WO2020080319A1 - Matériau thermoconducteur - Google Patents

Matériau thermoconducteur Download PDF

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Publication number
WO2020080319A1
WO2020080319A1 PCT/JP2019/040347 JP2019040347W WO2020080319A1 WO 2020080319 A1 WO2020080319 A1 WO 2020080319A1 JP 2019040347 W JP2019040347 W JP 2019040347W WO 2020080319 A1 WO2020080319 A1 WO 2020080319A1
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WO
WIPO (PCT)
Prior art keywords
conductive material
heat conductive
cellulose nanofibers
parts
mass
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PCT/JP2019/040347
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English (en)
Japanese (ja)
Inventor
尊史 川上
中村　哲也
佐藤　正史
中嶋　一雄
Original Assignee
株式会社オートネットワーク技術研究所
住友電装株式会社
住友電気工業株式会社
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Application filed by 株式会社オートネットワーク技術研究所, 住友電装株式会社, 住友電気工業株式会社 filed Critical 株式会社オートネットワーク技術研究所
Publication of WO2020080319A1 publication Critical patent/WO2020080319A1/fr

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    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L1/00—Compositions of cellulose, modified cellulose or cellulose derivatives
    • C08L1/02—Cellulose; Modified cellulose
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
    • C09K5/00—Heat-transfer, heat-exchange or heat-storage materials, e.g. refrigerants; Materials for the production of heat or cold by chemical reactions other than by combustion
    • C09K5/08—Materials not undergoing a change of physical state when used
    • C09K5/10—Liquid materials

Definitions

  • the present disclosure relates to thermally conductive materials.
  • thermoly conductive filler As this type of heat conductive material, it is generally known that resin, rubber or the like is highly filled with a heat conductive filler having high heat conductivity.
  • a ceramic material such as alumina, aluminum nitride, or silicon carbide is usually used as the thermally conductive filler (see, for example, Patent Documents 1 and 2).
  • Patent Document 3 discloses a heat conductive material composed of a composite material having cellulose nanofibers and a nanoparticle structure that densely coats the surface of the cellulose nanofibers.
  • conventionally known general heat conductive materials have the following problems. That is, when a ceramic material is used as the heat conductive filler, the specific gravity of the ceramic material is large, and thus the lightweight property which is a characteristic of resin, rubber and the like is impaired, and the light weight property of the heat conductive material is impaired.
  • the present disclosure has been made in view of the above background, and is intended to provide a heat conductive material having high heat conductivity without significantly impairing lightness.
  • One aspect of the present disclosure is a thermally conductive material including water and cellulose nanofibers.
  • FIG. 1 is a scanning electron microscope image (SEM image) of Sample 2.
  • FIG. 2 is an example of a scanning electron microscope (SEM image) used to measure the fiber length and fiber diameter when calculating the aspect ratio of the cellulose nanofibers in Sample 2.
  • FIG. 3 is a histogram of the aspect ratio of cellulose nanofibers in Sample 2.
  • the heat conductive material according to the present embodiment contains water and cellulose nanofibers.
  • Cellulose nanofibers have a smaller specific gravity than ceramic materials. Therefore, the heat conductive material according to the present embodiment is not significantly impaired in lightness as compared with the heat conductive material using the ceramic material.
  • the cellulose nanofibers have a high aspect ratio, the contact probability between the cellulose nanofibers is higher than that of spherical fillers such as alumina, and even if added in a small amount, high thermal conductivity can be imparted. Therefore, the heat conductive material according to the present embodiment can exhibit high heat conductivity.
  • cellulose nanofibers for example, wood fibers defibrated by chemical treatment, wood fibers defibrated by physical treatment, and the like can be used.
  • the cellulose nanofiber can have a hydrophilic group such as a hydroxyl group on the surface. Hydrophilic cellulose nanofibers are suitable because they are easily dispersed in water. It should be noted that this type of cellulose nanofiber is marketed, for example, by Dai-ichi Kogyo Seiyaku Co., Ltd. and Sugino Machine Co., Ltd.
  • the surface of the cellulose nanofibers is preferably exposed. If the surface of the cellulose nanofibers is densely covered with a ceramic material such as alumina as in the prior art, the specific gravity of the cellulose nanofibers increases correspondingly, which hinders the improvement of the weight reduction. On the other hand, according to the structure in which the surface of the cellulose nanofiber is exposed, since the surface of the cellulose nanofiber is not densely covered with the ceramic material, it is advantageous in improving the weight of the heat conductive material.
  • the average aspect ratio of cellulose nanofibers can be 180 or more and 260 or less. According to this structure, the three-dimensional network structure formed when dispersed in water becomes reliable, and the contact probability between the cellulose nanofibers is easily increased. Therefore, according to this structure, a heat conductive material that easily exhibits high heat conductivity can be obtained by adding a small amount of the water.
  • the average aspect ratio of the cellulose nanofibers can be preferably 190 or more, more preferably 200 or more, and further preferably 210 or more from the viewpoint of improving thermal conductivity.
  • the average aspect ratio of the cellulose nanofibers is preferably 250 or less, more preferably 240 or less, from the viewpoints of improving dispersibility, suppressing lowering of handling property due to high viscosity, deterioration of productivity, and the like. More preferably, it can be 230 or less.
  • the heat conductive material according to the present embodiment has the largest frequency of the class in which the aspect ratio of the cellulose nanofibers is 200 or more and 250 or less in the histogram when the histogram of the aspect ratio of the cellulose nanofibers is calculated. Good. That is, in the histogram, the frequency of the class in which the aspect ratio of the cellulose nanofibers is 200 or more and 250 or less is preferably the largest value as compared with the frequency of the other classes. According to this structure, the three-dimensional network structure formed when dispersed in water becomes reliable, and the contact probability between the cellulose nanofibers is easily increased. Therefore, according to this structure, a thermally conductive material that easily exhibits high thermal conductivity can be obtained by adding a small amount of cellulose nanofibers to water.
  • the aspect ratio is calculated from the formula of fiber length / fiber diameter of cellulose nanofiber.
  • the surface of the thermally conductive material is observed with a scanning electron microscope (SEM) (magnification: 10,000 times), and the length in the major axis direction of each cellulose nanofiber is measured. Required by that.
  • the fiber diameter of the cellulose nanofibers is calculated based on the resolution (pixel size) of the SEM image obtained by observing the surface of the heat conductive material with an SEM (magnification: 10,000 times).
  • the fiber diameter is 12.5 nm (12.5 nm ⁇ 1 pixel). To be done. If the width of the cellulose nanofiber is 1 pixel or more and 2 pixels or less, the fiber diameter is set to 25 nm (12.5 nm ⁇ 2 pixels).
  • the average aspect ratio of the cellulose nanofibers is the average value of the aspect ratios of the cellulose nanofibers calculated as described above.
  • a histogram of the aspect ratio of cellulose nanofibers can be obtained from the aspect ratio of cellulose nanofibers obtained as described above. Specifically, when the aspect ratio of the cellulose nanofibers is 50, the width of the class is set to 50, and a histogram is created. In the histogram, each grade on the horizontal axis is, from the smallest, the aspect ratio of the cellulose nanofibers is 50 or more and less than 100, 100 or more and less than 150, 150 or more and less than 200, 200 or more and less than 250, 250 or more and less than 300, 300 or more and 350 or more. Less than ... The vertical axis in the histogram is frequency (%).
  • the heat conductive material according to the present embodiment can be configured to include 0.1 parts by mass or more and 3 parts by mass or less of cellulose nanofibers with respect to 100 parts by mass of water. According to this structure, the heat conductive material having high heat conductivity can be secured without significantly impairing the lightness.
  • the thermally conductive material according to the present embodiment preferably contains cellulose nanofibers in an amount of 0.15 parts by mass or more, and more preferably 0.2 parts by weight with respect to 100 parts by mass of water. Parts by mass or more, more preferably 0.25 parts by mass or more, even more preferably 0.3 parts by mass or more, even more preferably 0.35 parts by mass or more, and most preferably 0.4 parts by mass or more.
  • the heat conductive material which concerns on this embodiment WHEREIN: 2.8 mass parts or less of cellulose nanofiber is preferable with respect to 100 mass parts of water, More preferably, it is 2. 5 parts by mass or less, more preferably 2.3 parts by mass or less, even more preferably 2.2 parts by mass or less, even more preferably 2.1 parts by mass or less, and most preferably 2 parts by mass or less. can do.
  • the thermally conductive material according to the present embodiment if necessary, for example, boron nitride, diamond, aluminum nitride, silicon nitride, silicon carbide, beryllium oxide, aluminum oxide, zinc oxide, magnesium oxide, silicon oxide, titanium oxide, One kind or two or more kinds of aluminum hydroxide, magnesium hydroxide and the like can be contained.
  • the heat conductive material according to this embodiment can be suitably used for vehicle parts. According to this configuration, heat generated from vehicle parts used in a hybrid vehicle, an electric vehicle, or the like can be efficiently radiated to the outside, and the heat conductive material does not easily impair the lightweight of the vehicle parts.
  • the vehicle component include a vehicle ECU (electronic control unit) board, a vehicle electrical relay component, and the like.
  • the heat conductive material according to the present embodiment can be configured to have a heat conductivity of 0.6 W / m ⁇ K or more at room temperature according to the heat ray method defined in JIS R2616. According to this structure, the usefulness as a heat conductive material is enhanced.
  • the thermal conductivity can be preferably 0.65 W / m ⁇ K or more, more preferably 0.7 W / m ⁇ K or more, and preferably 0.8 W / m ⁇ K or more.
  • the thermal conductivity is, for example, 2.5 W / m ⁇ K or less, preferably 2.0 W / m ⁇ K or less, from the viewpoint of ensuring high thermal conductivity while suppressing an increase in weight. You can
  • the heat conductive material according to the present embodiment may be used, for example, as it is, or may be used after being dried to remove water. Further, the heat conductive material according to the present embodiment can be suitably used as, for example, a heat conductive gel, a heat conductive putty, a heat conductive sheet, a heat conductive adhesive or the like used for vehicle parts.
  • the aqueous dispersion of the hydrophilic cellulose nanofibers was used as the heat conductive material of Sample 5.
  • Water was added to the heat conductive material of Sample 5 so that the weight ratio of the cellulose nanofibers would be the mixing ratio shown in Table 1, and the mixture was stirred and mixed for 1 hour using a homomixer to give cellulose nanofibers in water.
  • the fibers were sufficiently dispersed to obtain heat conductive materials of Samples 1 to 4.
  • water was used as the heat conductive material of Sample 6.
  • a heat conductive material of Sample 7 was obtained by mixing 100 parts by mass of water with 100 parts by mass of alumina and preparing the same as above.
  • Table 1 shows the blending ratio, thermal conductivity, and density of each heat conductive material.
  • the heat conductive material of Sample 2 was selected as a representative of the heat conductive materials of Samples 1 to 5. Then, the surface of the heat conductive material of Sample 2 was observed by SEM (magnification: 10,000 times), the fiber length and the fiber diameter of the cellulose nanofiber were measured by the above-mentioned method, and the fiber length / fiber diameter formula was used. The aspect ratio of each cellulose nanofiber was calculated. The results of SEM observation are shown in FIG. Moreover, the SEM image used for the measurement of fiber length and fiber diameter is shown in FIG. In addition, the black line in FIG. 2 is a line for measurement which traced the cellulose nanofiber.
  • the width of the cellulose nanofiber was within 1 pixel, or within 1 pixel to 2 pixels. Therefore, for the cellulose nanofibers having a width of 1 pixel or less, the fiber diameter was set to 12.5 nm (12.5 nm ⁇ 1 pixel).
  • the cellulose nanofibers having a width of 1 pixel or more and 2 pixels or less have a fiber diameter of 25 nm (12.5 nm ⁇ 2 pixels).
  • the average aspect ratio of the cellulose nanofibers was calculated to be 220.
  • the thermal conductivity of Sample 1 increased by 0.12 W / m ⁇ K as compared with Sample 1C. Further, in Samples 2 to 5, the thermal conductivity increased by about 0.3 W / m ⁇ K as compared with Sample 1C. This is because since the cellulose nanofibers have a high aspect ratio, the contact probability between the cellulose nanofibers is larger than that of spherical fillers such as alumina, and high thermal conductivity can be imparted even when added in a small amount. Is. In addition, Samples 2 to 5 had a smaller filler content, a density of about 60%, and a thermal conductivity equal to or higher than that of Comparative Example 2C. From the above results, it was confirmed that the heat conductive materials of Samples 1 to 5 could provide the heat conductive material having high heat conductivity without significantly impairing the lightness.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Organic Chemistry (AREA)
  • Physics & Mathematics (AREA)
  • Combustion & Propulsion (AREA)
  • Thermal Sciences (AREA)
  • Materials Engineering (AREA)
  • Health & Medical Sciences (AREA)
  • Medicinal Chemistry (AREA)
  • Polymers & Plastics (AREA)
  • Compositions Of Macromolecular Compounds (AREA)

Abstract

La présente invention concerne un matériau thermoconducteur qui présente une conductivité thermique élevée sans détériorer significativement la légèreté. Ce matériau thermoconducteur contient de l'eau et des nanofibres de cellulose. Le matériau thermoconducteur peut contenir de 0,1 partie en masse à 3 parties en masse (inclus) des nanofibres de cellulose pour 100 parties en masse d'eau. De préférence, les nanofibres de cellulose présentent un rapport d'aspect moyen de 180 à 260 (inclus). Ce matériau thermoconducteur est approprié pour être utilisé dans des composants pour véhicules.
PCT/JP2019/040347 2018-10-18 2019-10-14 Matériau thermoconducteur WO2020080319A1 (fr)

Applications Claiming Priority (2)

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JP2018196881A JP2020063390A (ja) 2018-10-18 2018-10-18 熱伝導性材料
JP2018-196881 2018-10-18

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WO2020080319A1 true WO2020080319A1 (fr) 2020-04-23

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Citations (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2006008077A (ja) * 2004-06-29 2006-01-12 Honda Motor Co Ltd 車両用内装材料及び車両用内装部材
JP2008248033A (ja) * 2007-03-29 2008-10-16 Hitachi Ltd 繊維強化複合樹脂組成物及びその製造方法
JP2011026531A (ja) * 2009-06-30 2011-02-10 Nippon Zeon Co Ltd 熱伝導性感圧接着剤組成物の製造方法、熱伝導性感圧接着性シート、及び電子部品
WO2011033815A1 (fr) * 2009-09-16 2011-03-24 株式会社カネカ Additif organique thermiquement conducteur, composition de résine et produit durci
WO2013031444A1 (fr) * 2011-08-26 2013-03-07 オリンパス株式会社 Nanofibres de cellulose et procédé de production de ces dernières, composition de résine composite, corps moulé
WO2016043146A1 (fr) * 2014-09-17 2016-03-24 国立大学法人名古屋大学 Composition thermoconductrice et son procédé de production
JP2016079202A (ja) * 2014-10-10 2016-05-16 株式会社Kri 放熱材
JP2018059057A (ja) * 2016-10-03 2018-04-12 国立研究開発法人産業技術総合研究所 複合材料とその製造方法及び熱伝導性材料

Patent Citations (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2006008077A (ja) * 2004-06-29 2006-01-12 Honda Motor Co Ltd 車両用内装材料及び車両用内装部材
JP2008248033A (ja) * 2007-03-29 2008-10-16 Hitachi Ltd 繊維強化複合樹脂組成物及びその製造方法
JP2011026531A (ja) * 2009-06-30 2011-02-10 Nippon Zeon Co Ltd 熱伝導性感圧接着剤組成物の製造方法、熱伝導性感圧接着性シート、及び電子部品
WO2011033815A1 (fr) * 2009-09-16 2011-03-24 株式会社カネカ Additif organique thermiquement conducteur, composition de résine et produit durci
WO2013031444A1 (fr) * 2011-08-26 2013-03-07 オリンパス株式会社 Nanofibres de cellulose et procédé de production de ces dernières, composition de résine composite, corps moulé
WO2016043146A1 (fr) * 2014-09-17 2016-03-24 国立大学法人名古屋大学 Composition thermoconductrice et son procédé de production
JP2016079202A (ja) * 2014-10-10 2016-05-16 株式会社Kri 放熱材
JP2018059057A (ja) * 2016-10-03 2018-04-12 国立研究開発法人産業技術総合研究所 複合材料とその製造方法及び熱伝導性材料

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
SHIMAZAKI, YUZURU ET AL.: "Development of Transparent High-Thermal-Conductivity Films Using Cellulose Nanofibers", MATERIAL TECHNOLOGIES FOR CONTROLLING HEAT/ELECTRICITY). POLYFILE, vol. 48, no. 9, 2011, pages 22 - 25 *

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