CN1195653A - Ceramic and metal part instant liquid phase connecting method - Google Patents

Ceramic and metal part instant liquid phase connecting method Download PDF

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CN1195653A
CN1195653A CN97106923A CN97106923A CN1195653A CN 1195653 A CN1195653 A CN 1195653A CN 97106923 A CN97106923 A CN 97106923A CN 97106923 A CN97106923 A CN 97106923A CN 1195653 A CN1195653 A CN 1195653A
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liquid phase
temperature
pottery
metal part
connecting method
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CN1059418C (en
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陈铮
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Abstract

The present invention relates to a method for joining ceramic material to metal material, and is characterized by that firstly, between the ceramic material and the metal material several layers of intermediate materials are placed, in which at least one layer of Ti, one layer of Cu and another layer of metal material which can be formed into uniform crystalline phase diagram relationship with Cu and its melting point is higher than that of Cu are included, then the above-mentioned materials are heated to implement first partial instantaneous liquid-phase joining, then also heated to make secondary partial instantaneous liquid-phase joining. As compared with existent techniques, said invention possesses the advantages of high joining strength, high jointed heat resistance and no brittle compound produced between several layers of intermediate materials after they are joined.

Description

Pottery and metal part instant liquid phase connecting method
The present invention relates to a kind of pottery and metal method of attachment.
In order to give full play to the performance complement between stupalith and the metallic substance, developing reliable and practical pottery and metal method of attachment is a high-tech research project that the essential industry application background is arranged.
Known method of attachment at present mainly contains: active metal brazing; Solid phase diffusion connects; Eutectic reaction connects; The glass-ceramic liquid phase connects; Connect behind the ceramic surface metallization; Friction welding (FW) connects; Ultrahigh vacuum(HHV) normal temperature connects; Laser and electrons leaves welding.Studies show that it is two kinds of methods of attachment that industrial application value and prospect are arranged most that active metal brazing is connected with solid phase diffusion.
Active metal brazing is to add active element at the plain metal solder, by the surface reaction between active element and the pottery, makes solder soak into and sprawl at ceramic surface, and realizes the method that chemistry connects.Studies show that the most effective active element is Ti and Zr, at present external existing Ag-Cu-Ti and the solder commercial distribution of Ag-Cu-Ti-In isoreactivity and on many actual industrial products (as ceramic engine) be applied.But because these active solder fusing points are low, generally be no more than 750K, also resistance to oxidation not with the use temperature of the joint of their solderings.Therefore, in recent years both at home and abroad all at active development high temperature active solder,, but also there is not sophisticated high temperature active solder to come out so far as Cu-Ti, Ni-Cu-Ti and Pd-Cu-Ti etc.
Solid phase diffusion connects, though can guarantee high high temperature strength of joint, but connecting, it needs under higher temperature and pressure, to carry out, this might increase distortion and the breakage that connects unrelieved stress and cause web member, also need simultaneously high precision processing is carried out on surface to be connected, to guarantee good initial contact between the joint face, required equipment is also complicated and expensive, and it is to be solved to also have many problems to have on using.
In recent years, people have developed a kind of new pottery and metal (or pottery) method of attachment under the inspiration of " connection of Ni based heat resistant alloy transient liquid phase ", be called " partial transient liquid phase connection ".This method of attachment fully combines active metal brazing and is connected both advantages with solid phase diffusion.By using the multilayer middle layer of microcosmic design, only near ceramic surface, form local liquid phase region in the connection procedure, play a part to be similar to solder, and then by the mutual diffusion mutually between liquid alloy and the refractory metal core layer, make liquid alloy isothermal solidification and further solid phase homogenization of composition, the fusing point of bonding land material is significantly improved, thereby show the heat-resistant quality of solid phase diffusion jointing.
Active soldering with all use homogeneous material (solder and/or middle layer) during solid phase diffusion is connected, the composition and the variation of melting point of solder are little before and after the soldering, and do not wish the undue corrosion of solder to metal mother metal or middle layer.Partial transient liquid phase is then selected inhomogeneous middle layer (B/A/B for use in connecting, the thickness of B is much smaller than the thickness of A), connecting under the temperature, only form local liquid phase region by the fusing of B or the interface of A/B at next-door neighbour's pottery place, joining region, play the effect of solder, and make liquid phase region isothermal solidification and solid phase homogenization of composition through long phase mutual diffusion, make joint have the heat-resistant quality that solid phase diffusion connects again.Because have liquid phase to participate in surface reaction, thereby partial transient liquid phase connects and soldering is similar, need not connect pressure in theory, it is much smaller that the actual pressure ratio solid phase of using connects, this also is the convenient part on using.
For realizing that pottery is connected with intermetallic chemistry, the fundamental principle that intermediate layer material was selected during partial transient liquid phase connected is as follows: the fundamental principle that a layer material is selected is as follows:
(1) surface reaction can take place with pottery and soak in B or A-B liquid alloy, and therefore, one of A and B must be active elements; When (2) relying on the A/B interfacial diffusion to form liquid phase, should have eutectic phasor relation between A, B, and moderate eutectic temperature (having determined the connection temperature) is arranged; And when only forming liquid phase by dissolving of B, connect temperature and then depend on the B fusing point, at this moment, between A and the B uniform grain or peritectoid phasor; (3) A (pure metal or A base alloy) should select according to performances such as hot strength, thermal expansion number, Young's modulus and scale resistances, and the middle layer test-results was to select the important evidence of A during solid phase diffusion connected; (4) high interdiffustion coefficient is arranged as far as possible between A, the B, to shorten whole process time; (5) do not produce frangible compounds between A, the B as far as possible.
Known intermediate layer material has at present: Cu/Ni/Cu, Cu/Pt/Cu and Cu/Ni-(20-22%Cr)/Cu is used for Al 2O 3The partial transient liquid phase of pottery connects; Ti/Ni/Ti, Au/Ni-22%Cr/Au are used for Si 3N 4The partial transient liquid phase of pottery connects, and the Ni base Alloy Foil of the useful plating of nearest test Au-Cu connects the Si that Ti has been plated on the surface 3N 4Pottery, strength of joint is up to 770MPa.As seen, reactive metal Ti is used for that partial transient liquid phase connects has only the Ti/Ni/Ti middle layer at present.According to the Ti-Ni phasor, when more than eutectic temperature, carrying out the partial transient liquid phase connection, compound between two kinds of friable metals that form between Ti and the Ni, Ni 3Ti and NiTi can reduce strength of joint significantly.Thereby still there is obvious deficiency in Ti/Ni/Ti multilayer middle layer in practicality.Because Ti is active to nearly all pottery (comprising oxide ceramics and non-oxide ceramics), therefore uses active element Ti to carry out partial transient liquid phase and connect significant and general applied value as intermediate layer material.
The present invention promptly is at above the deficiencies in the prior art part, and no frangible compounds produces in a kind of multilayer intermediate materials, strength of joint is high pottery and metal part instant liquid phase connecting method are provided.
The object of the present invention is achieved like this:
A kind of pottery and metal part instant liquid phase connecting method, elder generation's placement of multiple layers intermediate materials between pottery and metal, the connection of heating again, at least comprise one deck Ti, one deck Cu, one deck X material in the said multilayer intermediate materials, said X material is to become uniform grain phasor relation and the fusing point metallic substance higher than Cu fusing point with Cu, and above-mentioned trilaminate material is adjacent successively; After being placed on above-mentioned multilayer intermediate materials between pottery and the metal, carrying out first time partial transient liquid phase and connect, promptly heat to first connect temperature and on this temperature isothermal, said first connects temperature between the fusing point of the eutectic temperature of Ti and Cu and Cu; Above-mentioned first time partial transient liquid phase connect finish after, carry out second time partial transient liquid phase and connect, promptly further be warming up to second connect temperature and on this temperature isothermal, the said second connection temperature is between the fusing point of the fusing point of Cu and X material.
Said multilayer intermediate materials is five layer materials, and their adjacent order is followed successively by Ti, Cu, X, Cu, Ti.
Said X material is Ni.
The said first connection temperature is 1323K.
The said second connection temperature is 1373K.
Said X material is Au.
Said X material is Pd.
Said X material is Pt.
The present invention is further illustrated below in conjunction with accompanying drawing.
Fig. 1 is multilayer intermediate materials state graph in the present invention's partial transient liquid phase connection procedure first time;
Fig. 2 is multilayer intermediate materials state graph in the present invention's partial transient liquid phase connection procedure second time;
In the present embodiment, adopting Ti-Cu-Ni-Cu-Ti is the multilayer intermediate materials, then be eutectic phasor relation between Ti and the Cu, be uniform grain phasor relation between Cu and the Ni, after being placed on this multilayer intermediate materials between pottery and the metal, carrying out for the first time, partial transient liquid phase connects (a figure expression original state among Fig. 1), promptly heat to the first connection temperature, and continue to be incubated, this temperature is between the fusing point of the eutectic temperature of Ti and Cu and Cu, be advisable with 1323K, owing to be eutectic phasor relation between Ti and the Cu, at this moment by the mutual diffusion mutually between Ti and the Cu rapidly at the liquid phase region that forms Cu-Ti at the interface, and move to Ti side and Cu thruster simultaneously, when selecting thin Ti layer, liquid phase region makes the Ti layer all melt (dissolving) to the passing of Ti side the most at last, the state of this moment is shown in b figure among Fig. 1, and wherein 1 is the Cu-Ti liquid alloy, 2 is solid-state Cu layer.Further insulation will make liquid phase region generation isothermal solidification under the connection temperature after liquid phase region reaches maximum width, at this moment solid-liquid interface is moved in the other direction, after finishing, isothermal solidification also can carry out the solid phase homogenization of composition, the state of this moment is shown in C figure among Fig. 1, and wherein 3 be that responding layer, 4 is ceramic for solid-state Cu layer, 6 for the Cu-Ti solid solution layer of isothermal solidification, 5.Above-mentioned first time partial transient liquid phase connect finish after, carry out second time partial transient liquid phase and connect, promptly further be warming up to second and connect temperature, this temperature is advisable lasting insulation the on this temperature with 1373K between the fusing point of the fusing point of Cu and Ni.At this moment the solid-state Cu layer 5 in the first time, partial transient liquid phase connected and the Cu-Ti solid solution layer 4 of isothermal solidification just are melted, and the rich Cu of the liquid alloy of this moment only contains a spot of Ti.With previously described similar process, at this moment liquid phase region also can broadening and is reached maximum width, isothermal solidification and solid phase homogenization of composition then, thus increase substantially the fusing point of bonding land material.But the Cu-Ni phasor is the uniform grain phasor, is not incubated in this temperature and can forms frangible compounds; Simultaneously, owing to active Ti atom major part was consumed by the surface reaction with pottery in the partial transient liquid phase connection in the first time, thereby the possibility of formation Ti-Ni frangible compounds is also very little in the second time, partial transient liquid phase connected.In addition, responding layer can obviously not thicken yet in the second time, partial transient liquid phase connected, thereby can not reduce the joint strength of joint increasing substantially the stable on heating while of joint.Shown in the d among Fig. 2, e, f figure, wherein 7 is that liquid Cu layer (containing a small amount of Ti), 8 is that Cu-Ni liquid alloy, 9 is Cu-Ni sosoloid to each state in the partial transient liquid phase connection procedure respectively for the second time.In addition, need to prove that the Ni in the present embodiment can substitute with other metallic substance, these metallic substance are to become uniform grain relation and the fusing point metallic substance higher than Cu fusing point with Cu, as Au, Pd, Pt and their alloy.
Compared with prior art, the present invention is owing to adopted unique multilayer intermediate materials And double partial transient liquid phase bonding technology, no crisp in the multilayer intermediate materials after connecting The property compound produce thereby bonding strength height, jointing heat resistance height.

Claims (8)

1. pottery and metal part instant liquid phase connecting method, placement of multiple layers intermediate materials between pottery and metal earlier, the connection of heating again is characterized in that:
(1) comprise one deck Ti, one deck Cu, one deck X material in the said multilayer intermediate materials at least, said X material is to become uniform grain phasor relation and the fusing point metallic substance higher than Cu fusing point with Cu, and above-mentioned trilaminate material is adjacent successively;
(2) after being placed on above-mentioned multilayer intermediate materials between pottery and the metal, carry out the partial transient liquid phase connection first time, promptly heat to first connect temperature and on this temperature isothermal, said first connects temperature between the fusing point of the eutectic temperature of Ti and Cu and Cu;
(3) above-mentioned first time partial transient liquid phase connect finish after, carry out second time partial transient liquid phase and connect, promptly further be warming up to second connect temperature and on this temperature isothermal, the said second connection temperature is between the fusing point of the fusing point of Cu and X material.
2. pottery according to claim 1 and metal part instant liquid phase connecting method is characterized in that: said multilayer intermediate materials is five layer materials, and their adjacent order are followed successively by Ti, Cu, X, Cu, Ti.
3. pottery according to claim 1 and 2 and metal part instant liquid phase connecting method is characterized in that: said X material is Ni.
4. pottery according to claim 3 and metal part instant liquid phase connecting method is characterized in that: the said first connection temperature is 1323K.
5. pottery according to claim 3 and metal part instant liquid phase connecting method is characterized in that: the said second connection temperature is 1373K.
6. pottery according to claim 1 and 2 and metal part instant liquid phase connecting method is characterized in that: said X material is Au.
7. pottery according to claim 1 and 2 and metal part instant liquid phase connecting method is characterized in that: said X material is Pd.
8. pottery according to claim 1 and 2 and metal part instant liquid phase connecting method is characterized in that: said X material is Pt.
CN97106923A 1997-04-10 1997-04-10 Ceramic and metal part instant liquid phase connecting method Expired - Fee Related CN1059418C (en)

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Cited By (10)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN100361935C (en) * 2006-05-15 2008-01-16 西北工业大学 Connection method for carbon/carbon, carbon/silicon carbonate composite material and thermal-resisting alloy
CN101550020B (en) * 2009-05-13 2011-07-20 西北工业大学 Method for connecting carbon/carbon composite material with nickel-based high-temperature alloy
CN101580404B (en) * 2008-05-12 2011-08-03 铜陵市红星水暖有限责任公司 Manufacturing method of copper-plated porcelain
CN102336578A (en) * 2010-07-22 2012-02-01 鸿富锦精密工业(深圳)有限公司 Connection method for tin bronze and alumina ceramic and prepared connecting piece
CN103183520A (en) * 2013-03-01 2013-07-03 西北工业大学 Partial transient liquid phase bonding method for carbon/carbon composite material and nickel-base superalloy
CN103752973A (en) * 2014-02-14 2014-04-30 常州工学院 Middle layer assembly and method for connecting Si3N4 ceramic
CN108484200A (en) * 2018-06-26 2018-09-04 烟台柳鑫新材料科技有限公司 A kind of ceramic copper-clad plate and preparation method thereof
CN110524082A (en) * 2019-08-20 2019-12-03 西安交通大学 Using Fe as the method for carbon fiber in active element quick humidification ceramic matric composite
CN112338346A (en) * 2020-10-29 2021-02-09 河海大学常州校区 Method for connecting sapphire by adopting transient liquid phase diffusion welding
CN113182514A (en) * 2021-03-31 2021-07-30 北京科技大学 TiAl alloy ceramic welding part and integral forming preparation method thereof

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JPH0234908B2 (en) * 1985-08-06 1990-08-07 Sumitomo Denki Kogyo Kk HISANKABUTSUSERAMITSUKUSUTOKINZOKUNOSETSUGOTAI
JPS62171970A (en) * 1986-01-27 1987-07-28 株式会社東芝 Member for joining ceramic to metal
FR2616696B1 (en) * 1987-06-17 1993-05-07 Innovatique Sa METHOD OF BRAZING OVEN UNDER A RAREFIED OR CONTROLLED TWO-PIECE ATMOSPHERE
DE4320910C1 (en) * 1993-06-18 1994-09-08 Siemens Ag Method of producing a gastight soldered connection and use of this method in the production of components having a vacuum-tight housing
JP4092871B2 (en) * 2000-12-04 2008-05-28 住友金属工業株式会社 Composition for forming a lubricating coating suitable for lubricating treatment of threaded joints

Cited By (15)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN100361935C (en) * 2006-05-15 2008-01-16 西北工业大学 Connection method for carbon/carbon, carbon/silicon carbonate composite material and thermal-resisting alloy
CN101580404B (en) * 2008-05-12 2011-08-03 铜陵市红星水暖有限责任公司 Manufacturing method of copper-plated porcelain
CN101550020B (en) * 2009-05-13 2011-07-20 西北工业大学 Method for connecting carbon/carbon composite material with nickel-based high-temperature alloy
CN102336578B (en) * 2010-07-22 2014-10-15 鸿富锦精密工业(深圳)有限公司 Connection method for tin bronze and alumina ceramic and prepared connecting piece
CN102336578A (en) * 2010-07-22 2012-02-01 鸿富锦精密工业(深圳)有限公司 Connection method for tin bronze and alumina ceramic and prepared connecting piece
CN103183520A (en) * 2013-03-01 2013-07-03 西北工业大学 Partial transient liquid phase bonding method for carbon/carbon composite material and nickel-base superalloy
CN103183520B (en) * 2013-03-01 2014-04-02 西北工业大学 Partial transient liquid phase bonding method for carbon/carbon composite material and nickel-base superalloy
CN103752973A (en) * 2014-02-14 2014-04-30 常州工学院 Middle layer assembly and method for connecting Si3N4 ceramic
CN103752973B (en) * 2014-02-14 2015-11-04 常州工学院 A kind of connection Si 3n 4the mid-tier component of pottery and method
CN108484200A (en) * 2018-06-26 2018-09-04 烟台柳鑫新材料科技有限公司 A kind of ceramic copper-clad plate and preparation method thereof
CN108484200B (en) * 2018-06-26 2021-08-31 烟台柳鑫新材料科技有限公司 Ceramic copper-clad plate and preparation method thereof
CN110524082A (en) * 2019-08-20 2019-12-03 西安交通大学 Using Fe as the method for carbon fiber in active element quick humidification ceramic matric composite
CN110524082B (en) * 2019-08-20 2021-04-20 西安交通大学 Method for quickly wetting carbon fibers in ceramic matrix composite by taking Fe as active element
CN112338346A (en) * 2020-10-29 2021-02-09 河海大学常州校区 Method for connecting sapphire by adopting transient liquid phase diffusion welding
CN113182514A (en) * 2021-03-31 2021-07-30 北京科技大学 TiAl alloy ceramic welding part and integral forming preparation method thereof

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