Transient liquid phase ceramic bonding

• US 5,372,298 A
• Filed: 08/10/1993
• Issued: 12/13/1994
• Est. Priority Date: 01/07/1992
• Status: Expired due to Fees

• Current Assignee: Regents of the University of California (University of California)
• Original Assignee: Regents of the University of California (University of California)
• Inventors: Glaeser, Andreas M.
• Primary Examiner(s): Heinrich, Samuel M.
• Application Number:
  US08/105,049
• Time in Patent Office: 490 Days
• Field of Search: 228/121, 228/122.1, 228/124.1, 228/124.5, 228/124.6, 228/195
• US Class Current: 228/195
• CPC Class Codes: B23K 20/023 Thermo-compression bonding
• CPC Class Codes: B23K 20/16 with interposition of special material to facilitate connection of the parts, e.g. material for absorbing or producing gas
• CPC Class Codes: B23K 35/002 at least one of the workpieces being of light metal
• CPC Class Codes: B23K 35/005 at least one of the workpieces being of a refractory metal
• CPC Class Codes: C04B 2237/062 based on silica or silicates
• CPC Class Codes: C04B 2237/121 based on aluminium
• CPC Class Codes: C04B 2237/122 based on refractory metals
• CPC Class Codes: C04B 2237/123 based on iron group metals, e.g. steel
• CPC Class Codes: C04B 2237/124 based on copper
• CPC Class Codes: C04B 2237/125 based on noble metals, e.g. silver
• CPC Class Codes: C04B 2237/16 Silicon interlayers
• CPC Class Codes: C04B 2237/368 Silicon nitride
• CPC Class Codes: C04B 2237/60 Forming at the joining interface or in the joining layer specific reaction phases or zones, e.g. diffusion of reactive species from the interlayer to the substrate or from a substrate to the joining interface, carbide forming at the joining interface
• CPC Class Codes: C04B 2237/708 of one or more of the interlayers
• CPC Class Codes: C04B 2237/72 Forming laminates or joined articles comprising at least two interlayers directly next to each other
• CPC Class Codes: C04B 2237/76 Forming laminates or joined articles comprising at least one member in the form other than a sheet or disc, e.g. two tubes or a tube and a sheet or disc
• CPC Class Codes: C04B 2237/86 Joining of two substrates at their largest surfaces, one surface being complete joined and covered, the other surface not, e.g. a small plate joined at it's largest surface on top of a larger plate
• CPC Class Codes: C04B 37/003 by means of an interlayer consisting of a combination of materials selected from glass, or ceramic material with metals, metal oxides or metal salts
• CPC Class Codes: C04B 37/006 consisting of metals or metal salts
• CPC Class Codes: C04B 37/026 consisting of metals or metal salts
• CPC Class Codes: F28F 21/04 : of ceramic; of concrete; of natural stone

Abstract

Ceramics are joined to themselves or to metals using a transient liquid phase method employing three layers, one of which is a refractory metal, ceramic or alloy. The refractory layer is placed between two metal layers, each of which has a lower melting point than the refractory layer. The three layers are pressed between the two articles to be bonded to form an assembly. The assembly is heated to a bonding temperature at which the refractory layer remains solid, but the two metal layers melt to form a liquid. The refractory layer reacts with the surrounding liquid and a single solid bonding layer is eventually formed. The layers may be designed to react completely with each other and form refractory intermetallic bonding layers. Impurities incorporated into the refractory metal may react with the metal layers to form refractory compounds. Another method for joining ceramic articles employs a ceramic interlayer sandwiched between two metal layers. In alternative embodiments, the metal layers may include sublayers. A method is also provided for joining two ceramic articles using a single interlayer. An alternate bonding method provides a refractory-metal oxide interlayer placed adjacent to a strong oxide former. Aluminum or aluminum alloys are joined together using metal interlayers.

Claims

1. A method for bonding refractory materials, comprising:

(a) providing first and second articles, said first article including Si₃ N₄ ;

(b) placing at least three metal layers between said first and second articles, said first metal layer being located between said second and third metal layers, said first metal layer including a refractory metal, and said second and third metal layers each having a melting point which is lower than said refractory metal;

(c) pressing said first, second, and third metal layers between said first and second articles to form an assembly;

(d) heating said assembly to a first temperature sufficient to form a liquid from said second and third metal layers, but said first temperature being not sufficient to melt said first metal layer by itself; and

(e) maintaining said assembly at said first temperature until said liquid disappears and a solid bonding layer is formed between said first and second articles, said bonding layer having a higher melting point than said first temperature.

2. The method of claim 1 wherein said second article includes Si₃ N₄.

3. The method of claim 1 further including:

(f) heating said assembly at a second temperature until said bonding layer is homogenized.

4. The method of claim 3 wherein step (f) is performed immediately after step (e).

5. The method of claim 1 wherein at least one of said second and third metal layers includes at least two sublayers for forming an alloy.

6. The method of claim 1 wherein said second metal layer is comprised of a first sublayer having a first amount of gold, a second sublayer having a second amount of silicon, and a third sublayer having a third amount of titanium.

7. The method of claim 5 wherein said second metal layer is comprised of a first sublayer having a first amount of copper, a second sublayer having a second amount of silver, and a third sublayer having a third amount of titanium.

8. The method of claim 5 wherein said second metal layer is comprised of a first sublayer having a first amount of gold, a second sublayer having a second amount of copper, and a third sublayer having a third amount of titanium.

9. The method of claim 8 wherein said amount of gold in said first sublayer is approximately equivalent to said amount of copper in said second sublayer.

10. The method of claim 8 wherein said first, second, and third amounts are in ratios of approximately 48:

48;

4.

11. The method of claim 5 wherein a first of said three sublayers is deposited on said first article, said first sublayer being comprised of a metal which is reactive with Si₃ N₄ and which promotes wetting.

12. The method of claim 11 wherein said metal is selected from the group consisting of titanium, zirconium or chromium.

13. The method of claim 5 wherein a first of said three sublayers is deposited on said first article, said first sublayer being comprised of a metal which metallizes said first article.

14. The method of claim 13 wherein said metal is selected from the group consisting of tungsten, molybdenum, niobium, tantalum, rhenium, osmium, iridium, and rhodium.

15. The method of claim 5 wherein said second and third metal layers are deposited on said first metal layer prior to said step (c).

16. The method of claim 5 wherein said second metal layer is deposited on said first article prior to said step (c).

17. The method of claim 15 wherein said first sublayer of said second and third metal layers includes an amount of gold, said first sublayer being deposited furthest from said first metal layer relative to said second and third sublayers.

18. The method of claim 16 wherein said first sublayer of said second metal layer includes an amount of gold, said first sublayer being deposited furthest from said first article relative to said second and third sublayers.

19. The method of claim 16 wherein said first metal layer includes nickel.

20. The method of claim 1 wherein said three metal layers are composed of metals which, upon heating, react to form a bonding layer being more refractory than any of said three metal layers individually.

21. The method of claim 20 wherein said first metal layer includes nickel, and said second and third metal layers include aluminum.

22. A method for bonding refractory materials, comprising:

(a) providing first and second articles;

(b) placing at least three layers between said first and second articles, a first of said three layers being composed of a ceramic material;

(c) pressing said first, second, and third layers between said first and second articles to form an assembly;

(d) heating said assembly to a first temperature sufficient to melt said second and third layers; and

(e) maintaining said assembly at said first temperature until a solid bonding layer is formed between said first and second articles, said bonding layer having a higher melting point than said first temperature.

23. The method of claim 22 wherein said second and third layers are composed of a metal, said first layer being positioned between said second and third layers.

24. The method of claim 23 wherein said ceramic is composed of 3Al₂ O₃.2SiO₂, said second layer is composed of aluminum, and said third layer is composed of aluminum.

25. A method for bonding refractory materials, comprising:

(a) providing first and second articles;

(b) placing at least three metal layers between said first and second articles, said first metal layer being located between said second and third metal layers, said first metal layer including a refractory metal and impurities, said impurities reacting with said second metal Layer to form a compound having a melting temperature greater than said second metal layer;

(c) pressing said first, second, and third metal layers between said first and second articles to form an assembly;

(d) heating said assembly to a first temperature sufficient to form a liquid from said second and third metal layers, but said first temperature being not sufficient to melt said first metal layer; and

(e) maintaining said assembly at said first temperature until said liquid disappears and a solid bonding layer is formed between said first and second articles, said bonding layer having a higher melting point than said first temperature.

26. The method of claim 25 wherein said impurities are chosen from the group consisting of boron and carbon.

27. The method of claim 26 wherein said refractory metal includes nickel.

28. The method of claim 25 wherein said impurities react with said third metal layer to form a compound having a melting temperature greater than said third metal layer.

29. A method for bonding refractory materials, comprising:

(a) providing first and second articles;

(b) placing at least three layers between said first and second articles, said first layer being located between said second and third layers, said first layer including a refractory-metal oxide, said second and third layers including a metal being a strong oxide former to promote wetting, and said second and third layers having a melting point less than the melting point of said first layer;

(c) pressing said first, second, and third layers between said first and second articles to form an assembly;

(d) heating said assembly to a first temperature sufficient to form a liquid from said second and third layers, but said first temperature being not sufficient to melt said first layer; and

(e) maintaining said assembly at said first temperature until said liquid disappears and a solid bonding layer is formed between said first and second articles, said bonding layer having a higher melting point than said first temperature.

30. The method of claim 29 wherein said first layer includes iron oxide.

31. The method of claim 29 wherein said second and third metal layers are chosen from the group including aluminum and magnesium.