WO2022176725A1 - 熱伝導性シート、および電子機器 - Google Patents
熱伝導性シート、および電子機器 Download PDFInfo
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- WO2022176725A1 WO2022176725A1 PCT/JP2022/005029 JP2022005029W WO2022176725A1 WO 2022176725 A1 WO2022176725 A1 WO 2022176725A1 JP 2022005029 W JP2022005029 W JP 2022005029W WO 2022176725 A1 WO2022176725 A1 WO 2022176725A1
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- thermally conductive
- conductive sheet
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- filler
- heat
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- H01L23/36—Selection of materials, or shaping, to facilitate cooling or heating, e.g. heatsinks
- H01L23/373—Cooling facilitated by selection of materials for the device or materials for thermal expansion adaptation, e.g. carbon
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- H01L23/36—Selection of materials, or shaping, to facilitate cooling or heating, e.g. heatsinks
- H01L23/373—Cooling facilitated by selection of materials for the device or materials for thermal expansion adaptation, e.g. carbon
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- H01L2924/053—Oxides composed of metals from groups of the periodic table
- H01L2924/0543—13th Group
- H01L2924/05432—Al2O3
Definitions
- the present invention relates to thermally conductive sheets and electronic devices.
- the semiconductor is attached to a heat sink such as a heat dissipating fan or a heat dissipating plate via a heat conductive sheet.
- a heat conductive sheet a material in which a filler such as an inorganic filler is dispersed in silicone is widely used. In such heat dissipating members, there is a demand for further improvement in thermal conductivity.
- the filling rate of the inorganic filler to the thermally conductive sheet is increased, the flexibility of the thermally conductive sheet will be impaired, and the high filling rate of the inorganic filler will cause powder to fall off.
- inorganic fillers include alumina, aluminum nitride, and aluminum hydroxide.
- the matrix may be filled with scaly particles such as boron nitride or graphite, carbon fiber, or the like. This is due to the anisotropy of the thermal conductivity of the scaly particles and the like.
- carbon fiber in the case of carbon fiber, it has a thermal conductivity of about 600 to 1200 W/mK in the fiber direction.
- Boron nitride has a thermal conductivity of about 110 W/mK in the plane direction and about 2 W/mK in the direction perpendicular to the plane direction, and is known to have anisotropy. .
- the surface direction of the carbon fibers and scale-like particles is made the same as the thickness direction of the sheet, which is the direction of heat transfer. That is, by orienting the carbon fibers and the scale-like particles in the thickness direction of the sheet, the thermal conductivity can be dramatically improved.
- an insulating thermally conductive sheet is manufactured by filling a ceramic filler such as alumina, but since the thermal conductivity of the thermally conductive filler is low, a thermally conductive sheet with low thermal resistance cannot be obtained.
- Boron nitride is an example of a ceramic filler with high thermal conductivity. Since boron nitride has a scaly shape, high thermal conductivity cannot be obtained unless it is oriented in the thickness direction.
- boron nitride can be oriented in the thickness direction of the thermally conductive sheet.
- the thermal conductivity of the insulating filler is inferior to that of the conductive filler.
- the thermally conductive sheet according to the present invention includes a binder and an anisotropic thermally conductive filler, and the anisotropic thermally conductive filler is oriented in the thickness direction. It is a conductive sheet, and one surface of the thermally conductive sheet has an Sa of 5 ⁇ m or less, an Sz of 50 ⁇ m or less, and a dielectric breakdown voltage of 0.5 kV/mm or more.
- FIG. 1 is a diagram showing an example of a heat conductive sheet to which the present technology is applied.
- FIG. 2 is a perspective view showing an example of a process of slicing a thermally conductive compact.
- FIG. 3 is a diagram illustrating an example of a semiconductor device;
- FIG. 1 is a diagram showing an example of a thermally conductive sheet to which the present technology is applied.
- a thermally conductive sheet 1 shown in FIG. 1 has a sheet body 2 and a resin coating layer 5 .
- the sheet body 2 is obtained by curing a binder resin containing at least a polymer matrix component and a fibrous thermally conductive filler.
- the resin coating layer 5 is formed of an uncured component of the polymer matrix component exuded from the sheet body 2 .
- a first release film 3 is attached to one surface 2 a of the sheet body 2
- a second release film 4 is attached to the other surface 2 b of the sheet body 2 .
- the thermally conductive sheet 1 has a tackiness (adhesiveness) due to the resin coating layer 5 formed on one surface 2a and the other surface 2b. By peeling off 4, the sheet body 2 can be attached to a predetermined position. Thereby, the thermally conductive sheet 1 is excellent in workability and handleability. In addition, the thermally conductive sheet 1 is excellent in reworkability, such as correcting misalignment between the electronic component and the heat radiating member during assembly, dismantling for some reason after once assembled, and reassembling. .
- thermosetting polymer examples include crosslinked rubber, epoxy resin, polyimide resin, bismaleimide resin, benzocyclobutene resin, phenol resin, unsaturated polyester, diallyl phthalate resin, silicone resin, polyurethane, polyimide silicone, thermosetting type Polyphenylene ether, thermosetting modified polyphenylene ether, and the like can be mentioned. These may be used individually by 1 type, and may use 2 or more types together.
- crosslinked rubber examples include natural rubber, butadiene rubber, isoprene rubber, nitrile rubber, hydrogenated nitrile rubber, chloroprene rubber, ethylene propylene rubber, chlorinated polyethylene, chlorosulfonated polyethylene, butyl rubber, halogenated butyl rubber, fluorine rubber, urethane rubber, acrylic rubber, polyisobutylene rubber, silicone rubber and the like. These may be used individually by 1 type, and may use 2 or more types together.
- the silicone resin is preferably a silicone resin composed of a liquid silicone gel main agent and a curing agent.
- silicone resins include addition reaction type liquid silicone resins, heat vulcanization type millable type silicone resins using peroxide for vulcanization, and the like.
- the addition reaction type liquid silicone resin is particularly preferable as a heat dissipation member for electronic equipment, since adhesion between the heat generating surface of the electronic component and the heat sink surface is required.
- addition reaction type liquid silicone resin it is preferable to use a two-liquid addition reaction type silicone resin or the like in which polyorganosiloxane having a vinyl group is used as a main component and polyorganosiloxane having an Si—H group is used as a curing agent. .
- the liquid silicone component has a silicone A liquid component as a main agent and a silicone B liquid component containing a curing agent, and the silicone A liquid component and the silicone B liquid component are blended in a predetermined ratio.
- the mixing ratio of the silicone A liquid component and the silicone B liquid component can be adjusted as appropriate. 4
- the uncured component of the polymer matrix component is allowed to bleed and the resin coating layer 5 can be formed.
- the content of the polymer matrix component in the thermally conductive sheet 1 is not particularly limited and can be appropriately selected according to the purpose. From the point of view, it is preferably about 15% to 50% by volume, more preferably 20% to 45% by volume.
- the fibrous thermally conductive filler contained in the thermally conductive sheet 1 is a component for improving the thermal conductivity of the sheet.
- the type of thermally conductive filler is not particularly limited as long as it is a fibrous material with high thermal conductivity, but it is preferable to use carbon fiber from the viewpoint of obtaining higher thermal conductivity.
- the type of carbon fiber is not particularly limited, and can be appropriately selected according to the purpose.
- pitch-based, PAN-based, graphitized PBO fiber arc discharge method, laser evaporation method, CVD method (chemical vapor deposition method), CCVD method (catalytic chemical vapor deposition method), etc.
- CVD method chemical vapor deposition method
- CCVD method catalytic chemical vapor deposition method
- carbon fibers obtained by graphitizing PBO fibers and pitch-based carbon fibers are more preferable because high thermal conductivity can be obtained.
- the carbon fiber can be partially or wholly surface-treated as necessary.
- the surface treatment for example, oxidation treatment, nitriding treatment, nitration, sulfonation, or attaching or attaching a metal, a metal compound, an organic compound, etc. to the surface of the functional group or carbon fiber introduced to the surface by these treatments, or A process of combining, etc., may be mentioned.
- the functional group include hydroxyl group, carboxyl group, carbonyl group, nitro group, amino group and the like.
- the carbon fiber may be coated with an insulator at least part of its surface.
- Materials used for the coating include insulating inorganic substances such as SiO2, and thermosetting or UV-curable resins such as epoxy resins, (meth)acrylic resins, and divinylbenzene.
- coating methods include deposition on the surface of carbon fibers by a sol-gel method if the insulator is an inorganic material.
- thermosetting resins carbon fibers are added to a solution in which a monomer and a polymerization initiator or a curing agent are dissolved, and the polymerization reaction is carried out while stirring to deposit a solvent-insoluble polymer on the surface of the carbon fibers. A coating method and the like can be mentioned.
- a thermosetting resin it is preferable to use a bifunctional or higher monomer.
- the average fiber length (average long axis length) of the carbon fibers is not particularly limited and can be selected as appropriate. , more preferably in the range of 75 ⁇ m to 275 ⁇ m, and particularly preferably in the range of 90 ⁇ m to 250 ⁇ m.
- the average fiber diameter (average minor axis length) of the carbon fibers is not particularly limited and can be appropriately selected, but from the point of reliably obtaining high thermal conductivity, it is in the range of 4 ⁇ m to 20 ⁇ m. more preferably in the range of 5 ⁇ m to 14 ⁇ m.
- the aspect ratio (average major axis length/average minor axis length) of the carbon fibers is preferably 8 or more, more preferably 9 to 30, in order to reliably obtain high thermal conductivity. . If the aspect ratio is less than 8, the fiber length (major axis length) of the carbon fibers is short, and the thermal conductivity may decrease. Since the dispersibility at the temperature decreases, there is a possibility that sufficient thermal conductivity cannot be obtained.
- the content of the fibrous thermally conductive filler in the thermally conductive sheet 1 is not particularly limited and can be appropriately selected according to the purpose. is preferred, and 5% to 35% by volume is more preferred. If the content is less than 4% by volume, it may be difficult to obtain a sufficiently low thermal resistance. This may affect the orientation of the conductive filler.
- the content of the thermally conductive filler including the fibrous thermally conductive filler in the thermally conductive sheet 1 is preferably 15% by volume to 75% by volume.
- the thermally conductive sheet 1 may further contain an inorganic filler as a thermally conductive filler.
- an inorganic filler By containing the inorganic filler, the thermal conductivity of the thermally conductive sheet 1 can be further increased, and the strength of the sheet can be improved.
- the shape, material, average particle size, etc. of the inorganic filler are not particularly limited, and can be appropriately selected according to the purpose. Examples of the shape include spherical, ellipsoidal, massive, granular, flat, needle-like, and the like. Among these, a spherical shape and an elliptical shape are preferable from the viewpoint of filling properties, and a spherical shape is particularly preferable.
- Examples of materials for the inorganic filler include aluminum nitride (aluminum nitride: AlN), silica, alumina (aluminum oxide), boron nitride, titania, glass, zinc oxide, silicon carbide, silicon (silicone), silicon oxide, and metal particles. etc. These may be used individually by 1 type, and may use 2 or more types together. Among these, alumina, boron nitride, aluminum nitride, zinc oxide, and silica are preferred, and alumina and aluminum nitride are particularly preferred from the viewpoint of thermal conductivity.
- the inorganic filler can be surface-treated.
- the inorganic filler is treated with a coupling agent as the surface treatment, the dispersibility of the inorganic filler is improved and the flexibility of the thermally conductive sheet 1 is improved.
- the average particle size of the inorganic filler can be appropriately selected according to the type of inorganic material.
- the inorganic filler is alumina
- its average particle size is preferably 1 ⁇ m to 10 ⁇ m, more preferably 1 ⁇ m to 5 ⁇ m, and particularly preferably 4 ⁇ m to 5 ⁇ m. If the average particle size is less than 1 ⁇ m, the viscosity increases and mixing may become difficult. On the other hand, if the average particle size exceeds 10 ⁇ m, the thermal resistance of the thermally conductive sheet 1 may increase.
- the inorganic filler is aluminum nitride
- its average particle size is preferably 0.3 ⁇ m to 6.0 ⁇ m, more preferably 0.3 ⁇ m to 2.0 ⁇ m, and more preferably 0.5 ⁇ m to 1.0 ⁇ m. 5 ⁇ m is particularly preferred. If the average particle diameter is less than 0.3 ⁇ m, the viscosity may increase and mixing may become difficult.
- the average particle diameter of the inorganic filler can be measured, for example, with a particle size distribution meter or scanning electron microscope (SEM).
- the inorganic filler may be used instead of the fibrous thermally conductive filler.
- the shape is preferably needle-like or scale-like, and particularly preferably scale-like, because it is easy to exhibit thermal conductivity in the thickness direction.
- Boron nitride is preferable as the material for the scale-like inorganic filler.
- the thermally conductive sheet 1 can also contain other components as appropriate, depending on the purpose.
- Other components include, for example, magnetic powders, thixotropic agents, dispersants, curing accelerators, retarders, slight tackifiers, plasticizers, flame retardants, antioxidants, stabilizers, colorants, and the like.
- electromagnetic wave absorption performance may be imparted to the thermally conductive sheet 1 by adjusting the content of the magnetic powder.
- the thermally conductive sheet 1 may be imparted with electromagnetic wave absorption performance by adjusting the content of the magnetic powder.
- the type of the magnetic powder is not particularly limited as long as it has magnetic properties, and known magnetic powders can be appropriately selected.
- amorphous metal powder or crystalline metal powder can be used.
- amorphous metal powder include Fe--Si--B--Cr, Fe--Si--B, Co--Si--B, Co--Zr, Co--Nb and Co--Ta.
- the crystalline metal powder for example, pure iron, Fe-based, Co-based, Ni-based, Fe--Ni-based, Fe--Co-based, Fe--Al-based, Fe--Si-based, Fe--Si--Al-based , and Fe--Ni--Si--Al systems.
- a microcrystalline metal finely divided by adding a small amount of N (nitrogen), C (carbon), O (oxygen), B (boron), etc. may be used.
- the magnetic metal powder a mixture of two or more kinds of different materials or different average particle diameters may be used.
- the shape of the magnetic metal powder is spherical, flat, or the like.
- spherical magnetic metal powder having a particle size of several ⁇ m to several tens of ⁇ m.
- Such magnetic metal powder can be produced, for example, by an atomizing method or a method of thermally decomposing metal carbonyl.
- the atomization method has the advantage that it is easy to make spherical powder. Molten metal is flown out from a nozzle, and a jet stream of air, water, inert gas, etc. is blown onto the flown out molten metal to solidify it as droplets. It is a method of making powder.
- the cooling rate is preferably about 1 ⁇ 10 6 (K/s) in order to prevent the molten metal from crystallizing.
- the surface of the amorphous alloy powder can be made smooth.
- the filling property can be further improved by performing a coupling treatment.
- the manufacturing process of the thermally conductive sheet 1 to which the present technology is applied involves molding a thermally conductive resin composition containing a fibrous thermally conductive filler in a polymer matrix component into a predetermined shape and curing the composition. , a step of forming a thermally conductive molded body (step A), a step of slicing the thermally conductive molded body into sheets to form a molded body sheet (step B), and applying the molded body sheet to the first release film 3 and a second release film 4, and a step (step C) of smoothing the surface of the molded body sheet and forming a resin coating layer 5 by pressing.
- a fibrous thermally conductive filler will be described, but the same manufacturing process can be used when using a scale-like inorganic filler instead of the fibrous thermally conductive filler.
- the following steps can also be read appropriately.
- Step A the above-described polymer matrix component, fibrous thermally conductive filler, appropriately contained inorganic filler, and other components are blended to prepare a thermally conductive resin composition.
- the procedure for blending and preparing each component is not particularly limited.
- a fibrous thermally conductive filler, as appropriate, inorganic filler, magnetic powder, and other components are added to the polymer matrix component and mixed.
- the thermally conductive resin composition is prepared.
- a fibrous thermally conductive filler such as carbon fiber is oriented in one direction.
- the method for orienting the filler is not particularly limited as long as it can be oriented in one direction.
- the fibrous thermally conductive filler can be unidirectionally oriented relatively easily by extruding or press-fitting the thermally conductive resin composition into a hollow mold under high shearing force.
- the orientation of the fibrous thermally conductive filler is the same (within ⁇ 10°).
- Specific examples of the above-described method of extruding or press-fitting the thermally conductive resin composition into a hollow mold under a high shear force include an extrusion molding method and a mold molding method.
- the extrusion molding method when the thermally conductive resin composition is extruded from a die, or in the mold molding method, when the thermally conductive resin composition is pressed into a mold, the thermally conductive resin composition
- the fibrous thermally conductive filler is oriented along the flow direction. At this time, if a slit is attached to the tip of the die, the fibrous thermally conductive filler is more likely to be oriented.
- thermally conductive resin composition extruded or press-fitted into the hollow mold was molded into a block shape corresponding to the shape and size of the mold, and the orientation of the fibrous thermally conductive filler was maintained.
- a thermally conductive compact is formed by curing the polymeric matrix component as it is.
- a thermally conductive molded body refers to a base material (molded body) for sheet cutting, which is the basis of the thermally conductive sheet 1 obtained by cutting into a predetermined size.
- the size and shape of the hollow mold and the heat conductive molded body can be determined according to the required size and shape of the heat conductive sheet 1.
- the vertical size of the cross section is 0.5 cm to 0.5 cm.
- a rectangular parallelepiped with a width of 15 cm and a width of 0.5 cm to 15 cm is exemplified.
- the length of the rectangular parallelepiped may be determined as required.
- the method and conditions for curing the polymer matrix component can be changed according to the type of the polymer matrix component.
- the curing temperature in thermosetting can be adjusted.
- the thermosetting resin contains a base liquid silicone gel and a curing agent, it is preferable to cure at a curing temperature of 80°C to 120°C.
- the curing time in thermosetting is not particularly limited, but it can be 1 hour to 10 hours.
- Step B As shown in FIG. 2, in the step B of slicing the thermally conductive compact 6 into sheets to form a compact sheet 7, the longitudinal direction of the oriented fibrous thermally conductive filler is 0
- the thermally conductive molding 6 is cut into sheets at an angle of between 45° and 90°, preferably between 45° and 90°. Thereby, the fibrous thermally conductive filler is oriented in the thickness direction of the sheet body 2 .
- the cutting of the thermally conductive compact 6 is performed using a slicing device.
- the slicing device is not particularly limited as long as it can cut the thermally conductive compact 6, and a known slicing device can be used as appropriate.
- a known slicing device can be used as appropriate.
- an ultrasonic cutter, a planer, or the like can be used.
- the slice thickness of the thermally conductive molded body 6 is the thickness of the sheet body 2 of the thermally conductive sheet 1, and can be appropriately set according to the application of the thermally conductive sheet 1. For example, it is 0.5 to 3.0 mm. be.
- step C the first release film 3 is attached to one surface of the molded sheet 7, and the second release film 4 is attached to the other surface of the molded sheet 7 and pressed.
- the surface of the molded body sheet 7 is smoothed and the uncured component of the polymer matrix component is bled out, and the space between one surface of the molded body sheet 7 and the first release film 3 and between the molded body sheet 7 is removed.
- a resin coating layer 5 is formed between the other surface of and the second release film 4 .
- the surfaces 2a and 2b of the thermally conductive sheet 1 are sliced surfaces and pressed after being sliced.
- the thermally conductive sheet 1 is formed, and the unevenness of the sheet surface is reduced, and the exposed fibrous thermally conductive filler is coated to improve the adhesion with the heat source and the heat dissipating member. It is possible to reduce the interfacial contact resistance and improve the heat transfer efficiency.
- the pressing can be performed, for example, by using a pair of pressing devices consisting of a flat plate and a press head with a flat surface. Moreover, you may press using a pinch roll.
- the pressure at the time of pressing is not particularly limited and can be appropriately selected according to the purpose. Therefore, the pressure range is preferably 0.1 MPa to 100 MPa, more preferably 0.5 MPa to 95 MPa.
- first release film 3 and the second release film 4 attached to both sides of the molded sheet 7 for example, plastic films such as PET films and polyethylene films can be used.
- first release film 3 and the second release film 4 may be subjected to release treatment such as wax treatment or fluorine treatment on the surface to be attached to the surface of the molded body sheet 7 .
- first release film 3 and the second release film 4 may be embossed.
- the first release film 3 and the second release film 4 are formed to have different peel strengths (N) from the sheet body 2 by making the thickness and/or material different.
- N peel strengths
- a PET film having a thickness of 25 ⁇ m with wax treatment is used as the first release film 3
- an embossed polyethylene film with a thickness of 80 ⁇ m is used as the second release film 4 .
- the peel strength (N) from the sheet body 2 is the first
- the release film 3 is 0.03 (N) (bending radius of 3 mm)
- the second release film 4 is 0.05 (N) (bending radius of 0.5 mm or less).
- one surface 2a of the sheet body 2 where the resin coating layer 5 is exposed is attached to an electronic component such as a semiconductor device or a heat dissipation member such as a heat sink, and then the second release film 4 is attached to the sheet body 2. is peeled off from the other surface 2b.
- the thermally conductive sheet 1 is mounted on a semiconductor device 50 built in various electronic devices and sandwiched between a heat source and a heat radiating member.
- a semiconductor device 50 shown in FIG. 3 has at least an electronic component 51 , a heat spreader 52 , and a thermally conductive sheet 1 .
- the thermally conductive sheet 1 is sandwiched between the heat spreader 52 and the heat sink 53 , thereby forming a heat dissipation member for dissipating the heat of the electronic component 51 together with the heat spreader 52 .
- the electronic component 51 is not particularly limited and can be appropriately selected according to the purpose. Examples thereof include CPU, MPU, graphic processing elements, various semiconductor elements such as image sensors, antenna elements, and batteries.
- the heat spreader 52 is not particularly limited as long as it is a member that dissipates the heat generated by the electronic component 51, and can be appropriately selected according to the purpose.
- the thermally conductive sheet 1 the semiconductor device 50 has a high heat dissipation property and, depending on the content of the magnetic powder in the sheet body 2 , is also excellent in electromagnetic wave suppressing effect.
- the mounting location of the thermally conductive sheet 1 is not limited to between the heat spreader 52 and the electronic component 51 or between the heat spreader 52 and the heat sink 53, but can be appropriately selected according to the configuration of the electronic device or semiconductor device.
- any other heat dissipating member may be used as long as it conducts the heat generated from the heat source and dissipates it to the outside. , Peltier elements, heat pipes, metal covers, housings, and the like.
- Example 1 silicone resin (an example of a binder): 34% by volume, and scale-like boron nitride having a hexagonal crystal shape (D50 is 40 ⁇ m): 25 volumes %, aluminum nitride (D50 is 1.5 ⁇ m): 19% by volume, spherical alumina particles (D50 is 5 ⁇ m): 19% by volume, zinc oxide (D50 is 1 ⁇ m): 1% by volume, aluminum hydroxide (D50 8 ⁇ m): 1% by volume and a coupling agent: 1% by volume were uniformly mixed to prepare a resin composition for forming a thermally conductive sheet.
- silicone resin an example of a binder
- D50 scale-like boronitride having a hexagonal crystal shape
- the resin composition for forming a thermally conductive sheet is poured into a mold (opening: 50 mm ⁇ 50 mm) having a rectangular internal space, and heated in an oven at 60 ° C. for 4 hours. to form a molded body block (thermally conductive molded body 6 shown in FIG. 2).
- a release polyethylene terephthalate film was attached to the inner surface of the mold so that the release-treated surface faced the inside.
- Table 1 by slicing the obtained molded block into sheets with a superhard blade, a thermally conductive sheet 1 in which scaly boron nitride is oriented in the thickness direction of the sheet was obtained. .
- the molded block was sliced with a carbide cutter so that Sa on one side of the thermally conductive sheet 1 was 3.442 ⁇ m and Sz was 40.990 ⁇ m. A thermally conductive sheet 1 was obtained.
- Example 2 In this example, first, 100 g of pitch-based carbon fiber having an average fiber diameter of 9 ⁇ m and an average fiber length of 110 ⁇ m and 450 g of ethanol were put into a glass container and mixed with a stirring blade to obtain a slurry liquid. Flow rate: 25 g of divinylbenzene (93% divinylbenzene) was added to the slurry while nitrogen was added to the slurry liquid at a flow rate of 160 mL/min to effect inertization. Ten minutes after the addition of divinylbenzene, 0.500 g of a polymerization initiator (oil-soluble azo polymerization initiator) previously dissolved in 50 g of ethanol was added to the slurry liquid. After charging and stirring for 5 minutes, inertization with nitrogen was stopped.
- a polymerization initiator oil-soluble azo polymerization initiator
- silicone resin 28% by volume
- spherical alumina particles D50: 15 ⁇ m
- granular aluminum nitride D50: 1.5 ⁇ m
- aluminum hydroxide D50 is 8 ⁇ m
- a coupling agent 1 vol% to prepare a silicone composition.
- the molded block was sliced with a carbide cutter so that Sa on one side of the thermally conductive sheet 1 was 4.225 ⁇ m and Sz was 45.880 ⁇ m. A thermally conductive sheet 1 was obtained.
- silicone resin 28% by volume
- spherical alumina particles (D50 is 15 ⁇ m): 30% by volume
- spherical alumina particles (D50 is 5 ⁇ m): 1% by volume
- aluminum hydroxide (D50 is 8 ⁇ m): 1% by volume
- granular aluminum nitride (D50 is 1.5 ⁇ m): 33% by volume
- a coupling agent 1% by volume.
- the resin composition for forming a thermally conductive sheet is poured into a mold (opening: 50 mm ⁇ 50 mm) having a rectangular internal space, and heated in an oven at 100 ° C. for 6 hours. to form a compact block.
- a release polyethylene terephthalate film was adhered to the inner surface of the mold so that the release-treated surface faced the inside.
- Table 1 by slicing the resulting molded block into a desired thickness with a superhard blade, a thermally conductive sheet 1 having carbon fibers oriented in the thickness direction of the sheet was obtained.
- the molded block was sliced with a carbide cutter so that Sa on one side of the thermally conductive sheet 1 was 3.982 ⁇ m and Sz was 49.784 ⁇ m. A thermally conductive sheet 1 was obtained.
- the resin composition for forming a thermally conductive sheet is poured into a mold (opening: 50 mm ⁇ 50 mm) having a rectangular internal space, and heated in an oven at 100 ° C. for 6 hours. to form a compact block.
- a release polyethylene terephthalate film was attached to the inner surface of the mold so that the release-treated surface faced the inside.
- Table 1 by slicing the resulting molded block into a desired thickness with a superhard blade, a thermally conductive sheet 1 having carbon fibers oriented in the thickness direction of the sheet was obtained.
- the molded block was sliced with a carbide cutter so that Sa of one surface of the thermally conductive sheet 1 was 4.989 ⁇ m and Sz was 46.879 ⁇ m. A thermally conductive sheet 1 was obtained.
- Comparative Examples 1 to 4 thermally conductive sheets 1 having carbon fibers oriented in the thickness direction were obtained by slicing the molded blocks obtained in Examples 1 to 4 with a cutter knife (alloy tool steel). At that time, in Comparative Example 1, as shown in Table 1, the molded block was cut with a cemented carbide cutter so that Sa on either side of the thermally conductive sheet 1 was 5.687 ⁇ m and Sz was 71.652 ⁇ m. to obtain a thermally conductive sheet 1. Further, in Comparative Example 2, as shown in Table 1, the molded block was cut with a cemented carbide cutter so that Sa on either side of the thermally conductive sheet 1 was 5.899 ⁇ m and Sz was 65.050 ⁇ m.
- a heat conductive sheet 1 was obtained by slicing.
- Comparative Example 3 as shown in Table 1, the molded block was cut with a cemented carbide cutter so that Sa on either side of the thermally conductive sheet 1 was 5.680 ⁇ m and Sz was 57.380 ⁇ m. A heat conductive sheet 1 was obtained by slicing.
- Comparative Example 4 as shown in Table 1, the molded block was cut with a cemented carbide cutter so that Sa on either side of the thermally conductive sheet 1 was 7.761 ⁇ m and Sz was 65.230 ⁇ m. A heat conductive sheet 1 was obtained by slicing.
- the thermal resistance of the thermally conductive sheet 1 obtained in each of Examples 1-4 and Comparative Examples 1-4 was measured by the following procedure.
- the heat conductive sheet 1 having the above thickness was processed into a circular shape with a diameter of 20 mm to obtain a test piece.
- the obtained test piece was sandwiched between copper sheets, and thermal resistance [°C.cm2/W] was measured with a load of 1 kgf/cm2.
- the thickness at the time of measurement was plotted on the horizontal axis and the thermal resistance value was plotted on the vertical axis, and the contact thermal resistance was obtained from the intercept.
- the surface roughness of the thermally conductive sheet 1 obtained in each of Examples 1-4 and Comparative Examples 1-4 was measured with a one-shot 3D shaping machine VR5200 manufactured by KEYENCE CORPORATION.
- Sa (arithmetic mean height) is a parameter obtained by extending Ra (arithmetic mean height of lines) to a plane, and represents the mean of the absolute values of the height differences of each point with respect to the mean plane of the surface. Sa is generally used when evaluating surface roughness.
- Sz maximum height represents the distance from the highest point to the lowest point on the surface.
- Example 1 and Comparative Example 1, Example 2 and Comparative Example 2, Example 3 and Comparative Example 3, and Example 4 and Comparative Example 4 are compared, the heat conduction of the comparative examples Thermal conductivity and dielectric breakdown voltage of Thermally Conductive Sheet 1 of Example were higher than that of Thermally Conductive Sheet 1.
- the thermally conductive sheet 1 containing the binder and the illegal thermally conductive filler and having the anisotropic thermally conductive filler oriented in the thickness direction has an Sa of 5 ⁇ m or less, an Sz of 50 ⁇ m or less, and a dielectric breakdown voltage of 0.5 ⁇ m.
- the thermally conductive sheet 1 of Examples 1 to 4 is combined with an electronic component 51 (an example of a heating element) constituting the electronic device, a heat dissipation fan, a heat dissipation plate, etc. (an example of a heat dissipation member), By sandwiching between them, it is possible to improve the thermal conductivity with respect to the heat dissipating member, and to efficiently dissipate the heat.
- an electronic component 51 an example of a heating element
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Abstract
Description
図1は、本技術が適用された熱伝導性シートの一例を示す図である。図1に示す熱伝導性シート1は、シート本体2と、樹脂被覆層5を有する。シート本体2は、少なくとも高分子マトリックス成分と繊維状の熱伝導性充填剤とを含むバインダ樹脂が硬化されたものである。樹脂被覆層5は、シート本体2から滲み出た高分子マトリックス成分の未硬化成分によって形成されている。シート本体2の一方の面2aには、第1剥離フィルム3が貼り付けられ、シート本体2の他方の面2bは、第2剥離フィルム4が貼り付けられている。
シート本体2を構成する高分子マトリックス成分は、熱伝導性シート1の基材となる高分子成分のことである。その種類については、特に限定されず、公知の高分子マトリックス成分を適宜選択することができる。例えば、高分子マトリックス成分の一つとして、熱硬化性ポリマーが挙げられる。
熱伝導性シート1に含まれる繊維状の熱伝導性充填剤は、シートの熱伝導性を向上させるための成分である。熱伝導性充填剤の種類については、熱伝導性の高い繊維状の材料であれば特に限定はされないが、より高い熱伝導性を得られる点からは、炭素繊維を用いることが好ましい。
熱伝導性シート1は、熱伝導性充填剤として、無機物フィラーをさらに含有させてもよい。無機物フィラーを含有させることにより、熱伝導性シート1の熱伝導性をより高め、シートの強度を向上できる。前記無機物フィラーとしては、形状、材質、平均粒径等については特に制限がされず、目的に応じて適宜選択することができる。前記形状としては、例えば、球状、楕円球状、塊状、粒状、扁平状、針状等が挙げられる。これらの中でも、球状、楕円形状が充填性の点から好ましく、球状が特に好ましい。
熱伝導性シート1は、上述した、高分子マトリックス成分および繊維状熱伝導性充填剤、適宜含有される無機物フィラーに加えて、目的に応じてその他の成分を適宜含むこともできる。その他の成分としては、例えば、磁性粉、チキソトロピー性付与剤、分散剤、硬化促進剤、遅延剤、微粘着付与剤、可塑剤、難燃剤、酸化防止剤、安定剤、着色剤等が挙げられる。また、磁性粉の含有量を調整することにより、熱伝導性シート1に電磁波吸収性能を付与してもよい。
熱伝導性シート1は、磁性粉の含有量を調整することにより、熱伝導性シート1に電磁波吸収性能を付与してもよい。
次いで、熱伝導性シート1の製造工程について説明する。本技術が適用された熱伝導性シート1の製造工程は、高分子マトリックス成分に繊維状の熱伝導性充填剤等が含有された熱伝導性樹脂組成物を所定の形状に成型して硬化させ、熱伝導性成形体を形成する工程(工程A)と、前記熱伝導性成形体をシート状にスライスし、成形体シートを形成する工程(工程B)と、成形体シートを第1剥離フィルム3と第2剥離フィルム4とで挟持しプレスすることにより、成形体シート表面を平滑化するとともに樹脂被覆層5を形成する工程(工程C)とを有する。なお、ここでは、繊維状の熱伝導性充填剤を用いた場合について説明するが、繊維状の熱伝導性充填剤に替えて鱗片状の無機物フィラーを用いる場合も同様の製造工程が利用でき、以下の工程に於いても適宜読み替えが可能である。
この工程Aでは、上述した高分子マトリックス成分および繊維状熱伝導性充填剤、適宜含有される無機物フィラー、その他の成分を配合し、熱伝導性樹脂組成物を調製する。なお、各成分を配合、調製する手順については特に限定はされず、例えば、高分子マトリックス成分に、繊維状熱伝導性充填剤、適宜、無機物フィラー、磁性粉、その他成分を添加し、混合することにより、熱伝導性樹脂組成物の調製が行われる。
図2に示すように、熱伝導性成形体6をシート状にスライスし、成形体シート7を形成する工程Bでは、配向した繊維状の熱伝導性充填剤の長軸方向に対して、0°~90°の角度となるように、より好ましくは45°~90°の角度となるように、熱伝導性成形体6をシート状に切断する。これにより、繊維状熱伝導性充填剤は、シート本体2の厚み方向に配向される。
工程Cでは、成形体シート7の一方の面に第1剥離フィルム3を貼り付け、成形体シート7の他方の面に第2剥離フィルム4を貼り付けてプレスする。このプレスにより、成形体シート7の表面を平滑化するとともに高分子マトリックス成分の未硬化成分をブリードさせ、成形体シート7の一方の面と第1剥離フィルム3との間と、成形体シート7の他方の面と第2剥離フィルム4との間に樹脂被覆層5を形成する。ここで、熱伝導性シート1の面2aと面2bは、スライスされた面であり、スライスされた後にプレスされた面である。これにより、熱伝導性シート1が形成され、シート表面の凹凸を低減させるとともに、露出する繊維状の熱伝導性充填剤を被覆させ、熱源や放熱部材との密着性を向上し、軽荷重時の界面接触抵抗を軽減させ、熱伝導効率を向上させることができる。
実使用時においては、熱伝導性シート1は、例えば、半導体装置等の電子部品や、ヒートシンク等の各種放熱部材に実装される。このとき、熱伝導性シート1は、シート本体2からの剥離強度が小さい方の剥離フィルム、例えば上述した例で言えば、第1剥離フィルム3から剥離する。これにより、第1剥離フィルム3に付着してシート本体2の全部が第2剥離フィルム4から剥離することがなく、第2剥離フィルム4に支持された状態でシート本体2の一方の面2aを露出させることができる。熱伝導性シート1は、樹脂被覆層5が露出したシート本体2の一方の面2aを半導体装置等の電子部品またはヒートシンク等の放熱部材に貼り付け、その後、第2剥離フィルム4をシート本体2の他方の面2bから剥離する。
本実施例では、下記の表1に示すように、まず、シリコーン樹脂(バインダの一例):34体積%と、結晶形状が六方晶型である鱗片状の窒化ホウ素(D50が40μm):25体積%と、窒化アルミニウム(D50が1.5μm):19体積%と、球状アルミナ粒子(D50が5μm):19体積%と、酸化亜鉛(D50が1μm):1体積%と、水酸化アルミ(D50が8μm):1体積%と、カップリング剤:1体積%と、を均一に混合することにより、熱伝導性シート形成用の樹脂組成物を調製した。
本実施例では、まず、ガラス容器に、平均繊維径:9μm、平均繊維長:110μmのピッチ系炭素繊維を100g、エタノールを450g投入し、撹拌翼にて混合してスラリー液を得た。流量:160mL/minで窒素をスラリー液に加えてイナート化を行いながら、スラリーにジビニルベンゼン(93%ジビニルベンゼン)を25g加えた。ジビニルベンゼンを加えた10分後に、予め50gのエタノールに溶解させておいた0.500gの重合開始剤(油溶性アゾ重合開始剤)をスラリー液に投入した。投入後、5分間撹拌した後に、窒素によるイナート化を停止させた。
本実施例では、まず、ポリエチレン製容器に、平均繊維径9μm、平均繊維長110μmのピッチ系炭素繊維を100g、テトラエトキシシラン(TEOS)200g、エタノール900gを投入し、撹拌翼にて混合した。その後、50℃まで加温しながら、反応開始剤(10%アンモニア水)176gを5分かけて投入した。溶媒の投入が完了した時点を0分として、3時間撹拌を行った。撹拌終了後、降温させ、吸引濾過して固形分を回収し、固形分を水とエタノールを用いて洗浄し、再度吸引濾過を行い、固形分を回収した。回収した固形分を100℃にて2時間乾燥後、更に200℃で8時間焼成を行うことで、SiO2絶縁被覆炭素繊維(表面を絶縁物で被覆した炭素繊維の一例)を得た。
本実施例では、下記の表1に示すように、シリコーン樹脂:28体積%と、炭素繊維:6体積%、球状アルミナ粒子(D50が15μm):30体積%と、球状アルミナ粒子(D50が5μm):1体積%と、粒状窒化アルミ(D50が1.5μm):33体積%と、水酸化アルミ(D50が8μm):1体積%と、カップリング剤:1体積%と、を混合し、シリコーン組成物を調製した。
比較例1~4では、実施例1~4で得られた成形体ブロックをカッターナイフ(合金工具鋼)でスライスすることにより、炭素繊維が厚み方向に配向した熱伝導性シート1を得た。その際、比較例1では、表1に示すように、熱伝導性シート1のいずれか一方の面のSaが5.687μmかつSzが71.652μmとなるように、成形体ブロックを超硬刃物でスライスして熱伝導性シート1を得た。また、比較例2では、表1に示すように、熱伝導性シート1のいずれか一方の面のSaが5.899μmかつSzが65.050μmとなるように、成形体ブロックを超硬刃物でスライスして熱伝導性シート1を得た。また、比較例3では、表1に示すように、熱伝導性シート1のいずれか一方の面のSaが5.680μmかつSzが57.380μmとなるように、成形体ブロックを超硬刃物でスライスして熱伝導性シート1を得た。また、比較例4では、表1に示すように、熱伝導性シート1のいずれか一方の面のSaが7.761μmかつSzが65.230μmとなるように、成形体ブロックを超硬刃物でスライスして熱伝導性シート1を得た。
実施例1~4および比較例1~4のそれぞれで得られた熱伝導性シート1の熱抵抗は、以下の手順で測定した。上記の厚みの熱伝導性シート1を直径20mmの円形になるように加工し、テストピースを得た。次いで、得られたテストピースを銅の間に挟み、熱抵抗[℃・cm2/W]を1kgf/cm2の荷重で測定した。横軸に測定時厚み、縦軸に熱抵抗値としてプロットし、切片から接触熱抵抗を求めた。
実施例1~4および比較例1~4のそれぞれで得られた熱伝導性シート1の表面粗さは、株式会社キーエンス製ワンショット3D形状機VR5200で測定した。Sa(算術平均高さ)は、Ra(線の算術平均高さ)を面に拡張したパラメーターであり、表面の平均面に対して、各点の高さの差の絶対値の平均を表す。Saは、面粗さを評価する際に一般的に利用する。Sz(最大高さ)は、表面の最も高い点から最も低い点までの距離を表す。そして、表1に示すように、実施例1と比較例1、実施例2と比較例2、実施例3と比較例3、および実施例4と比較例4を比較すると、比較例の熱伝導性シート1と比較すると、実施例の熱伝導性シート1の熱伝導率および絶縁破壊電圧が高くなった。これにより、バインダと違法性熱伝導フィラーを含み、当該異方性熱伝導フィラーが厚み方向に配向した熱伝導性シート1のSaが5μm以下かつSzが50μm以下であり、絶縁破壊電圧が0.5kV/mm以上とすることにより、絶縁性を有しながらも低熱抵抗の熱伝導性シート1を得ることができることが分かる。すなわち、絶縁性材料を用いてもSaとSzを所定の値以下とすることで厚み方向に良好に伝熱させることが可能な熱伝導性シート1が得られる。そして、電子機器において、実施例1~4の熱伝導性シート1を、当該電子機器を構成する電子部品51(発熱体の一例)と、放熱ファンや放熱板等(放熱部材の一例)と、の間に挟むことにより、放熱部材に対する熱伝導率を向上させることができ、効率良く放熱させることができる。
Claims (5)
- バインダと異方性熱伝導フィラーとを含み、前記異方性熱伝導フィラーが厚み方向に配向した熱伝導性シートであり、
当該熱伝導性シートのいずれか一方の面のSaが5μm以下、Szが50μm以下であり、絶縁破壊電圧が0.5kV/mm以上である、熱伝導性シート。 - 前記異方性熱伝導フィラーが、窒化ホウ素、炭素繊維、および、表面を絶縁物で被覆した炭素繊維のいずれかである、請求項1に記載の熱伝導性シート。
- さらに、アルミナ、窒化アルミ、酸化亜鉛、および水酸化アルミのいずれかを含有する、請求項1または2に記載の熱伝導性シート。
- 前記バインダがシリコーンである、請求項1~3のいずれかに記載の熱伝導性シート。
- 請求項1~4記載の熱伝導性シートを、発熱体と放熱部材の間に挟んだ、電子機器。
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JP2017130652A (ja) * | 2016-01-14 | 2017-07-27 | デクセリアルズ株式会社 | 熱伝導シート、熱伝導シートの製造方法、放熱部材及び半導体装置 |
JP2017135211A (ja) * | 2016-01-26 | 2017-08-03 | デクセリアルズ株式会社 | 熱伝導シート、熱伝導シートの製造方法、放熱部材及び半導体装置 |
JP2017135371A (ja) * | 2016-01-26 | 2017-08-03 | デクセリアルズ株式会社 | 熱伝導シート、熱伝導シートの製造方法、放熱部材及び半導体装置 |
JP2018067695A (ja) * | 2016-10-21 | 2018-04-26 | 日本ゼオン株式会社 | 熱伝導シートおよびその製造方法 |
JP6755421B1 (ja) * | 2019-03-22 | 2020-09-16 | 帝人株式会社 | 絶縁シート |
JP2020196828A (ja) * | 2019-06-04 | 2020-12-10 | リンテック株式会社 | 粘着性放熱シート |
JP2021004284A (ja) * | 2019-06-25 | 2021-01-14 | 日本ゼオン株式会社 | 熱伝導シートおよびその製造方法 |
JP6983345B1 (ja) * | 2021-02-18 | 2021-12-17 | デクセリアルズ株式会社 | 熱伝導性シート、および電子機器 |
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JP2017130652A (ja) * | 2016-01-14 | 2017-07-27 | デクセリアルズ株式会社 | 熱伝導シート、熱伝導シートの製造方法、放熱部材及び半導体装置 |
JP2017135211A (ja) * | 2016-01-26 | 2017-08-03 | デクセリアルズ株式会社 | 熱伝導シート、熱伝導シートの製造方法、放熱部材及び半導体装置 |
JP2017135371A (ja) * | 2016-01-26 | 2017-08-03 | デクセリアルズ株式会社 | 熱伝導シート、熱伝導シートの製造方法、放熱部材及び半導体装置 |
JP2018067695A (ja) * | 2016-10-21 | 2018-04-26 | 日本ゼオン株式会社 | 熱伝導シートおよびその製造方法 |
JP6755421B1 (ja) * | 2019-03-22 | 2020-09-16 | 帝人株式会社 | 絶縁シート |
JP2020196828A (ja) * | 2019-06-04 | 2020-12-10 | リンテック株式会社 | 粘着性放熱シート |
JP2021004284A (ja) * | 2019-06-25 | 2021-01-14 | 日本ゼオン株式会社 | 熱伝導シートおよびその製造方法 |
JP6983345B1 (ja) * | 2021-02-18 | 2021-12-17 | デクセリアルズ株式会社 | 熱伝導性シート、および電子機器 |
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JP2022126076A (ja) | 2022-08-30 |
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