method for preparing a thermally conductive insulating packaging material, comprising the following steps:

[0034] Step (1), mixing alkenyl carbon nanotubes and nano aluminum nitride / ethylene propylene diene monomer rubber composite material in a mass ratio of 1:10 to obtain a thermal conductive additive;

[0035] Wherein, the olefin-based carbon nanotubes are prepared by the following steps:

[0036] S11, carboxylated carbon nanotubes, dicyclohexylcarbodiimide, and ethylenediamine were mixed at a mass ratio of 0.15:1:170, ultrasonically dispersed for 20 minutes, reacted at 100°C for 26 hours, and after the reaction was completed, filtered to obtain a filter cake, washed with ethanol 6 times the mass of the filter cake, and dried at 50°C for 28 hours to obtain amino carbon nanotubes;

[0037] The aminated carbon nanotubes, 3,5-diaminobenzoic acid, pyridine, triphenyl phosphite and N-methylpyrrolidone were mixed in a mass ratio of 5.5:0.55:6:6:60, reacted for 6 hours at 70°C in a nitrogen atmosphere, and after the reaction was completed, filtered to obtain the filter cake, and washed with methanol and N,N-dimethylformamide in an amount 6 times the mass of the filter cake, and dried at 50°C for 28 hours to obtain hyperbranched polymer modified carbon nanotubes;

[0038] S12, mixing the hyperbranched polymer modified carbon nanotubes with dichloromethane and triethylamine in a nitrogen atmosphere, adding acryloyl chloride solution dropwise at 0°C for 15 min, reacting at 0°C for 2 h, removing the solvent dichloromethane by rotary evaporation at 20°C, adding chloroform 6 times the mass of the filter cake for washing, and drying at 50°C for 28 h to obtain olefinic carbon nanotubes;

[0039] The mass ratio of the hyperbranched polymer modified carbon nanotubes, dichloromethane, triethylamine and acryloyl chloride solution is 1:23:0.15:4, and the acryloyl chloride solution is prepared by mixing acryloyl chloride and dichloromethane in a mass ratio of 1:8;

[0040] The nano aluminum nitride / ethylene propylene diene monomer rubber composite material is prepared by the following steps:

[0041] S21, mixing amino nano aluminum nitride with dichloromethane, ultrasonically dispersing for 20 minutes, adding 2-bromoisobutyric acid and triethylamine, reacting at 0°C for 3 hours, and then continuing to react at 20°C for 12 hours. After the reaction is completed, filtering, taking the filter cake, adding dichloromethane 6 times the mass of the filter cake to wash three times, and drying at 70°C for 28 hours to obtain modified nano aluminum nitride;

[0042] Among them, the mass ratio of amino nano-aluminum nitride, dichloromethane, 2-bromoisobutyric acid, and triethylamine is 15:160:9:10;

[0043] S22, mixing EPDM rubber, cyclohexane and modified nano-aluminum nitride at 50°C, adding N,N,N',N",N"-pentamethyldiethylenetriamine and cuprous bromide in a nitrogen atmosphere, reacting at 60°C for 24 hours in a nitrogen atmosphere, filtering after the reaction, taking the filter cake, adding acetone 6 times the mass of the filter cake to wash three times, and drying at 70°C for 28 hours to obtain a nano-aluminum nitride / EPDM rubber composite material;

[0044] Among them, the mass ratio of EPDM rubber, cyclohexane, modified nano-aluminum nitride, N,N,N',N",N"-pentamethyldiethylenetriamine, and cuprous bromide is 4:140:10:2:1.6;

[0045] Step (2), mixing the polyolefin elastomer and ethylene propylene diene monomer rubber at a speed of 50 r / min and a temperature of 50° C., adding γ-methacryloxypropyl trimethoxysilane, styrene, an antioxidant, a light stabilizer, a thermal conductive additive and tert-butyl peroxycarbonate-2-ethylhexyl ester and mixing evenly, discharging the material, and vulcanizing it at a temperature of 135° C. for 12 minutes to obtain a thermally conductive insulating packaging material;

[0046] The mass ratio of polyolefin elastomer, EPDM rubber, γ-methacryloxypropyl trimethoxysilane, styrene, antioxidant, light stabilizer, thermal conductive additive, and tert-butyl peroxycarbonate-2-ethylhexyl is: 40:60:0.1: 1.5:0.2:0.15:25:0.8 The nano aluminum nitride / ethylene propylene diene monomer rubber composite material used in the preparation of the thermal conductive additive is the same as the ethylene propylene diene monomer rubber used in the preparation of the thermal conductive insulating packaging material.

[0047] Example 2

[0048] This embodiment discloses a method for preparing a thermally conductive insulating packaging material, comprising the following steps:

[0049] Step (1), mixing alkenyl carbon nanotubes and nano aluminum nitride / ethylene propylene diene monomer rubber composite material in a mass ratio of 1:9.5 to obtain a thermal conductive additive;

[0050] Wherein, the olefin-based carbon nanotubes are prepared by the following steps:

[0051] S11, carboxylated carbon nanotubes, dicyclohexylcarbodiimide, and ethylenediamine were mixed at a mass ratio of 0.16:1:190, ultrasonically dispersed for 25 minutes, reacted at 110°C for 26 hours, and after the reaction, filtered, took the filter cake, added ethanol 7 times the mass of the filter cake for washing, and dried at 55°C for 26 hours to obtain amino carbon nanotubes;

[0052] The aminated carbon nanotubes, 3,5-diaminobenzoic acid, pyridine, triphenyl phosphite and N-methylpyrrolidone were mixed in a mass ratio of 5.8:0.58:6.5:6.5:65, reacted for 6 hours in a nitrogen atmosphere at 75°C, and after the reaction was completed, filtered to obtain the filter cake, and washed with methanol and N,N-dimethylformamide in an amount 8 times the mass of the filter cake, and dried at 55°C for 26 hours to obtain hyperbranched polymer modified carbon nanotubes;

[0053] S12, the hyperbranched polymer modified carbon nanotubes were mixed with dichloromethane and triethylamine in a nitrogen atmosphere, and the acryloyl chloride solution was added dropwise at 3°C ​​for 15 min. After the addition was completed, the mixture was reacted at 3°C ​​for 2 h. After the reaction was completed, the solvent dichloromethane was removed by rotary evaporation at 25°C, chloroform in an amount of 8 times the mass of the filter cake was added for washing, and the mixture was dried at 55°C for 26 h to obtain olefinic carbon nanotubes;

[0054] The mass ratio of the hyperbranched polymer modified carbon nanotubes, dichloromethane, triethylamine and acryloyl chloride solution is 1:26:0.20:4.3, and the acryloyl chloride solution is prepared by mixing acryloyl chloride and dichloromethane in a mass ratio of 1:8.5.

[0055] The nano aluminum nitride / ethylene propylene diene monomer rubber composite material is prepared by the following steps:

[0056] S21, mixing amino nano aluminum nitride with dichloromethane, ultrasonically dispersing for 25 minutes, adding 2-bromoisobutyric acid and triethylamine, reacting at 3°C ​​for 3 hours, and then continuing to react at 25°C for 12 hours. After the reaction is completed, filtering, taking the filter cake, adding dichloromethane 7 times the mass of the filter cake to wash three times, and drying at 75°C for 26 hours to obtain modified nano aluminum nitride;

[0057] Among them, the mass ratio of amino nano-aluminum nitride, dichloromethane, 2-bromoisobutyric acid, and triethylamine is 15:170:9.3:10.5;

[0058] S22, mixing EPDM rubber, cyclohexane and modified nano-aluminum nitride at 55°C, adding N,N,N',N",N"-pentamethyldiethylenetriamine and cuprous bromide in a nitrogen atmosphere, reacting at 65°C for 24 hours in a nitrogen atmosphere, filtering after the reaction, taking the filter cake, adding acetone 7 times the mass of the filter cake to wash three times, and drying at 75°C for 26 hours to obtain a nano-aluminum nitride / EPDM rubber composite material;

[0059] Among them, the mass ratio of EPDM rubber, cyclohexane, modified nano-aluminum nitride, N,N,N',N",N"-pentamethyldiethylenetriamine, and cuprous bromide is 4.3:145:10:2.2:1.7;

[0060] Step (2), mixing the polyolefin elastomer and EPDM rubber at a speed of 55 r / min and a temperature of 55° C., adding γ-methacryloxypropyl trimethoxysilane, styrene, an antioxidant, a light stabilizer, a thermal conductive additive and tert-butyl peroxycarbonate-2-ethylhexyl ester and mixing evenly, discharging the material, and vulcanizing it at a temperature of 140° C. for 10 minutes to obtain a thermally conductive insulating packaging material;

[0061] The mass ratio of polyolefin elastomer, EPDM rubber, γ-methacryloxypropyl trimethoxysilane, styrene, antioxidant, light stabilizer, thermal conductive additive, and tert-butyl peroxycarbonate-2-ethylhexyl is: 33:67: 0.13:1.6:0.23:0.16:26:0.9 The nano aluminum nitride / ethylene propylene diene monomer rubber composite material used in the preparation of the thermal conductive additive is the same as the ethylene propylene diene monomer rubber used in the preparation of the thermal conductive insulating packaging material.

[0062] Example 3

[0063] This embodiment discloses a method for preparing a thermally conductive insulating packaging material, comprising the following steps:

[0064] Step (1), mixing alkenyl carbon nanotubes and nano aluminum nitride / ethylene propylene diene monomer rubber composite material in a mass ratio of 1:9 to obtain a thermal conductive additive;

[0065] Wherein, the olefin-based carbon nanotubes are prepared by the following steps:

[0066] S11, carboxylated carbon nanotubes, dicyclohexylcarbodiimide, and ethylenediamine were mixed in a mass ratio of 0.18:1:210, ultrasonically dispersed for 25 minutes, reacted at 110°C for 25 hours, and after the reaction, filtered to obtain a filter cake, washed with 7 times the mass of the filter cake using ethanol, and dried at 55°C for 26 hours to obtain amino carbon nanotubes;

[0067] The aminated carbon nanotubes, 3,5-diaminobenzoic acid, pyridine, triphenyl phosphite and N-methylpyrrolidone were mixed in a mass ratio of 6:0.6:7:7:70, reacted for 5.5 hours in a nitrogen atmosphere at 75°C, and after the reaction was completed, the filter cake was filtered and washed with methanol and N,N-dimethylformamide in an amount 8 times the mass of the filter cake, and dried at 55°C for 26 hours to obtain hyperbranched polymer modified carbon nanotubes;

[0068] S12, the hyperbranched polymer modified carbon nanotubes were mixed with dichloromethane and triethylamine in a nitrogen atmosphere, and the acryloyl chloride solution was added dropwise at 3°C ​​for 18 min. After the addition was completed, the mixture was reacted at 3°C ​​for 1.5 h. After the reaction was completed, the solvent dichloromethane was removed by rotary evaporation at 25°C, chloroform 8 times the mass of the filter cake was added for washing, and the mixture was dried at 55°C for 26 h to obtain olefinic carbon nanotubes;

[0069] The mass ratio of the hyperbranched polymer modified carbon nanotubes, dichloromethane, triethylamine and acryloyl chloride solution is 1:30:0.23:4.5, and the acryloyl chloride solution is prepared by mixing acryloyl chloride and dichloromethane in a mass ratio of 1:9;

[0070] The nano aluminum nitride / ethylene propylene diene monomer rubber composite material is prepared by the following steps:

[0071] S21, mixing amino nano aluminum nitride with dichloromethane, ultrasonically dispersing for 25 minutes, adding 2-bromoisobutyric acid and triethylamine, reacting at 3°C ​​for 2.5 hours, and then continuing to react at 25°C for 11 hours. After the reaction is completed, filtering, taking the filter cake, adding dichloromethane 7 times the mass of the filter cake to wash three times, and drying at 75°C for 26 hours to obtain modified nano aluminum nitride;

[0072] Among them, the mass ratio of amino nano-aluminum nitride, dichloromethane, 2-bromoisobutyric acid, and triethylamine is 15:180:9.5:11;

[0073] S22, mixing EPDM rubber, cyclohexane and modified nano-aluminum nitride at 55°C, adding N,N,N',N",N"-pentamethyldiethylenetriamine and cuprous bromide in a nitrogen atmosphere, reacting for 22 hours at 65°C in a nitrogen atmosphere, filtering after the reaction, taking the filter cake, adding acetone 7 times the mass of the filter cake to wash three times, and drying at 75°C for 26 hours to obtain a nano-aluminum nitride / EPDM rubber composite material;

[0074] Among them, the mass ratio of EPDM rubber, cyclohexane, modified nano-aluminum nitride, N,N,N',N",N"-pentamethyldiethylenetriamine, and cuprous bromide is 4.5:150:10:2.3:1.8;

[0075] Step (2), mixing the polyolefin elastomer and ethylene propylene diene monomer rubber at a speed of 55 r / min and a temperature of 55° C., adding γ-methacryloxypropyl trimethoxysilane, styrene, an antioxidant, a light stabilizer, a thermal conductive additive and tert-butyl peroxycarbonate-2-ethylhexyl ester and mixing evenly, discharging the material, and vulcanizing it at a temperature of 145° C. for 10 minutes to obtain a thermally conductive insulating packaging material;

[0076] The mass ratio of polyolefin elastomer, EPDM rubber, γ-methacryloxypropyl trimethoxysilane, styrene, antioxidant, light stabilizer, thermal conductive additive, and tert-butyl peroxycarbonate-2-ethylhexyl is: 35:65: 0.15:1.8:0.25:0.18:28:1.1 The nano aluminum nitride / ethylene propylene diene monomer rubber composite material used in the preparation of the thermal conductive additive is the same as the ethylene propylene diene monomer rubber used in the preparation of the thermal conductive insulating packaging material.

[0077] Example 4

[0078] This embodiment discloses a method for preparing a thermally conductive insulating packaging material, comprising the following steps:

[0079] Step (1), mixing alkenyl carbon nanotubes and nano aluminum nitride / ethylene propylene rubber composite material in a mass ratio of 1:8.5 to obtain a thermal conductive additive;

[0080] Wherein, the olefin-based carbon nanotubes are prepared by the following steps:

[0081] S11, carboxylated carbon nanotubes, dicyclohexylcarbodiimide, and ethylenediamine were mixed at a mass ratio of 0.19:1:230, ultrasonically dispersed for 25 minutes, reacted at 110°C for 24 hours, and after the reaction, filtered, took the filter cake, added ethanol 7 times the mass of the filter cake for washing, and dried at 55°C for 26 hours to obtain amino carbon nanotubes;

[0082] The aminated carbon nanotubes, 3,5-diaminobenzoic acid, pyridine, triphenyl phosphite and N-methylpyrrolidone were mixed in a mass ratio of 6.3:0.63:7.5:7.5:75, reacted for 5 hours in a nitrogen atmosphere at 75°C, and after the reaction was completed, filtered to obtain the filter cake, and washed with methanol and N,N-dimethylformamide in an amount 8 times the mass of the filter cake, and dried at 55°C for 26 hours to obtain hyperbranched polymer modified carbon nanotubes;

[0083] S12, the hyperbranched polymer modified carbon nanotubes were mixed with dichloromethane and triethylamine in a nitrogen atmosphere, and the acryloyl chloride solution was added dropwise at 3°C ​​for 25 min. After the addition was completed, the mixture was reacted at 3°C ​​for 1 h. After the reaction was completed, the solvent dichloromethane was removed by rotary evaporation at 25°C, chloroform in an amount of 8 times the mass of the filter cake was added for washing, and the mixture was dried at 55°C for 26 h to obtain olefinic carbon nanotubes;

[0084] The mass ratio of the hyperbranched polymer modified carbon nanotubes, dichloromethane, triethylamine and acryloyl chloride solution is 1:30:0.23:4.5, and the acryloyl chloride solution is prepared by mixing acryloyl chloride and dichloromethane in a mass ratio of 1:9;

[0085] The nano aluminum nitride / ethylene propylene diene monomer rubber composite material is prepared by the following steps:

[0086] S21, mixing amino nano aluminum nitride with dichloromethane, ultrasonically dispersing for 25 minutes, adding 2-bromoisobutyric acid and triethylamine, reacting at 3°C ​​for 2 hours, and then continuing to react at 25°C for 10 hours. After the reaction is completed, filtering, taking the filter cake, adding dichloromethane 7 times the mass of the filter cake to wash three times, and drying at 75°C for 26 hours to obtain modified nano aluminum nitride;

[0087] Among them, the mass ratio of amino nano-aluminum nitride, dichloromethane, 2-bromoisobutyric acid, and triethylamine is 15:190:9.8:11.5;

[0088] S22, mixing EPDM rubber, cyclohexane and modified nano-aluminum nitride at 55°C, adding N,N,N',N",N"-pentamethyldiethylenetriamine and cuprous bromide in a nitrogen atmosphere, reacting for 20 hours at 65°C in a nitrogen atmosphere, filtering after the reaction, taking the filter cake, adding acetone 7 times the mass of the filter cake to wash three times, and drying at 75°C for 26 hours to obtain a nano-aluminum nitride / EPDM rubber composite material;

[0089] Among them, the mass ratio of EPDM rubber, cyclohexane, modified nano-aluminum nitride, N,N,N',N",N"-pentamethyldiethylenetriamine, and cuprous bromide is 4.8:155:10:2.4:1.9;

[0090] Step (2), mixing the polyolefin elastomer and ethylene propylene diene monomer rubber at a speed of 55 r / min and a temperature of 55° C., adding γ-methacryloxypropyl trimethoxysilane, styrene, an antioxidant, a light stabilizer, a thermal conductive additive and tert-butyl peroxycarbonate-2-ethylhexyl ester and mixing evenly, discharging the material, and vulcanizing it at a temperature of 150° C. for 10 minutes to obtain a thermally conductive insulating packaging material;

[0091] The mass ratio of polyolefin elastomer, EPDM rubber, γ-methacryloxypropyl trimethoxysilane, styrene, antioxidant, light stabilizer, thermal conductive additive, and tert-butyl peroxycarbonate-2-ethylhexyl is: 38:62: 0.18:1.9:0.28:0.19:29:1.3 The nano aluminum nitride / ethylene propylene diene monomer rubber composite material used in the preparation of the thermal conductive additive is the same as the ethylene propylene diene monomer rubber used in the preparation of the thermal conductive insulating packaging material.

[0092] Example 5

[0093] This embodiment discloses a method for preparing a thermally conductive insulating packaging material, comprising the following steps:

[0094] Step (1), mixing alkenyl carbon nanotubes and nano aluminum nitride / ethylene propylene diene monomer rubber composite material in a mass ratio of 1:8 to obtain a thermal conductive additive;

[0095] Wherein, the olefin-based carbon nanotubes are prepared by the following steps:

[0096] S11, carboxylated carbon nanotubes, dicyclohexylcarbodiimide, and ethylenediamine were mixed at a mass ratio of 0.2:1:250, ultrasonically dispersed for 30 minutes, reacted at 120°C for 24 hours, and after the reaction, filtered to obtain a filter cake, washed with ethanol 8 times the mass of the filter cake, and dried at 60°C for 24 hours to obtain amino carbon nanotubes;

[0097] The aminated carbon nanotubes, 3,5-diaminobenzoic acid, pyridine, triphenyl phosphite and N-methylpyrrolidone were mixed in a mass ratio of 6.5:0.65:8:8:80, reacted at 80°C in a nitrogen atmosphere for 5 hours, and after the reaction was completed, filtered to obtain the filter cake, and washed with methanol and N,N-dimethylformamide in an amount 10 times the mass of the filter cake, and dried at 60°C for 24 hours to obtain hyperbranched polymer modified carbon nanotubes;

[0098] S12, the hyperbranched polymer modified carbon nanotubes were mixed with dichloromethane and triethylamine in a nitrogen atmosphere, and the acryloyl chloride solution was added dropwise at 5°C for 30 min. After the addition was completed, the mixture was reacted at 5°C for 1 h. After the reaction was completed, the solvent dichloromethane was removed by rotary evaporation at 30°C, chloroform 10 times the mass of the filter cake was added for washing, and the mixture was dried at 60°C for 24 h to obtain olefinic carbon nanotubes;

[0099] The mass ratio of the hyperbranched polymer modified carbon nanotubes, dichloromethane, triethylamine and acryloyl chloride solution is 1:35:0.3:5, and the acryloyl chloride solution is prepared by mixing acryloyl chloride and dichloromethane in a mass ratio of 1:10;

[0100] The nano aluminum nitride / ethylene propylene diene monomer rubber composite material is prepared by the following steps:

[0101] S21, mixing amino nano aluminum nitride with dichloromethane, ultrasonically dispersing for 30 minutes, adding 2-bromoisobutyric acid and triethylamine, reacting at 5°C for 2 hours, and then continuing to react at 30°C for 10 hours. After the reaction is completed, filtering, taking the filter cake, adding dichloromethane 8 times the mass of the filter cake to wash three times, and drying at 80°C for 24 hours to obtain modified nano aluminum nitride;

[0102] The mass ratio of amino nano-aluminum nitride, dichloromethane, 2-bromoisobutyric acid, and triethylamine is 15:200:10:12;

[0103] S22, mixing EPDM rubber, cyclohexane and modified nano-aluminum nitride at 60°C, adding N,N,N',N",N"-pentamethyldiethylenetriamine and cuprous bromide in a nitrogen atmosphere, reacting for 20 hours at 70°C in a nitrogen atmosphere, filtering after the reaction, taking the filter cake, adding acetone 8 times the mass of the filter cake to wash three times, and drying at 80°C for 24 hours to obtain a nano-aluminum nitride / EPDM rubber composite material;

[0104] The mass ratio of EPDM rubber, cyclohexane, modified nano-aluminum nitride, N,N,N',N",N"-pentamethyldiethylenetriamine, and cuprous bromide is 5:160:10:2.5:2;

[0105] Step (2), mixing the polyolefin elastomer and ethylene propylene diene monomer rubber at a speed of 60 r / min and a temperature of 60° C., adding γ-methacryloxypropyl trimethoxysilane, styrene, an antioxidant, a light stabilizer, a thermal conductive additive and tert-butyl peroxycarbonate-2-ethylhexyl ester and mixing evenly, discharging the material, and vulcanizing it at a temperature of 155° C. for 8 minutes to obtain a thermally conductive insulating packaging material;

[0106] The mass ratio of polyolefin elastomer, EPDM rubber, γ-methacryloxypropyl trimethoxysilane, styrene, antioxidant, light stabilizer, thermal conductive additive, and tert-butyl peroxycarbonate-2-ethylhexyl is: 30:70:0.2: 2:0.3:0.2:30:1.5 The nano aluminum nitride / ethylene propylene diene monomer rubber composite material used in the preparation of the thermal conductive additive is the same as the ethylene propylene diene monomer rubber used in the preparation of the thermal conductive insulating packaging material.

[0107] Comparative Example 1

[0108] This comparative example discloses a method for preparing a packaging material, comprising the following steps:

[0109] Step (1), mixing carbon nanotubes and nano-aluminum nitride in a mass ratio of 1:10 to obtain a thermal conductive additive;

[0110] Step (2), mixing the polyolefin elastomer and ethylene propylene diene monomer rubber at a speed of 50 r / min and a temperature of 50° C., adding γ-methacryloxypropyl trimethoxysilane, styrene, an antioxidant, a light stabilizer, a thermal conductive additive and tert-butyl peroxycarbonate-2-ethylhexyl ester and mixing evenly, discharging the material, and vulcanizing it at a temperature of 135° C. for 12 minutes to obtain a packaging material;

[0111] The mass ratio of polyolefin elastomer, EPDM rubber, γ-methacryloxypropyl trimethoxysilane, styrene, antioxidant, light stabilizer, thermal conductive additive, and tert-butyl peroxycarbonate-2-ethylhexyl is: 40:60:0.1: 1.5:0.2:0.15:25:0.8 .

[0112] Comparative Example 2

[0113] This comparative example discloses a method for preparing a packaging material, comprising the following steps:

[0114] Step (1), mixing amino nano aluminum nitride with dichloromethane, ultrasonically dispersing for 20 minutes, adding 2-bromoisobutyric acid and triethylamine, reacting at 0°C for 3 hours, and continuing to react at 20°C for 12 hours. After the reaction is completed, filtering, taking the filter cake, adding dichloromethane 6 times the mass of the filter cake to wash three times, and drying at 70°C for 28 hours to obtain modified nano aluminum nitride;

[0115] Among them, the mass ratio of amino nano-aluminum nitride, dichloromethane, 2-bromoisobutyric acid, and triethylamine is 15:160:9:10;

[0116] The EPDM rubber, cyclohexane and modified nano-aluminum nitride were mixed at a temperature of 50°C, N,N,N',N",N"-pentamethyldiethylenetriamine and cuprous bromide were added in a nitrogen atmosphere, and the mixture was reacted at a temperature of 60°C for 24 hours. After the reaction was completed, the mixture was filtered, the filter cake was taken, acetone of 6 times the mass of the filter cake was added for washing three times, and the mixture was dried at a temperature of 70°C for 28 hours to obtain a nano-aluminum nitride / EPDM rubber composite material;

[0117] Among them, the mass ratio of EPDM rubber, cyclohexane, modified nano-aluminum nitride, N,N,N',N",N"-pentamethyldiethylenetriamine, and cuprous bromide is 4:140:10:2:1.6;

[0118] Step (2), mixing the polyolefin elastomer and ethylene propylene diene monomer rubber at a speed of 50 r / min and a temperature of 50° C., adding γ-methacryloxypropyl trimethoxysilane, styrene, an antioxidant, a light stabilizer, a thermal conductive additive and tert-butyl peroxycarbonate-2-ethylhexyl ester and mixing evenly, discharging the material, and vulcanizing it at a temperature of 135° C. for 12 minutes to obtain a packaging material;

[0119] The mass ratio of polyolefin elastomer, EPDM rubber, γ-methacryloxypropyl trimethoxysilane, styrene, antioxidant, light stabilizer, nano aluminum nitride / EPDM rubber composite material, and tert-butyl peroxycarbonate-2-ethylhexyl is: 40:60:0.1:1.5:0.2:0.15:25:0.8 The EPDM rubber used in preparing the nano-aluminum nitride / EPDM rubber composite material is the same as the EPDM rubber used in preparing the packaging material.

[0120] In the above embodiments and comparative examples: carboxylated carbon nanotubes are from Suzhou Beike Nanotechnology Co., Ltd., product name carboxylated single-walled carbon nanotubes, outer diameter 2nm, length 20-30μm; dicyclohexylcarbodiimide is from Shanghai MacLean Biochemical Technology Co., Ltd., CAS No.: 538-75-0; 3,5-diaminobenzoic acid is from Shandong Poly Chemical Co., Ltd., CAS No.: 535-87-5; triphenyl phosphite is from Jinan Feiyue Chemical Co., Ltd., CAS No.: 101-02-0; acryloyl chloride is from Shanghai Aladdin Biochemical Technology Co., Ltd., CAS No.: 814-68-6; amino nano-aluminum nitride is from Lianyungang Rongbai New Materials Co., Ltd., specification aminosilane coupling agent KH550 modified nano-aluminum nitride, particle size 100nm; 2-bromoisobutyric acid is from Shanghai Aladdin Biochemical Technology Co., Ltd., CAS No.: 2052-01-9; ethylene propylene diene monomer rubber is from German Lanxess, product name EPDM K512; N,N,N',N",N"-pentamethyldiethylenetriamine is from Shandong Xiya Chemical Co., Ltd., CAS No.: 3030-47-5; cuprous bromide is from Shandong Guohua Chemical Co., Ltd., CAS No.: 7787-70-4; polyolefin elastomer is from ExxonMobil, product name POE 6102FL; γ-methacryloxypropyltrimethoxysilane is from Wuhan Lanabai Pharmaceutical Chemical Co., Ltd., product name silane coupling agent KH570, CAS No.: 2530-85-0; antioxidant is from Nanjing Milan Chemical Co., Ltd., product name antioxidant 1010; light stabilizer is from Changzhou Youfeng Chemical Co., Ltd., product name light stabilizer UV-531; tert-butyl peroxycarbonate-2-ethylhexyl ester is from Hubei Tosoh Chemical Technology Co., Ltd., CAS No.: 34443-12-4.

[0121] Test example

[0122] The packaging materials prepared in the embodiments and comparative examples were subjected to comprehensive performance tests, and the specific test results are shown in Table 1:

[0123] Table 1

[0124]

[0125] The detection of each index in Table 1 is based on the following standards: the volume resistivity is measured with reference to GB / T1410-2006 "Test Method for Volume Resistivity and Surface Resistivity of Solid Insulating Materials"; the bonding performance is represented by the peel strength, which is measured with reference to GB / T2790-1995 "Test Method for 180° Peel Strength of Adhesives - Flexible Materials to Rigid Materials"; the resistance to wet heat aging is represented by the peel strength retention rate, and the test conditions are: relative humidity 85%, temperature 85°C, and test time 1000h. It can be seen from the test results in Table 1 that the packaging material prepared by the present invention has excellent thermal conductivity and insulation performance, and good bonding performance.

[0126] It can be seen from the test results in Table 1 that the packaging material prepared by the present invention has excellent thermal conductivity and insulation performance, and good bonding performance.

[0127] The invention generates a hyperbranched polyaromatic amide polymer by polymerization on the surface of a carbon nanotube, and then performs end-capping by acryloyl chloride. The obtained olefinic carbon nanotube not only improves the compatibility of the olefinic carbon nanotube in a polymer matrix, but also forms a polymer layer on the surface of the carbon nanotube, which can hinder the contact between the carbon nanotubes and reduce the electrical conductivity of the carbon nanotubes. The olefinic carbon nanotubes can be used as a thermal conductive filler component to improve the thermal conductivity of the polymer matrix. Moreover, since the olefinic carbon nanotubes contain carbon-carbon double bond functional groups, they can participate in the vulcanization reaction between the components in the polymer matrix to generate a network cross-linked structure, further improving the dispersibility of the olefinic carbon nanotubes in the matrix. The nano aluminum nitride / ethylene propylene diene monomer rubber composite material is compounded with the olefinic carbon nanotubes to obtain a thermal conductive additive. The nano aluminum nitride / ethylene propylene diene monomer rubber composite material has good compatibility with the ethylene propylene diene monomer rubber component, can be uniformly dispersed in the polymer matrix, improves the insulation performance of the material, and cooperates with the olefinic carbon nanotubes to form a thermal conductive path in the polymer matrix, thereby improving the thermal conductivity of the material.

[0128] In Comparative Example 1, the carbon nanotubes and nano-aluminum nitride surfaces are not modified, the thermal conductive additives are not compatible with the polymer matrix, and since the carbon nanotubes have a low resistivity and are conductive, the resistivity of the polymer matrix will be reduced without surface modification, which will have an adverse effect on its insulation properties. Therefore, the thermal conductivity, insulation and mechanical properties of Comparative Example 1 are all reduced;

[0129] In Comparative Example 2, no olefinic carbon nanotubes are added to the thermal conductive additive, and the synergistic improvement effect of carbon nanotubes on thermal conductivity is lacking. However, since the resistivity of carbon nanotubes is relatively low, the resistivity of the material is not increased after the addition of olefinic carbon nanotubes. Therefore, the thermal conductivity of Comparative Example 2 is lower than that of the embodiment, and the resistivity is higher than that of the embodiment.

[0130] Although embodiments of the present invention have been shown and described, it will be appreciated by those skilled in the art that various changes, modifications, substitutions and variations may be made to the embodiments without departing from the principles and spirit of the present invention, and that the scope of the present invention is defined by the appended claims and their equivalents.

Claims

1. A method for preparing a thermally conductive insulating packaging material, characterized in that: The following steps are involved: Step (1), mixing alkenyl carbon nanotubes and nano aluminum nitride / ethylene propylene diene monomer rubber composite material to obtain a thermal conductive additive; Wherein, the olefin-based carbon nanotubes are prepared by the following steps: The hyperbranched polymer modified carbon nanotubes are uniformly mixed with dichloromethane and triethylamine in a nitrogen atmosphere, and the acryloyl chloride solution is added dropwise. After the addition is complete, the mixture is reacted. After the reaction is completed, the solvent dichloromethane is removed by rotary evaporation, and the mixture is washed and dried to obtain olefinic carbon nanotubes. The nano aluminum nitride / ethylene propylene diene monomer rubber composite material is prepared by the following steps: The EPDM rubber, cyclohexane and modified nano-aluminum nitride are mixed, and N,N,N',N",N"-pentamethyldiethylenetriamine and cuprous bromide are added in a nitrogen atmosphere to react. After the reaction is completed, the mixture is filtered, washed and dried to obtain a nano-aluminum nitride / EPDM rubber composite material; Step (2), mixing the polyolefin elastomer and EPDM rubber evenly, adding γ-methacryloxypropyl trimethoxysilane, styrene, antioxidant, light stabilizer, thermal conductive additive and tert-butyl peroxycarbonate-2-ethylhexyl ester and mixing evenly, discharging and vulcanizing to obtain a thermally conductive insulating packaging material.

2. The method for preparing a thermally conductive insulating packaging material according to claim 1, characterized in that: In the step (1), the mass ratio of the olefinic carbon nanotubes to the nano-aluminum nitride / ethylene propylene diene monomer rubber composite material is 1:8-10.

3. The method for preparing a thermally conductive insulating packaging material according to claim 1, characterized in that: When preparing alkenyl carbon nanotubes in step (1), the hyperbranched polymer modified carbon nanotubes are prepared by the following steps: The carboxylated carbon nanotubes, dicyclohexylcarbodiimide and ethylenediamine are mixed, ultrasonically dispersed, reacted, and after the reaction is completed, filtered, washed and dried to obtain the amino carbon nanotubes; The aminated carbon nanotubes, 3,5-diaminobenzoic acid, pyridine, triphenyl phosphite and N-methylpyrrolidone are mixed and reacted, and after the reaction is completed, the mixture is filtered, washed and dried to obtain the hyperbranched polymer modified carbon nanotubes.

4. The method for preparing a thermally conductive insulating packaging material according to claim 3, characterized in that: When preparing the hyperbranched polymer modified carbon nanotubes, the mass ratio of carboxylated carbon nanotubes, dicyclohexylcarbodiimide and ethylenediamine is 0.15-0.2:1:170-250; when preparing the amino carbon nanotubes, the reaction conditions are: reacting at a temperature of 100-120°C for 24-26h; the mass ratio of the amino carbon nanotubes, 3,5-diaminobenzoic acid, pyridine, triphenyl phosphite and N-methylpyrrolidone is 5.5-6.5:0.55-0.65:6-8:6-8:60-80; when preparing the hyperbranched polymer modified carbon nanotubes, the reaction conditions are: reacting at a temperature of 70-80°C in a nitrogen atmosphere for 5-6h.

5. The method for preparing a thermally conductive insulating packaging material according to claim 1, characterized in that: When preparing alkenyl carbon nanotubes in step (1): the mass ratio of hyperbranched polymer modified carbon nanotubes, dichloromethane, triethylamine and acryloyl chloride solution is 1:23-35:0.15-0.3:4-5, the acryloyl chloride solution is prepared by mixing acryloyl chloride and dichloromethane in a mass ratio of 1:8-10, and the dripping condition is dripping at a temperature of 0-5°C for 15-30min; the reaction condition is: reacting at a temperature of 0-5°C for 1-2h.

6. The method for preparing a thermally conductive insulating packaging material according to claim 1, characterized in that: When the nano aluminum nitride / ethylene propylene diene monomer rubber composite material is prepared in step (1), the modified nano aluminum nitride is prepared by the following steps: The amino nano-aluminum nitride is mixed with dichloromethane, ultrasonically dispersed, 2-bromoisobutyric acid and triethylamine are added, reacted, and after the reaction is completed, the reaction is continued. After the reaction is completed, the modified nano-aluminum nitride is obtained by filtering, washing, and drying. Among them, the mass ratio of amino nano-aluminum nitride, dichloromethane, 2-bromoisobutyric acid and triethylamine is 15:160-200:9-10:10-12; the reaction conditions are: react at 0-5°C for 2-3h; the continued reaction conditions are: continue to react at 20-30°C for 10-12h.

7. The method for preparing a thermally conductive insulating packaging material according to claim 1, characterized in that: When preparing the nano aluminum nitride / ethylene propylene rubber composite material in the step (1), the mass ratio of ethylene propylene rubber, cyclohexane, modified nano aluminum nitride, N,N,N',N",N"-pentamethyldiethylenetriamine and cuprous bromide is 4-5:140-160:10:2-2.5:1.6-2; the reaction conditions are: reacting in a nitrogen atmosphere at a temperature of 60-70°C for 20-24h.

8. The method for preparing a thermally conductive insulating packaging material according to claim 1, characterized in that: In the step (2), the mass ratio of polyolefin elastomer, ethylene propylene diene monomer rubber, γ-methacryloxypropyl trimethoxysilane, styrene, antioxidant, light stabilizer, thermal conductive additive, and tert-butyl peroxycarbonate-2-ethylhexyl is: 30-40:60-70:0.1- 0.2:1.5-2:0.2-0.3:0.15-0.2:25-30:0.8-1.5 ; Mixing conditions: mix evenly at a speed of 50-60r / min and a temperature of 50-60℃.

9. The method for preparing a thermally conductive insulating packaging material according to claim 1, characterized in that: In the step (2), the nano aluminum nitride / ethylene propylene diene monomer rubber composite material in the preparation of the thermal conductive additive is the same as the ethylene propylene diene monomer rubber used in the preparation of the thermal conductive insulating packaging material; the vulcanization conditions are: vulcanization at a temperature of 135-155° C. for 8-12 minutes.

10. A thermally conductive insulating packaging material prepared by the method for preparing a thermally conductive insulating packaging material according to any one of claims 1 to 9.

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