TWI546374B - Thermally conductive molded body - Google Patents

Description

Thermally conductive formed body

The present invention relates to a thermally conductive molded body in which an electronic article attached to heat is used as a heat countermeasure component for heat release and cooling of the above electronic article.

A liquid-mixed composition in which a large amount of a thermally conductive filler is mixed with a low-viscosity liquid polymer is known to have a heat-conductive molded article having a high thermal conductivity by curing the liquid mixed composition.

As the above-mentioned liquid polymer, tannin extract can be suitably used, but the contact point of low molecular naphthenes is induced, and therefore there is a strong demand in the market for replacement with a non-lanthanum liquid polymer. Japanese Patent Publication No. 2006-312708 (Patent Document 1) describes an example in which a poly-α-olefin-based resin is used as a non-fluorene-based liquid polymer.

However, in order to increase the thermal conductivity, it is necessary to contain a large amount of the thermally conductive filler, but the liquid polymer filled with a large amount of the thermally conductive filler is difficult to produce due to high viscosity. On the other hand, in order to reduce the viscosity, adding a large amount of plasticizer causes a problem of oil release. Further, in the case where a low-viscosity plasticizer and a heat-conductive molded body having a low ignition point are selected, there is a problem that flame retardancy is lowered. Patent Document 1 JP-A-2006-312708

An object of the present invention is to provide a liquid mixed composition which is a raw material for a thermally conductive molded body and which can prevent a liquid polymer from containing a thermally conductive filler. A thermally conductive molded body having a viscosity and capable of suppressing oil release. Further, a thermally conductive molded body excellent in flame retardancy is provided.

In order to achieve the above object, the content of the present invention is as follows.

In a thermally conductive molded body comprising a polymer matrix, a plasticizer, and a thermally conductive filler, the polymer matrix is a hardened body of an olefin-based liquid resin, and the plasticizer contains a dialkyl carbonate and a ignition point of 250 ° C. The above non-antimony oil; characterized in that the weight ratio of the dialkyl carbonate to the total of the dialkyl carbonate and the non-antimony oil is 0.05 or more and less than 0.85, and the content of the dialkyl carbonate is high as described above. The molecular weight of the molecular matrix 100 is less than 100 parts by weight.

The plasticizer comprises a dialkyl carbonate and a non-antimony oil having a firing point of 250 ° C or more, and a weight ratio of the dialkyl carbonate to a total of the dialkyl carbonate of the dialkyl carbonate and the non-lanthanum oil having a firing point of 250 ° C or higher. When the amount is less than 0.85, a thermally conductive molded body having a high heat-insulating filler which is excellent in flame retardancy and has low oil release can be obtained.

Even if the content of the plasticizer in the dialkyl carbonate is small, the viscosity of the liquid mixed composition can be lowered. Therefore, the content of the plasticizer can be lowered to the extent that the oil release is suppressed. When a thermally conductive molded body is produced, oxygen bubbles can be easily removed, and a high-quality thermally conductive molded body can be easily produced. In other words, when the range of the viscosity at which the liquid mixed composition can be produced is set to be the maximum, when the non-antimony oil having a firing point of 250 ° C or more is used as the plasticizer, the heat conductive filler can be highly filled and can be improved. The thermal conductivity of the thermally conductive molded body.

Also, because of the weight of the polymer matrix 100 parts of the dialkyl carbonate When the content is less than 100 parts by weight, it can be a thermally conductive molded body excellent in flame retardancy. When the content of the dialkyl carbonate exceeds 100 parts by weight, the flame retardancy of the thermally conductive molded body is lowered.

The total content of the dialkyl carbonate and the non-antimony oil may be from 121 parts by weight to 257 parts by weight to 100 parts by weight of the polymer matrix. When the amount is less than the weight of 121, the thermally conductive filler cannot be filled high, and the thermal conductivity of the thermally conductive molded article cannot be sufficiently improved. On the other hand, when it exceeds 257 parts by weight, oil release occurs.

The thermally conductive filler may contain a metal hydroxide. In other words, a part of the thermally conductive filler may contain a metal hydroxide, and all of the thermally conductive filler may be a metal hydroxide. When a metal hydroxide is used for the heat conductive filler, the flame retardancy of the heat conductive molded body can be improved, and the amount of the heat conductive filler which the heat conductive molded body occupies can be relatively increased.

Further, the polymer matrix is preferably composed of polyisobutylene as a main component. Polybutene has high heat resistance in olefin hydrazine resin because of its high mechanical strength. Therefore, it is suitable as a thermally conductive molded body which is used at a high temperature and used for a long period of time.

Further, paraffin can be used as the non-antimony oil having a firing point of 250 ° C or higher. The plasticizer combined with the paraffin wax and the dialkyl carbonate can suppress the decrease in flame retardancy and effectively reduce the viscosity because of the synergistic effect of the lower viscosity of each of the individual viscosity average values.

Therefore, by using such a combination, a liquid mixed composition excellent in workability can be obtained by blending with higher thermal conductivity, and a heat conductive molded body having high flame retardancy which is easy to manufacture and can suppress oil release of a plasticizer can be obtained. .

According to the thermally conductive molded article of the present invention, even if the thermally conductive filler is highly filled, a liquid mixed composition having good workability can be obtained, and it can be easily produced, and the thermally conductive molded article can be suppressed. Further, it is also a thermally conductive molded body excellent in flame retardancy.

The contents of the present invention are not limited to the above description, and the objects, advantages, features, and uses of the present invention will become more apparent from the following description. Further, it is to be appropriately included in the scope of the invention without departing from the spirit and scope of the invention.

The thermally conductive molded article of the present invention is a polymer matrix of an olefin-based liquid resin, and a non-antimony oil having a dialkyl carbonate and a pyrophoric point of 250 ° C or higher contains a plasticizer in a predetermined ratio, and a thermally conductive filler. A hardened body in which the liquid combination mixture hardens. Each of the above components will be described below.

Polymer matrix: The polymer matrix is an olefin-based liquid resin. Since the olefin-based liquid resin is a non-cerium oxide polymer, contact failure due to low molecular weight enthalpy does not occur. Further, the olefin-based liquid resin is excellent in defoaming property in the production stage of the mixed thermally conductive filler even in the non-fluorene-based polymer, and the curing system having a long activation period can be adjusted. Further, heat resistance necessary for the thermally conductive molded body can be achieved.

By using a liquid resin having a reactive functional group in the molecule, the liquid mixed composition can be cured to form a thermally conductive molded body. Specifically, an olefin-based liquid resin having an acryl group, a vinyl group or the like can be used, and a liquid tree having a propylene group end is preferred in terms of a balance between reactivity and activation period. fat.

The number average molecular weight of the liquid resin is preferably in the range of 1,000 to 20,000, more preferably in the range of 5,000 to 7,000. When the number average molecular weight is less than 1,000, sufficient cross-linking structure cannot be obtained after hardening, and the mechanical strength of the thermally conductive molded body is lowered, and the brittleness becomes brittle. On the other hand, when the number average molecular weight exceeds 20,000, the viscosity is increased, and it is difficult to highly fill the thermally conductive filler.

The olefin-based liquid resin is, for example, a polyisobutylene or an ethylene-propylene polymer.

Thermal Conductive Filler: The thermally conductive filler may use a metal having high thermal conductivity, a metal oxide, a metal nitride, a metal carbide, a metal hydroxide, a carbon filler, or the like. Specifically, aluminum oxide, magnesium oxide, lead oxide, boron nitride, aluminum nitride, tantalum carbide, aluminum hydroxide, magnesium hydroxide, carbon fiber, black lead, and the like. Among the above-mentioned thermally conductive fillers, metal oxides, metal nitrides, metal carbides, and metal hydroxides are suitably used for applications requiring electrical insulation, and among these, high flame retardancy is used. It is preferred to use a metal hydroxide. On the other hand, carbon fibers are preferably used from the viewpoint of improving thermal conductivity. Carbon fiber is a diamagnetic body and can be easily aligned in any direction according to the average direction of the magnetic field. In the case of arranging a thermally conductive filler in accordance with a magnetic field, in particular, a permanent magnet and an electromagnet may be used, and a superconducting magnet is used as a magnetic field generating device.

Although a single thermally conductive filler can be used alone, the mixture of coatings can improve the balance of thermal conductivity and flame retardancy. Further, in order to impart considerations such as improvement in insulation and filling properties and suppression of cracking, a thermally conductive filler to which a surface treatment is applied may be used.

The content of the thermally conductive filler is preferably in the range of from 150 parts by weight to 5,400 parts by weight based on 100 parts by weight of the polymer substrate. When the amount is less than 150 parts by weight, the thermal conductivity of the thermally conductive molded body cannot be improved. When the amount is more than 5,400 parts by weight, the viscosity is increased to deteriorate the formability, and the hardness is increased to deteriorate the contact heat resistance.

Although the shape is not particularly limited, a thermally conductive filler such as a scaly shape, a needle shape, a granular shape or the like can be used. Among the above shapes, it is preferably a granular form which can be easily filled in a polymer matrix, and can be oriented in a fiber shape in any direction depending on a magnetic field and an electric field, or a flow field and a shear field.

The particle diameter of the thermally conductive filler is preferably from 0.1 μm to 100 μm, more preferably from 1 μm to 50 μm. When the viscosity is lower than 0.1 μm, the viscosity of the liquid mixed composition rises, which may make it difficult to form into a sheet. When it is larger than 100 μm, the hardening of the thermally conductive molded body becomes hard. Although the average particle diameter can be used for the particle diameter, it is preferable to mix two or more kinds of thermally conductive fillers having different average particle diameters because of high filling or softening of the hardness of the thermally conductive molded body.

Plasticizer: The first component is a component for reducing the viscosity of the liquid combination mixture of the thermally conductive filler contained in the liquid resin. The second is a component for making the hardness of the thermally conductive molded body soft. The above plasticizer contains a dialkyl carbonate and a non-antimony oil having a firing point of 250 ° C or higher.

The dynamic viscosity of the non-antimony oil having a firing point of 250 ° C or higher is preferably in the range of 70 mm ² /s to 400 mm ² /s, and the liquid mixed composition can be made low in viscosity. Further, the flame-retardant property of the thermally conductive molded article is hard to be deteriorated, and even when 300 parts by weight of the non-antimony oil is added to the weight portion of the polymer substrate 100, high flame retardancy (UL94 V-0) can be easily obtained. Examples of the non-antimony oil include a process oil, an aromatic processing oil, a naphthene processing oil, a co-oligomer of ethylene and an alpha olefin, and the like. mixture.

The dynamic viscosity of the dialkyl carbonate is preferably from 10 mm ² /s to 40 mm ² /s, and a low-viscosity liquid mixed composition having a low viscosity is added in a small amount. When the temperature is lower than 10 mm ² /s, the volatility is high because the low viscosity is excellent, and the hardness of the thermally conductive molded body may harden over time. On the other hand, when it is higher than 40 mm ² /s, the effect of low viscosity is lowered. The dialkyl carbonate is preferably ROCOOR (R is an alkyl group having 10 to 18 carbon atoms). The dialkyl carbonate is more effective in reducing the viscosity than the non-lanthanide oil. For example, a liquid mixed composition of 150 parts by weight of a dialkyl carbonate is added to 100 parts by weight of the polymer matrix, and 300 parts by weight is added to the non-anthraquinone oil. The liquid mixed composition has a lower viscosity.

The weight ratio of the dialkyl carbonate to the dialkyl carbonate in combination with the non-antimony oil having a firing point of 250 ° C or higher is 0.05 or more and less than 0.85. When it is blended in the above range, it is possible to obtain a thermally conductive composition which is not only low in viscosity in the liquid mixed composition but also suppresses deterioration in flame retardancy. The weight ratio of the dialkyl carbonate is less than 0.05, and the plasticizer cannot be stopped in the undischarged content while sufficiently reducing the viscosity of the liquid mixed composition. At 0.85 or more, the flame retardancy is liable to be lowered, and it is difficult to establish a suitable viscosity and flame retardancy.

The content of the dialkyl carbonate is less than 100 parts by weight to 100 parts by weight of the polymer matrix. When the content of the dialkyl carbonate exceeds 100 parts by weight, the flame retardancy of the thermally conductive molded body is lowered. Furthermore, for 100 parts by weight of the polymer matrix, less than 100 parts by weight, dialkyl carbonate is necessary The composition is such that the content is more than 0 parts by weight.

The total content of the dialkyl carbonate and the non-ruthenium oil may be from 121 parts by weight to 257 parts by weight to 100 parts by weight of the polymer matrix. When the weight is less than 121 parts, the thermally conductive filler cannot be filled high, and the thermal conductivity of the thermally conductive molded body cannot be improved. On the other hand, when it exceeds 257 parts by weight, the oil release of the plasticizer increases.

Further, the plasticizer is generally preferably a lower viscosity plasticizer suitable for a non-reactive plasticizer which is hard to harden after hardening. However, the low-viscosity plasticizer has a low ignition point, and when mixed with the polymer matrix, there is a problem that the flame retardancy is liable to be lowered, and when the non-reactive plasticizer is added in a large amount, there is a problem that the thermally conductive molded body releases oil. In particular, in order to improve the thermal conductivity, it is necessary to fill a large amount of the thermally conductive filler, and the problem that the amount of the plasticizer added increases must be solved. Dialkyl carbonates are also disadvantages of low viscosity plasticizers which deteriorate the flame retardancy. The principle is unknown, but the addition of a small amount of other plasticizers of the same viscosity makes the liquid mixed composition particularly low in viscosity. Therefore, by using the above characteristics, the combination of the dialkyl carbonate and the non-antimony oil in the above-mentioned predetermined ratio can solve the above problems.

Other components: In order to improve the flame retardancy of the thermally conductive molded body, it is preferred to add a flame retardant. As the flame retardant, a phosphorus-based flame retardant, a nitrogen-based flame retardant, a metal hydroxide or the like can be used, and a suitable flame retardant auxiliary can also be used in combination. Further, in order to improve the dispersibility of the thermally conductive filler, a dispersant and a coupling may be mixed. Further, in order to improve weather resistance, an oxidation preventive agent and an aging preventive agent may be added. Further, the liquid mixed composition may further contain a catalyst, a hardening retarder, and the like for the purpose of improving productivity, weather resistance, heat resistance, and the like. Deterioration inhibitors, etc. In addition to the above, various additives for various lifting functions can be added within the range not impairing the object of the present invention.

A method for producing a thermally conductive molded body: a raw material olefin-based liquid resin in which a thermally conductive molded body is mixed, a plasticizer, and a thermally conductive filler can be used to disperse the liquid conductive composition. And a method in which the liquid mixed composition is injected into a mold and then cured to form a thermally conductive molded body. Further, a method in which a liquid mixed composition is discharged onto a substrate such as a resin film or a metal plate to be cured is obtained.

Example

Preparation of sample: Samples 1 to 11 prepared in Examples of the present invention or Comparative Examples were described. The repeated parts of the description of the samples are omitted. The combination of Sample 1 to Sample 11 is shown in Table 1.

[sample 1]

In the polymer matrix, polyisopropene having a propylene group at the end (number average molecular weight = 5000): 67 parts by weight of a plasticizer dialkyl carbonate (C ₁₄ H ₂₉ OCOOC ₁₄ H ₂₉ , dynamic viscosity at 40 ° C 17.6) Mm ² /s ignition point 210 ° C): 33 parts by weight, thermal conductive filler, aluminum hydroxide having an average particle diameter of 10 μm: 240 parts by weight, aluminum hydroxide having an average particle diameter of 1 μm: 10 parts by weight, and an average fiber length of 100 μm Asphalt-based carbon fiber: 55 parts by weight, hardener (CR300, force Co., Ltd.): 2.5 parts by weight, platinum catalyst (PT-CS-3.2cS, manufactured by Ferro (USA)): 0.2 parts by weight, flame retardant red phosphorus ( 120 UF, manufactured by Phosphorus Chemical Co., Ltd.): 10 parts by weight was mixed by a vibrating stirrer to prepare a liquid mixed composition. A titanate coupling agent can also be used as a surface treatment agent in the thermally conductive filler. Further, the thermally conductive filler and other additives may be added in a certain amount to the total amount of the polymer matrix and the plasticizer.

After the liquid mixed composition was vacuum-deaerated, a mold cavity having a sheet shape was injected, and a magnetic field having a magnetic flux density of 8 Tesla was applied to align the carbon fibers in the thickness direction. Thereafter, the mixture was heated in an atmosphere of 130 ° C for 1 hour to cure the liquid mixed composition to obtain a sheet-shaped thermally conductive molded body.

[sample 2, sample 3]

A sample in which the amount of dialkyl carbonate added to the sample 1 was changed.

[sample 4 ~ sample 8]

Paraffin oil (PW-90, manufactured by Idemitsu Kosan Co., Ltd., 40 ° C dynamic viscosity 90 mm ² /s, ignition point 272 ° C) and non-antimony oil with a fire point of 250 ° C or higher is added as a plasticity to the aforementioned dialkyl carbonate. The mixture is mixed into a sample.

[sample 9 ~ sample 11]

Use only non-lanthanum oil as a plasticizer sample.

Evaluation of samples:

Each of the thermally conductive molded articles prepared in the above samples 1 to 11 and each of the liquid mixed compositions obtained in the production process were subjected to various tests and evaluated. The evaluation method is as follows, and the evaluation results are shown in Table 1.

[Viscosity of liquid mixed composition]

Using a rotary viscometer (manufactured by Brooks Field, Inc., product: DV-E type, No. 14), the viscosity of the liquid mixed composition was measured at a number of revolutions of 10 rpm in an atmosphere of 25 °C.

[oil release]

The degree of oil release of the thermally conductive shaped body was evaluated.

The thermally conductive molded body was placed in a thermostatic chamber at 100 ° C for 24 hours, and then the surface of the thermally conductive molded body was visually observed. In the "release oil" column of the table, "Yes" indicates that the test piece has oil release, and "None" means that the test piece does not release oil.

[flammability]

The flame retardancy of thermally conductive shaped bodies is based on the US UL (UnderWriters) The combustion test (UL94) developed by Laboratories Inc) was evaluated.

A test piece (length: 127 mm x width: 12.7 mm x thickness: 1 mm or 0.5 mm) of each sample was placed so that the longitudinal direction of the test piece was placed in a straight direction with a fixing jig, and the burner (caliber: 10 mm, length: about 10 cm) was fired. After 10 seconds, the flame was recorded to record the burning time of each test piece. Then, after the second contact with the flame, the holding time of the fire (glow time) is recorded whether there is a drop of the absorbent cotton that is placed under the test piece. The above operation was carried out for each test piece, and one group was made 5 times. Based on the criteria in Table 2, it is judged whether or not it meets "V-0" (Table 2 is "94V-0") or "V-1" (Table 2 is "94V-1"). In the above-mentioned criteria for determining the flame retardancy, "V-0" indicates that the flame retardancy is higher than "V-1", and the test standard for "V-1" is a test piece that fails the test, and it is judged that there is no flame retardancy. The "flame retardance" column in the middle is described as "X".

[thermal impedance]

The thermal impedance of the thermally conductive molded body was measured.

As shown in Fig. 7, the heating element (25) and the heat radiator (26) on the substrate (24) (Heatsink Co., Ltd.) Manufactured FH-60-30), and a fan (air volume: 0.01 kg/sec, wind pressure: 49 Pa) provided on the upper part thereof, and clamped the test piece (27) of sample 1 to sample 11 (cut to a size of 10 mm x 10 mm) ), a load (28) was placed on the heat radiator (26) and a certain weight (40 N) was applied to the test piece (27). After the heat generating body (25) was left in a state of being heated for 10 minutes, the outer surface temperature T1 of the heat generating body (25) side of the test piece (27) and the outer surface temperature T2 of the heat radiating body (26) side were detected by the detecting machine (29). Further, the thermal resistance value of the test piece (27) was calculated by the following formula (1). The heating element (25) is usually an electronic component representing a CPU. The heat generation of the heating element (25) of this test is a heater using 25 W because of the simplification and rapid evaluation of the sheet performance.

Thermal resistance value (°C/W)=(T1(°C)-T2(°C))/heating capacity (W).........Formula (I)

Analysis of the results of each test evaluation: [Viscosity of liquid mixed composition]

Figure 2 is a graph showing the viscosity of a liquid mixed composition, the X-axis is the ratio of the dialkyl carbonate in the plasticizer, and the Y-axis is the amount of the plasticizer.

When the weight ratio of the dialkyl carbonate in the plasticizer composed of the non-antimony oil and the dialkyl carbonate is large, the viscosity of the liquid mixed composition can be low, even if the total amount of the plasticizer is small. The values of these viscosities are evaluated for viscosity from actual workability. Specifically, the foaming property of the liquid mixed composition was excellent, and when the sheet was produced by a hybrid coater, the thickness of the sheet was the same as the set thickness, and the "evaluation of viscosity" in Table 1 was "○". Further, in particular, in a relationship in which the viscosity is relatively low, a person who has a high setting speed at the time of sheet formation and can produce a heat conductive molded body having a desired thickness is "◎". On the other hand, off When the foaming property is deteriorated to affect the defoaming time, or when a sheet is produced by a blend coater, the fluidity of the liquid mixed composition is deteriorated, and it is difficult to adjust the thickness of the sheet to a desired thickness, and it is represented by "X".

Next, the viscosity of the liquid mixed composition was analyzed in detail, and the relationship between the blending amount of the plasticizers of Samples 1 to 11 and the viscosity was shown in Fig. 1 .

In Fig. 1, "DAC" means a dialkyl carbonate, and the following figures are the ratio of the dialkyl carbonate of the dialkyl carbonate and the non-lanthanide oil in the plasticizer. For example, "DAC1.0" means that the ratio of dialkyl carbonate is 1.0 (dialkyl carbonate is 100% and does not contain non-antimony oil), and "DAC0.5" means that the ratio of dialkyl carbonate is 0.5. (Dialkyl carbonate is 50% but not lanthanide oil is 50%).

According to the measurement results, when the ratio of the dialkyl carbonate in the plasticizer is constant, the relationship between the amount of the plasticizer and the viscosity can be calculated by the following formulas (2) to (5).

y=1.78×10 ⁴ x ^-0.460 formula (2). The ratio of dialkyl carbonate is 1.0

y=2.72×10 ⁴ x ^-0.684 Equation (3). The ratio of dialkyl carbonate is 0.5

y=8.63×10 ⁴ x ^-0.778 formula (4). The ratio of dialkyl carbonate is 0.33

y=3.64×10 ⁴ x ^-0.658 Equation (5). The ratio of dialkyl carbonate is 0

However, x represents the viscosity (mPa.s) of the liquid mixed composition, and y represents the amount (weight portion) of the plasticizer to the weight portion of the polymer matrix 100.

However, there is only one sample with a ratio of dialkyl carbonate of 0.1. It cannot be approximated. Further, in the present invention, the approximate expressions are all the least squares method.

The approximated formula is substituted for any viscosity value, and the viscosity of the liquid mixed composition can estimate the amount of the plasticizer blended as described above. For example, the substitution viscosity is 56000mPa. s, the ratio of each dialkyl carbonate, the viscosity can be calculated 56000mPa. The amount of plasticizer when s.

Then, using the approximate expressions obtained in Fig. 1, the viscosity is calculated from equations (2) to (5) and the viscosity is 56000 mPa. S and viscosity 42000mPa. The amount of the plasticizer in the case of S, the X-axis in the figure is "the ratio of the dialkyl carbonate in the plasticizer", and the Y-axis "the amount of the plasticizer (weight portion)". Thus, as shown in Figure 2, the viscosity is 56000mPa. The viscosity curve of S (curve 1) and the viscosity of 42000mPa. The equivalent viscosity curve of S (curve 2). Furthermore, 56000mPa. S is the viscosity of sample 4, 42000 mPa. S is the viscosity of the sample 5.

Then, as shown in Fig. 2, sample 1 to sample 11 are drawn to have a viscosity of 56000 mPa. The iso-viscosity curve of S (curve 1) is a reference, and a sample having a lower viscosity than the viscosity curve is a sample having a better viscosity, and a sample having a higher viscosity than the viscosity curve is a third-figure as a position of a high-viscosity sample. As can be seen from Fig. 3, the viscosity of the sample mixed with the paraffin oil and the paraffin oil was lower than that of the above-mentioned respective samples used alone. Therefore, the combination of a dialkyl carbonate and a paraffin oil is seen to have a synergistic effect of a decrease in viscosity.

[flammability]

Fig. 4 is a test result of the flame retardancy when the sample 1 to the sample 11 are drawn, the X-axis is "the ratio of the dialkyl carbonate in the plasticizer", and the Y-axis is "plastic" The amount of the compound (weight portion) is "○" for the sample having flame retardancy, and "●" for the case of non-flammability.

When the weight ratio of the dialkyl carbonate is large, the flame retardancy tends to deteriorate rapidly.

The evaluation result of the flame retardancy was estimated based on the evaluation results of the sample 2, the sample 4, and the sample 8. In other words, the sample 2 and the sample 8 in which the dialkyl carbonate in the plasticizer having a polymer base value of 100 parts by weight is 100 parts by weight is not flame retardant, and the sample 2 when the dialkyl carbonate is 97 parts by weight Flame retardant V-0. In addition, even with the influence of the paraffin oil, the sample 2 having less paraffin oil than the sample 5 and the sample 8 having a large amount of paraffin oil have different evaluation results of flame retardancy, and therefore paraffin wax within the scope of the present invention The amount of oil blended has little effect on flame retardancy. From the above, it can be seen that the weight portion of the dialkyl carbonate 100 is not flammable. According to the above analysis, Fig. 4 shows a curve 3 (flame retardation boundary value curve) of 100 parts by weight of the dialkyl carbonate.

[oil release]

Fig. 5 shows the evaluation results of the oil release of each sample. The compounding amount of the plasticizer was 300 parts by weight, and a large amount of the sample 8 and the sample 11 were found to release oil, and the other samples did not cause oil release. In the evaluation results, when the weight ratio of the sample dialkyl carbonate having the same amount of the plasticizer is increased, there is no sample which is easy to release oil, and at least 257 parts by weight of the sample 10 is the upper limit, and the following plasticizer is blended. The amount can be seen as not causing oil release. Therefore, the auxiliary line for the "existing" oil release sample and the "no" oil release sample is represented by a straight line 4 (y = 257 straight line) (an oil release line value straight line).

The above experimental example (production and evaluation of the sample) is an example of the present invention, for example, by using the polymer base value and the viscosity of the plasticizer, the blending amount of the flame retardant and the heat conductive filler, the liquid mixed composition The viscosity and the amount most suitable for the plasticizer will vary. However, the thermal conductivity of the thermally conductive molded body is improved, and even if the blending is adjusted, the boundary between the moldability, the release of oil, and the flame retardancy is naturally matched. For the blending of the boundary, the plasticizer "dialkyl" The carbonate is mixed with a non-antimony oil having a firing point of 250 ° C or higher, and the amount of the dialkyl carbonate is less than 100 parts by weight based on 100 parts by weight of the polymer base value, and a liquid which is easier to form than the conventional one can be obtained. In the case of a mixed composition, a thermally conductive composition which is excellent in flame retardancy can be obtained by blending a plurality of thermally conductive fillers to improve thermal conductivity and suppressing oil release of a plasticizer.

From the above viewpoint, the evaluation results of the experimental examples are reviewed using the sixth figure, from "the intersection of the curve 1 indicating the viscosity of 56000 mPa‧s and the straight line of the oil release boundary line (line 4)" to "the curve 1 indicating the viscosity of 56000 mPa‧s and the difficulty When the ratio of the flammability boundary value straight line (curve 3) (but not including the intersection point), that is, the ratio of the dialkyl carbonate to 0.05 or more and less than 0.85, the above result is a more appropriate ratio. In the above range, the amount of the plasticizer blended in the materials used in this experimental example can be estimated to be 121 to 257 parts by weight.

When the range of the dialkyl carbonate is in the range of 0.21 to 0.60, the thermal conductivity is improved, and the moldability and oil release are suppressed, and the flame retardancy characteristics can be satisfied. 2, when the amount of the thermally conductive filler is large, the viscosity of the liquid mixed composition is a low viscosity. In this case, the curve 2 indicating the viscosity of 42000 mPa·s and the line of the oil release boundary are straight. straight line 4) The intersection point)" to "the intersection of the curve 2 indicating the viscosity of 42000mPa‧s and the line of the flame retardant boundary line (curve 3) (but not including the intersection point)", that is, the ratio of the dialkyl carbonate is 0.21 or more and less than 0.60. Time. In the above range, the amount of the plasticizer to be used in the material used in the experimental example can be estimated to be 166 to 257 parts by weight.

Furthermore, the above-described embodiment is an example of the present invention, and is not limited to the above-described embodiment, and any modification can be made without departing from the gist of the present invention.

24‧‧‧Substrate

25‧‧‧heating body

26‧‧‧ Heat sink

27‧‧‧Test piece

28‧‧‧Load

29‧‧‧Measurement machine

Figure 1 is a graph showing the relationship between the amount of plasticizer and the viscosity.

Figure 2 is a graph illustrating the iso-viscosity curve.

Fig. 3 is a graph plotting the iso-viscosity curves of Sample 1 to Sample 11.

Fig. 4 is a graph showing the range of the amount of the dialkyl carbonate not exceeding 100 parts by weight.

Figure 5 is a graph illustrating the boundary value of the oil release.

Figure 6 is a graph illustrating the range of ratios of the most suitable dialkyl carbonates.

Fig. 7 is an explanatory view showing a device for evaluating thermal impedance.

Claims (5)

A thermally conductive molded body comprising a polymer matrix, a plasticizer and a thermally conductive filler, wherein the polymer matrix is a hardened body of an olefin-based liquid resin, and the hardened body of the olefin-based liquid resin comprises a propylene group a vinyl olefin-based liquid resin; the plasticizer is a non-anthracene oil comprising a dialkyl carbonate and a pyrophoric point of 250 ° C or higher; and a dialkyl carbonate of a dialkyl carbonate and a non-lanthanide oil; The weight ratio is 0.05 or more and less than 0.85, and the content of the dialkyl carbonate is less than 100 parts by weight to the weight portion of the polymer matrix 100, and the thermally conductive filler includes metal, metal oxide, metal nitride, metal carbonization. Matter, metal hydroxide, carbon filler. The thermally conductive molded article according to claim 1, wherein the content of the dialkyl carbonate and the non-antimony oil is from 121 parts by weight to 257 parts by weight to the weight portion of the polymer matrix 100. The thermally conductive molded article according to claim 1, wherein the thermally conductive filler is a thermally conductive filler comprising a metal hydroxide. The thermally conductive molded article according to claim 1, wherein the polymer matrix is a polymer matrix mainly composed of polyisobutylene. The thermally conductive molded body according to claim 1, wherein the non-antimony oil is paraffin oil.