CN112592197A - Ceramic-metal sealing ceramic sheet prepared by tape casting method - Google Patents
Ceramic-metal sealing ceramic sheet prepared by tape casting method Download PDFInfo
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- CN112592197A CN112592197A CN202011446052.3A CN202011446052A CN112592197A CN 112592197 A CN112592197 A CN 112592197A CN 202011446052 A CN202011446052 A CN 202011446052A CN 112592197 A CN112592197 A CN 112592197A
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- ceramic
- casting method
- metal sealing
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- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B37/00—Joining burned ceramic articles with other burned ceramic articles or other articles by heating
- C04B37/02—Joining burned ceramic articles with other burned ceramic articles or other articles by heating with metallic articles
- C04B37/023—Joining burned ceramic articles with other burned ceramic articles or other articles by heating with metallic articles characterised by the interlayer used
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- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B37/00—Joining burned ceramic articles with other burned ceramic articles or other articles by heating
- C04B37/003—Joining 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
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- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B2237/00—Aspects relating to ceramic laminates or to joining of ceramic articles with other articles by heating
- C04B2237/02—Aspects relating to interlayers, e.g. used to join ceramic articles with other articles by heating
- C04B2237/10—Glass interlayers, e.g. frit or flux
Abstract
The invention discloses a ceramic-metal sealing ceramic sheet prepared by a tape casting method, which comprises the following sealing butt joint process flow: (1) drying the inorganic powder at 110 ℃ for 4 hours; (2) weighing powder by using a ball mill according to requirements, and crushing to obtain glass powder to be sealed; (3) adding the prepared glass powder into a ball milling tank according to a pulping formula to prepare glass slurry; the ceramic-metal sealing ceramic chip prepared by the tape casting method is different from the prior art, the glass sealing material prepared by the tape casting method and suitable for high-temperature use has uniform density, is suitable for cutting and processing, is well attached to a plane for plating, has good sealing performance after sintering, has high chemical stability in an oxidizing gas environment, has thermal expansion amount which is uniformly matched with each part of the solid oxide fuel cell, and cannot lose efficacy due to the difference of local thermal expansion amount, thereby greatly improving the air tightness, the insulativity, the thermal stability and the chemical stability of the solid oxide fuel cell.
Description
Technical Field
The invention relates to the technical field of ceramic-metal sealing under a high-temperature working condition, in particular to a ceramic-metal sealing ceramic sheet prepared by a tape casting method.
Background
Solid Oxide Fuel Cells (SOFCs) are a new green generation technology that convert the chemical energy generated by combining a Fuel (e.g., H2, natural gas) on an oxygen ion conducting ceramic with an oxidizing gas (e.g., air) into electrical and thermal energy. Because the working environment of the solid oxide fuel cell is severe and the working temperature is high, the sealing material of the fuel cell stack is required to have good air tightness, insulation, thermal stability, chemical stability and the like, but until now, no material can meet all conditions, so that the sealing becomes a bottleneck limiting the development of the flat SOFC.
At present, the traditional technology of ceramic-metal sealing is mainly characterized in that a ceramic sealing material is made into sealing slurry, and after coating, the sealing slurry is combined and co-fired, and the coating technology is adopted, and after the slurry is coated on an SUS 430 steel groove and a ceramic plane, the sealing slurry and the ceramic plane are combined together and co-sintered.
However, the conventional process has poor coating uniformity and non-uniform structure of the formed sealing layer, which makes it difficult to ensure the airtightness of the high-temperature solid oxide fuel cell, and therefore, we propose a ceramic-metal sealing ceramic sheet prepared by a casting method.
Disclosure of Invention
The invention aims to provide a ceramic-metal sealing ceramic sheet prepared by a tape casting method, so as to solve the problems in the background technology.
In order to achieve the purpose, the invention provides the following technical scheme: a ceramic-metal sealing ceramic sheet prepared by a tape casting method comprises the following sealing butt joint process flow:
(1) drying the inorganic powder at 110 ℃ for 4 hours;
(2) weighing powder by using a ball mill according to requirements, and crushing to obtain glass powder to be sealed;
(3) adding the prepared glass powder into a ball milling tank according to a pulping formula to prepare glass slurry;
(4) preparing a biscuit by adopting a casting machine, casting for 1 time, and drying at the temperature of 60 ℃;
(5) cutting into pieces as required;
(6) and adding the superposed casting sealing sheet between the metal connector and the ceramic plate, and sintering to form sealing.
Preferably, in step (1)The inorganic powder comprises the following components: SiO 22：35％、B2O3：10％、Al2O3： 5％、BaO：35％、CaO：15％。
Preferably, in the step (2), the inorganic powder is firstly ball-milled for 3-6 hours (zirconium balls, diameter 5mm, ball/material volume ratio: 2/1), and after ball-milling and grinding, the inorganic powder is further ball-milled for 5-8 hours in a ball mill, and then sieved by a 400-mesh sieve, so as to obtain the glass powder to be sealed.
Preferably, in step (3), the mixture is ball-milled for 24 hours (zirconium balls, diameter 5mm, ball/material volume ratio: 2/1).
Preferably, the slurry in the step (3) comprises the following components: 100g of inorganic glass powder, 60ml of ethanol, 20ml of butanone, 2.5ml of triethanolamine, 4ml of diethyl phthalate, 6.4g of polyvinyl butyral, 3.2g of polyethylene glycol and 0.51 of solid content.
Preferably, in the step (4), the casting speed is 0.3m/min-0.5m/min, and the height of the flat scraper is 0.5 mm.
Preferably, in the slicing step (5), the material is laminated to a desired thickness of 15MPa, typically 1.5 mm.
Preferably, the sintering in step (6) requires heating at 2.5 ℃/min and sintering at 850 ℃ for 1 h.
Compared with the prior art, the invention has the beneficial effects that:
compared with the prior art, the glass sealing material prepared by adopting the tape casting method and suitable for high-temperature use has uniform density, is suitable for cutting and processing, is well attached to a plane for plating, has good sealing performance after sintering, has high chemical stability in an oxidizing gas environment, has thermal expansion amount which is uniformly matched with each part of a Solid Oxide Fuel Cell (SOFC), and cannot lose efficacy due to local thermal expansion difference, thereby greatly improving the air tightness, the insulativity, the thermal stability and the chemical stability of the SOFC.
Drawings
FIG. 1 is a schematic view of a ceramic-metal seal assembly of the present invention;
FIG. 2 is a schematic view of the operation of the casting machine of the present invention;
fig. 3 is a schematic view of the operation of the casting machine of the present invention.
Detailed Description
The technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the drawings in the embodiments of the present invention, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all of the embodiments. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
Referring to fig. 1-3, the present invention provides a technical solution: a ceramic-metal sealing ceramic sheet prepared by a tape casting method comprises the following sealing butt joint process flow:
(1) drying the inorganic powder at 110 ℃ for 4 hours;
(2) weighing powder according to requirements by using a ball mill, putting inorganic powder into the ball mill for ball milling for 3-6 hours (zirconium balls with the diameter of 5mm and the ball/material volume ratio of 2/1), grinding, ball milling for 5-8 hours in the ball mill, and sieving with a 400-mesh sieve to obtain glass powder to be sealed;
(3) adding the prepared glass powder into a ball milling tank according to a pulping formula to prepare glass slurry, and carrying out ball milling for 24 hours (zirconium balls with the diameter of 5mm and the ball/material volume ratio of 2/1);
(4) preparing biscuit by using a casting machine, casting for 1 time at the casting speed of 0.3-0.5 m/min and the height of a flat scraper of 0.5mm, and drying at the temperature of 60 ℃;
(5) cutting into pieces as required, and laminating under 15Mpa to obtain a required thickness of 1.5 mm;
(6) adding a superposed casting sealing sheet between a metal connector and a ceramic plate, heating at 2.5 ℃/min, and sintering at 850 ℃ for 1h to form sealing, wherein in the temperature rise process, the heating rate cannot be too fast, because glass and a battery element to be sealed are required to be fully wetted before crystals are precipitated and grown, if the heating rate is too high, the crystals are precipitated and cured under the condition of insufficient wetting, so that poor contact is caused, and the sealing effect is influenced.
In the step (1), the inorganic powder comprises the following components: SiO 22：35％、B2O3：10％、Al2O3：5％、BaO： 35％、CaO：15％。
The slurry in the step (3) comprises the following components: 100g of inorganic glass powder, 60ml of ethanol, 20ml of butanone, 2.5ml of triethanolamine, 4ml of diethyl phthalate, 6.4g of polyvinyl butyral, 3.2g of polyethylene glycol and 0.51 of solid content.
It is noted that, herein, relational terms such as first and second, and the like may be used solely to distinguish one entity or action from another entity or action without necessarily requiring or implying any actual such relationship or order between such entities or actions. Also, the terms "comprises," "comprising," or any other variation thereof, are intended to cover a non-exclusive inclusion, such that a process, method, article, or apparatus that comprises a list of elements does not include only those elements but may include other elements not expressly listed or inherent to such process, method, article, or apparatus.
Although embodiments of the present invention have been shown and described, it will be appreciated by those skilled in the art that changes, modifications, substitutions and alterations can be made in these embodiments without departing from the principles and spirit of the invention, the scope of which is defined in the appended claims and their equivalents.
Claims (8)
1. A ceramic-metal sealing ceramic sheet prepared by a tape casting method comprises the following sealing butt joint process flow:
(1) drying the inorganic powder at 110 ℃ for 4 hours;
(2) weighing powder by using a ball mill according to requirements, and crushing to obtain glass powder to be sealed;
(3) adding the prepared glass powder into a ball milling tank according to a pulping formula to prepare glass slurry;
(4) preparing a biscuit by adopting a casting machine, casting for 1 time, and drying at the temperature of 60 ℃;
(5) cutting into pieces as required;
(6) and adding the superposed casting sealing sheet between the metal connector and the ceramic plate, and sintering to form sealing.
2. The ceramic-metal sealing ceramic sheet prepared by a casting method according to claim 1, wherein: in the step (1), the inorganic powder comprises the following components: SiO 22：35％、B2O3：10％、Al2O3：5％、BaO：35％、CaO：15％。
3. The ceramic-metal sealing ceramic sheet prepared by a casting method according to claim 1, wherein: in the step (2), the inorganic powder is firstly ball-milled for 3-6 hours (zirconium balls with the diameter of 5mm and the ball/material volume ratio of 2/1), and is further ball-milled for 5-8 hours in a ball mill after ball-milling and crushing, and then is sieved by a 400-mesh sieve, so that the glass powder to be sealed is obtained.
4. The ceramic-metal sealing ceramic sheet prepared by a casting method according to claim 1, wherein: in step (3), ball milling was carried out for 24 hours (zirconium balls, diameter 5mm, ball/material volume ratio: 2/1).
5. The ceramic-metal sealing ceramic sheet prepared by a casting method according to claim 1, wherein: the slurry in the step (3) comprises the following components: 100g of inorganic glass powder, 60ml of ethanol, 20ml of butanone, 2.5ml of triethanolamine, 4ml of diethyl phthalate, 6.4g of polyvinyl butyral, 3.2g of polyethylene glycol and 0.51 of solid content.
6. The ceramic-metal sealing ceramic sheet prepared by a casting method according to claim 1, wherein: in the step (4), the casting speed is 0.3m/min-0.5m/min, and the height of the flat scraper is 0.5 mm.
7. The ceramic-metal sealing ceramic sheet prepared by a casting method according to claim 1, wherein: in the slicing process in the step (5), the material is laminated to a required thickness of 15MPa, generally 1.5 mm.
8. The ceramic-metal sealing ceramic sheet prepared by a casting method according to claim 1, wherein: in the step (6), the sintering is required to be heated at 2.5 ℃/min and sintered for 1h at 850 ℃.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202011446052.3A CN112592197A (en) | 2020-12-09 | 2020-12-09 | Ceramic-metal sealing ceramic sheet prepared by tape casting method |
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| Application Number | Priority Date | Filing Date | Title |
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| CN202011446052.3A CN112592197A (en) | 2020-12-09 | 2020-12-09 | Ceramic-metal sealing ceramic sheet prepared by tape casting method |
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| CN112592197A true CN112592197A (en) | 2021-04-02 |
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN115000449A (en) * | 2022-06-24 | 2022-09-02 | 西安石油大学 | Method for preparing SOFC (solid oxide Fuel cell) galvanic pile sealing coating by spraying-casting process |
-
2020
- 2020-12-09 CN CN202011446052.3A patent/CN112592197A/en active Pending
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN115000449A (en) * | 2022-06-24 | 2022-09-02 | 西安石油大学 | Method for preparing SOFC (solid oxide Fuel cell) galvanic pile sealing coating by spraying-casting process |
| CN115000449B (en) * | 2022-06-24 | 2023-07-04 | 西安石油大学 | Method for preparing SOFC (solid oxide Fuel cell) stack sealing coating through spraying-casting process |
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