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GB2114040A - Sealing ceramic to ceramic or to metal - Google Patents

Sealing ceramic to ceramic or to metal Download PDF

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Publication number
GB2114040A
GB2114040A GB08203497A GB8203497A GB2114040A GB 2114040 A GB2114040 A GB 2114040A GB 08203497 A GB08203497 A GB 08203497A GB 8203497 A GB8203497 A GB 8203497A GB 2114040 A GB2114040 A GB 2114040A
Authority
GB
United Kingdom
Prior art keywords
seal
tin
ceramic
articles
article
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
Application number
GB08203497A
Other versions
GB2114040B (en
Inventor
Willia Dunn Hepburn
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Ferranti International PLC
Original Assignee
Ferranti PLC
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by Ferranti PLC filed Critical Ferranti PLC
Priority to GB08203497A priority Critical patent/GB2114040B/en
Publication of GB2114040A publication Critical patent/GB2114040A/en
Application granted granted Critical
Publication of GB2114040B publication Critical patent/GB2114040B/en
Expired legal-status Critical Current

Links

Classifications

    • CCHEMISTRY; METALLURGY
    • C04CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04BLIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B37/00Joining burned ceramic articles with other burned ceramic articles or other articles by heating
    • C04B37/02Joining burned ceramic articles with other burned ceramic articles or other articles by heating with metallic articles
    • C04B37/023Joining burned ceramic articles with other burned ceramic articles or other articles by heating with metallic articles characterised by the interlayer used
    • C04B37/026Joining burned ceramic articles with other burned ceramic articles or other articles by heating with metallic articles characterised by the interlayer used consisting of metals or metal salts
    • CCHEMISTRY; METALLURGY
    • C03GLASS; MINERAL OR SLAG WOOL
    • C03CCHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
    • C03C27/00Joining pieces of glass to pieces of other inorganic material; Joining glass to glass other than by fusing
    • C03C27/04Joining glass to metal by means of an interlayer
    • C03C27/042Joining glass to metal by means of an interlayer consisting of a combination of materials selected from glass, glass-ceramic or ceramic material with metals, metal oxides or metal salts
    • C03C27/046Joining glass to metal by means of an interlayer consisting of a combination of materials selected from glass, glass-ceramic or ceramic material with metals, metal oxides or metal salts of metals, metal oxides or metal salts only
    • CCHEMISTRY; METALLURGY
    • C03GLASS; MINERAL OR SLAG WOOL
    • C03CCHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
    • C03C27/00Joining pieces of glass to pieces of other inorganic material; Joining glass to glass other than by fusing
    • C03C27/06Joining glass to glass by processes other than fusing
    • C03C27/08Joining glass to glass by processes other than fusing with the aid of intervening metal
    • CCHEMISTRY; METALLURGY
    • C04CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04BLIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B37/00Joining burned ceramic articles with other burned ceramic articles or other articles by heating
    • C04B37/003Joining burned ceramic articles with other burned ceramic articles or other articles by heating by means of an interlayer consisting of a combination of materials selected from glass, or ceramic material with metals, metal oxides or metal salts
    • C04B37/006Joining burned ceramic articles with other burned ceramic articles or other articles by heating by means of an interlayer consisting of a combination of materials selected from glass, or ceramic material with metals, metal oxides or metal salts consisting of metals or metal salts
    • CCHEMISTRY; METALLURGY
    • C04CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04BLIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2237/00Aspects relating to ceramic laminates or to joining of ceramic articles with other articles by heating
    • C04B2237/02Aspects relating to interlayers, e.g. used to join ceramic articles with other articles by heating
    • C04B2237/12Metallic interlayers
    • CCHEMISTRY; METALLURGY
    • C04CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04BLIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2237/00Aspects relating to ceramic laminates or to joining of ceramic articles with other articles by heating
    • C04B2237/02Aspects relating to interlayers, e.g. used to join ceramic articles with other articles by heating
    • C04B2237/12Metallic interlayers
    • C04B2237/126Metallic interlayers wherein the active component for bonding is not the largest fraction of the interlayer
    • C04B2237/127The active component for bonding being a refractory metal
    • CCHEMISTRY; METALLURGY
    • C04CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04BLIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2237/00Aspects relating to ceramic laminates or to joining of ceramic articles with other articles by heating
    • C04B2237/30Composition of layers of ceramic laminates or of ceramic or metallic articles to be joined by heating, e.g. Si substrates
    • C04B2237/32Ceramic
    • CCHEMISTRY; METALLURGY
    • C04CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04BLIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2237/00Aspects relating to ceramic laminates or to joining of ceramic articles with other articles by heating
    • C04B2237/30Composition of layers of ceramic laminates or of ceramic or metallic articles to be joined by heating, e.g. Si substrates
    • C04B2237/40Metallic
    • C04B2237/405Iron metal group, e.g. Co or Ni

Landscapes

  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Ceramic Engineering (AREA)
  • Materials Engineering (AREA)
  • Organic Chemistry (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Geochemistry & Mineralogy (AREA)
  • Structural Engineering (AREA)
  • Joining Of Glass To Other Materials (AREA)
  • Gasket Seals (AREA)

Abstract

A satisfactory seal between two ceramic articles, or between a ceramic article and a metal article, the articles being of materials each having a low coefficient of linear expansion less than 2 x 10<-6> per degree Kelvin, at 20 DEG C, the seal being provided by forming layers of an alloy of tin with titanium or zirconium adjacent to the article surfaces, and with unalloyed tin between the alloy layers. A ceramic article may be of a glass ceramic, or of fused silica; and a metal article may be of a suitable nickel-iron alloy.

Description

SPECIFICATION Seals between ceramic articles or between ceramic articles and metal articles This invention relates to seals between two ceramic articles, or between a ceramic article and a metal article, and in particular to such seals associated with articles of materials having low coefficients of linear expansion, each less than 2 x 10-6 per degree Kelvin at 200C.
The articles may be of a glass ceramic, or of fused silica, or of a nickel-iron alloy.
Titanium or zirconium reacts with the surfaces of such articles, but titanium or zirconium alone is unsuitable to comprise such a seal, being too reactive for this purpose, being capable of damaging the articles. However, an alloy containing titanium or zirconium can be provided, and is suitable for this purpose.
It is known to provide seals between such articles by providing an assembly including titanium or zirconium to form a liquid alloy with a larger quantity of an alloying material, when the alloying material is melted. The liquid alloy including the titanium or zirconium reacts with the article surfaces, and wets these surfaces, the alloy layers adhering to the article surfaces when solidified, and substantially only sufficient titanium or zirconium is provided for this purpose. Known alloying materials include the copper-silver eutectic, and pure silver. The liquid alloy including the titanium or zirconium is formed, at least, at the melting point of the alloying material.
For convenience, in this specification and the accompanying claims, the term alloy is employed to include a reference to a solution of the material referred to above as the alloying material and either the titanium or zirconium.
Also for convenience, in this specification and the accompanying claims, such a seal containing an alloy of titanium or zirconium is referred to as a seal of the type referred to.
Usually, pure titanium or zirconium is not provided initially on the article surfaces, but instead a compound, such as the hydride thereof, is provided, and when the compound decomposes the element thereby provided is capable of forming the required liquid alloy. The liquid alloy may be formed immediately, or at a higher temperature. Thus, it is required that the alloying material is stable, at least, at the temperature at which the compound decomposes. Usually, the whole of the seal providing operation is performed in a substantial vacuum.
Further, it is required that the temperature at which the compound decomposes, and the time the materials are held at this, or at a higher temperature, are sufficient to cause any surface oxide to be absorbed.
It is essential that the articles are not damaged by being held at the temperature referred to in the preceding paragraph. Thus, this temperature may be required to be lower than that associated with the use of the copper-silver eutectic, or of pure silver, in forming a seal of the type referred to.
In addition, the higher the solidification temperature of the composite seal the greater the effect of any differences between the coefficients of expansion of the different materials of the composite body comprising the articles, and the constituent parts of the formed composite seal of the type referred to between the articles.
In contrast, the solidification temperature may not be required to be so low that the composite body, comprising the articles with the formed composite seal of the type referred to therebetween, cannot be effectively outgassed, if such outgassing is desirable.
Other desirable properties of the alloying material are that it is soft when solidified, to enable it to accommodate any differential thermal expansion within the composite body; and it is required to have a low vapour pressure at the temperature at which the assembly is held.
It is an object of the present invention to provide a novel and advantageous alloying material, for forming an alloy with titanium or zirconium, in order to provide a seal of the type referred to between two ceramic articles, or between a ceramic article and a metal article, such that an advantageous combination of the desirable criteria referred to above for such an alloying material is obtained.
According to the present invention a seal of the type referred to, between two ceramic articles, or between a ceramic article and a metal article, the articles being of materials having low coefficients of linear expansion, each less than 2 x 10-6 per degree Kelvin at 200 C, includes an alloying material comprising tin, there being alloy layers of tin with titanium or zirconium adjacent to the article surfaces, with soft tin, containing little or no titanium or zirconium, between the alloy layers.
Such a seal is satisfactory, and the composite body so provided readily can be baked in vacuo at 2000C for several hours, in order to outgas the composite body.
According to another aspect, the present invention comprises a method of providing a seal of the type referred to, the method comprising coating the articles with layers containing titanium or zirconium, providing tin between the titanium or zirconium containing layers, and heating the assembly to cause the tin to alloy with the titanium, or zirconium, the alloy to wet the article surfaces, and there is provided the required seal between the articles when the composite body, thereby obtained, is cooled.
Usually the titanium or zirconium layers are provided by coating the articles with a suspension of a titanium or zirconium compound, such as the hydride thereof, in a suitable binder, and allowing the suspension to dry. Subsequently, the binder and the hydrogen are removed by the heating, the titanium or zirconium, and the tin, forming the liquid alloy.
An oxide layer readily forms on tin, and such an oxide layer is deleterious for the required seal.
Consequently, the tin is coated with a thin layer of silver, or is washed in an acid to remove the oxide layer, before the tin is incorporated into the seal.
The present invention will now be described by way of example with reference to the following Examples.
EXAMPLE 1 An article of a glass ceramic, having a low coefficient of linear expansion of 0.03 x 10-6 per degree Kelvin at 200 C, is coated in any convenient way with a suspension of titanium hydride in a nitrocellulose binder, and is allowed to dry.
Another article of the glass ceramic is similarly coated. A layer of tin foil, or tin wire, coated with a thin layer of silver, and approximately, 10 times the volume of the provided titanium, is p!aced between the titanium hydride layers. The whole is then placed in a vacuum furnace, with an atmosphere of less than 1 x 1 0-6 newtons per square metre, and a small load is applied to the assembly. The furnace is heated at a temperature of 6000C for 1 5 minutes, and is allowed to cool to 2000 C, before being gas cooled to 1 000C, and fast cooled from 1000C to room temperature.
During the heating process step, the binder and the hydrogen are removed from the titanium hydride layers, and the titanium alioys with the tin, adjacent to the article surfaces, the element immediately forming the liquid alloy. Any surface impurity on the silver is absorbed in the melt; and the titanium-tin alloy wets the surfaces of the articles. Soft tin, containing little or no titanium, remains between the alloy layers. Upon cooling, a satisfactory seal is provided between the two articles. The composite body is then outgassed by being heated at a temperature of 2000C for 3 hours in vacuo.
EXAMPLE 2 Example 1 is repeated, except that one of the glass ceramic articles is replaced by an article of a nickel-iron alloy, having a composition of 36% by weight of nickel, 64% by weight of iron, together with incidental impurities. This alloy has a low coefficient of linear expansion of less than 1 x 10-6 per degree Kelvin at 200C. The titaniumtin alloy wets the surface of the nickel-iron alloy article. A satisfactory seal is provided between the two articles.
The required titanium containing layers on the articles may be provided on the articles in any convenient way.
One, or both, of the articles may be of fused silica, having a coefficient of linear expansion of 0.4 x 10-6 per degree Kelvin at 200C.
Zirconium may replace the titanium.
The tin is coated with silver to prevent a deleterious oxide layer being formed on the tin.
Alternatively, such an oxide layer is removed by washing the tin in an acid immediately before the tin is incorporated into the seal.

Claims (14)

1. A seal of the type referred to, between two ceramic articles, or between a ceramic article and a metal article, the articles being of materials having low coefficients of linear expansion, each less than 2 x 10-6 per degree Kelvin at 200C. the seal including an alloying material comprising tin, there being alloy layers of tin with titanium or zirconium adjacent to the article surfaces, with soft tin, containing little or no titanium or zirconium, between the alloy layers.
2. A seal as claimed in claim 1 in which a ceramic article is of a glass ceramic, or of fused silica.
3. A seal as claimed in claim 1 or claim 2 in which a metal article is of a nickel-iron alloy.
4. A method of providing a seal of the type referred to, and of a form claimed in any one of the preceding claims, the method comprising coating the articles with layers containing titanium or zirconium, providing tin between the titanium or zirconium containing layers, and heating the assembly to cause the tin to alloy with the titanium or zirconium, the alloy to wet the article surfaces, and there is provided the required seal between the articles when the composite body, thereby obtained, is cooled.
5. A method as claimed in claim 4 in which initially the articles are coated with a suspension of a titanium or zirconium compound in a suitable binder, and allowing the suspension to dry, and the compound is caused to decompose, the element forming the alloy with tin.
6. A method as claimed in claim 5 in which the compound is the hydride thereof.
7. A method as claimed in any one of claims 4 to 6 in which the seal is formed in a substantial vacuum.
8. A method as claimed in any one of the claims 4 to 7 in which the assembly is heated at a temperature of 6000C for 1 5 minutes.
9. A method as claimed in any one of claims 4 to 8 in which the tin is coated with a layer of silver before being incorporated in the seal.
10. A method as claimed in any one of claims 4 to 8 in which the tin is washed in an acid to remove any oxide layer on the tin, before the tin is incorporated in the seal.
11. A seal between two ceramic articles substantially as described herein with reference to Example 1.
12. A seal between a ceramic article and a metal article substantially as described herein with reference to Example 2.
13. A method of providing a seal between two ceramic articles substantially as described herein with reference to Example 1.
14. A method of providing a seal between a ceramic article and a metal article substantially as described herein with reference to Example 2.
GB08203497A 1982-02-06 1982-02-06 Sealing ceramic to ceramic or to metal Expired GB2114040B (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
GB08203497A GB2114040B (en) 1982-02-06 1982-02-06 Sealing ceramic to ceramic or to metal

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
GB08203497A GB2114040B (en) 1982-02-06 1982-02-06 Sealing ceramic to ceramic or to metal

Publications (2)

Publication Number Publication Date
GB2114040A true GB2114040A (en) 1983-08-17
GB2114040B GB2114040B (en) 1985-08-07

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GB08203497A Expired GB2114040B (en) 1982-02-06 1982-02-06 Sealing ceramic to ceramic or to metal

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Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS62192295A (en) * 1986-02-19 1987-08-22 デグツサ・アクチエンゲゼルシヤフト Soft solder alloy for mutual bonding of ceramic part or bonding with part consisting of metal
FR2619562A1 (en) * 1987-08-18 1989-02-24 Ferranti Int Signal METHOD FOR SEALING TWO CERAMIC OR CERAMIC AND METALLIC ARTICLES
EP1065180A3 (en) * 1999-06-30 2002-08-07 Bormioli Rocco &amp; Figlio S.p.A. A method for treating a glass container for the adhesion of a thermoplastic polymer

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS62192295A (en) * 1986-02-19 1987-08-22 デグツサ・アクチエンゲゼルシヤフト Soft solder alloy for mutual bonding of ceramic part or bonding with part consisting of metal
EP0235546A3 (en) * 1986-02-19 1988-09-14 Degussa Aktiengesellschaft Use of a solder alloy for bounding ceramic parts
FR2619562A1 (en) * 1987-08-18 1989-02-24 Ferranti Int Signal METHOD FOR SEALING TWO CERAMIC OR CERAMIC AND METALLIC ARTICLES
EP1065180A3 (en) * 1999-06-30 2002-08-07 Bormioli Rocco &amp; Figlio S.p.A. A method for treating a glass container for the adhesion of a thermoplastic polymer

Also Published As

Publication number Publication date
GB2114040B (en) 1985-08-07

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Legal Events

Date Code Title Description
732 Registration of transactions, instruments or events in the register (sect. 32/1977)
PCNP Patent ceased through non-payment of renewal fee

Effective date: 19940206