JP2001064080A - Silicon nitride sintered body and its production - Google Patents
Silicon nitride sintered body and its productionInfo
- Publication number
- JP2001064080A JP2001064080A JP2000108937A JP2000108937A JP2001064080A JP 2001064080 A JP2001064080 A JP 2001064080A JP 2000108937 A JP2000108937 A JP 2000108937A JP 2000108937 A JP2000108937 A JP 2000108937A JP 2001064080 A JP2001064080 A JP 2001064080A
- Authority
- JP
- Japan
- Prior art keywords
- sintered body
- silicon nitride
- temperature
- nitride sintered
- raw material
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Granted
Links
- 229910052581 Si3N4 Inorganic materials 0.000 title claims abstract description 75
- HQVNEWCFYHHQES-UHFFFAOYSA-N silicon nitride Chemical compound N12[Si]34N5[Si]62N3[Si]51N64 HQVNEWCFYHHQES-UHFFFAOYSA-N 0.000 title claims abstract description 75
- 238000004519 manufacturing process Methods 0.000 title claims abstract description 23
- 238000005245 sintering Methods 0.000 claims abstract description 28
- 239000002994 raw material Substances 0.000 claims abstract description 26
- 239000000843 powder Substances 0.000 claims abstract description 20
- 150000001875 compounds Chemical class 0.000 claims abstract description 10
- 239000012299 nitrogen atmosphere Substances 0.000 claims abstract description 5
- 238000000034 method Methods 0.000 claims description 16
- 238000010304 firing Methods 0.000 claims description 13
- 239000013078 crystal Substances 0.000 claims description 8
- 230000000052 comparative effect Effects 0.000 description 22
- 238000010292 electrical insulation Methods 0.000 description 16
- 238000000465 moulding Methods 0.000 description 12
- 239000004065 semiconductor Substances 0.000 description 12
- 239000000203 mixture Substances 0.000 description 8
- 238000010438 heat treatment Methods 0.000 description 7
- 239000000463 material Substances 0.000 description 7
- 239000002245 particle Substances 0.000 description 7
- 239000012071 phase Substances 0.000 description 7
- 230000000694 effects Effects 0.000 description 6
- 239000012535 impurity Substances 0.000 description 6
- 238000006243 chemical reaction Methods 0.000 description 5
- 238000009413 insulation Methods 0.000 description 5
- NIPNSKYNPDTRPC-UHFFFAOYSA-N N-[2-oxo-2-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)ethyl]-2-[[3-(trifluoromethoxy)phenyl]methylamino]pyrimidine-5-carboxamide Chemical compound O=C(CNC(=O)C=1C=NC(=NC=1)NCC1=CC(=CC=C1)OC(F)(F)F)N1CC2=C(CC1)NN=N2 NIPNSKYNPDTRPC-UHFFFAOYSA-N 0.000 description 4
- 239000011230 binding agent Substances 0.000 description 4
- 229910001404 rare earth metal oxide Inorganic materials 0.000 description 4
- 238000003756 stirring Methods 0.000 description 4
- 239000000758 substrate Substances 0.000 description 4
- VZSRBBMJRBPUNF-UHFFFAOYSA-N 2-(2,3-dihydro-1H-inden-2-ylamino)-N-[3-oxo-3-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)propyl]pyrimidine-5-carboxamide Chemical compound C1C(CC2=CC=CC=C12)NC1=NC=C(C=N1)C(=O)NCCC(N1CC2=C(CC1)NN=N2)=O VZSRBBMJRBPUNF-UHFFFAOYSA-N 0.000 description 3
- WZFUQSJFWNHZHM-UHFFFAOYSA-N 2-[4-[2-(2,3-dihydro-1H-inden-2-ylamino)pyrimidin-5-yl]piperazin-1-yl]-1-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)ethanone Chemical compound C1C(CC2=CC=CC=C12)NC1=NC=C(C=N1)N1CCN(CC1)CC(=O)N1CC2=C(CC1)NN=N2 WZFUQSJFWNHZHM-UHFFFAOYSA-N 0.000 description 3
- YJLUBHOZZTYQIP-UHFFFAOYSA-N 2-[5-[2-(2,3-dihydro-1H-inden-2-ylamino)pyrimidin-5-yl]-1,3,4-oxadiazol-2-yl]-1-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)ethanone Chemical compound C1C(CC2=CC=CC=C12)NC1=NC=C(C=N1)C1=NN=C(O1)CC(=O)N1CC2=C(CC1)NN=N2 YJLUBHOZZTYQIP-UHFFFAOYSA-N 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 3
- 239000002202 Polyethylene glycol Substances 0.000 description 3
- 239000012298 atmosphere Substances 0.000 description 3
- 239000002131 composite material Substances 0.000 description 3
- 229920001223 polyethylene glycol Polymers 0.000 description 3
- 239000006104 solid solution Substances 0.000 description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 3
- HMUNWXXNJPVALC-UHFFFAOYSA-N 1-[4-[2-(2,3-dihydro-1H-inden-2-ylamino)pyrimidin-5-yl]piperazin-1-yl]-2-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)ethanone Chemical compound C1C(CC2=CC=CC=C12)NC1=NC=C(C=N1)N1CCN(CC1)C(CN1CC2=C(CC1)NN=N2)=O HMUNWXXNJPVALC-UHFFFAOYSA-N 0.000 description 2
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 2
- 229910017493 Nd 2 O 3 Inorganic materials 0.000 description 2
- 239000004372 Polyvinyl alcohol Substances 0.000 description 2
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 2
- 239000007864 aqueous solution Substances 0.000 description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 2
- 239000002981 blocking agent Substances 0.000 description 2
- 239000000919 ceramic Substances 0.000 description 2
- 229910052802 copper Inorganic materials 0.000 description 2
- 239000010949 copper Substances 0.000 description 2
- 238000000354 decomposition reaction Methods 0.000 description 2
- 230000007423 decrease Effects 0.000 description 2
- 238000000280 densification Methods 0.000 description 2
- 238000004090 dissolution Methods 0.000 description 2
- 238000011156 evaluation Methods 0.000 description 2
- 239000007789 gas Substances 0.000 description 2
- 238000000462 isostatic pressing Methods 0.000 description 2
- 239000012778 molding material Substances 0.000 description 2
- 230000003647 oxidation Effects 0.000 description 2
- 238000007254 oxidation reaction Methods 0.000 description 2
- 239000001301 oxygen Substances 0.000 description 2
- 229910052760 oxygen Inorganic materials 0.000 description 2
- 229920002451 polyvinyl alcohol Polymers 0.000 description 2
- 229910052710 silicon Inorganic materials 0.000 description 2
- 239000010703 silicon Substances 0.000 description 2
- 239000002002 slurry Substances 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- JQMFQLVAJGZSQS-UHFFFAOYSA-N 2-[4-[2-(2,3-dihydro-1H-inden-2-ylamino)pyrimidin-5-yl]piperazin-1-yl]-N-(2-oxo-3H-1,3-benzoxazol-6-yl)acetamide Chemical compound C1C(CC2=CC=CC=C12)NC1=NC=C(C=N1)N1CCN(CC1)CC(=O)NC1=CC2=C(NC(O2)=O)C=C1 JQMFQLVAJGZSQS-UHFFFAOYSA-N 0.000 description 1
- IHCCLXNEEPMSIO-UHFFFAOYSA-N 2-[4-[2-(2,3-dihydro-1H-inden-2-ylamino)pyrimidin-5-yl]piperidin-1-yl]-1-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)ethanone Chemical compound C1C(CC2=CC=CC=C12)NC1=NC=C(C=N1)C1CCN(CC1)CC(=O)N1CC2=C(CC1)NN=N2 IHCCLXNEEPMSIO-UHFFFAOYSA-N 0.000 description 1
- YLZOPXRUQYQQID-UHFFFAOYSA-N 3-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)-1-[4-[2-[[3-(trifluoromethoxy)phenyl]methylamino]pyrimidin-5-yl]piperazin-1-yl]propan-1-one Chemical compound N1N=NC=2CN(CCC=21)CCC(=O)N1CCN(CC1)C=1C=NC(=NC=1)NCC1=CC(=CC=C1)OC(F)(F)F YLZOPXRUQYQQID-UHFFFAOYSA-N 0.000 description 1
- CONKBQPVFMXDOV-QHCPKHFHSA-N 6-[(5S)-5-[[4-[2-(2,3-dihydro-1H-inden-2-ylamino)pyrimidin-5-yl]piperazin-1-yl]methyl]-2-oxo-1,3-oxazolidin-3-yl]-3H-1,3-benzoxazol-2-one Chemical compound C1C(CC2=CC=CC=C12)NC1=NC=C(C=N1)N1CCN(CC1)C[C@H]1CN(C(O1)=O)C1=CC2=C(NC(O2)=O)C=C1 CONKBQPVFMXDOV-QHCPKHFHSA-N 0.000 description 1
- 238000007088 Archimedes method Methods 0.000 description 1
- 229910021578 Iron(III) chloride Inorganic materials 0.000 description 1
- AFCARXCZXQIEQB-UHFFFAOYSA-N N-[3-oxo-3-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)propyl]-2-[[3-(trifluoromethoxy)phenyl]methylamino]pyrimidine-5-carboxamide Chemical compound O=C(CCNC(=O)C=1C=NC(=NC=1)NCC1=CC(=CC=C1)OC(F)(F)F)N1CC2=C(CC1)NN=N2 AFCARXCZXQIEQB-UHFFFAOYSA-N 0.000 description 1
- 101100371219 Pseudomonas putida (strain DOT-T1E) ttgE gene Proteins 0.000 description 1
- 229910004298 SiO 2 Inorganic materials 0.000 description 1
- 238000002441 X-ray diffraction Methods 0.000 description 1
- 238000005299 abrasion Methods 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 238000004220 aggregation Methods 0.000 description 1
- 230000002776 aggregation Effects 0.000 description 1
- 239000003125 aqueous solvent Substances 0.000 description 1
- 238000005219 brazing Methods 0.000 description 1
- 230000015556 catabolic process Effects 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 238000013329 compounding Methods 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- LPLMZAJYUPAYQZ-UHFFFAOYSA-N diazanium;difluoride Chemical compound [NH4+].[NH4+].[F-].[F-] LPLMZAJYUPAYQZ-UHFFFAOYSA-N 0.000 description 1
- 229910001873 dinitrogen Inorganic materials 0.000 description 1
- 239000006185 dispersion Substances 0.000 description 1
- 239000010419 fine particle Substances 0.000 description 1
- 239000011521 glass Substances 0.000 description 1
- 238000000227 grinding Methods 0.000 description 1
- 230000017525 heat dissipation Effects 0.000 description 1
- 239000011261 inert gas Substances 0.000 description 1
- RBTARNINKXHZNM-UHFFFAOYSA-K iron trichloride Chemical compound Cl[Fe](Cl)Cl RBTARNINKXHZNM-UHFFFAOYSA-K 0.000 description 1
- 239000004973 liquid crystal related substance Substances 0.000 description 1
- 239000007791 liquid phase Substances 0.000 description 1
- 230000007257 malfunction Effects 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- 230000008018 melting Effects 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 239000011368 organic material Substances 0.000 description 1
- 230000002093 peripheral effect Effects 0.000 description 1
- 238000013001 point bending Methods 0.000 description 1
- 239000011164 primary particle Substances 0.000 description 1
- 230000001737 promoting effect Effects 0.000 description 1
- 239000007921 spray Substances 0.000 description 1
Landscapes
- Ceramic Products (AREA)
Abstract
Description
【０００１】[0001]
【発明の属する技術分野】 本発明は、熱伝導率が高
く、かつ、高温における電気絶縁性に優れた窒化珪素焼
結体及びその製造方法に関する。The present invention relates to a silicon nitride sintered body having high thermal conductivity and excellent electrical insulation at high temperatures, and a method for producing the same.
【０００２】[0002]
【従来の技術】 窒化珪素焼結体は、強度、靭性等の機
械的特性をはじめ、耐摩耗性、耐酸化性、電気絶縁性
等、種々の特性に優れているため、例えばディーゼル、
ガスタービンのような熱機関用構造材料として汎用され
る一方、ＢｅＯ，ＡｌＮ，ＳｉＣ等の焼結体に比して熱
伝導特性が劣るため、放熱性を要求される部材（例えば
回路基板）には使用されていなかった。2. Description of the Related Art Sintered silicon nitride is excellent in various properties such as mechanical properties such as strength and toughness, abrasion resistance, oxidation resistance, and electrical insulation.
While it is widely used as a structural material for heat engines such as gas turbines, it has poor heat conduction characteristics as compared with sintered bodies of BeO, AlN, SiC, etc. Was not used.
【０００３】 しかしながら、本出願人は窒化珪素焼結
体の優れた機械的特性や電気絶縁性を生かしつつ、熱伝
導特性を向上させることができれば、回路基板等として
好適に用いることができると考え、種々の改良を行って
きた。例えば、窒化珪素多結晶体の結晶粒の大きさと不
純物であるＡｌの含有量とを制御することにより、優れ
た機械的特性と良好な熱伝導特性を併有する窒化珪素焼
結体が得られることを既に開示している（特開平3-2189
75号公報）。However, the present applicant considers that a silicon nitride sintered body can be suitably used as a circuit board and the like if the heat conduction property can be improved while utilizing the excellent mechanical properties and electrical insulation properties. And various improvements have been made. For example, by controlling the size of the crystal grains of the silicon nitride polycrystal and the content of Al as an impurity, a silicon nitride sintered body having both excellent mechanical properties and good heat conduction properties can be obtained. (Japanese Unexamined Patent Publication No. Hei 3-2189)
No. 75 gazette).
【０００４】 また、最近では、窒化珪素多結晶体の結
晶粒を粗粒と微粒の複合組織にし、粗粒の比率を制御す
ることにより、良好な機械的特性を満足し、かつ、高熱
伝導性を有する窒化珪素焼結体が得られることが開示さ
れている（特開平9-30866号公報）。Further, recently, the crystal grains of the silicon nitride polycrystal are formed into a composite structure of coarse grains and fine grains, and by controlling the ratio of the coarse grains, satisfactory mechanical properties are satisfied and high thermal conductivity is obtained. It is disclosed that a silicon nitride sintered body having the following can be obtained (JP-A-9-30866).
【０００５】[0005]
【発明が解決しようとする課題】 上記のような熱伝導
特性に優れる窒化珪素焼結体は、素子からの発熱を速や
かに放熱し、かつ、基板表裏及び基板上の配線間を確実
に絶縁することが要求される回路基板として好適に用い
ることができる。例えば、当該窒化珪素焼結体を基板と
して金属回路を設け、更に半導体素子を載置してなる半
導体モジュールなどが検討されている。SUMMARY OF THE INVENTION A silicon nitride sintered body having excellent heat conduction characteristics as described above rapidly radiates heat generated from the element and reliably insulates the wiring on the front and back surfaces of the substrate and the wiring on the substrate. It can be suitably used as a circuit board which is required. For example, a semiconductor module in which a metal circuit is provided using the silicon nitride sintered body as a substrate and a semiconductor element is mounted thereon is being studied.
【０００６】 しかしながら、上述の窒化珪素焼結体は
室温条件では充分な電気絶縁性を示すものの、高温条件
においては著しく電気絶縁性が低下する場合があるた
め、例えば１００℃以上の高温条件における電気絶縁性
を必要とする車載用の回路基板としては不十分なもので
あった。特にサイリスタのような大電流制御用の半導体
素子に使用する場合には、通常の回路基板に比して、一
層高い電気絶縁性が要求されるため、上記の問題は極め
て顕著なものとなる。However, although the above-mentioned silicon nitride sintered body shows sufficient electrical insulation at room temperature, the electrical insulation may be significantly reduced at high temperature conditions. It was insufficient as a circuit board for vehicles requiring insulation. In particular, when used in a semiconductor device for controlling a large current, such as a thyristor, the above problem becomes extremely remarkable because higher electric insulation is required as compared with a normal circuit board.
【０００７】 即ち、高温条件下で使用する回路基板と
して良好な特性を備えた窒化珪素焼結体は未だ見出され
ておらず、熱伝導特性と高温条件における電気絶縁性の
双方を満足する窒化珪素焼結体が切望されている。本発
明は、このような従来技術の問題点に鑑みてなされたも
のであって、その目的とするところは、熱伝導率が高
く、かつ、高温における電気絶縁性に優れた窒化珪素焼
結体及びその製造方法を提供することにある。That is, a silicon nitride sintered body having good characteristics as a circuit board used under high-temperature conditions has not yet been found, and nitrided silicon that satisfies both heat conduction characteristics and electrical insulation under high-temperature conditions has been found. There is a long-awaited demand for silicon sintered bodies. The present invention has been made in view of such problems of the related art, and it is an object of the present invention to provide a silicon nitride sintered body having high thermal conductivity and excellent electrical insulation at high temperatures. And a method for manufacturing the same.
【０００８】[0008]
【課題を解決するための手段】 即ち、本発明によれ
ば、窒化珪素結晶粒及び粒界相からなり、酸化物換算で
０．３〜１０重量％のＭｇを含む焼結体であって、当該
焼結体の熱伝導率が６０Ｗ／ｍＫ以上、１２５℃におけ
る電気抵抗率が１Ｅ＋１３Ωｃｍ以上であることを特徴
とする窒化珪素焼結体が提供される。That is, according to the present invention, there is provided a sintered body comprising silicon nitride crystal grains and a grain boundary phase and containing 0.3 to 10% by weight of Mg in terms of oxide, A silicon nitride sintered body is provided, wherein the sintered body has a thermal conductivity of 60 W / mK or more and an electrical resistivity at 125 ° C. of 1E + 13 Ωcm or more.
【０００９】 本発明の窒化珪素焼結体は、４００℃に
おける電気抵抗率が１Ｅ＋１１Ωｃｍ以上であることが
好ましく、Ａｌ単体の含有率が０．２５重量％以下であ
ることが好ましい。また、本発明によれば、上記の窒化
珪素焼結体からなることを特徴とする回路基板が提供さ
れる。The silicon nitride sintered body of the present invention preferably has an electric resistivity at 400 ° C. of 1E + 11 Ωcm or more, and preferably has a content of Al alone of 0.25% by weight or less. Further, according to the present invention, there is provided a circuit board comprising the above silicon nitride sintered body.
【００１０】 更に、本発明によれば、窒化珪素粉末
と、Ｍｇ化合物と、焼結助剤とを含む成形原料を成形
し、当該成形体を窒素雰囲気下において１８００〜２０
００℃で焼成する、窒化珪素焼結体の製造方法であっ
て、前記成形原料を、酸化物換算で０．３〜１０重量％
のＭｇを含むように調製し、かつ、１４００〜１７００
℃の温度範囲において、０．５時間以上、一定温度に保
持した後、前記焼成温度まで昇温することを特徴とする
窒化珪素焼結体の製造方法が提供される。Further, according to the present invention, a forming raw material containing a silicon nitride powder, a Mg compound, and a sintering aid is formed, and the formed body is formed in a nitrogen atmosphere at 1800 to 20%.
A method for producing a silicon nitride sintered body which is fired at 00 ° C., wherein the forming raw material is 0.3 to 10% by weight in terms of oxide.
Of Mg, and 1400-1700
A method for producing a silicon nitride sintered body, characterized in that after maintaining a constant temperature in a temperature range of 0.5 ° C. for 0.5 hours or more, the temperature is raised to the firing temperature.
【００１１】[0011]
【発明の実施の形態】 本発明は、酸化物換算で０．３
〜１０重量％のＭｇを含み、熱伝導率が６０Ｗ／ｍＫ以
上、１２５℃における電気抵抗率が１Ｅ＋１３Ωｃｍ以
上であることを特徴とする窒化珪素焼結体である。この
ような窒化珪素焼結体は、熱伝導率が高く、かつ、高温
における電気絶縁性に優れるため、例えば車載用の回路
基板、特にサイリスタのような大電流制御用の半導体素
子に使用する回路基板として好適に用いることができ
る。以下、本発明の窒化珪素焼結体について詳細に説明
する。BEST MODE FOR CARRYING OUT THE INVENTION
A silicon nitride sintered body containing 10 to 10% by weight of Mg, having a thermal conductivity of 60 W / mK or more and an electric resistivity at 125 ° C. of 1E + 13 Ωcm or more. Since such a silicon nitride sintered body has high thermal conductivity and excellent electrical insulation at high temperatures, it is used for a circuit board used for a vehicle, particularly a semiconductor element for controlling a large current such as a thyristor. It can be suitably used as a substrate. Hereinafter, the silicon nitride sintered body of the present invention will be described in detail.
【００１２】 本発明の窒化珪素焼結体は、粒径０．１
〜１００μｍ程度の窒化珪素の結晶粒の間隙に、酸化
物、酸窒化物等からなる粒界相を有する焼結体であり、
通常は、相対密度が９７〜１００％程度、１０μｍ当た
りの粒界個数が５〜３０個程度であるのが通常である。The silicon nitride sintered body of the present invention has a particle size of 0.1
A sintered body having a grain boundary phase composed of an oxide, an oxynitride, or the like in a gap between silicon nitride crystal grains of about 100 μm;
Usually, the relative density is about 97 to 100%, and the number of grain boundaries per 10 μm is usually about 5 to 30.
【００１３】 本発明の窒化珪素焼結体は、酸化物換算
で０．３〜１０重量％のＭｇを含有することを特徴とす
る。少なくとも０．３重量％以上のＭｇを含有せしめた
焼結体は高温における電気抵抗率が高く、回路基板とし
て必要な電気絶縁性を有するからである。但し、Ｍｇを
過剰に含有する場合には焼結体が緻密化しないことに起
因して、熱伝導率が低下するため、含有率は多くとも１
０重量％以下とすることが必要である。[0013] The silicon nitride sintered body of the present invention is characterized by containing 0.3 to 10% by weight of Mg in terms of oxide. This is because a sintered body containing at least 0.3% by weight or more of Mg has a high electric resistivity at a high temperature and has an electric insulation required for a circuit board. However, when Mg is excessively contained, the thermal conductivity is reduced due to the densification of the sintered body, so that the content is at most 1%.
It is necessary that the content be 0% by weight or less.
【００１４】 また、本発明の窒化珪素焼結体は、熱伝
導率が６０Ｗ／ｍＫ以上であることを特徴とする。熱伝
導率が６０Ｗ／ｍＫ未満では、回路基板として用いる場
合に充分な放熱性が得られず、その用途が限定されるか
らである。Further, the silicon nitride sintered body of the present invention is characterized in that the thermal conductivity is 60 W / mK or more. If the thermal conductivity is less than 60 W / mK, sufficient heat dissipation cannot be obtained when used as a circuit board, which limits its use.
【００１５】 更に、本発明の窒化珪素焼結体は、１２
５℃における電気抵抗率が１Ｅ＋１３Ωｃｍ以上である
ことを特徴とする。通常の回路基板等において電気絶縁
性を確保するためには、１Ｅ＋１１Ωｃｍ程度の電気抵
抗率であれば充分であるが、サイリスタのような大電流
制御用の半導体素子の回路基板として用いる場合には一
層高い電気絶縁性が要求されるからである。なお、電気
抵抗率の測定温度を１２５℃としたのは、車載用の回路
基板は１００〜１５０℃程度の高温条件下で使用される
からである。Further, the silicon nitride sintered body of the present invention
The electrical resistivity at 5 ° C. is 1E + 13 Ωcm or more. An electrical resistivity of about 1E + 11 Ωcm is sufficient to secure electrical insulation in a normal circuit board or the like. However, when it is used as a circuit board of a semiconductor device for controlling a large current such as a thyristor, it is more required. This is because high electrical insulation is required. The reason why the measurement temperature of the electric resistivity was set to 125 ° C. is that the circuit board for vehicle use is used under a high temperature condition of about 100 to 150 ° C.
【００１６】 本発明の窒化珪素焼結体は、少なくとも
１２５℃における電気抵抗率が１Ｅ＋１３Ωｃｍ以上で
あることが必要であるが、４００℃における電気抵抗率
が１Ｅ＋１１Ωｃｍ以上であることが好ましい。４００
℃程度の高温条件においては絶縁破壊されないまでも絶
縁性低下によるリーク電流が流れる場合が生じ得る。こ
のような場合にあっても１Ｅ＋１１Ωｃｍ以上の電気抵
抗率を確保することにより、後述する高温ヒータ、グロ
ープラグ等のヒータ端子間、或いはヒータと被加熱物と
の間のリーク電流を抑制することが可能となる。即ち、
高温ヒータ、グロープラグ等をより高温で使用すること
ができる点において好ましい。The silicon nitride sintered body of the present invention needs to have an electric resistivity at least at 125 ° C. of 1E + 13 Ωcm or more, and preferably has an electric resistivity at 400 ° C. of 1E + 11 Ωcm or more. 400
Under a high temperature condition of about ° C., a leak current may flow due to a decrease in insulation even if dielectric breakdown does not occur. Even in such a case, by securing an electrical resistivity of 1E + 11 Ωcm or more, it is possible to suppress a leak current between heater terminals such as a high-temperature heater and a glow plug, which will be described later, or between the heater and the object to be heated. It becomes possible. That is,
This is preferable in that a high-temperature heater, a glow plug, or the like can be used at a higher temperature.
【００１７】 本発明の窒化珪素焼結体は、不純物とし
て存在するＡｌ単体の含有率が０．２５重量％以下であ
ることが好ましい。Ａｌ単体の含有率が０．２５重量％
超の場合、Ａｌが窒化珪素粒子に固溶し、焼結体の熱伝
導率が低下するという不具合を生ずるからである。In the silicon nitride sintered body of the present invention, the content of Al alone as an impurity is preferably 0.25% by weight or less. Al content of 0.25% by weight
This is because, in the case where the content is excessive, Al dissolves in the silicon nitride particles, which causes a problem that the thermal conductivity of the sintered body is reduced.
【００１８】 上述した本発明の窒化珪素焼結体は、熱
伝導率が高く、かつ、高温における電気絶縁性に優れる
ため、例えば高温条件下で使用される車載用の回路基
板、特にサイリスタのように高い電気絶縁性が必要とさ
れる、大電流制御用の半導体素子に使用する回路基板と
して好適に用いることができる。The above-described silicon nitride sintered body of the present invention has a high thermal conductivity and an excellent electrical insulation property at a high temperature. Therefore, for example, a circuit board for a vehicle used under a high-temperature condition, such as a thyristor, is used. It can be suitably used as a circuit board used for a semiconductor element for controlling a large current, which requires high electric insulation.
【００１９】 また、本発明の窒化珪素焼結体は、回路
基板のみならず、半導体製造装置用ヒータ等の高温ヒー
タ、或いはグロープラグ等の材料としても好適に用いる
ことができる。高温における端子間の電気絶縁性を向上
させること可能となり、より高温での使用が可能となる
ことに加え、熱伝導率が高いため均熱性にも優れるから
である。窒化珪素焼結体は耐食性にも優れるため、ＣＶ
Ｄ等の腐食性雰囲気下で使用される半導体製造装置用ヒ
ータの材料としては特に好適に用いることができる。Further, the silicon nitride sintered body of the present invention can be suitably used not only as a circuit board but also as a material for a high-temperature heater such as a heater for a semiconductor manufacturing apparatus or a glow plug. This is because it is possible to improve the electrical insulation between the terminals at a high temperature and to use the terminal at a higher temperature, and also to have excellent thermal uniformity due to its high thermal conductivity. Since silicon nitride sintered body has excellent corrosion resistance, CV
As a material for a heater for a semiconductor manufacturing apparatus used in a corrosive atmosphere such as D, it can be particularly preferably used.
【００２０】 本発明の窒化珪素焼結体は、従来の製造
方法のように、窒化珪素粉末と、Ｙ2Ｏ3等の焼結助剤等
を含む成形原料を成形し、当該成形体を窒素雰囲気或い
は不活性ガス雰囲気中で焼成するのみでは得ることがで
きないが、所定量のＭｇ化合物を成形原料に含有せし
め、かつ、焼成前の昇温過程において所定時間一定温度
に保持する工程を導入することにより製造することが可
能となる。以下、本発明の製造方法について詳細に説明
する。The silicon nitride sintered body of the present invention is obtained by molding a molding raw material containing silicon nitride powder and a sintering aid such as Y 2 O 3 as in a conventional production method, and forming the molded body with nitrogen. Although it cannot be obtained only by firing in an atmosphere or an inert gas atmosphere, a step of incorporating a predetermined amount of a Mg compound into a forming raw material and maintaining a constant temperature for a predetermined time in a heating process before firing is introduced. By doing so, it becomes possible to manufacture. Hereinafter, the production method of the present invention will be described in detail.
【００２１】 本発明の製造方法では、まず、成形原料
を成形して成形体を製造する。本発明で使用する成形原
料は、少なくとも窒化珪素粉末と、Ｍｇ化合物と、焼結
助剤とを含有する。窒化珪素は難焼結性のセラミックで
あるため、成形原料を構成する窒化珪素粉末は、粒径が
２μｍ以下の微粒子を用いることが好ましい。粒径を小
さくすることにより、表面張力が大きくなり、焼結が容
易となるからである。In the production method of the present invention, first, a molding raw material is molded to produce a molded body. The forming raw material used in the present invention contains at least a silicon nitride powder, a Mg compound, and a sintering aid. Since silicon nitride is a hardly sinterable ceramic, it is preferable to use fine particles having a particle size of 2 μm or less as the silicon nitride powder constituting the forming raw material. This is because by reducing the particle size, the surface tension increases and sintering becomes easy.
【００２２】 窒化珪素は結晶構造としてα相、β相が
存在するが、成形原料となる窒化珪素粉末のβ化率は特
に限定されず、β化率が１％程度の低いものでも使用で
きる。本発明の製造方法においては１８００℃以上の高
温で焼成を行うため、α相は不可逆的にβ相に相変化す
るためである。窒化珪素粉末中に不純物として存在する
酸素の含有量も特に限定されないが、通常は０．５〜
２．０％程度のものが用いられる。Silicon nitride has an α phase and a β phase as a crystal structure, but the β conversion rate of the silicon nitride powder used as a forming raw material is not particularly limited, and a β conversion rate as low as about 1% can be used. This is because in the production method of the present invention, since the firing is performed at a high temperature of 1800 ° C. or more, the α phase irreversibly changes to the β phase. The content of oxygen present as an impurity in the silicon nitride powder is not particularly limited, but is usually 0.5 to
About 2.0% is used.
【００２３】 また、本発明の成形原料には、酸化物換
算で０．３〜１０重量％のＭｇを含むようにＭｇ化合物
を含有せしめることが必要である。既述のように、この
範囲でＭｇを含有することにより焼結体の電気抵抗率を
向上させることが可能となり、かつ、焼結体を緻密化す
る効果をも得ることができるからである。Ｍｇ化合物の
種類は特に限定されないが、後述する焼結助剤として添
加するＭｇＯを兼用することができる。Further, it is necessary that the forming material of the present invention contains an Mg compound so as to contain 0.3 to 10% by weight of Mg in terms of oxide. As described above, by containing Mg in this range, the electrical resistivity of the sintered body can be improved, and the effect of densifying the sintered body can be obtained. The type of the Mg compound is not particularly limited, but MgO added as a sintering aid described later can also be used.
【００２４】 更に、本発明の成形原料には、難焼結性
のセラミックである窒化珪素の焼結を容易にするため、
焼結助剤を含有せしめることが必要である。焼結助剤の
種類は特に限定されず、例えばＭｇＯ、ＺｒＯ2等の酸
化物を用いることができる。ＭｇＯは、窒化珪素の緻密
化を促進する効果が高く、焼結体の電気抵抗率を向上さ
せる効果をも有する点において、ＺｒＯ2は焼結体の機
械的強度を向上させられる点において好ましい。Further, in order to facilitate the sintering of silicon nitride, which is a hard-to-sinter ceramic,
It is necessary to include a sintering aid. The type of the sintering aid is not particularly limited, and for example, oxides such as MgO and ZrO 2 can be used. Since MgO has a high effect of promoting the densification of silicon nitride and also has an effect of improving the electrical resistivity of the sintered body, ZrO 2 is preferable in that the mechanical strength of the sintered body can be improved.
【００２５】 また、希土類酸化物であるＹ2Ｏ3、Ｙｂ
2Ｏ3、Ｎｄ2Ｏ3を前記焼結助剤と併用することも好まし
い。希土類酸化物は窒化珪素粒子の界面に均一に分布し
て不純物のＳｉＯ2や他の焼結助剤であるＭｇＯ等と結
合し、高融点の液相又は結晶を形成するため、焼結体を
緻密化し、高強度化する効果を有するからである。Also, rare earth oxides such as Y 2 O 3 and Yb
It is also preferable to use 2 O 3 and Nd 2 O 3 in combination with the sintering aid. The rare earth oxide is uniformly distributed at the interface of the silicon nitride particles and combines with impurities such as SiO 2 and other sintering aids such as MgO to form a high melting point liquid phase or crystal. This is because it has the effect of densifying and increasing the strength.
【００２６】 成形原料全体に対する焼結助剤全体の含
有率は特に限定されないが酸化物換算で１〜１０重量％
であることが好ましい。焼結助剤が少なすぎれば焼結が
進行しない一方、多すぎれば窒化珪素粒子間に多量のガ
ラス相が形成され、焼結体の熱伝導率が低下するためで
ある。The content of the entire sintering aid relative to the entire forming raw material is not particularly limited, but is 1 to 10% by weight in terms of oxide.
It is preferable that If the amount of the sintering aid is too small, sintering does not proceed, while if it is too large, a large amount of glass phase is formed between the silicon nitride particles, and the thermal conductivity of the sintered body decreases.
【００２７】 なお、本発明の成形原料は、窒化珪素粉
末、Ｍｇ化合物、焼結助剤を含有する限りにおいて、他
の物質を添加してもよい。例えば焼結体に遮光性を付与
するためにＭｏ2Ｃ，ＳｉＣを添加することも可能であ
る。これらの物質の添加は、焼結体を回路基板とした際
に、可視光近傍の波長を有する電磁波による半導体素子
の誤動作を防止できる点において好ましい。The molding raw material of the present invention may contain other substances as long as it contains silicon nitride powder, Mg compound and sintering aid. For example, Mo 2 C or SiC can be added to impart light shielding properties to the sintered body. The addition of these substances is preferable in that when a sintered body is used as a circuit board, malfunction of a semiconductor element due to electromagnetic waves having a wavelength near visible light can be prevented.
【００２８】 上記の成形原料は従来公知の成形方法に
より成形体とすることができる。例えば、上記成形原料
に水を加え、撹拌槽型撹拌ミル（商品名：アトライタ
（三井三池化工機（株））等）により混合・粉砕してス
ラリーを形成し、バインダを添加した後スプレードライ
ヤにて造粒乾燥し、当該造粒粉を成形型に投入して静水
圧加圧成形する方法等が挙げられる。The above-mentioned molding raw material can be formed into a molded body by a conventionally known molding method. For example, water is added to the above molding material, and the mixture is mixed and pulverized with a stirring tank type stirring mill (trade name: Attritor (Mitsui Miike Kakoki Co., Ltd.) or the like) to form a slurry. Granulated and dried, and then the granulated powder is charged into a mold and subjected to isostatic pressing.
【００２９】 このような成形方法は、成形原料界面で
の凝集を防止し、均一な分散が可能となるとともに、成
形原料に流動性を付与することが可能である点において
好ましい。[0029] Such a molding method is preferable in that aggregation at the interface of the molding raw material can be prevented, uniform dispersion can be achieved, and fluidity can be imparted to the molding raw material.
【００３０】 また、バインダの添加は１次粒子間の摩
擦抵抗を減少させ、造粒粉をつぶれ易くするため、生成
される欠陥を小さくすることができる点においても好ま
しい。バインダの種類は特に限定されないが、例えばポ
リビニルアルコール、ポリエチレングリコール等の有機
質材料が挙げられる。Further, the addition of the binder is preferable in that the frictional resistance between the primary particles is reduced and the granulated powder is easily crushed, so that the generated defects can be reduced. The type of the binder is not particularly limited, and examples thereof include organic materials such as polyvinyl alcohol and polyethylene glycol.
【００３１】 上記成形体は、窒化珪素の分解、酸化を
防止するため、窒素雰囲気中において焼成して焼結体と
するが、１〜２０気圧の窒素ガス加圧下で焼成を行って
も良い。焼成温度については、高密度焼結体を得るため
１８００℃以上とする必要があるが、窒化珪素の分解を
防止するべく２０００℃以下としなければならない。The above-mentioned molded body is fired in a nitrogen atmosphere to form a sintered body in order to prevent decomposition and oxidation of silicon nitride, but firing may be performed under a nitrogen gas pressure of 1 to 20 atm. The firing temperature must be 1800 ° C. or higher to obtain a high-density sintered body, but must be 2000 ° C. or lower to prevent decomposition of silicon nitride.
【００３２】 また、本発明の製造方法においては、焼
成前の昇温過程、即ち、１４００〜１７００℃の温度範
囲において、０．５時間以上、一定温度（例えば１５０
０℃）に保持した後、前記焼成温度まで昇温することを
特徴とする。このような方法によれば、焼結体の高温条
件での電気抵抗率を向上させることが可能となる。Further, in the manufacturing method of the present invention, a constant temperature (for example, 150 ° C.) for at least 0.5 hour in a temperature increasing process before firing, ie, in a temperature range of 1400 to 1700 ° C.
(0 ° C.), and then the temperature is raised to the firing temperature. According to such a method, the electrical resistivity of the sintered body under high temperature conditions can be improved.
【００３３】 本発明の方法により焼結体の電気抵抗率
が上昇する理由の詳細は不明であるが、焼結初期に一定
温度で焼結を進行させることにより、成形原料中に添加
したＭｇＯが窒化珪素結晶粒に微量固溶し、或いはＭｇ
Ｏが溶解して窒化珪素結晶粒の全体を均一に被包するこ
とにより焼結体の電気抵抗率が向上するものと推定され
る。Although the details of the reason why the electrical resistivity of the sintered body is increased by the method of the present invention are unknown, by allowing sintering to proceed at a constant temperature in the early stage of sintering, MgO added to the forming raw material can be reduced. A small amount of solid solution in silicon nitride crystal grains or Mg
It is presumed that the electric resistivity of the sintered body is improved by dissolving O and uniformly covering the entire silicon nitride crystal grains.
【００３４】 即ち、１４００℃未満では温度不足によ
り、１７００℃を超える場合には焼結初期の焼結速度が
速すぎるため、いずれもＭｇＯの固溶或いは溶解がうま
く進行しない。また、ＭｇＯの固溶や溶解にはある程度
の時間を必要とするため、０．５時間以上、当該温度で
保持する必要がある。That is, when the temperature is lower than 1400 ° C., the temperature is insufficient, and when the temperature exceeds 1700 ° C., the sintering speed in the initial stage of sintering is too high, and the solid solution or dissolution of MgO does not proceed well. Since a certain time is required for the solid solution or dissolution of MgO, it is necessary to maintain the temperature at the temperature for 0.5 hour or more.
【００３５】 なお、本発明の方法において「一定温
度」というときは、１４００〜１７００℃の温度範囲を
厳守する限りにおいて、設定温度±２０℃程度で制御さ
れていれば許容される。The term “constant temperature” in the method of the present invention is acceptable as long as the temperature is controlled at a set temperature of about ± 20 ° C. as long as the temperature range of 1400 to 1700 ° C. is strictly adhered to.
【００３６】 以上説明したように本発明の製造方法に
よれば、例えば車載用の半導体素子、特にサイリスタの
ような大電流制御用の半導体素子に使用する回路基板と
して好適に用いることができる、熱伝導率が高く、か
つ、高温における電気絶縁性に優れた窒化珪素焼結体を
簡便に製造することができる。As described above, according to the manufacturing method of the present invention, for example, heat can be suitably used as a circuit board used for a semiconductor element for vehicle mounting, particularly a semiconductor element for large current control such as a thyristor. A silicon nitride sintered body having high conductivity and excellent electrical insulation at high temperatures can be easily manufactured.
【００３７】[0037]
【実施例】 以下、本発明について実施例により更に詳
細に説明する。但し、本発明はこれらの実施例に限定さ
れるものではない。なお、以下の実施例、比較例で使用
する窒化珪素粉末、焼結助剤、遮光性付与剤は、いずれ
も不純物として含まれるＡｌ単体が０．０１重量％以下
のものを使用した。EXAMPLES Hereinafter, the present invention will be described in more detail with reference to Examples. However, the present invention is not limited to these examples. The silicon nitride powder, the sintering aid, and the light-blocking agent used in the following Examples and Comparative Examples used were those in which Al alone contained as an impurity was 0.01% by weight or less.
【００３８】（焼結体の評価方法）製造された窒化珪素
焼結体は以下に示す評価方法により相対密度、熱伝導
率、電気抵抗率、粒界個数、β化率、室温強度、破壊靭
性値を測定して評価した。(Evaluation Method of Sintered Body) The manufactured silicon nitride sintered body was evaluated by the following evaluation methods for relative density, thermal conductivity, electric resistivity, number of grain boundaries, β conversion, room temperature strength, fracture toughness. The values were measured and evaluated.
【００３９】（１）相対密度：水溶媒のアルキメデス法
により測定した。各助剤組成における理論密度は、窒化
珪素及び各助剤の単独での密度の配合重量により重み付
け平均により算出した。 （２）熱伝導率：直径１０ｍｍ×厚さ３ｍｍの円筒状に
加工した焼結体をサンプルとし、JIS R1611に記載の方
法に準拠してレーザーフラッシュ法で測定した。(1) Relative density: Measured by the Archimedes method of an aqueous solvent. The theoretical density in each auxiliary composition was calculated by weighted average based on the compounding weight of the density of silicon nitride and each auxiliary alone. (2) Thermal conductivity: A sintered body processed into a cylindrical shape having a diameter of 10 mm and a thickness of 3 mm was used as a sample and measured by a laser flash method in accordance with the method described in JIS R1611.
【００４０】（３）電気抵抗率：縦５０ｍｍ×横５０ｍ
ｍ×厚さ１ｍｍの板状に加工した焼結体にＡｇペースト
を塗布焼き付けしたものをサンプルとし、JIS C2141に
記載の方法に準拠して、真空中において３端子法により
５００ｍＶ／ｍｍの電界強度で測定した。(3) Electric resistivity: length 50 mm × width 50 m
A sample obtained by applying and baking an Ag paste to a sintered body processed into a plate having a size of mx 1 mm and having a thickness of 500 mV / mm by a three-terminal method in a vacuum according to the method described in JIS C2141. Was measured.
【００４１】（４）粒界個数：走査型電子顕微鏡にて、
焼結体の任意断面における微構造を窒化珪素粒子が個々
に識別できる倍率で写真撮影し、写真に直線を描き、直
線が横切る粒界の個数を計測した。粒界の数が１０００
個を超えるまで視野を変えて直線を引き、１０００個の
粒界を計測するのに要した直線の総距離Ｌ（μｍ）から
（１０００／Ｌ）×１０により１０μｍ当たりの個数に
換算した。例えば１０００個の粒界を計測するのに５０
０μｍを要したとすれば１０μｍ当たりの粒界の個数は
２０個となる。(4) Number of grain boundaries:
The microstructure in an arbitrary cross section of the sintered body was photographed at a magnification at which the silicon nitride particles could be individually identified, a straight line was drawn on the photograph, and the number of grain boundaries crossed by the straight line was measured. 1000 grain boundaries
Lines were drawn by changing the field of view until the number exceeded the number, and the total distance L (μm) of the lines required to measure 1000 grain boundaries was converted to the number per 10 μm by (1000 / L) × 10. For example, 50 to measure 1000 grain boundaries
If 0 μm is required, the number of grain boundaries per 10 μm is 20.
【００４２】（５）β化率：Ｘ線回折により、α−Ｓｉ
3Ｎ4の（２１０），（２０１）面の回折強度α（２１
０），α（２０１）と、β−Ｓｉ3Ｎ4の（１０１），
（２１０）面の回折強度β（１０１），β（２１０）よ
り次式により求めた。(5) β conversion: α-Si by X-ray diffraction
The diffraction intensity α (21) of the (210) and (201) planes of 3 N 4
0), α (201) and (101), β-Si 3 N 4
The diffraction intensity was obtained from the diffraction intensity β (101) and β (210) of the (210) plane by the following equation.
【００４３】[0043]
【数１】 (Equation 1)
【００４４】（６）室温強度：縦４ｍｍ×横３ｍｍ×長
さ４０ｍｍの棒状に加工した焼結体をサンプルとし、JI
S R1601に記載の方法に準拠して、４点曲げ強度を測定
した。 （７）破壊靭性値：JIS R1607に記載の方法に準拠し
て、ＳＥＰＢ法により測定した。(6) Room temperature strength: A sintered body processed into a rod shape of 4 mm long × 3 mm wide × 40 mm long was used as a sample,
The four-point bending strength was measured according to the method described in SR1601. (7) Fracture toughness: Measured by the SEPB method according to the method described in JIS R1607.
【００４５】（実施例１）実施例１では、定温保持工程
の適正温度について検証した。Example 1 In Example 1, the appropriate temperature in the constant temperature holding step was verified.
【００４６】 表１記載のβ化率、不純物酸素量であっ
て、比表面積１１ｍ2／ｇの市販の窒化珪素粉末と、焼
結助剤であるＭｇＯ，Ｙ2Ｏ3とからなる成形原料に、更
に焼結助剤としてＺｒＯ2を、遮光性を付与するための
添加剤としてＭｏ2Ｃを添加し、表１に記載の比率で調
合した。なお、表１においては、ＭｇＯ、Ｙ2Ｏ3につい
ては成形原料中の含有率で、ＺｒＯ2、Ｍｏ2Ｃについて
は成形原料に対する添加率で表記した。A molding raw material comprising a commercially available silicon nitride powder having a β conversion ratio and an impurity oxygen amount shown in Table 1 having a specific surface area of 11 m 2 / g and sintering aids of MgO and Y 2 O 3 was used. Further, ZrO 2 was added as a sintering aid, and Mo 2 C was added as an additive for imparting light-shielding properties. In Table 1, MgO and Y 2 O 3 are represented by the content in the forming material, and ZrO 2 and Mo 2 C are represented by the addition ratio to the forming material.
【００４７】 上記成形原料に水を加え、撹拌槽型撹拌
ミル（商品名；アトライタ（三井三池化工機（株））
等）により混合・粉砕してスラリーを形成し、ＰＶＡ
（ポリビニルアルコール）及びＰＥＧ（ポリエチレング
リコール）をバインダとして添加した後スプレードライ
ヤにて造粒乾燥し、更に当該造粒粉を成形型に投入し、
６９０ＭＰａで静水圧加圧成形することにより、６０×
６０×６ｍｍの成形体を作製した。Water is added to the above molding material, and a stirring tank type stirring mill (trade name: Attritor (Mitsui Miike Kakoki Co., Ltd.))
) To form a slurry,
(Polyvinyl alcohol) and PEG (polyethylene glycol) are added as binders, and then granulated and dried by a spray dryer.
60 × by isostatic pressing at 690 MPa
A molded body of 60 × 6 mm was produced.
【００４８】 得られた成形体はバインダを消失させた
後、Ｎ2雰囲気中、図１に示す実施例１−１の昇温スケ
ジュールに準じて焼成を行い、実施例１−１〜１−３、
比較例１−１，１−２の焼結体を得た。原料組成及び製
造条件を表１に、焼結体特性を表２に示す。After the binder was removed from the obtained molded body, the molded body was fired in an N 2 atmosphere in accordance with the heating schedule of Example 1-1 shown in FIG. 1 to obtain Examples 1-1 to 1-3. ,
The sintered bodies of Comparative Examples 1-1 and 1-2 were obtained. Table 1 shows the raw material composition and production conditions, and Table 2 shows the characteristics of the sintered body.
【００４９】[0049]
【表１】 [Table 1]
【００５０】[0050]
【表２】 [Table 2]
【００５１】（結果）実施例１−１〜１−３に示すよう
に定温保持工程の温度が本発明の範囲内である限り、熱
伝導率、電気抵抗率が良好な焼結体を得ることができ
た。一方、比較例１−１に示すように保持温度が１４０
０℃未満の場合には、１２５℃、４００℃における電気
抵抗率がいずれも低く、比較例１−２に示すように保持
温度を１７００℃超とした場合には焼結が進行せず、焼
結体の相対密度が９５％と低かったことに起因して、熱
伝導率が低かった。(Results) As shown in Examples 1-1 to 1-3, as long as the temperature in the constant temperature holding step is within the range of the present invention, a sintered body having good thermal conductivity and electric resistivity can be obtained. Was completed. On the other hand, as shown in Comparative Example 1-1, the holding temperature was 140
When the temperature is lower than 0 ° C., the electrical resistivity at 125 ° C. and 400 ° C. are both low. When the holding temperature is higher than 1700 ° C. as shown in Comparative Example 1-2, sintering does not proceed, and The thermal conductivity was low due to the low relative density of the compacts of 95%.
【００５２】（実施例２）実施例２では、定温保持後の
焼成温度について検証した。表１に記載の条件で実施例
１と同様に焼結体を製造し、実施例２−１〜２−３、比
較例２−１，２−２の焼結体を得た。原料組成及び製造
条件を表１に、焼結体特性を表２に示す。Example 2 In Example 2, the firing temperature after holding at a constant temperature was verified. A sintered body was manufactured in the same manner as in Example 1 under the conditions shown in Table 1, and sintered bodies of Examples 2-1 to 2-3 and Comparative Examples 2-1 and 2-2 were obtained. Table 1 shows the raw material composition and production conditions, and Table 2 shows the characteristics of the sintered body.
【００５３】（結果）実施例２−１〜２−３に示すよう
に定温保持が適正に行われ、かつ、焼成温度が本発明の
範囲内である場合には、熱伝導率、電気抵抗率が良好な
焼結体を得ることができた。一方、定温保持が適正に行
われた場合であっても、比較例２−１に示すように焼成
温度が１８００℃未満では焼結体の熱伝導率が低く、比
較例２−２に示すように２０００℃超では電気抵抗率が
低かった。(Results) As shown in Examples 2-1 to 2-3, when the constant temperature was properly maintained and the firing temperature was within the range of the present invention, the thermal conductivity and the electrical resistivity However, a good sintered body could be obtained. On the other hand, even when the constant temperature holding is properly performed, the thermal conductivity of the sintered body is low when the sintering temperature is lower than 1800 ° C. as shown in Comparative Example 2-1 and as shown in Comparative Example 2-2. Above 2000 ° C, the electrical resistivity was low.
【００５４】（実施例３）実施例３ではＭｇ化合物添加
の効果について検証した。表３に記載の条件で実施例１
と同様に焼結体を製造し、実施例３−１〜３−３、比較
例３−１，３−２の焼結体を得た。原料組成及び製造条
件を表３に、焼結体特性を表４に示す。なお、比較例３
−１においては、Ｙ2Ｏ3以外の希土類酸化物としてＹｂ
2Ｏ3を使用した。また、成形原料に対し１重量％のＳｉ
Ｃ及び２重量％のＭｏ2Ｃを遮光性付与剤として添加し
た。Example 3 In Example 3, the effect of adding a Mg compound was examined. Example 1 under the conditions described in Table 3
A sintered body was manufactured in the same manner as in Example 1 to obtain sintered bodies of Examples 3-1 to 3-3 and Comparative examples 3-1 and 3-2. Table 3 shows the raw material composition and production conditions, and Table 4 shows the properties of the sintered body. Comparative Example 3
In -1, Yb as a rare earth oxides other than Y 2 O 3
2 O 3 was used. In addition, 1% by weight of Si based on
C and 2% by weight of Mo 2 C were added as light-blocking agents.
【００５５】[0055]
【表３】 [Table 3]
【００５６】[0056]
【表４】 [Table 4]
【００５７】（結果）実施例３−１〜３−３に示すよう
にＭｇを本発明の範囲内で含む場合には、高い熱伝導率
と電気抵抗率を有する焼結体を得られる一方、比較例３
−１，３−２に示すように、Ｍｇが含まれていない焼結
体は電気抵抗率が低かった。(Results) As shown in Examples 3-1 to 3-3, when Mg is contained within the scope of the present invention, a sintered body having high thermal conductivity and electrical resistivity can be obtained, Comparative Example 3
As shown in -1, 3-2, the sintered body containing no Mg had a low electric resistivity.
【００５８】 図３は、本発明の範囲内でＭｇを含有す
る実施例１−３の焼結体と、Ｍｇを含有しない比較例３
−１の焼結体についての、焼結体の電気抵抗率と温度と
の相関を示すグラフである。図３から明らかなようにＭ
ｇを含有する実施例１−３の焼結体は常温から４００℃
程度の高温領域まで高い電気抵抗率を示した。FIG. 3 shows the sintered body of Example 1-3 containing Mg within the scope of the present invention and Comparative Example 3 not containing Mg.
2 is a graph showing the correlation between the electrical resistivity of the sintered body and the temperature for the sintered body of -1. As is apparent from FIG.
g of the sintered body of Example 1-3 containing room temperature
High electrical resistivity was exhibited up to a high temperature range.
【００５９】（実施例４）実施例４では、温度保持工程
導入の効果について検証した。表３に記載の条件で実施
例１と同様に焼結体を製造し、実施例４−１〜４−３の
焼結体を得た。但し、比較例４−１〜４−３は図２に示
すような昇温スケジュールにより焼成を行った。Example 4 In Example 4, the effect of introducing the temperature holding step was verified. A sintered body was manufactured in the same manner as in Example 1 under the conditions shown in Table 3 to obtain sintered bodies of Examples 4-1 to 4-3. However, in Comparative Examples 4-1 to 4-3, baking was performed according to a heating schedule as shown in FIG.
【００６０】 即ち、昇温過程において温度保持工程を
入れず、１５００℃にてＮ2ガスの圧力を１．５ａｔｍ
から１０ａｔｍ若しくは１００ａｔｍに変更することの
みを行った。原料組成及び製造条件を表３に、焼結体特
性を表４に示す。なお、Ｙ2Ｏ3以外の希土類酸化物とし
て、実施例４−３においてはＹｂ2Ｏ3を、実施例４−
２，比較例４−１〜４−３においてはＮｄ2Ｏ3を使用し
た。That is, the temperature of the N 2 gas was increased to 1.5 atm
Only 10 atm or 100 atm. Table 3 shows the raw material composition and production conditions, and Table 4 shows the properties of the sintered body. In addition, in Example 4-3, as a rare earth oxide other than Y 2 O 3 , Yb 2 O 3 was used.
2, were used Nd 2 O 3 in Comparative Examples 4-1 to 4-3.
【００６１】（結果）実施例４−１〜４−３に示すよう
に温度保持工程が適正に行われた場合には、熱伝導率、
電気抵抗率が良好な焼結体を得ることができた。一方、
比較例４−１〜４−３に示すように、昇温過程における
温度保持を行わない場合には焼結体の電気抵抗率が低下
した。(Results) As shown in Examples 4-1 to 4-3, when the temperature holding step was properly performed, the thermal conductivity,
A sintered body having good electric resistivity was obtained. on the other hand,
As shown in Comparative Examples 4-1 to 4-3, when the temperature was not maintained during the heating process, the electrical resistivity of the sintered body decreased.
【００６２】（実施例５）実施例５では、原料粉末にお
ける窒化珪素粉末の種類による影響を検証した。表３に
記載の条件で実施例１と同様に焼結体を製造し、実施例
５−１〜５−３の焼結体を得た。Example 5 In Example 5, the influence of the type of silicon nitride powder in the raw material powder was verified. A sintered body was manufactured in the same manner as in Example 1 under the conditions described in Table 3, and sintered bodies of Examples 5-1 to 5-3 were obtained.
【００６３】 但し、実施例５−１では比表面積５．５
ｍ2／ｇの市販の窒化珪素粉末を、実施例５−２では比
表面積３．４ｍ2／ｇの市販の窒化珪素粉末を、実施例
５−３では比表面積１１．２ｍ2／ｇの市販の窒化珪素
粉末を使用した。原料組成及び製造条件を表３に、焼結
体特性を表４に示す。なお、実施例５−１，５−２にお
いては、成形原料に対し０．１重量％のＭｏ 2Ｃを遮光
性付与剤として添加した。However, in Example 5-1 the specific surface area was 5.5.
mTwo/ G of commercially available silicon nitride powder in Example 5-2
Surface area 3.4mTwo/ G of commercially available silicon nitride powder in the Examples
For 5-3, specific surface area 11.2mTwo/ G commercial silicon nitride
Powder was used. Table 3 shows the raw material composition and manufacturing conditions.
Table 4 shows the body characteristics. In Examples 5-1 and 5-2,
In addition, 0.1% by weight of Mo TwoShade C
It was added as a property imparting agent.
【００６４】（結果）実施例５−１〜５−３に示すよう
に、窒化珪素粉末の種類を変更した場合でも、Ｍｇ化合
物の量、定温保持条件、焼成条件が本発明の範囲内であ
る限りにおいて高いい熱伝導率と電気抵抗率を達成する
ことができた。(Results) As shown in Examples 5-1 to 5-3, even when the type of the silicon nitride powder was changed, the amount of the Mg compound, the condition for maintaining the constant temperature, and the firing condition were within the scope of the present invention. As far as possible, high thermal conductivity and electrical resistivity could be achieved.
【００６５】（実施例６）実施例１−３、比較例３−
１、比較例４−１と同一組成の成形用粉末を１５０ＭＰ
ａで金型成形することにより、５０×６０×１ｍｍの成
形体とし、実施例１−３、比較例３−１、比較例４−１
と同一の条件にて焼成し、最後に研削加工することによ
り４０×５０×０．６ｍｍの平板状焼結体を得た。Example 6 Example 1-3, Comparative Example 3-
1. A molding powder having the same composition as that of Comparative Example 4-1 was 150 MPa
A molded product of 50 × 60 × 1 mm was obtained by molding with a in Example a, Example 1-3, Comparative Example 3-1 and Comparative Example 4-1.
By baking under the same conditions as described above, and finally grinding, a plate-like sintered body of 40 × 50 × 0.6 mm was obtained.
【００６６】 これらの焼結体に、市販のＡｇ−Ｃｕ−
Ｔｉロウを外周５ｍｍ幅を除いて両面にスクリーン印刷
し、０．３ｍｍ厚の銅板を両面に張り付けた状態で、真
空下８５０℃で１０分間熱処理を行うことにより窒化珪
素／銅の複合接合体を得た。次いで、複合接合体の一方
の面に回路形成用レジストを印刷し、硬化した後、塩化
第２鉄水溶液でエッチングし、回路パターンを形成し
た。A commercially available Ag—Cu—
A silicon nitride / copper composite joined body is obtained by performing a heat treatment at 850 ° C. for 10 minutes under vacuum in a state where a Ti wax is screen-printed on both sides except for a 5 mm outer peripheral width and a copper plate having a thickness of 0.3 mm is stuck on both sides. Obtained. Next, a circuit forming resist was printed on one surface of the composite joint, cured, and then etched with a ferric chloride aqueous solution to form a circuit pattern.
【００６７】 更に、回路間のロウ材を除くため、酸性
フッ化アンモニウム水溶液にて洗浄し、その後数回水洗
して回路基板を作製した（各々を、実施例６−１，比較
例６−１，６−２の回路基板と称する。）。Further, in order to remove the brazing material between the circuits, the circuit boards were washed with an aqueous solution of ammonium ammonium fluoride, and then washed with water several times to prepare circuit boards (each of Example 6-1 and Comparative Example 6-1). , 6-2.).
【００６８】 前記３種の回路基板について、大気中１
２５℃において、表面−裏面間に６００Ｖの電圧を印加
したところ、実施例６−１の回路基板の電気抵抗値は２
００ＧΩで充分な電気絶縁性を確保できたのに対し、比
較例６−１，６−２の回路基板の電気抵抗値はそれぞれ
３０ＭΩ，１ＧΩであった。即ち、比較例６−１，６−
２の回路基板は、絶縁破壊はされていないものの十分な
電気絶縁性が確保できず、大電流制御素子用の回路基板
としては不適であった。Regarding the three types of circuit boards,
At 25 ° C., when a voltage of 600 V was applied between the front surface and the back surface, the electric resistance of the circuit board of Example 6-1 was 2
While sufficient electrical insulation was ensured at 00 GΩ, the electrical resistance values of the circuit boards of Comparative Examples 6-1 and 6-2 were 30 MΩ and 1 GΩ, respectively. That is, Comparative Examples 6-1 and 6-
The circuit board No. 2 did not break down, but could not secure sufficient electrical insulation, and was not suitable as a circuit board for a large current control element.
【００６９】[0069]
【発明の効果】 以上説明したように、本発明の窒化珪
素焼結体は、熱伝導率が高く、かつ、高温における電気
絶縁性に優れるため、例えば車載用の回路基板、特にサ
イリスタのような大電流制御用の半導体素子に使用する
回路基板として好適に用いることができる。As described above, the silicon nitride sintered body of the present invention has high thermal conductivity and excellent electrical insulation at high temperatures, and therefore, for example, a circuit board for a vehicle, particularly a thyristor. It can be suitably used as a circuit board used for a semiconductor element for controlling a large current.
【図１】 実施例１−１の昇温スケジュールを示すグラ
フである。FIG. 1 is a graph showing a heating schedule of Example 1-1.
【図２】 比較例４−１の昇温スケジュールを示すグラ
フである。FIG. 2 is a graph showing a heating schedule of Comparative Example 4-1.
【図３】 焼結体の電気抵抗率と温度との相関を示すグ
ラフである。FIG. 3 is a graph showing the correlation between the electrical resistivity of a sintered body and the temperature.
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Claims (5)
化物換算で０．３〜１０重量％のＭｇを含む焼結体であ
って、 当該焼結体の熱伝導率が６０Ｗ／ｍＫ以上、１２５℃に
おける電気抵抗率が１Ｅ＋１３Ωｃｍ以上であることを
特徴とする窒化珪素焼結体。1. A sintered body comprising silicon nitride crystal grains and a grain boundary phase and containing 0.3 to 10% by weight of Mg in terms of oxide, wherein the sintered body has a thermal conductivity of 60 W / mK. As described above, the silicon nitride sintered body has an electric resistivity at 125 ° C. of 1E + 13 Ωcm or more.
１Ωｃｍ以上である請求項１に記載の窒化珪素焼結体。2. The electric resistivity at 400 ° C. is 1E + 1.
The silicon nitride sintered body according to claim 1, wherein the silicon nitride sintered body has a resistivity of 1 Ωcm or more.
下である請求項１又は２に記載の窒化珪素焼結体。3. The silicon nitride sintered body according to claim 1, wherein the content of Al alone is 0.25% by weight or less.
化珪素焼結体からなることを特徴とする回路基板。4. A circuit board comprising the silicon nitride sintered body according to claim 1.
剤とを含む成形原料を成形し、当該成形体を窒素雰囲気
中において１８００〜２０００℃で焼成する、窒化珪素
焼結体の製造方法であって、 前記成形原料を、酸化物換算で０．３〜１０重量％のＭ
ｇを含むように調製し、かつ、１４００〜１７００℃の
温度範囲において、０．５時間以上、一定温度に保持し
た後、前記焼成温度まで昇温することを特徴とする窒化
珪素焼結体の製造方法。5. A method for manufacturing a silicon nitride sintered body, comprising forming a forming raw material containing a silicon nitride powder, a Mg compound, and a sintering aid, and firing the formed body at 1800 to 2000 ° C. in a nitrogen atmosphere. The method according to claim 1, wherein the forming raw material is prepared by mixing 0.3 to 10% by weight of M
g, and maintained at a constant temperature for at least 0.5 hour in a temperature range of 1400 to 1700 ° C., and then heated to the firing temperature. Production method.
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|---|---|---|---|---|
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Citations (12)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH01160870A (en) * | 1987-12-18 | 1989-06-23 | Ngk Spark Plug Co Ltd | Silicon nitride sintered compact and production thereof |
| JPH03218975A (en) * | 1990-01-23 | 1991-09-26 | Ngk Insulators Ltd | Silicon nitride body and production thereof |
| JPH04212441A (en) * | 1990-09-18 | 1992-08-04 | Ngk Insulators Ltd | Ceramic wiring board |
| JPH061663A (en) * | 1992-06-23 | 1994-01-11 | Toyota Motor Corp | Method for manufacturing silicon nitride sintered body |
| JPH06305837A (en) * | 1993-04-21 | 1994-11-01 | Sumitomo Electric Ind Ltd | Sintered silicon nitride |
| JPH0930866A (en) * | 1995-07-21 | 1997-02-04 | Nissan Motor Co Ltd | High thermal conductivity silicon nitride sintered body, method for producing the same, and insulating substrate made of silicon nitride sintered body |
| JPH09157030A (en) * | 1995-12-07 | 1997-06-17 | Denki Kagaku Kogyo Kk | Production of silicon nitride sintered compact |
| JPH09157054A (en) * | 1995-12-07 | 1997-06-17 | Denki Kagaku Kogyo Kk | Circuit board |
| JPH09268070A (en) * | 1996-04-03 | 1997-10-14 | Honda Motor Co Ltd | Manufacturing method of ceramic sintered body |
| JPH11100274A (en) * | 1997-09-26 | 1999-04-13 | Denki Kagaku Kogyo Kk | Silicon nitride sintered compact, its production and circuit board |
| JP2000128654A (en) * | 1998-10-28 | 2000-05-09 | Sumitomo Electric Ind Ltd | Silicon nitride composite substrate |
| JP2000351673A (en) * | 1999-06-10 | 2000-12-19 | Hitachi Metals Ltd | High thermal conductive silicon nitride sintered body and method for producing the same |
-
2000
- 2000-04-11 JP JP2000108937A patent/JP4571728B2/en not_active Expired - Lifetime
Patent Citations (12)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH01160870A (en) * | 1987-12-18 | 1989-06-23 | Ngk Spark Plug Co Ltd | Silicon nitride sintered compact and production thereof |
| JPH03218975A (en) * | 1990-01-23 | 1991-09-26 | Ngk Insulators Ltd | Silicon nitride body and production thereof |
| JPH04212441A (en) * | 1990-09-18 | 1992-08-04 | Ngk Insulators Ltd | Ceramic wiring board |
| JPH061663A (en) * | 1992-06-23 | 1994-01-11 | Toyota Motor Corp | Method for manufacturing silicon nitride sintered body |
| JPH06305837A (en) * | 1993-04-21 | 1994-11-01 | Sumitomo Electric Ind Ltd | Sintered silicon nitride |
| JPH0930866A (en) * | 1995-07-21 | 1997-02-04 | Nissan Motor Co Ltd | High thermal conductivity silicon nitride sintered body, method for producing the same, and insulating substrate made of silicon nitride sintered body |
| JPH09157030A (en) * | 1995-12-07 | 1997-06-17 | Denki Kagaku Kogyo Kk | Production of silicon nitride sintered compact |
| JPH09157054A (en) * | 1995-12-07 | 1997-06-17 | Denki Kagaku Kogyo Kk | Circuit board |
| JPH09268070A (en) * | 1996-04-03 | 1997-10-14 | Honda Motor Co Ltd | Manufacturing method of ceramic sintered body |
| JPH11100274A (en) * | 1997-09-26 | 1999-04-13 | Denki Kagaku Kogyo Kk | Silicon nitride sintered compact, its production and circuit board |
| JP2000128654A (en) * | 1998-10-28 | 2000-05-09 | Sumitomo Electric Ind Ltd | Silicon nitride composite substrate |
| JP2000351673A (en) * | 1999-06-10 | 2000-12-19 | Hitachi Metals Ltd | High thermal conductive silicon nitride sintered body and method for producing the same |
Non-Patent Citations (1)
| Title |
|---|
| 阿部弘 他, セラミックサイエンスシリーズ５ エンジニアリングセラミックス, vol. １版１刷, JPN7010002398, 25 September 1984 (1984-09-25), JP, pages 7, ISSN: 0001691484 * |
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