Method for sealing an oxygen transport membrane assembly

• US 9,969,645 B2
• Filed: 12/19/2013
• Issued: 05/15/2018
• Est. Priority Date: 12/19/2012
• Status: Active Grant

• Current Assignee: Praxair Technology Incorporated (Linde Plc)
• Original Assignee: Praxair Technology Incorporated (Linde Plc)
• Inventors: Gonzalez, Javier E., Grant, Arthur F.
• Primary Examiner(s): Aftergut, Jeffry H
• Assistant Examiner(s): Lee, Jaeyun
• Application Number:
  US14/134,276
• Publication Number:
  US 20140169862A1
• Time in Patent Office: 1,608 Days
• CPC Class Codes: B01D 65/003 Membrane bonding or sealing
• CPC Class Codes: B01D 71/024 Oxides
• CPC Class Codes: B01D 71/0271 Perovskites
• CPC Class Codes: C03C 10/0018 containing SiO2, Al2O3 and monovalent metal oxide as main constituents
• CPC Class Codes: C03C 8/24 Fusion seal compositions being frit compositions having non-frit additions, i.e. for use as seals between dissimilar materials, e.g. glass and metal; Glass solders
• CPC Class Codes: C04B 2235/6562 Heating rate
• CPC Class Codes: C04B 2235/6565 Cooling rate
• CPC Class Codes: C04B 2237/10 Glass interlayers, e.g. frit or flux
• CPC Class Codes: C04B 2237/348 Zirconia, hafnia, zirconates or hafnates
• CPC Class Codes: C04B 2237/40 Metallic
• CPC Class Codes: C04B 2237/401 Cermets
• 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 2237/765 at least one member being a tube
• CPC Class Codes: C04B 35/6264 Mixing media, e.g. organic solvents
• CPC Class Codes: C04B 35/632 Organic additives
• CPC Class Codes: C04B 35/6342 Polyvinylacetals, e.g. polyvinylbutyral [PVB]
• CPC Class Codes: C04B 35/638 Removal thereof
• CPC Class Codes: C04B 37/005 consisting of glass or ceramic material
• CPC Class Codes: C04B 37/025 consisting of glass or ceramic material
• CPC Class Codes: H01M 8/0282 : Inorganic material
• CPC Class Codes: H01M 8/0286 : Processes for forming seals
• CPC Class Codes: Y02E 60/50 : Fuel cells
• CPC Class Codes: Y10T 403/477 : Fusion bond, e.g., weld, etc.

Abstract

An improved method of sealing a ceramic part to a solid part made of ceramic, metal, cermet or a ceramic coated metal is provided. The improved method includes placing a bond agent comprising an Al₂O₃ and SiO₂ based glass-ceramic material and organic binder material on adjoining surfaces of the ceramic part and the solid part. The assembly is heated to a first target temperature that removes or dissolves the organic binder material from the bond agent and the assembly is subjected to a second induction heating step at a temperature ramp rate of between about 100° C. and 200° C. per minute to temperatures where the glass-ceramic material flows and wets the interface between adjoining surfaces. The assembly is rapidly cooled at a cooling rate of about 140° C. per minute or more to induce nucleation and re-crystallization of the glass-ceramic material to form a dense, durable and gas-tight seal.

Claims

1. A method of sealing a first ceramic part to a second ceramic part configured to receive the first ceramic part, the method comprising the steps of:

placing a glass-ceramic bond agent comprising a glass-ceramic material and organic binder material in a volumetric ratio of from about 4;

1 to about 1.5;

1 on one or more adjoining surfaces of the first ceramic part and the second ceramic part, wherein said glass-ceramic bond agent comprises a blend of from about 2 mol % to about 15 mol % of Al₂O₃, from about 40 mol % to about 70 mol % SiO₂ and from about 20 mol % to 55 mol % BaO, SrO, CaO, MgO or combinations thereof;

heating the first ceramic part, the second ceramic part and the bond agent to remove or dissolve the organic binder material;

further heating the first ceramic part and the second ceramic part at a rate of greater than about 100°

C. per minute to temperatures where the glass-ceramic material reacts with carbon from the organic binder material and the glass-ceramic material flows into or wets the interface between adjoining surfaces of the first ceramic part and the second ceramic part; and

cooling the first ceramic part and the second ceramic part at a rate of greater than about 100°

C. per minute to nucleate and re-crystallize the glass-ceramic material disposed between adjoining surfaces of the first ceramic part and the second ceramic part and form a hermetic or gas-tight seal between the first ceramic part and the second ceramic part, said seal able to withstand temperatures of >

800°

C. and pressures of >

100 psi, wherein the steps of heating and cooling the first ceramic part and the second ceramic part further comprise using an induction heating element to effect the temperature changes.

2. The method of claim 1 wherein the organic binder material is a combination of phosphate ester, polyvinyl butyrai and butyl benzyl phthalate, and said glass-ceramic bond agent is a paste, slurry, film, ribbon, or tape disposed on one or more adjoining surfaces of the first ceramic part and the second ceramic part.

3. The method of claim 1 wherein the step of cooling the first ceramic part and the second ceramic part further comprises cooling the first ceramic part and the second ceramic part at a rate of between about 120°

C. per minute to about 160°

C. per minute to nucleate and re-crystallize the glass-ceramic material disposed between adjoining surfaces of the first ceramic part and the second ceramic solid part.

4. The method of claim 1 wherein the step of heating the first ceramic part and the second ceramic part to temperatures effective to flow and wet the glass-ceramic material further comprises heating the first ceramic part, the second ceramic part and the glass-ceramic material at a rate of between about 200°

C. per minute to about 250°

C. per minute.

5. The method of claim 1 further comprising the step of maintaining the temperature of the first ceramic part and the second ceramic part for a prescribed duration of between about 30 seconds to 360 seconds, the step of maintaining the temperature to be effected between or during the heating and cooling steps.

6. The method of claim 1, wherein the first ceramic part is a tubular oxygen transport membrane.