TW201400437A - 碳材-陶瓷材接合體的製造方法、及碳材-陶瓷材接合體 - Google Patents
碳材-陶瓷材接合體的製造方法、及碳材-陶瓷材接合體 Download PDFInfo
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- TW201400437A TW201400437A TW102116989A TW102116989A TW201400437A TW 201400437 A TW201400437 A TW 201400437A TW 102116989 A TW102116989 A TW 102116989A TW 102116989 A TW102116989 A TW 102116989A TW 201400437 A TW201400437 A TW 201400437A
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- 229910010293 ceramic material Inorganic materials 0.000 title claims abstract description 151
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 122
- 229910052799 carbon Inorganic materials 0.000 title claims abstract description 120
- 238000004519 manufacturing process Methods 0.000 title claims abstract description 27
- 238000000034 method Methods 0.000 title abstract description 27
- 239000003575 carbonaceous material Substances 0.000 claims abstract description 117
- 238000005245 sintering Methods 0.000 claims abstract description 96
- 239000000919 ceramic Substances 0.000 claims abstract description 46
- 238000005304 joining Methods 0.000 claims abstract description 6
- 229910000420 cerium oxide Inorganic materials 0.000 claims description 33
- BMMGVYCKOGBVEV-UHFFFAOYSA-N oxo(oxoceriooxy)cerium Chemical compound [Ce]=O.O=[Ce]=O BMMGVYCKOGBVEV-UHFFFAOYSA-N 0.000 claims description 33
- 239000010410 layer Substances 0.000 claims description 20
- 239000002344 surface layer Substances 0.000 claims description 17
- NFFIWVVINABMKP-UHFFFAOYSA-N methylidynetantalum Chemical compound [Ta]#C NFFIWVVINABMKP-UHFFFAOYSA-N 0.000 claims description 9
- 229910003468 tantalcarbide Inorganic materials 0.000 claims description 9
- 229920000049 Carbon (fiber) Polymers 0.000 claims description 7
- 239000004917 carbon fiber Substances 0.000 claims description 7
- 239000011521 glass Substances 0.000 claims description 7
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims description 7
- 239000002131 composite material Substances 0.000 claims description 6
- 239000007770 graphite material Substances 0.000 claims description 6
- 229910052751 metal Inorganic materials 0.000 claims description 6
- 239000002184 metal Substances 0.000 claims description 6
- 239000011148 porous material Substances 0.000 claims description 6
- 239000013078 crystal Substances 0.000 claims description 5
- 230000000717 retained effect Effects 0.000 claims description 5
- 229910052582 BN Inorganic materials 0.000 claims description 3
- PZNSFCLAULLKQX-UHFFFAOYSA-N Boron nitride Chemical compound N#B PZNSFCLAULLKQX-UHFFFAOYSA-N 0.000 claims description 3
- 229910026551 ZrC Inorganic materials 0.000 claims description 3
- OTCHGXYCWNXDOA-UHFFFAOYSA-N [C].[Zr] Chemical compound [C].[Zr] OTCHGXYCWNXDOA-UHFFFAOYSA-N 0.000 claims description 3
- 229910052810 boron oxide Inorganic materials 0.000 claims description 3
- BRPQOXSCLDDYGP-UHFFFAOYSA-N calcium oxide Chemical compound [O-2].[Ca+2] BRPQOXSCLDDYGP-UHFFFAOYSA-N 0.000 claims description 3
- 239000000292 calcium oxide Substances 0.000 claims description 3
- ODINCKMPIJJUCX-UHFFFAOYSA-N calcium oxide Inorganic materials [Ca]=O ODINCKMPIJJUCX-UHFFFAOYSA-N 0.000 claims description 3
- PMHQVHHXPFUNSP-UHFFFAOYSA-M copper(1+);methylsulfanylmethane;bromide Chemical compound Br[Cu].CSC PMHQVHHXPFUNSP-UHFFFAOYSA-M 0.000 claims description 3
- JKWMSGQKBLHBQQ-UHFFFAOYSA-N diboron trioxide Chemical compound O=BOB=O JKWMSGQKBLHBQQ-UHFFFAOYSA-N 0.000 claims description 3
- 239000007772 electrode material Substances 0.000 claims description 3
- FUJCRWPEOMXPAD-UHFFFAOYSA-N lithium oxide Chemical compound [Li+].[Li+].[O-2] FUJCRWPEOMXPAD-UHFFFAOYSA-N 0.000 claims description 3
- 229910001947 lithium oxide Inorganic materials 0.000 claims description 3
- 239000000395 magnesium oxide Substances 0.000 claims description 3
- CPLXHLVBOLITMK-UHFFFAOYSA-N magnesium oxide Inorganic materials [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 claims description 3
- AXZKOIWUVFPNLO-UHFFFAOYSA-N magnesium;oxygen(2-) Chemical compound [O-2].[Mg+2] AXZKOIWUVFPNLO-UHFFFAOYSA-N 0.000 claims description 3
- 150000004767 nitrides Chemical class 0.000 claims description 3
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 claims description 3
- 238000009628 steelmaking Methods 0.000 claims description 3
- MZLGASXMSKOWSE-UHFFFAOYSA-N tantalum nitride Chemical compound [Ta]#N MZLGASXMSKOWSE-UHFFFAOYSA-N 0.000 claims description 3
- 229910003470 tongbaite Inorganic materials 0.000 claims description 3
- MTPVUVINMAGMJL-UHFFFAOYSA-N trimethyl(1,1,2,2,2-pentafluoroethyl)silane Chemical compound C[Si](C)(C)C(F)(F)C(F)(F)F MTPVUVINMAGMJL-UHFFFAOYSA-N 0.000 claims description 3
- UONOETXJSWQNOL-UHFFFAOYSA-N tungsten carbide Chemical compound [W+]#[C-] UONOETXJSWQNOL-UHFFFAOYSA-N 0.000 claims description 3
- 238000003763 carbonization Methods 0.000 claims description 2
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 claims 2
- ZOXJGFHDIHLPTG-UHFFFAOYSA-N Boron Chemical compound [B] ZOXJGFHDIHLPTG-UHFFFAOYSA-N 0.000 claims 1
- 229910052684 Cerium Inorganic materials 0.000 claims 1
- 229910052796 boron Inorganic materials 0.000 claims 1
- GWXLDORMOJMVQZ-UHFFFAOYSA-N cerium Chemical compound [Ce] GWXLDORMOJMVQZ-UHFFFAOYSA-N 0.000 claims 1
- UFGZSIPAQKLCGR-UHFFFAOYSA-N chromium carbide Chemical compound [Cr]#C[Cr]C#[Cr] UFGZSIPAQKLCGR-UHFFFAOYSA-N 0.000 claims 1
- 229910010272 inorganic material Inorganic materials 0.000 description 37
- 239000011147 inorganic material Substances 0.000 description 37
- 238000001878 scanning electron micrograph Methods 0.000 description 23
- 238000009826 distribution Methods 0.000 description 16
- 239000012071 phase Substances 0.000 description 14
- 239000000463 material Substances 0.000 description 10
- 239000000853 adhesive Substances 0.000 description 7
- 230000001070 adhesive effect Effects 0.000 description 7
- 239000000203 mixture Substances 0.000 description 7
- PIGFYZPCRLYGLF-UHFFFAOYSA-N Aluminum nitride Chemical compound [Al]#N PIGFYZPCRLYGLF-UHFFFAOYSA-N 0.000 description 6
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 5
- 229910052782 aluminium Inorganic materials 0.000 description 5
- SIWVEOZUMHYXCS-UHFFFAOYSA-N oxo(oxoyttriooxy)yttrium Chemical compound O=[Y]O[Y]=O SIWVEOZUMHYXCS-UHFFFAOYSA-N 0.000 description 5
- 230000000052 comparative effect Effects 0.000 description 4
- 239000010439 graphite Substances 0.000 description 4
- 229910002804 graphite Inorganic materials 0.000 description 4
- 239000002245 particle Substances 0.000 description 4
- 229910052727 yttrium Inorganic materials 0.000 description 4
- WSFSSNUMVMOOMR-UHFFFAOYSA-N Formaldehyde Chemical compound O=C WSFSSNUMVMOOMR-UHFFFAOYSA-N 0.000 description 3
- 238000002844 melting Methods 0.000 description 3
- 230000008018 melting Effects 0.000 description 3
- 239000000843 powder Substances 0.000 description 3
- 229910052580 B4C Inorganic materials 0.000 description 2
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 description 2
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 2
- 238000002441 X-ray diffraction Methods 0.000 description 2
- 238000004873 anchoring Methods 0.000 description 2
- INAHAJYZKVIDIZ-UHFFFAOYSA-N boron carbide Chemical compound B12B3B4C32B41 INAHAJYZKVIDIZ-UHFFFAOYSA-N 0.000 description 2
- WXANAQMHYPHTGY-UHFFFAOYSA-N cerium;ethyne Chemical compound [Ce].[C-]#[C] WXANAQMHYPHTGY-UHFFFAOYSA-N 0.000 description 2
- 239000011651 chromium Substances 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 238000010438 heat treatment Methods 0.000 description 2
- 239000007788 liquid Substances 0.000 description 2
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 description 2
- 230000035515 penetration Effects 0.000 description 2
- 229910052710 silicon Inorganic materials 0.000 description 2
- 239000002002 slurry Substances 0.000 description 2
- 238000002490 spark plasma sintering Methods 0.000 description 2
- 229910001220 stainless steel Inorganic materials 0.000 description 2
- 239000010935 stainless steel Substances 0.000 description 2
- 229910001928 zirconium oxide Inorganic materials 0.000 description 2
- ZWEHNKRNPOVVGH-UHFFFAOYSA-N 2-Butanone Chemical compound CCC(C)=O ZWEHNKRNPOVVGH-UHFFFAOYSA-N 0.000 description 1
- LJKDOMVGKKPJBH-UHFFFAOYSA-N 2-ethylhexyl dihydrogen phosphate Chemical compound CCCCC(CC)COP(O)(O)=O LJKDOMVGKKPJBH-UHFFFAOYSA-N 0.000 description 1
- 229920002799 BoPET Polymers 0.000 description 1
- ISWSIDIOOBJBQZ-UHFFFAOYSA-N Phenol Chemical compound OC1=CC=CC=C1 ISWSIDIOOBJBQZ-UHFFFAOYSA-N 0.000 description 1
- 239000002202 Polyethylene glycol Substances 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 1
- 238000005452 bending Methods 0.000 description 1
- -1 benzyl benzyl butyl citrate Chemical compound 0.000 description 1
- 239000011230 binding agent Substances 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 238000010000 carbonizing Methods 0.000 description 1
- 239000004927 clay Substances 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 239000002270 dispersing agent Substances 0.000 description 1
- 229920006332 epoxy adhesive Polymers 0.000 description 1
- 238000010304 firing Methods 0.000 description 1
- 230000004927 fusion Effects 0.000 description 1
- 238000007731 hot pressing Methods 0.000 description 1
- 229910052746 lanthanum Inorganic materials 0.000 description 1
- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 description 1
- 239000011777 magnesium Substances 0.000 description 1
- 238000010297 mechanical methods and process Methods 0.000 description 1
- 239000000155 melt Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 239000005011 phenolic resin Substances 0.000 description 1
- 229920002037 poly(vinyl butyral) polymer Polymers 0.000 description 1
- 229920001223 polyethylene glycol Polymers 0.000 description 1
- 229920005989 resin Polymers 0.000 description 1
- 239000011347 resin Substances 0.000 description 1
- 239000007790 solid phase Substances 0.000 description 1
- 239000002904 solvent Substances 0.000 description 1
- 238000009864 tensile test Methods 0.000 description 1
- RUDFQVOCFDJEEF-UHFFFAOYSA-N yttrium(III) oxide Inorganic materials [O-2].[O-2].[O-2].[Y+3].[Y+3] RUDFQVOCFDJEEF-UHFFFAOYSA-N 0.000 description 1
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- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B18/00—Layered products essentially comprising ceramics, e.g. refractory products
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- C04B35/522—Graphite
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Abstract
本發明提供一種新穎之碳材-陶瓷材接合體的製造方法,係接合碳材10與陶瓷材12而成之碳材-陶瓷材接合體2的製造方法,係藉由於碳材10上形成含有陶瓷及燒結助劑之層11並進行燒結,俾得到碳材-陶瓷材接合體2。
Description
本發明係關於一種碳材-陶瓷材接合體之製造方法、及碳材-陶瓷材接合體。
碳材係在常壓不具有融點。又,陶瓷一般係高融點材料。因而,要使碳材與陶瓷藉融接法接合可謂很困難。
又,碳材或陶瓷一般為脆性材料。因此,要使碳材與陶瓷材藉壓接法接合係很困難。碳材與陶瓷材之接合一般藉由使用螺絲等之機械方法,或使用蠟材、黏著劑等之方法來完成。
例如,在專利文獻1中揭示一種使用酚/甲醛樹脂黏著石墨材之方法。於專利文獻2中揭示一種使用酚樹脂等之碳系黏著劑黏著石墨材。在專利文獻3中揭示一種使用蠟材接合石墨與鋁系材料之方法。
[專利文獻1]特開平6-345553號公報
[專利文獻2]特開2002-321987號公報
[專利文獻3]特開平4-26567號公報
然而,例如在使用有機物之黏著劑的方法中,要製造於高溫加熱之用途所使用的碳材-陶瓷材接合體係很困難。又,即使在使如上述之黏著劑碳化的方法中,亦顧慮已碳化之黏著劑會降低導熱性。使用蠟材時,碳材-陶瓷材接合體在蠟材之融點以上係無法使用,而要製造於高溫加熱之用途所使用的碳材-陶瓷材接合體係很困難。如此之狀況下,尋求碳材與無機材更有力之接合方法。
本發明之主要目的在於提供一種新穎的碳材-陶瓷材接合體之製造方法。
本發明係接合碳材與陶瓷材而成之碳材-陶瓷材接合體的製造方法。在本發明中係藉由於碳材上形成含有陶瓷及燒結助劑之層,並燒結,俾得到碳材-陶瓷材接合體。
本發明之碳材-陶瓷材接合體之製造方法中,燒結助劑宜使用由氧化釔、氧化鋁、氧化鈣、氧化鋰、氧化矽、氧化硼、氧化鋯、氧化鎂、氧化鈰、氧化釓、氧化銪、氧化鑭、氧化鎦、氧化釹、氧化鉺、氧化鏑、及氧化釤所構成之群中選出的至少一種。
本發明之碳材-陶瓷材接合體之製造方法中,宜藉由
燒結,使燒結助劑浸入於碳材之表層的凹部或氣孔,並使其冷卻,藉此使燒結助劑滯留於碳材之表層。
本發明之碳材-陶瓷材接合體之製造方法中,宜於前述陶瓷及/或前述燒結助劑含有矽元素,藉前述燒結,於前述碳材與前述陶瓷材之界面形成結晶相或非晶質玻璃相。
本發明之碳材-陶瓷材接合體之製造方法中,宜使含有陶瓷及燒結助劑之層中的燒結助劑之含量為2質量%以上。
本發明之碳材-陶瓷材接合體之製造方法中,就前述陶瓷而言,宜使用金屬氮化物及金屬碳化物之至少一者。
本發明之碳材-陶瓷材接合體之製造方法中,陶瓷宜使用由氮化鋁、氮化硼、氮化矽、碳化矽、碳化硼、碳化鉭、碳化鋯、碳化鎢、碳化鈦、碳化鉻、及碳化鈮所構成之群中選出的至少一種。
本發明之碳材-陶瓷材接合體之製造方法中,碳材宜使用由製鋼用電極材、等方性石墨材、多孔質碳材、碳纖維集合體、碳纖維複合材料、及碳纖維強化碳複合材料所構成之群中選出的至少一種。
本發明之第1碳材-陶瓷材接合體,具備碳材與陶瓷材。陶瓷材係與碳材接合。於碳材之陶瓷材側之表層、與陶瓷材之碳材側之表層的兩方,含有可使用於陶瓷材之燒結的燒結助劑。
本發明之第1碳材-陶瓷材接合體中,於碳材之陶瓷材側之表層中之燒結助劑的含量,亦可高於陶瓷材之碳材側之燒結助劑的含量。
本發明之第2碳材-陶瓷材接合體,具備碳材及與前
述碳材接合之陶瓷材。於前述碳材與前述陶瓷材之接合界面,設有藉燒結而形成之結晶相或非晶質玻璃相。
若依本發明,可提供一種新穎之碳材-陶瓷材接合體的製造方法。
1‧‧‧碳材-陶瓷層合材
2‧‧‧碳材-陶瓷材接合體
10‧‧‧碳材
11‧‧‧陶瓷層
12‧‧‧陶瓷材
第1圖係用以說明本發明之一實施形態中的碳材-陶瓷材接合體之製造方法的簡略截面圖。
第2圖係本發明之一實施形態中的碳材-陶瓷材接合體之簡略截面圖。
第3圖係在實施例1所得到之碳材-陶瓷材接合體A中的碳材與陶瓷材之界面部分的SEM像。
第4圖係在實施例1所得到之碳材-陶瓷材接合體A中的碳材與無機材之界面部分的Al元素之分布的SEM像。
第5圖係在實施例1所得到之碳材-陶瓷材接合體A中的碳材與無機材之界面部分的C元素之分布的SEM像。
第6圖係在實施例1所得到之碳材-陶瓷材接合體A中的碳材與無機材之界面部分的Y元素之分布的SEM像。
第7圖係在實施例2所得到之碳材-陶瓷材接合體B中的碳材與無機材之界面部分的SEM像。
第8圖係在實施例2所得到之碳材-陶瓷材接合體B中的碳材與無機材之界面部分的Al元素之分布的SEM像。
第9圖係在實施例2所得到之碳材-陶瓷材接合體B中的碳
材與無機材之界面部分的C元素之分布的SEM像。
第10圖係在實施例2所得到之碳材-陶瓷材接合體B中的碳材與無機材之界面部分的Y元素之分布的SEM像。
第11圖係在實施例5所得到之碳材-陶瓷材接合體E中的碳材與陶瓷材之界面部分的SEM像。
第12圖係在比較例2所得到之碳材-陶瓷材接合體H中的碳材與陶瓷材之界面部分的SEM像。
第13圖係表示在實施例4至6所得到之碳材-陶瓷材接合體D至F的界面部分之X線繞射的譜峯強度圖形。
第14圖係在實施例4所得到之碳材-陶瓷材接合體D中的碳材與無機材之界面部分的Si元素之分布的SEM像。
第15圖係在實施例4所得到之碳材-陶瓷材接合體D中的碳材與無機材之界面部分的Al元素之分布的SEM像。
第16圖係在實施例4所得到之碳材-陶瓷材接合體D中的碳材與無機材之界面部分的Y元素之分布的SEM像。
第17圖係在實施例6所得到之碳材-陶瓷材接合體F中的碳材與無機材之界面部分的Si元素之分布的SEM像。
第18圖係在實施例6所得到之碳材-陶瓷材接合體F中的碳材與無機材之界面部分的Al元素之分布的SEM像。
第19圖係在實施例6所得到之碳材-陶瓷材接合體F中的碳材與無機材之界面部分的Y元素之分布的SEM像。
以下,說明有關實施本發明較佳形態的一例。但,下述之實施形態係僅例示。本發明係不受下述之實施形態任何限
定。
在實施形態等參照之圖面係被模式性記載者,被描繪於圖面之物體的尺寸之比率等係有時與現實物體之尺寸的比率等相異。具體之物體的尺寸比率等係參酌以下之說明而判斷。
第1圖係用以說明本實施形態中的碳材-陶瓷材接合體之製造方法的簡略截面圖。第2圖係本實施形態中的碳材-陶瓷材接合體之簡略截面圖。參照第1圖及第2圖,同時說明有關本實施形態中之碳材-陶瓷材接合體2的製造方法及構成。
(碳材-陶瓷材接合體2之製造方法)
在碳材-陶瓷材接合體2之製造方法中,首先準備第1圖所示之碳材10。
碳材10係只要為以碳為主成分者,並無特別限定。碳材10材係宜使用由製鋼用電極材、等方性石墨材、多孔質碳材、碳纖維集合體、碳纖維複合材料、及碳纖維強化碳複合材料所構成之群中選出的至少一種。碳材10之形狀,並無特別限定。碳材係可為碳質,亦可為石墨質。
然後,於碳材之上形成含有陶瓷及燒結助劑之層的陶瓷層11,得到碳材-陶瓷層合體1。陶瓷層11係藉由陶瓷及燒結助劑之混合物所構成。陶瓷層11係例如可為陶瓷粒子與燒結助劑粒子之混合物,亦可為燒結助劑分散之板狀的陶瓷等。陶瓷層11係亦可含有陶瓷及燒結助劑以外之成分。
陶瓷之種類並無特別限定。陶瓷宜為使用金屬氮化物及金屬碳化物之至少一者。陶瓷以使用由氮化鋁、氮化硼、氮化矽、碳化矽、碳化硼、碳化鉭、碳化鋯、碳化鎢、碳化鈦、碳
化鉻、及碳化鈮所構成之群中選出的至少一種較佳。
繼而,加熱碳材-陶瓷層合體1而燒結陶瓷層11。藉此,可得到接合第2圖所示之碳材10與陶瓷材12之碳材-陶瓷材接合體2。
燒結陶瓷層11之方法係並無特別限定。燒結方法可舉例如放電電漿燒結法、熱壓法、常壓燒結法等。燒結時之溫度宜為1600℃以上,更宜為1800℃以上。燒結時之溫度一般為2100℃以下。燒結時之壓力宜為1MPa以上,更宜為10MPa以上。燒結時之壓力一般為40MPa以下。
陶瓷層11之燒結時,燒結助劑及源自燒結助劑之成分的至少一者(以下,有時稱為「燒結助劑等」)之至少一部分從陶瓷層11移動至碳材10。茲認為此係起因於燒結助劑等在燒結之高溫下成為液狀,浸入於碳材10之表層的凹部或氣孔等,使其冷卻,藉此使燒結助劑等固化而滯留於碳材10。亦即,在本實施形態中係藉燒結,藉由使燒結助劑浸入於碳材10之表層的凹部或氣孔,使其冷卻,俾使燒結助劑滯留於碳材10之表層。
燒結助劑係例如可使用被用於陶瓷之燒結之一般燒結助劑。為更牢固碳材-陶瓷材接合體2中之碳材10與陶瓷材12的接合,燒結助劑宜使用由氧化釔、氧化鋁、氧化鈣、氧化鋰、氧化矽、氧化硼、氧化鋯、氧化鎂、氧化鈰、氧化釓、氧化銪、氧化鑭、氧化鎦、氧化釹、氧化鉺、氧化鏑、及氧化釤所構成之群中選出的至少一種。
為更牢固碳材10-陶瓷材12之接合,陶瓷層11中之燒結助劑的含量宜為2質量%以上,更宜為3質量%左右。陶瓷
層11中之燒結助劑的含量宜為15質量%以下,更宜為10質量%以下。
如以上做法,可製造碳材-陶瓷材接合體2。
(碳材-陶瓷材接合體2)
如第2圖所示般,碳材-陶瓷材接合體2係具備碳材10與陶瓷材12。陶瓷材12係與碳材10接合。
於碳材10之陶瓷材12側之表層、與陶瓷材12之碳材10側之表層的兩者,含有可使用於陶瓷12材之燒結的燒結助劑。有時於碳材10之陶瓷材12側之表層之燒結助劑的含量高於陶瓷材12之碳材10側之燒結助劑的含量。認為此係在燒結之高溫下,成為液體之燒結助劑等係易浸入於碳材10之表層中的凹部或氣孔等,滯留於碳材10之比率高之故。
在碳材-陶瓷材接合體2中,碳材10與陶瓷材12係牢固地接合。此理由之內容係未必明確,但例如,可如下般認為。如上述般,陶瓷層11之燒結時,於陶瓷層11所含有的燒結助劑等係成為液狀,浸入於碳材10之表層中的凹部或氣孔等,藉其後之冷卻而固化。認為此時,在碳材10與陶瓷材12之界面部分燒結助劑等固化,俾介由燒結助劑等而使碳材10與陶瓷材12牢固地接合。
又,碳材-陶瓷材接合體2係未必需要使用蠟材或黏著劑等。因此,碳材-陶瓷材接合體2係例如即使在1000℃以上之高溫下亦可使用。
又因未必需要使用蠟材或黏著劑等,故在碳材-陶瓷材接合體2中係未形成熱阻抗層。因而,碳材-陶瓷材接合體2
具有良好之導熱率。
以下,有關本發明,依據具體之實施例,更詳細說明。本發明係不受以下之實施例任何限定。在不變更本發明之旨意的範圍中,可適當變更而實施。
(實施例1)
就碳材而言,使用體密度為1.8Mg/m3、彎曲強度為40MPa、線熱膨脹係數為4.7×10-6/K之等方性石墨。無機材料係使用氮化鋁(AlN)粉末。燒結助劑係使用氧化釔(Y2O3)。以無機材料與燒結助劑就質量比成為95:5之方式混合,使此混合物配置於碳材上而製作層合體。使所得到之層合體藉放電電漿燒結法在約30MPa之壓力下,以約1900℃加熱,製作碳材-陶瓷材接合體A。
繼而,為了測定碳材-陶瓷材接合體之接合強度之目的,實施抗拉試驗。在上述碳材之上下分別以與上述相同之方法,製作接合無機材之3層構造體。於上下各別之無機材使不銹鋼治具以環氧系黏著劑黏著。此時,黏著條件係以80℃保持24小時以上。以強度試驗機使被固定於試驗片之不銹鋼製治具以0.5分/mm拉張,測定石墨材與無機材之接合強度。其結果,接合強度為13MPa。碳材-陶瓷材接合體A中,碳材與無機材係牢固地接合。
在碳材-陶瓷材接合體A中的碳材與無機材之界面部分的SEM像表示於第3圖。又,將Al、C及Y元素之分布分別表示於第4圖、第5圖、第6圖中。從第3圖至6明顯可知,於碳材側存在許多燒結助劑。
(實施例2)
就無機材料與燒結助劑之混合物而言,除使用含有氧化釔
(Y2O3)之氮化鋁(AlN)燒結板以外,其餘係與實施例1同樣做法製作碳材-陶瓷材接合體B。
與實施例1同樣做法,測定碳材-陶瓷材接合體B之接合強度為10MPa。在碳材-陶瓷材接合體B中,碳材與無機材牢固地接合。
在碳材-陶瓷材接合體B中的碳材與無機材之界面部分的SEM像表示於第7圖。又,將Al、C及Y元素之分布分別表示於第8圖、第9圖、第10圖中。從第7至10圖明顯可知,於碳材側存在許多燒結助劑。
(實施例3)
使作為無機材料之氮化鋁(AlN)粉末(平均粒徑0.6μm、比表面積2.7m2/g)與作為燒結助劑之氧化釔(Y2O3),就質量比(無機材料:燒結助劑)成為95:5之方式混合。然後,於此混合物中添加作為分散劑之磷酸2-乙基己酯、作為溶劑之2-丁酮/乙醇混合物(體積比67:33)、作為黏結劑之聚乙烯基丁縮醛、作為可塑劑之聚乙二醇/酞酸苯甲基丁基醇混合物(質量比50:50),以自轉/公轉混合機混合而得到漿液。所得到之漿液使用刮刀塗佈於PET膜上,乾燥而得到140μm之薄片。除了將此薄片配置於在實施例2使用之碳材與氮化鋁(AlN)燒結板之間而形成層合體以外,其餘與實施例1同樣做法藉放電電漿燒結法製作碳材-陶瓷材接合體C。
與實施例1同樣做法,測定碳材-陶瓷材接合體C之接合強度為14MPa。在碳材-陶瓷材接合體C中,碳材與無機材牢固地接合。
在實施例1至3中,燒結或燒成時燒結助劑熔融,滲出於碳材與陶瓷材之接合部分,但添加Y2O3或Al2O3作為相燒結助劑進行燒結時,推論在接合界面中產生Al2Y4O9之結晶相。除了燒結助劑於碳材之浸透外,此結晶相於碳材與陶瓷材埋入碳材與陶瓷材界面之間隙,同時產生咬入碳材表面之凹凸部的錨定效果,可得到牢固之接合強度。
(實施例4)
使用作為無機材料之碳化矽(SiC)粉末(平均粒徑0.8μm、比表面積13m2/g至15m2/g),使用氧化釔(Y2O3)與氧化鋁(Al2O3)作為燒結助劑,以重量比成為SiC:Y2O3:Al2O3=91:3:6之方式混合,除使放電電漿燒結法之溫度為1800℃以外,其餘係與實施例1同樣做法製作碳材-陶瓷材接合體D。
與實施例1同樣做法,測定碳材-陶瓷材接合體D之接合強度為18MPa。在碳材-陶瓷材接合體D中,碳材與無機材牢固地接合。
(實施例5)
除使放電電漿燒結法之溫度為1900℃以外,其餘係與實施例4同樣做法製作碳材-陶瓷材接合體E。與實施例1同樣做法,測定碳材-陶瓷材接合體E之接合強度為18MPa。在碳材-陶瓷材接合體E中,碳材與無機材牢固地接合。
(實施例6)
除使放電電漿燒結法之溫度為2000℃以外,其餘係與實施例4同樣做法製作碳材-陶瓷材接合體F。與實施例1同樣做法,測定碳材-陶瓷材接合體F之接合強度為12MPa。在碳材-陶瓷材接
合體F中,碳材與無機材牢固地接合。
(實施例7)
除使氮化鋁(AlN)與氧化釔(Y2O3)之摻合比率就質量比成為97.5:2.5以外,其餘係與實施例1同樣做法製作碳材-陶瓷材接合體I。與實施例1同樣做法,測定碳材-陶瓷材接合體I之接合強度為9MPa。在碳材-陶瓷材接合體I中,碳材與無機材牢固地接合。
(實施例8)
除使氮化鋁(AlN)與氧化釔(Y2O3)之摻合比率就質量比成為90:10以外,其餘係與實施例1同樣做法製作碳材-陶瓷材接合體J。與實施例1同樣做法,測定碳材-陶瓷材接合體J之接合強度為19MPa。在碳材-陶瓷材接合體J中,碳材與無機材牢固地接合。
(比較例1)
除不使用燒結助劑以外,與實施例1同樣做法,使層合體以放電電漿燒結法接合,製作碳材-陶瓷材接合體G。
與實施例1同樣做法,測定碳材-陶瓷材接合體G之接合強度為5MPa。在碳材-陶瓷材接合體G中,碳材與無機材之接合強度小。
(比較例2)
除不使用燒結助劑以外,與實施例5同樣做法,使層合體以放電電漿燒結法接合,製作碳材-陶瓷材接合體H。
與實施例1同樣做法,測定碳材-陶瓷材接合體H之接合強度為5MPa。在碳材-陶瓷材接合體H中,碳材與無機材之
接合強度小。
第11圖係實施例5之碳材-陶瓷材之界面部分的SEM像。第12圖係比較例2之碳材-陶瓷材之界面部分的SEM像。由第11圖可知碳材與陶瓷材之接合部分看不到間隙而牢固地結合。然而在第12圖中可知碳材與陶瓷材之接合部分可看到間隙而接合不充分。
第13圖係表示在實施例4至6所得到之碳材-陶瓷材的界面部分之X線繞射的譜峯強度之圖形。燒結或燒成時燒結助劑熔融,滲出於碳材與陶瓷材之接合部分,但在第13圖中係看不到在35°及43°附近被檢出之Al2O3的譜峯或在29°及49°附近被檢出之Y2O3的譜峯。又,一般於SiC添加Y2O3或Al2O3作為相燒結助劑進行燒結時,已知形成Si-Al-Y-O系之相,但除了石墨、SiC以外未看到結晶相(黏土之譜峯係使用於試料固定者)。因此,推論於界面部分形成Si-Al-Y-O之非晶質玻璃相,該非晶質玻璃相於碳材與陶瓷材埋入碳材與陶瓷材界面之間隙,同時產生咬入於碳材表面之凹凸部的錨定效果,可得到牢固之接合強度。
於第14至16圖係在實施例4所得到之碳材-陶瓷材接合體D中的碳材與無機材之界面部分的Si、Al及Y元素之分布的SEM像。在實施例4中係雖可看到界面部分牢固地接合,但燒結助劑對碳材之浸透未明顯看到,故推論上述之非晶質玻璃相的形成有助於接合。
於第17至19圖係在實施例6所得到之碳材-陶瓷材接合體F中的碳材與無機材之界面部分的Si、Al及Y元素之分布的SEM像。在實施例6中係可看到界面部分牢固地接合,同時明
白燒結助劑浸透於碳材、於碳材側存在許多燒結助劑。
本案圖式為實施形態之簡略截面圖、SEM像及譜峯強度表,不足以代表本案技術特徵。
Claims (11)
- 一種碳材-陶瓷材接合體之製造方法,係接合碳材與陶瓷材而成之碳材-陶瓷材接合體的製造方法,藉由於前述碳材上形成含有陶瓷及燒結助劑之層並進行燒結,俾得到前述碳材-陶瓷材接合體。
- 如申請專利範圍第1項所述之碳材-陶瓷材接合體之製造方法,其中,前述燒結助劑係使用由氧化釔、氧化鋁、氧化鈣、氧化鋰、氧化矽、氧化硼、氧化鋯、氧化鎂、氧化鈰、氧化釓、氧化銪、氧化鑭、氧化鎦、氧化釹、氧化鉺、氧化鏑、及氧化釤所構成之群中選出的至少一種。
- 如申請專利範圍第1或2項所述之碳材-陶瓷材接合體之製造方法,其中,藉由前述燒結,使前述燒結助劑浸入於前述碳材之表層的凹部或氣孔,並進行冷卻,藉此使前述燒結助劑滯留於碳材之表層。
- 如申請專利範圍第1至3項中任一項所述之碳材-陶瓷材接合體之製造方法,其中,於前述陶瓷及/或前述燒結助劑含有矽元素,藉由前述燒結,於前述碳材與前述陶瓷材之界面形成結晶相或非晶質玻璃相。
- 如申請專利範圍第1至4項中任一項所述之碳材-陶瓷材接合體之製造方法,其中,使含有前述陶瓷及前述燒結助劑之層中的前述燒結助劑之含量為2質量%以上。
- 如申請專利範圍第1至5項中任一項所述之碳材-陶瓷材接合體之製造方法,其中,前述陶瓷係使用金屬氮化物及金屬碳化物之至少一者。
- 如申請專利範圍第1至6項中任一項所述之碳材-陶瓷材接合體之製造方法,其中,前述陶瓷係使用由氮化鋁、氮化硼、氮化矽、碳化矽、碳化硼、碳化鉭、碳化鋯、碳化鎢、碳化鈦、碳化鉻、及碳化鈮所構成之群中選出的至少一種。
- 如申請專利範圍第1至7項中任一項所述之碳材-陶瓷材接合體之製造方法,其中,前述碳材係使用由製鋼用電極材、等方性石墨材、多孔質碳材、碳纖維集合體、碳纖維複合材料、及碳纖維強化碳複合材料所構成之群中選出的至少一種。
- 一種碳材-陶瓷材接合體,係具備:碳材及與前述碳材接合之陶瓷材;於前述碳材之前述陶瓷材側之表層、以及前述陶瓷材之前述碳材側之表層的兩方,含有可使用於前述陶瓷材之燒結的燒結助劑。
- 如申請專利範圍第9項所述之碳材-陶瓷材接合體,其中,於前述碳材之前述陶瓷材側之表層中之前述燒結助劑的含量高於前述陶瓷材之前述碳材側之燒結助劑的含量。
- 一種碳材-陶瓷材接合體,係具備:碳材及與前述碳材接合之陶瓷材;於前述碳材與前述陶瓷材之接合界面,設有藉燒結所形成之結晶相或非晶質玻璃相。
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CA2897496A1 (en) * | 2013-02-04 | 2014-08-07 | Toyo Tanso Co., Ltd. | Joined material and method of manufacturing same |
US20160023956A1 (en) * | 2014-07-28 | 2016-01-28 | The Curators Of The University Of Missouri | Ceramic-ceramic welds |
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WO2021090759A1 (ja) * | 2019-11-05 | 2021-05-14 | 三菱マテリアル株式会社 | グラフェン含有炭素質部材/セラミックス接合体、および、銅/グラフェン含有炭素質部材/セラミックス接合体 |
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