JPS5950085A - Ceramic,cermet or metal composite body - Google Patents

Abstract

(57) [Summary] This bulletin contains application data before electronic filing, so abstract data is not recorded.

Description

DETAILED DESCRIPTION OF THE INVENTION The present invention relates to the use of nitrides, oxides, arsenides, borides, phosphides, tellurides, titanates, silicides, carbides, etc. of metals or metalloids as substrates or basic elements. or compression molded products thereof. These include tin, lead, indium, or their alloys as a coating, film layer, or intermediate layer forming body. The substrate can be used in admixture with the former and bonded to a variety of other substrates, such as coatings, in a carbon monoxide atmosphere.

In the previous application (Japanese Patent Application No. Sho JA-f♂711-/), we have proposed an adhesive coating on the substrate described in the said application, consisting of a mixture of tin, lead, indium or their alloys and carbides or cartenyl formers. Various substrate and alloy combinations have been disclosed that have been found to be particularly useful in producing. Our method was developed while exploiting and investigating various aspects of the invention of the above-mentioned application, and was applied to substrates that have traditionally been known to be very difficult to bond to different materials and substrates. It is based on the following discoveries, which are commonly known to be particularly useful in applied applications.

As disclosed in the previous application, tin, lead, indium or alloys thereof and carbides and cal? The combination with nil formers has yielded previously unknown and completely unexpected results when they are properly mixed and then bonded to the substrate in a carbon monoxide atmosphere. This discovery opens the door to the possibility of bonding metals to substrates that have hitherto been the most difficult to bond. By carrying out the above method on a variety of substrates on which it was not previously possible to easily form good bonds that are virtually void-free and have great adhesion and an unmeasurable increase in durability, excellent yields can be obtained. was found to be formed. This is possible with the substrate, and the tin, lead, and indium alloys on the substrate can further be combined with other substrates or metals in various ways, making it suitable for many applications such as in the electronics industry for purposes such as heat dissipation, current conduction, etc. Provides a novel, previously unknown substrate that is useful and has virtually no pores (with no contamination between these devices).
[by microscopic examination] forms a bond. Other devices, such as piezoelectrics, such as barium titanate, and laser beam vibrators, such as those based on aluminum gallium arsenide, use a substrate of an electrically conductive material or a thermally conductive but electrically insulating substrate, such as beryllium oxide. They can be easily bonded and fabricated by easy means for the desired application at a fraction of the cost required to successfully bond them.

In view of the foregoing, the disclosure in the earlier application is hereby incorporated by reference, but need not be repeated. Generally, the same atmospheric conditions
Applied together with the same temperature range, these are established for the substrate at the required conditions. Similarly, the residence time provided by the reducing atmosphere of carbon monoxide for suitable bonding is established as necessary, but is generally within the ranges described in the earlier application. The particular temperatures and residence times used are optimal for the particular substrate, and the mere predetermined establishment of the necessary conditions is not sufficient when the practice of the invention is carried out in the industrial installation to which it is sought to be applied. It is carried out even in the case of

Although carbon monoxide is an excellent reducing agent, it can be mixed with other compatible reducing agents. Similarly, −
It can also be diluted with other gases compatible with carbon monoxide that do not affect the reaction mechanism or reducibility of the carbon oxide. After a reducing atmosphere has been established and a suitable bond has been formed, e.g. by substantially porosity free, sufficient wetting and intimate adhesion as described above, the reducing atmosphere is suitably removed and other inert The atmosphere is replaced and the formed composite is cooled. The initial heating is performed in an inert atmosphere by the same means as the subsequent cooling, although preheating of the substrate and material can also be done in a reducing gas such as hydrogen. However, the most effective means, and especially the best, are to combine substrates, layers, etc. with tin, lead, indium and/or alloys thereof and carbides or cals with nil formers in the presence of carbon monoxide. , it appears to interact synergistically with the substrate, tin etc. and/or carbide or carbide formers.

Carbide or CalΔ? Although the nil formers are used in a variety of forms, they are most advantageously used in colloidal to fine particulate form up to 1.5 inches. These microparticles are dispersed in metals such as brocades under conditions assisted by, for example, forging and/or thermoforming or similar methods; likewise, the dispersoids of one in their extremely fine form are Suitably mixed in vehicles such as rosin oil or various freons that evaporate more easily than dispersions. The dispersion is then coated onto the substrate or applied to it by screening or printing, depending on the thickness of the substrate. Thereafter, the material is inserted under appropriate conditions in a reducing atmosphere as described above. In this way, different patterns (master turns) are formed on the substrate, eg conductive paths and the like forming circuits and the like.

Some of the example substrates given in the earlier application combine equally well with previously undisclosed substrates in this application. Accordingly, the various substrates as disclosed and claimed in this application can be combined in distinct and novel combinations useful for purposes as disclosed in and. Thus, lanthanum boride, LaB5, useful as a highly effective electron source used in electron microscopy, is significantly bonded to electrical devices when first coated with tin-vanadium. The substrate is better bonded or coated with the composition at about 1000 DEG C. in a carbon monoxide atmosphere with about 1/2 to 2 parts vanadium, balance tin.

The homogeneous mixing of these powders, their easy dispersibility in finely divided form, and their easy application to substrates lend their combination to the purpose of application to a variety of other substrates as mentioned above.

For example, beryllium oxide is easily combined with a substrate having tin as an intermediate layer to the other of the two layers such as lanthanum boride or carbide or carbunyl formers such as gallium arsenide or carboxylic acid as an intermediate layer in a mixture with vanadium. Other equally easy methods of forming films, layers, etc. on gallium arsenide and/or bonding gallium arsenide or gallium alponium arsenide with various substrates include tin and carbide or gallium arsenide. was discovered when using combinations with nil formers. Some of these are, for example, Cr-3n.

V-Sn%Mo-! 3n, W-Sn, A-8n,
7'j-5n.

Ta-Sn, Mn-sn, Nl-Sn
and co-5n.

The above combination is about /j~.2 carbide or carbnyl formers, the remainder being tin, with a preferred range of about 10% when combined with gallium arsenide or aluminum gallium arsenide.
~73% carbide or calyt"nyl formers. Similar to the above, the 5n-V combination in particular is readily used to form adhesive coatings on silicon, silicon nitride or silicon oxide, thus A combination of three different layers is formed (and these, in turn, are bonded to other aforementioned substrates).

In addition to the carbides or car&nyl formers mentioned above, mixtures thereof are likewise useful. For example, Cr, V, MO and 2
Addition of 10 Ti of nickel to a cobalt mixture of 10 fl of CO to 0% Sn produces similarly pronounced adhesion to substrates such as tungsten carbide in combination with substrates as described herein.

Additionally, a light emitting diode (light emlttln)
Phosphate, which is used at high frequencies such as for gdlode, is a tin, indium, and lead alloy with carbide or carbnyl formers, 7% V and 7% N1 monoxide. The coating is carried out at 00° C. in a carbon atmosphere. A highly adhesive bond was formed.

In a similar manner, vanadium is used in the same ratio as above to tin, etc., and nickel, zirconium ortho-
The silicates themselves or in mixtures with magnesium silicate and also with aluminum silicate are well coated with remarkable adhesion properties in carbon monoxide under the same conditions.

In the same manner as above, various titanates such as barium titanate; silicon nitride-oxides such as boron oxide; arsenides; silicides: tellurides and the like are tin-containing disasters or carbonyl formers such as carbon, such as graphite. bonded to a substrate such as a metal such as stainless steel; an oxide such as beryllium oxide;

According to Mizuyoshi, the composite has excellent mechanical and/or electrical and/or thermal conductive properties.

There is no need to use new metals, no scalpel ring is required, and an extremely solid and strong bond is formed. Temperatures are regulated in various substrates such that high temperature requirements are encountered in special cases such as when bonding to steel in a slump where these temperature limits have hitherto not been achievable. Ru.

In general, the present invention covers all ceramic type materials, including mixtures of ceramics and metals known as cermets, and oxides, nitrides, arsenides, and metals or metalloids.
It has been discovered that the same compounds can be applied including titanates, tellurides, silicides, borides, phosphides and carbides. When in powder form they are, for example, hydrostatically compressed into a very solid mass under very high pressure (when the powder is subjected to high static pressures, as is well known in the art), It has been discovered that it is particularly useful as a substrate material.

These base materials can also be distributed as powders in the form of forming fine dispersions with either compatible or incompatible but strong mutually or other similar forms, and then completely densified with remarkable properties. is compressed statically into a shape. These may thus be ceramics or cermets (ceramic, metal lamination) which are subsequently bonded to other metals, ceramics, cermets and the like by means of pots and the like and carbide or carbonyl formations. These substrates have strong bonds with each other or with other metals and cermets when subsequently bonded with tin, lead, indium or alloys thereof mixed with carbides or carbonyl formers as described herein. and used for the various purposes mentioned above.

In a previous application, we also describe the use of carbides or carbides to form adhesive composites with carbon such as graphite, diamond, etc. and others that are very difficult to bond to substrates.
Various tin, lead, indium compositions with t''nyl formers are disclosed. In addition, these substrates have tin, lead, indium compositions thereon as disclosed in the earlier application. When deposited and processed, these have the hitherto undiscovered ability to bond other metals that are difficult to bond to substrates, such as steel when bonded in this way to tin alloys. forms bronze compositions with enhanced temperature properties, and composites such as graphite, tin, and copper, when the last λ is converted to bronze, have useful temperature limits far in excess of those achievable with tin alone. form a graphite-bronze composite having

We further demonstrate that these and other substrates are Nl-Cu-N
It has been discovered that additional beneficial properties are obtained and temperature limits are further improved when used with metals in the form of a sandwich such as I.

Furthermore, we use boron nitride, titanium diboride (T482
) or a mixture thereof is used as a substrate,
They have also discovered that tin, lead, indium and their alloys can be mixed with carbide or carbonyl formers to form adhesive composites with remarkable properties. These complexes then serve a purpose and resistor as described above.
It is also used for other purposes such as resistors in atmospheres where the absence of contamination from ance elements is required. That type of contamination is highly undesirable, for example, in the manufacture of semiconductors or in the manufacture of silicon metals, i.e., single crystal growth or vitreous silicon growth where silicon is used, for example, in solar cells.

Among the many composites mentioned above, the aforementioned methods of processing composites can be equally applied to the deposition of mixtures, the deposition of compacted powder preforms or the deposition of metals into powder mixtures or preforms. Both can be made on a substrate or metal to form a composite.

Since the earlier application describes various process details in addition to carbide or carbonyl formers, the earlier application is hereby incorporated by reference.
It serves as a reference and forms part of this application.

Next, examples of the present invention will be shown, but the present invention is not limited thereto.

Example / When boron nitride is used as the substrate, a Sn-Cr composition (Sn 90 wt.
Cr/Owt%, /00% Co atmosphere)
An adhesive coating of is formed on the surface of the boron nitride. This composition does not reduce wetting. Similar to the graphite substrate, the copper layer on its tin coating forms bronze. In addition to boron nitride, titanium diboride exhibits excellent structural properties such as strength when coated with the aforementioned compositions (or when a sandwich with copper is formed in the coating). Mixtures of boron nitride and Tc B 2 are likewise combined with tin and carbide or cartenyl-forming elements or mixtures thereof, such as the glue 0'1oan-101rCr compositions described above. Boron nitride is an excellent abrasive and the boron nitride-TtB2 mixture is an excellent resistor.

Examples λ Carbides or carbides with tin, lead or indium alloys, e.g. Cr, TL, Hf, Zr, C
o , FbN l s Mn , Re , Ru1Rh
< Os % l r, vs Nb-”as W, M
O or mixtures thereof are optional such as boron nitride or titanium diboride substrates, or these substrates are mixtures of each other, such as /:l mixtures.

To these substrate compositions other metals are bonded as adhesive composites (as for the substrates described above), for example Cu and N1, such as Monel metal type in volatile proportions or a thickness of 7.
~10mil Ni and 2~! Mil~0,/inch Cu
A Nl -Cu -Nl vnduinote with is placed, for example, on a brocade. / mil Ni, j mil Cu, /
Mill Ni works particularly well to form the above composites in 70% 5N-10 Ti Cr compact compositions on graphite. Various other sandwich overlays are used, such as Nl, Cu, Mo.

Procedural amendment (formality) 1. Indication of the case 1939 patent application No. 170g2
．． No. 1, No. 2 Invention (D title: Ceramic, cermet or metal composite 3, Relationship with the person making the amendment case: Applicant 4, Agent)

Claims (1)

[Scope of Claims] (1) Consisting of a metal or metalloid nitride, oxide, arsenide, titanate, silicide, oxide, telluride, phosphide or carbide, or a compression molded product thereof Composites consisting of tin, lead, indium, tin alloys, lead alloys as components in combination with carbide or carbide formers as an adhesive coating, film or layer on a substrate. The adhesive coating has no wetting property even when heated,
A composite wherein the contact angle between the film or layer and the substrate is zero to negative, and the interface between the coating, film or layer and the substrate is substantially void-free. (2) The carbide former or carbunyl former is chromium,
Titanium, hafnium, zirconium, iron, nickel, manganese, rhenium, ruthenium, rhodium,
The composite according to claim 1, which is osmium, iridium, vanadium, niobium, tantalum, tungsten or molybdenum, or a mixture thereof. (3) The composite according to claim (1), wherein the base structure is gallium arsenide or the phosphide is rieux. (4) The composite according to claim (1), wherein the base structure is aluminum gallium arsenide. (5) The substrate is La day. The composite according to claim 1, which is lanthanum boride represented by: (6) The composite according to claim (1), wherein the substrate is barium titanate, zirconium orthosilicate, magnesium silicate, aluminum silicate, or a mixture of these silicates. (7) Claim No. (1) in which the substrate is silicon nitride
Complexes described in Section. (8) The composite according to claim (1), wherein the substrate is a torment. (9) A patent in which the substrate is a compression molded body of oxides, nitrides, borides, arsenides, tellurides, phosphides, silicides, titanium rv & salts of metals, metalloids or mixtures thereof, or mixtures thereof. A composite according to claim (1). (g) The carbide-forming body or the Cal-Nyl-forming body is 7j~
, two predominant elements are chromium, vanadium, molybdenum, tungsten, iron, titanium, tal/tal, manganese, nickel or cobalt, or a mixture thereof, and the remainder is tin or indium or an alloy thereof. ). Ql) A composite according to claim 1, wherein the iron is a carbide former or a car/nil former with tin in a ratio of about j to 7j. 2) Claim No. 1, wherein the carbide former is chromium.
). (2) The composite according to claim (1), wherein the carbide former is vanadium. The composite according to claim 1, wherein the α◆ carginyl former is nickel mixed with vanadium. (g) Claim No. 1 in which the tin alloy is a tin-lead alloy
). (b) The composite according to claim (1), wherein the alloy is an indium alloy. 0 - The can assembly according to claim αQ, in which indium is mixed with vanadium. A claim further comprising an overlay overlying a coating, film or layer on the substrate of seven substrate materials, wherein the overlay is a metal that is alloyable with the coating, film or layer on the substrate. The complex according to item (1). (to) A composite according to claim 1, wherein the overlay is copper on a tin-chromium arsenide composite. The composite according to claim 1, wherein the top layer is an epsilon compound. 6!9 The composite according to claim 1, wherein the substrate is gallium arsenide, the coating is made of tin and vanadium, and the overlay is chromium oxide. (b) The composite according to claim Q1, wherein the substrate is lanthanum boride and the overlay is ihyperylium acid. (c) A sandwich consisting of beryllia, a tin-vanadium coating, film or layer thereon, and a gallium arsenide or alkalivanadium arsenide overlay. complex. (c) tin, lead, indium, tin as a component in combination with carbide or carbinyl formers as an adhesive coating, film or layer on a substrate consisting of boron nitride or titanium diboride or mixtures thereof; composites consisting of alloys, lead alloys or in-chromium alloys. (c) The carbide former or carbinyl former is chromium, titanium, hafnium, zirconium, cobalt, iron,
Nickel, manganese, rhenium, ruthenium, rhodium, osmium, iridium. The composite according to claim (c), which is panazome, niobium, tantalum, tungsten or molybdenum, or a mixture thereof. (c) The adhesive coating, film or layer is further overlaid with an adhesive layer of copper, nickel, molybdenum or a sandwich layer of these metals.
The complex described in section c). (b) The composite according to claim (c), wherein the adhesive overlay layer is a nickel-copper-nickel composite material. The composite according to claim (c), wherein the substrate is a mixture of boron nitride and titanium diboride. (iv) The composite according to claim (c), wherein the substrate is boron nitride. (7) The composite according to claim (c), wherein the substrate is titanium diboride. A composite as claimed in claim (c) in which tin is combined with chromium as an adhesive coating on a boron nitride substrate. 0. The composite according to claim (c), wherein the substrate is a mixture of boron nitride and titanium diboride in a weight ratio of /v//. The composite according to claim (b), wherein the top layer is on graphite. (b) The carbide-forming body or cartenyl-forming body in the form of a metal is composed of a nyl-forming body and a “tin group” metal such as tin, tin alloy, lead, lead alloy, indium or indium alloy, and is the carbide-forming body or cartenyl-forming body. ~tios, the remainder being said tin group metal, wherein - in a carbon oxide atmosphere, nitrides, oxides, arsenides, titanates, silicides, borides, tellurides of metals or metalloids; , forming a layer on a substrate made of a phosphide or carbide, or a compression molded product thereof, which has a zero or negative contact angle and does not have wettability even after repeated heating cycles. Alloy with properties. (to) The alloy according to claim (b), which is a chromium-tin alloy containing 5 to 13% chromium and the balance being tin. (b) The alloy according to claim (b), which is a molybdenum-tin alloy containing 10% to 10% molybdenum and the remainder being tin. (b) A carbide-forming body on a substrate consisting of a metal or metalloid nitride, oxide, arsenide, titanate, silicide, boride, telluride, phosphide or carbide, or a compression molded body thereof; Process for the preparation of adhesive coatings, films or layers consisting of tin, lead, indium or their respective alloys in combination with cartenil formers, in which granular tin, lead, indium or their respective alloys and carbide formers in the form of finely granular metals are used. or calyt
rnyl former in a suitable vehicle to form a dispersoid for a dispersion provided on the substrate, - the melting point of the mixture in the presence of carbon oxide; reacting the mixture up to and at its melting point;
- cooling the acid mixture in the presence of a carbon oxide atmosphere or a mixture of carbon monoxide and an inert gas, or cooling the mixture in an inert atmosphere of hydrogen or hydrogen and nitrogen; ” A preparation method characterized by a process of recovering it as an alloy. A process according to claim (b), wherein the granules are a colloidal mixture with a particle size range of 330 mesh/inch (3,/-73 square centimeters). (2) The vehicle is a rosin, oil, or freon composition.
The preparation method according to claim 0η, which is applied onto a substrate by painting, spraying or printing.