CN113072389B - Low-temperature connection method of oxide ceramics - Google Patents

Low-temperature connection method of oxide ceramics Download PDF

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CN113072389B
CN113072389B CN202110380989.3A CN202110380989A CN113072389B CN 113072389 B CN113072389 B CN 113072389B CN 202110380989 A CN202110380989 A CN 202110380989A CN 113072389 B CN113072389 B CN 113072389B
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geopolymer
temperature
low
precursor
oxide ceramics
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CN113072389A (en
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金柏希
康雨航
王愉瑾
毛样武
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Wuhan Institute of Technology
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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
    • 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
    • C04B12/00—Cements not provided for in groups C04B7/00 - C04B11/00
    • C04B12/005—Geopolymer cements, e.g. reaction products of aluminosilicates with alkali metal hydroxides or silicates
    • 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
    • C04B2237/30—Composition of layers of ceramic laminates or of ceramic or metallic articles to be joined by heating, e.g. Si substrates
    • C04B2237/32—Ceramic
    • C04B2237/34—Oxidic
    • C04B2237/341—Silica or silicates
    • 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
    • C04B2237/30—Composition of layers of ceramic laminates or of ceramic or metallic articles to be joined by heating, e.g. Si substrates
    • C04B2237/32—Ceramic
    • C04B2237/34—Oxidic
    • C04B2237/343—Alumina or aluminates
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P40/00—Technologies relating to the processing of minerals
    • Y02P40/10—Production of cement, e.g. improving or optimising the production methods; Cement grinding

Abstract

The invention discloses a low-temperature connection method of oxide ceramics, which comprises the steps of generating a geopolymer precursor by reacting an alkali activator with metakaolin and the like, solidifying part of the precursor at low temperature, grinding the solidified precursor into powder and carrying out heat treatment to obtain a granular geopolymer reinforcing phase. And then mixing and stirring the geopolymer particles and the geopolymer precursor uniformly to obtain the geopolymer particle reinforced geopolymer precursor. The geopolymer particle reinforced geopolymer precursor is uniformly coated on the connecting surface of the oxide ceramic, and finally the particle reinforced geopolymer precursor and the surface of the oxide ceramic form bonding through low-temperature connection in a sealed container, so that connection is realized. The low-temperature connection method of the oxide ceramics can improve the density of the connection region of the oxide ceramic joint, thereby improving the joint strength. In addition, the invention can successfully connect the oxide ceramics at a lower temperature, has low connection cost, and is energy-saving and environment-friendly.

Description

Low-temperature connection method of oxide ceramics
Technical Field
The invention relates to the technical field of connection of oxide ceramics, in particular to a low-temperature connection method of oxide ceramics.
Background
Oxide ceramics such as Al 2 O 3 And SiO 2 And the like, because of having excellent properties such as high resistivity, high thermal conductivity, corrosion resistance, wear resistance and the like, have wide application in many fields. Due to its poor processability, it is necessary to join them when making large-sized and complex-shaped articles.
The common methods for connecting oxide ceramics mainly include brazing, diffusion welding and the like, for example, chinese patent CN111644739A discloses a brazing filler metal system and a brazing method for brazing YSZ ceramics in an air atmosphere, and the method solves the problems of large joint brittleness, low mechanical strength and poor high-temperature oxidation/reduction atmosphere tolerance in the existing YSZ ceramic brazing process. The method of brazing YSZ ceramics is as follows: 1. polishing the to-be-welded surface of the YSZ ceramic; 2. mixing Ag powder with nano SiO 2 Grinding and mixing glass particles to prepare Ag-SiO 2 Brazing filler metal powder; 3. preparing an ethyl cellulose-terpineol solution binder; 4. Ag-SiO 2 Mixing the mixed powder with a binder; 5. coating solder paste on the surface to be welded; 6. brazing was performed in a muffle furnace. The invention can directly obtain reliable YSZ ceramic soldered joint in air atmosphere without high vacuum or protective atmosphere, and SiO in solder 2 The particles have excellent high-temperature oxidation/reduction atmosphere tolerance, hydrogen-induced reduction cavities can not occur, and the air tightness of the soldered joint is good. Chinese patent CN87101570A discloses a method for connecting oxide superconductors, which is mainly characterized in that the surfaces of superconductors are mechanically ground flat and then coated or not coated with solder, superconductor parts (plates, rods, wires and the like) are clamped by a clamp, certain pressure is applied, then the superconductor parts are heated at a certain speed, the superconductor parts are insulated for a certain time to realize diffusion welding, and finally the superconductor parts are cooled to room temperature at a certain speed.
The method for connecting the oxide ceramics has the following defects: brazing is usually carried out in a high-temperature sintering furnace by using brazing filler metal, and the main problem is that the required connection temperature is high, so the cost is high and the energy consumption is high. Diffusion welding has high requirements on the preparation and assembly of the surface of a weldment, the size of the weldment is limited by equipment, and the temperature and pressure required during diffusion are high, so that the requirements on the equipment are high, and the cost is high.
Disclosure of Invention
In order to overcome the above-mentioned disadvantages of the prior art, it is an object of the present invention to provide a low-temperature bonding method of oxide ceramics.
In order to solve the problems, the invention adopts the following technical scheme:
a low-temperature bonding method of oxide ceramics comprises the following steps:
1) Preparing potassium silicate, KOH and deionized water into an alkali activator;
2) Mixing metakaolin and the alkali activator, and stirring to obtain a geopolymer precursor A;
3) Solidifying the geopolymer precursor A, grinding the solidified geopolymer precursor A into fine powder, and then putting the fine powder into a muffle furnace for heat treatment to obtain a geopolymer particle reinforced phase;
4) Mixing metakaolin and the alkali activator, and stirring to obtain a geopolymer precursor B; adding the geopolymer particle reinforced phase into the geopolymer precursor B, and continuously stirring to obtain a geopolymer particle reinforced geopolymer precursor;
5) Coating the geopolymer particle reinforced geopolymer precursor prepared in the step 4) on the surface of the oxide ceramic after pretreatment, butting the two coated surfaces to form a connecting piece, and then connecting the connecting piece to obtain the oxide ceramic connecting piece.
Preferably, the mass ratio of potassium silicate, KOH and deionized water in the alkali activator is 100: (8 to 10): (70 to 90).
Preferably, the mass ratio of the metakaolin to the alkali activator in the geopolymer precursor A is (70 to 90): (178 to 200).
Preferably, the mass ratio of the metakaolin to the alkali activator in the geopolymer precursor B is (70 to 90): (178 to 200).
Preferably, in the geopolymer particle-reinforced geopolymer precursor, the mass ratio of the geopolymer particle reinforcing phase to the geopolymer precursor B is (5 to 10): (248 to 290).
Preferably, the heat treatment temperature is 500-600 ℃, and the time is 30-60 min.
Preferably, the temperature of the curing treatment is 50 to 80 ℃, and the time is 24 to 72 hours.
Preferably, the temperature of the connection processing is 50 to 80 ℃, and the time is 24 to 72 hours.
Preferably, the alkali-activator is prepared by the following method: mixing potassium silicate, KOH and deionized water uniformly, and standing for 12 to 24 hours at the temperature of 30 to 40 ℃ to obtain the alkali activator.
Preferably, the pretreatment comprises a polishing or cleaning degreasing treatment.
Compared with the prior art, the invention has the technical effects that:
according to the low-temperature connection method of the oxide ceramics, the geopolymer precursor is enhanced by adding the granular geopolymer enhancement phase, so that the shrinkage of the geopolymer precursor during curing can be reduced, and the density of a joint connection region is improved; in addition, the low-temperature connection method of the oxide ceramics can successfully connect the oxide ceramics at a lower temperature, and has the advantages of low connection cost, energy conservation and environmental protection.
The low-temperature connection method of the oxide ceramic is simple to operate, low in cost of required raw materials and suitable for industrial large-scale production, and the obtained oxide ceramic connecting piece is firm in combination, free of cracks on a connection interface and high in joint strength.
Additional advantages, objects, and features of the invention will be set forth in part in the description which follows and in part will become apparent to those having ordinary skill in the art upon examination of the following or may be learned from practice of the invention.
It will be appreciated by those skilled in the art that the objects and advantages that can be achieved with the present invention are not limited to what has been particularly described hereinabove, and that the above and other objects that can be achieved with the present invention will be more clearly understood from the following detailed description.
Drawings
The accompanying drawings, which are included to provide a further understanding of the invention and are incorporated in and constitute a part of this specification, illustrate embodiments of the invention and together with the description serve to explain the principles of the invention and not to limit the invention. In the drawings:
fig. 1 is a flow diagram of a preparation process for a geopolymer particle reinforced geopolymer precursor provided by an embodiment of the present invention;
FIG. 2 is a schematic diagram of Al connection by using geopolymer particles to reinforce geopolymer precursors according to an embodiment of the present invention 2 O 3 Assembly drawing of ceramics;
FIG. 3 is an infrared spectrum of a geopolymer reinforced with geopolymer particles after heat treatment at 500 ℃ for 30 min and a metakaolin material prepared in example 1 of the present invention;
figure 4 is an X-ray diffraction pattern of the geopolymer particle reinforced geopolymer with metakaolin material after heat treatment at 500 ℃ for 30 min as prepared in example 1 of the present invention.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is further described in detail with reference to the following embodiments. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention.
The endpoints of the ranges and any values disclosed herein are not limited to the precise range or value, and such ranges or values should be understood to encompass values close to those ranges or values. For numerical ranges, each range between its endpoints and individual point values, and each individual point value can be combined with each other to give one or more new numerical ranges, and such numerical ranges should be construed as specifically disclosed herein.
Before describing the present invention in detail, it is to be understood that the terminology used herein is for the purpose of describing particular embodiments only, and is not intended to limit the scope of the present invention which will be limited only by the appended claims. For a more complete understanding of the invention described herein, the following terms are used, and their definitions are set forth below. Unless defined otherwise, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs.
All the starting materials mentioned in the following examples are commercially available, unless otherwise specified.
The embodiment of the invention provides a low-temperature connection method of oxide ceramics, which comprises the following steps:
1) Preparing potassium silicate, KOH and deionized water into an alkali activator;
2) Mixing metakaolin and an alkali activator, and stirring to obtain a geopolymer precursor A;
3) Curing the geopolymer precursor A, grinding the cured geopolymer precursor A into fine powder, and then putting the fine powder into a muffle furnace for heat treatment to obtain a geopolymer particle reinforced phase;
4) Mixing metakaolin and an alkali activator, and stirring to obtain a geopolymer precursor B; adding the geopolymer particle reinforced phase into the geopolymer precursor B, and continuously stirring to obtain a geopolymer particle reinforced geopolymer precursor;
5) Coating the geopolymer particle reinforced geopolymer precursor prepared in the step 4) on the surface of the oxide ceramic after pretreatment, butting the two coated surfaces to form a connecting piece, and then connecting the connecting piece to obtain the oxide ceramic connecting piece.
Fig. 1 shows a flow chart of preparation of a geopolymer particle-reinforced geopolymer precursor according to an embodiment of the present invention (corresponding to steps 1) to 4); FIG. 2 shows an Al-bonded Geopolymer precursor reinforced with Geopolymer particles according to an embodiment of the present invention 2 O 3 Assembly drawing of ceramic (corresponding to step 5) described above).
The invention relates to a low-temperature connection method of oxide ceramics, which is based on the following design principle: the geopolymer precursor is generated by the reaction of an alkali activator and metakaolin and the like, and a part of the precursor is ground into powder after being solidified at low temperature and is subjected to heat treatment to obtain the granular geopolymer reinforcing phase. And then mixing and stirring the geopolymer particles and the geopolymer precursor uniformly to obtain the geopolymer particle reinforced geopolymer precursor. The geopolymer particle reinforced geopolymer precursor is uniformly coated on the connecting surface of the oxide ceramic, and finally the particle reinforced geopolymer precursor and the surface of the oxide ceramic form bonding through low-temperature connection in a sealed container, so that connection is realized. The particle-reinforced geopolymer reinforcing phase can reduce the shrinkage of the solidified geopolymer precursor, so that the compactness of the connecting region of the oxide ceramic joint can be improved, and the joint strength is improved. The thickness of the solder of the oxide ceramic connecting piece obtained by the connecting method is about 300 to 400 mu m, and the maximum average shear strength of the joint can reach 59 MPa.
Wherein, the alkali activator in the step 1) can be prepared by the following method: mixing potassium silicate and KOH and deionized water are uniformly mixed, and the mixture is kept stand for 12 to 24 hours at the temperature of 30 to 40 ℃ to obtain the alkali activator. The mass ratio of potassium silicate, KOH and deionized water in the prepared alkali activator is 100: (8 to 10): (70 to 90). The potassium silicate adopted by the embodiment of the invention comprises the following components: k 2 O•3.3SiO 2 88 wt%，H 2 O2 wt%, and the others are oxide impurities.
The mass ratio of the metakaolin to the alkali activator in the geopolymer precursor A in the step 2) is preferably (70 to 90): (178: 200). The metakaolin adopted in the embodiment of the invention has the component of SiO 2 54 wt%，Al 2 O 3 43 wt%, and the others are oxide impurities. The stirring speed is 700 to 1000 r/min, and the stirring time is 10 to 15 min.
The conditions of the curing treatment in step 3) are preferably: the temperature is 50 to 80 ℃, and the time is 24 to 72 hours. The conditions of the heat treatment are preferably: the temperature is 500-600 ℃, and the time is 30-60 min.
The mass ratio of the metakaolin to the alkali activator in the geopolymer precursor B in the step 4) is preferably (70 to 90): (178 to 200). In the geopolymer particle reinforced geopolymer precursor, the mass ratio of the geopolymer particle reinforced phase to the geopolymer precursor B is preferably (5 to 10): (248 to 290).
The conditions of the ligation treatment in step 5) are preferably: the temperature is 50 to 80 ℃, and the time is 24 to 72 hours. The joining process is carried out in a sealed container. The oxide ceramic surface pretreatment comprises polishing or cleaning degreasing treatment.
According to the low-temperature connection method of the oxide ceramics, the geopolymer precursor is enhanced by adding the granular geopolymer enhancement phase, so that the shrinkage of the geopolymer precursor during curing can be reduced, and the density of a joint connection region is improved; in addition, the low-temperature connection method of the oxide ceramics can successfully connect the oxide ceramics at a lower temperature, and has the advantages of low connection cost, energy conservation and environmental protection.
The low-temperature connection method of the oxide ceramic is simple to operate, low in cost of required raw materials and suitable for industrial large-scale production, and the obtained oxide ceramic connecting piece is firm in combination, free of cracks on a connection interface and high in joint strength.
The following is a further description with reference to specific examples.
Example 1
Embodiment 1 of the present invention provides a low-temperature connection method for oxide ceramics, which specifically includes the following steps:
1) 100 g of potassium silicate (containing 88 wt.% of K) are weighed out 2 O•3.3SiO 2 2% by weight of H 2 O, the other is oxide impurities), 9.6 g of KOH and 90 g of deionized water, then uniformly mixing, placing in a 40 ℃ oven, and standing for 24 hours to obtain a transparent alkali activator;
2) 7.9 g of metakaolin (54% by weight SiO in it) were weighed out 2 43 wt% of Al 2 O 3 And 3 wt% of impurities) and 18.6 g of the alkali activator, and mixing the two in a stirrer at the rotating speed of 900 r/min for 10 min to obtain a geopolymer precursor A which is uniformly mixed;
3) Sealing the geopolymer precursor A, placing in a 75 ℃ oven for heat preservation for 72 h for solidification, grinding the solidified geopolymer into fine powder, then placing in a muffle furnace for heat treatment at 500 ℃ for 30 min to obtain a granular geopolymer particle reinforced phase;
4) Weighing 7.9 g of metakaolin and 18.6 g of alkali activator, mixing the metakaolin and the alkali activator in a stirrer at the rotating speed of 900 r/min for 10 min to obtain a geological polymer precursor B which is uniformly mixed; taking 0.5 g of the geopolymer particle reinforced phase obtained in the step 3), adding the geopolymer particle reinforced phase into the geopolymer precursor B, and continuously stirring for 10 min to obtain a geopolymer particle reinforced geopolymer precursor;
5) Coating the geopolymer particle reinforced geopolymer precursor prepared in the step 4) on the surface of the pretreated aluminum oxide, butting the two coated surfaces to form a connecting piece, then sealing and placing the connecting piece into an oven for low-temperature connection, and keeping the temperature for 48 hours under the condition that the connection temperature is 75 ℃ to obtain the aluminum oxide connecting piece. The maximum shearing strength of the aluminum oxide connecting piece prepared by the embodiment can reach 59 MPa.
Fig. 3 is an infrared spectrum of the geopolymer particle reinforced geopolymer prepared in this example (i.e., the particulate geopolymer particle reinforced phase prepared in step 3) and metakaolin material, and it can be seen from fig. 3 that the Si-O-Si bond is significantly shifted, indicating the formation of the geopolymer.
Figure 4 is an X-ray diffraction pattern of the geopolymer particles reinforced geopolymer produced in this example (i.e. the particulate geopolymer particle reinforcing phase produced in step 3) with a metakaolin starting material. As can be seen in fig. 4, the amorphous peak of the geopolymer is significantly shifted compared to the amorphous peak of metakaolin, further confirming the formation of geopolymer.
Example 2
Embodiment 2 of the present invention provides a low temperature connection method of oxide ceramics, which specifically includes the following steps:
1) 100 g of potassium silicate (88 wt.% K) was weighed out 2 O•3.3SiO 2 2% by weight of H 2 O, the other is oxide impurities), 8.9 g of KOH and 90 g of deionized water, then uniformly mixing, placing in a 35 ℃ oven, and standing for 24 hours to obtain a transparent alkali activator;
2) 8.5 g of metakaolin (containing 54% by weight of SiO) were weighed out 2 43 wt% of Al 2 O 3 And 3 wt% of impurities) and 20.0 g of the alkali activator, and mixing the two in a stirrer at the rotating speed of 700 r/min for 14 min to obtain a geological polymer precursor A which is uniformly mixed;
3) Sealing the geopolymer precursor A, placing in a 60 ℃ oven for heat preservation for 64 h for solidification, grinding the solidified geopolymer into fine powder, then placing in a muffle furnace for heat treatment at 500 ℃ for 30 min to obtain a granular geopolymer particle reinforced phase;
4) Weighing 8.5 g of metakaolin and 20.0 g of alkali activator, and mixing the metakaolin and the alkali activator in a stirrer at the rotating speed of 700 r/min for 14 min to obtain a geopolymer precursor B which is uniformly mixed; taking 0.8 g of the geopolymer particle reinforced phase obtained in the step 3), adding the geopolymer particle reinforced phase into the geopolymer precursor B, and continuously stirring for 10 min to obtain a geopolymer particle reinforced geopolymer precursor;
5) Coating the geopolymer particle reinforced geopolymer precursor prepared in the step 4) on the surface of pretreated silicon dioxide, butting the two coated surfaces to form a connecting piece, then hermetically placing the connecting piece into an oven for low-temperature connection, and keeping the temperature for 64 h under the condition that the connection temperature is 60 ℃ to obtain the silicon dioxide connecting piece. The interface of the silicon dioxide connecting piece manufactured by the embodiment is firmly combined, the connecting interface has no crack, and the joint strength is higher.
Example 3
Embodiment 3 of the present invention provides a low temperature connection method of oxide ceramics, which specifically includes the following steps:
1) 100 g of potassium silicate (88 wt.% K) was weighed out 2 O•3.3SiO 2 2% by weight of H 2 O, the rest is oxide impurities), 8.2 g of KOH and 70 g of deionized water, then uniformly mixing, placing in a 30 ℃ oven, and standing for 12 hours to obtain a transparent alkali activator;
2) 7.1g of metakaolin (54% by weight SiO in it) were weighed out 2 43 wt% of Al 2 O 3 And 3 wt% impurities) and 18.0 g of the alkali activator, and mixing the two in a stirrer at a rotating speed of 800 r/min for 15 min to obtain a geopolymer precursor A which is uniformly mixed;
3) Sealing the geopolymer precursor A, placing in an oven at 55 ℃ for heat preservation for 48 h for solidification, grinding the solidified geopolymer into fine powder, then placing in a muffle furnace, and preserving the heat at 600 ℃ for 60 min for heat treatment to obtain a granular geopolymer particle reinforced phase;
4) Weighing 7.1g of metakaolin and 18.0 g of alkali activator, mixing the metakaolin and the alkali activator in a stirrer at the rotating speed of 800 r/min for 15 min to obtain a geological polymer precursor B which is uniformly mixed; taking 1.0 g of the geopolymer particle reinforced phase obtained in the step 3), adding the geopolymer particle reinforced phase into the geopolymer precursor B, and continuously stirring for 10 min to obtain a geopolymer particle reinforced geopolymer precursor;
5) Coating the geopolymer particle reinforced geopolymer precursor prepared in the step 4) on the surface of the pretreated aluminum oxide, butting the two coated surfaces to form a connecting piece, then hermetically placing the connecting piece into an oven for low-temperature connection, and keeping the temperature for 72 hours under the condition that the connection temperature is 50 ℃ to obtain the aluminum oxide connecting piece. The alumina connecting piece prepared by the embodiment has the advantages of firm interface combination, no obvious crack on the connecting interface and higher joint strength.
Example 4
Embodiment 4 of the present invention provides a low-temperature connection method for oxide ceramics, which specifically includes the following steps:
1) 100 g of potassium silicate (88 wt.% K) was weighed out 2 O•3.3SiO 2 2% by weight of H 2 O, the rest is oxide impurities), 9.0 g of KOH and 80 g of deionized water, then uniformly mixing, placing in a 30 ℃ oven, and standing for 24 hours to obtain a transparent alkali activator;
2) 8.8 g of metakaolin (which contains 54 wt% SiO) were weighed out again 2 43 wt% of Al 2 O 3 And 3 wt% of impurities) and 19.0 g of the alkali activator, and mixing the two in a stirrer at the rotating speed of 700 r/min for 15 min to obtain a geological polymer precursor A which is uniformly mixed;
3) Sealing the geopolymer precursor A, placing the sealed geopolymer precursor A in a 50 ℃ drying oven, preserving heat for 72 h for curing, grinding the cured geopolymer into fine powder, then placing the fine powder in a muffle furnace, preserving heat for 45 min at 550 ℃, and carrying out heat treatment to obtain a granular geopolymer particle reinforced phase;
4) Weighing 8.8 g of metakaolin and 19.0 g of alkali activator, and mixing the metakaolin and the alkali activator in a stirrer at the rotating speed of 700 r/min for 15 min to obtain a geopolymer precursor B which is uniformly mixed; taking 0.6 g of the geopolymer particle reinforced phase obtained in the step 3), adding the geopolymer particle reinforced phase into the geopolymer precursor B, and continuously stirring for 10 min to obtain a geopolymer particle reinforced geopolymer precursor;
5) Coating the geopolymer particle reinforced geopolymer precursor prepared in the step 4) on the surface of the pretreated silicon dioxide, butting the two coated surfaces to form a connecting piece, and then hermetically placing the connecting piece into an oven for low-temperature connection, wherein the connection temperature is 80 ℃, and keeping the temperature for 24 hours to obtain the silicon dioxide connecting piece. The interface of the silicon dioxide connecting piece manufactured by the embodiment is firmly combined, the connecting interface has no crack, and the joint strength is higher.
In addition, any combination of the various embodiments of the present invention can be made, and the same should be considered as the disclosure of the present invention as long as the idea of the present invention is not violated.
The present invention is not limited to the above-described specific embodiments, and various modifications and variations are possible. Any modifications, equivalents, improvements and the like made to the above embodiments in accordance with the technical spirit of the present invention should be included in the scope of the present invention.

Claims (10)

1. A low-temperature connection method of oxide ceramics is characterized by comprising the following steps:
1) Preparing potassium silicate, KOH and deionized water into an alkali activator;
2) Mixing metakaolin and the alkali activator, and stirring to obtain a geopolymer precursor A;
3) Solidifying the geopolymer precursor A, grinding the solidified geopolymer precursor A into fine powder, and then putting the fine powder into a muffle furnace for heat treatment to obtain a geopolymer particle reinforced phase; the heat treatment temperature is 500-600 ℃;
4) Mixing metakaolin and the alkali activator, and stirring to obtain a geopolymer precursor B; adding the geopolymer particle reinforced phase into the geopolymer precursor B, and continuously stirring to obtain a geopolymer particle reinforced geopolymer precursor;
5) Coating the geopolymer particle reinforced geopolymer precursor prepared in the step 4) on the surface of the oxide ceramic after pretreatment, butting the two coated surfaces to form a connecting piece, and then connecting the connecting piece to obtain an oxide ceramic connecting piece; the temperature of the connection treatment is 50 to 80 ℃.
2. The method for connecting oxide ceramics at low temperature according to claim 1, wherein the alkali activator contains potassium silicate, KOH and deionized water at a mass ratio of 100: (8 to 10): (70 to 90).
3. The low-temperature connection method of oxide ceramics according to claim 1, wherein the mass ratio of metakaolin to the alkali activator in the geopolymer precursor A is (70 to 90): (178: 200).
4. The low-temperature connection method of oxide ceramics according to claim 1, wherein the mass ratio of metakaolin to the alkali activator in the geopolymer precursor B is (70-90): (178: 200).
5. The low-temperature connection method of oxide ceramics according to claim 1, wherein the mass ratio of the geopolymer particle reinforced phase to the geopolymer precursor B in the geopolymer particle reinforced geopolymer precursor is (5 to 10): (248 to 290).
6. The method for connecting oxide ceramics at low temperature according to claim 1, wherein the heat treatment time is 30 to 60 min.
7. The low-temperature connection method of oxide ceramics according to claim 1, wherein the temperature of the curing process is 50 to 80 ℃ and the time is 24 to 72 hours.
8. The method for connecting oxide ceramics at low temperature according to claim 1, wherein the connection processing time is 24 to 72 hours.
9. The method for low-temperature bonding of oxide ceramics according to claim 1, wherein the alkali activator is prepared by the following method: and (3) uniformly mixing potassium silicate, KOH and deionized water, and standing for 12-24 h at the temperature of 30-40 ℃ to obtain the alkali activator.
10. The method for low-temperature bonding of oxide ceramics according to claim 1, wherein the pretreatment comprises polishing or cleaning degreasing treatment.
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