CN116161979B - Method for connecting Ti-Al-C system MAX phase ceramic and zirconium alloy - Google Patents
Method for connecting Ti-Al-C system MAX phase ceramic and zirconium alloy Download PDFInfo
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- 239000000919 ceramic Substances 0.000 title claims abstract description 85
- 229910001093 Zr alloy Inorganic materials 0.000 title claims abstract description 61
- 238000000034 method Methods 0.000 title claims abstract description 28
- 229910002110 ceramic alloy Inorganic materials 0.000 title claims abstract description 20
- 239000010949 copper Substances 0.000 claims abstract description 20
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims abstract description 19
- 229910052802 copper Inorganic materials 0.000 claims abstract description 18
- 229910052751 metal Inorganic materials 0.000 claims abstract description 18
- 239000002184 metal Substances 0.000 claims abstract description 18
- 238000005498 polishing Methods 0.000 claims abstract description 16
- 229910045601 alloy Inorganic materials 0.000 claims description 27
- 239000000956 alloy Substances 0.000 claims description 27
- 244000137852 Petrea volubilis Species 0.000 claims description 10
- 238000001816 cooling Methods 0.000 claims description 8
- 239000011888 foil Substances 0.000 claims description 8
- 238000005304 joining Methods 0.000 claims description 7
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- 238000004140 cleaning Methods 0.000 claims description 3
- 238000010438 heat treatment Methods 0.000 claims description 3
- 239000006104 solid solution Substances 0.000 claims description 3
- 229910004298 SiO 2 Inorganic materials 0.000 claims description 2
- 238000003825 pressing Methods 0.000 claims description 2
- 239000010953 base metal Substances 0.000 abstract description 9
- 229910000765 intermetallic Inorganic materials 0.000 abstract description 6
- 238000007796 conventional method Methods 0.000 abstract 1
- 239000012071 phase Substances 0.000 description 46
- 239000010410 layer Substances 0.000 description 16
- 239000000463 material Substances 0.000 description 9
- 238000003466 welding Methods 0.000 description 8
- 230000005496 eutectics Effects 0.000 description 6
- 239000007791 liquid phase Substances 0.000 description 6
- 238000009792 diffusion process Methods 0.000 description 4
- 230000007704 transition Effects 0.000 description 4
- 230000005540 biological transmission Effects 0.000 description 3
- 150000001875 compounds Chemical class 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- 238000002844 melting Methods 0.000 description 3
- 229910017985 Cu—Zr Inorganic materials 0.000 description 2
- 230000009471 action Effects 0.000 description 2
- 238000006243 chemical reaction Methods 0.000 description 2
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- 239000011229 interlayer Substances 0.000 description 2
- 238000004321 preservation Methods 0.000 description 2
- 238000007711 solidification Methods 0.000 description 2
- 230000008023 solidification Effects 0.000 description 2
- 101100136092 Drosophila melanogaster peng gene Proteins 0.000 description 1
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 1
- 229910004349 Ti-Al Inorganic materials 0.000 description 1
- 229910004692 Ti—Al Inorganic materials 0.000 description 1
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 description 1
- 238000010521 absorption reaction Methods 0.000 description 1
- 230000003471 anti-radiation Effects 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000015556 catabolic process Effects 0.000 description 1
- 229910010293 ceramic material Inorganic materials 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 238000005520 cutting process Methods 0.000 description 1
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- 230000002542 deteriorative effect Effects 0.000 description 1
- 238000006073 displacement reaction Methods 0.000 description 1
- 238000002003 electron diffraction Methods 0.000 description 1
- 238000007731 hot pressing Methods 0.000 description 1
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- 230000008018 melting Effects 0.000 description 1
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- 230000000630 rising effect Effects 0.000 description 1
- 238000004098 selected area electron diffraction Methods 0.000 description 1
- 238000002490 spark plasma sintering Methods 0.000 description 1
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- 238000006467 substitution reaction Methods 0.000 description 1
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- 229910052726 zirconium Inorganic materials 0.000 description 1
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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
- 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
- C04B2237/12—Metallic interlayers
- C04B2237/124—Metallic interlayers based on copper
-
- 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
- C04B2237/40—Metallic
- C04B2237/407—Copper
-
- 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
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E30/00—Energy generation of nuclear origin
- Y02E30/30—Nuclear fission reactors
Abstract
The invention discloses a method for connecting Ti-Al-C system MAX phase ceramic and zirconium alloy, which aims to solve the problem that the strength of an obtained welded joint is low due to the fact that Zr-Al brittle intermetallic compounds with larger difference of thermal expansion coefficients with a base metal are inevitably generated between connecting surfaces in the conventional method for connecting Ti-Al-C system MAX phase ceramic and zirconium alloy. The connection method comprises the following steps: 1. pure copper is used as an intermediate layer; 2. mechanically polishing and polishing the surface to be connected of the Ti-Al-C system MAX phase ceramic and the zirconium alloy to be welded; 3. sequentially stacking the Ti-Al-C series MAX phase ceramic/intermediate layer/zirconium alloy in sequence to obtain a fitting to be welded; 4. and placing the assembly to be welded into a high-temperature vacuum furnace, and preserving heat at the temperature of 885-950 ℃. The invention avoids the generation of Zr-Al brittle phase, generates ZrC ceramic phase matched with the thermal expansion coefficient of the parent metal instead, and obviously improves the joint strength.
Description
Technical Field
The invention belongs to the field of metal and ceramic connection, and particularly relates to a connection method of Ti-Al-C series MAX phase ceramic and zirconium alloy.
Background
MAX phase is M n+1 AX n Is the generic name of a ternary layered ceramic of a chemical general formula, wherein M is a transition group metal, A is mainly a group IIIA and IVA element, X is C or N, and n=1 to 3. The MAX phase ceramic material has the excellent performances of ceramic and metal, wherein the Ti-Al-C system MAX phase ceramic has the excellent performances of good high-temperature oxidation resistance, damage resistance, high electrical conductivity, high thermal conductivity, easy processing and the like, is widely focused and researched, and particularly the Ti-Al-C system MAX phase ceramic has the excellent anti-radiation characteristic, thus becoming a nuclear energy structure candidate material with great prospect. Zirconium alloys are an indispensable material in nuclear power plants because zirconium has a low thermal neutron absorption cross section. Therefore, the realization of high-quality connection of Ti-Al-C series MAX phase ceramic and zirconium alloy is of great significance for the rapid development of the nuclear industry.
Barsoum team, university of American German patent Lei Saier, 2015 (TallmanDJ, yangJ, panL, et al, activity of zirconium-4 witti) 3 SiC 2 andTi 2 AlCInhe 1100-1300 ℃ temperature equipment, journal Nuclear materials,2015, 460:122-129) was previously reported with Ti 2 And connecting AlC ceramic with Zr-4 alloy. The test is carried out by adopting a vacuum hot-pressing furnace, the connection temperature is 1100-1300 ℃, the connection time is 1-30 h, and the vacuum degree is 10 -1 Pa, the connection pressure is 2.5MPa, and the literature finds that the Al element diffused in the MAX phase and Zr-4 alloy react at the interface to generate a large amount of Zr-Al brittle intermetallic compounds, and the joint is directly cracked after welding due to the overlarge difference between the thermal expansion coefficient of the Zr-Al intermetallic compounds and the difference between the thermal expansion coefficients of parent metals at two sides, so that connection cannot be realized. In addition, the connection temperature is higher than the phase transition temperature of the Zr-4 alloy (alpha-Zr at a temperature lower than 825 ℃ and two-phase coexistence area at 825-975 ℃ and converted into beta-Zr at a temperature higher than 975 ℃), and the heat preservation time is as long as several tens of hours at a temperature higher than the phase transition temperature, seriously deteriorating the performance of the base material. Subsequently, lu Bo of Tianjin university and Huang Qing of Ningbo Material institute of Chinese sciences et al successively reported the study of Ti using the Spark Plasma Sintering (SPS) method 3 AlC 2 Connection of ceramic to Zr-4 (Lu Bo. Current-assisted zirconium alloy to MAX phase Material Ti 3 AlC 2 Influence of connection and regulation study of connection interface thereof, university of Tianjin, 2016; boLu, xianjinYang, jieZhou the number of the individual pieces of the plastic,etal.Effect ofElectricCurrentonDiffusionofAluminuminTi 3 AlC 2 intozirconium malloy. Journal wuhan UniversityofTechnology (MaterialScienceEdition), 2017,32 (3): 645-649; yang Hui, lu Bo, yang Xianjin, shi Wen, zhou Xiaobing, li Peng, yellow peak, huang Qing. Ti under Current assisted heating 3 AlC 2 Zr interface study modern technical ceramics, 2017,38 (1): 48-56). It was found that Ti was achieved at a pressure of 22.2MPa and a temperature of 885 to 1050 ℃C 3 AlC 2 The connection with Zr-4, but the still brittle Zr-Al intermetallic compound generated between the interfaces, only the thickness of the obtained compound is reduced compared with Barsoum et Al, so that the obtained compound is not directly cracked after welding, but the strength test shows that the shear strength of the joint is extremely low, only 6.38MPa, and the use requirement cannot be met. In addition, the method aims at making Ti 3 AlC 2 Closely contacts with Zr-4 to provide a path for the diffusion of Al and Zr-4 in the ceramic, thus generally requiring a large pressure>10 MPa), but the high pressure applied during high temperature joining may cause severe plastic deformation of Zr-4 due to the low elastic modulus of Zr-4 alloy.
In summary, the method for connecting Ti-Al-C series MAX phase ceramic and zirconium alloy disclosed and reported at present has the following defects: 1. the joint connection strength is extremely low: because brittle Zr-Al intermetallic compounds with larger difference of thermal expansion coefficients with a base metal are inevitably generated in the joint, the joint strength is seriously weakened, even the joint is directly cracked after welding, and a firm joint cannot be obtained; 2. the connection temperature is higher or the heat preservation is carried out for a long time at the temperature higher than the phase transition temperature of the zirconium alloy, so that the performance degradation of the zirconium alloy parent metal is easy to cause; 3. the connecting pressure is high, the zirconium alloy base metal can be seriously plastically deformed at high temperature due to the high connecting pressure, and the ceramic is embedded into the zirconium alloy base metal under the action of pressure, so that the joint is formed poorly. There is therefore a need to develop a new type of connection method, which allows both a connection at a relatively low temperature and a low pressure and a high strength of the resulting joint.
Disclosure of Invention
The invention provides a method for connecting Ti-Al-C MAX phase ceramic and zirconium alloy, which aims to solve the problems that the existing method for connecting Ti-Al-C MAX phase ceramic and zirconium alloy uses high connecting temperature and high connecting pressure, and the strength of an obtained welded joint is extremely low and even cracks directly after welding due to unavoidable generation of Zr-Al brittle intermetallic compounds with larger difference of thermal expansion coefficients with a base metal between connecting surfaces.
The method for connecting the Ti-Al-C system MAX phase ceramic and the zirconium alloy is realized according to the following steps:
1. pure copper is used as an intermediate layer;
2. mechanically polishing and polishing surfaces to be connected of Ti-Al-C system MAX phase ceramic and zirconium alloy to be welded respectively, and then ultrasonically cleaning to obtain Ti-Al-C system MAX phase ceramic and zirconium alloy to be welded;
3. sequentially stacking the middle layer in the first step and the to-be-welded Ti-Al-C system MAX phase ceramic and the to-be-welded zirconium alloy in the sequence of the Ti-Al-C system MAX phase ceramic/middle layer/zirconium alloy, and applying certain pressure to obtain a to-be-welded assembly;
4. and (3) placing the assembly to be welded into a high-temperature vacuum furnace, preserving heat for 5-45 min at 885-950 ℃, and cooling to room temperature to finish the connection of the Ti-Al-C series MAX phase ceramic and the zirconium alloy.
The invention provides a method for connecting Ti-Al-C series MAX phase ceramic and zirconium alloy, which uses pure copper as an intermediate layer and connects at relatively low temperature and pressure, wherein the main connecting mechanism is as follows: on the zirconium alloy side, the copper interlayer and the zirconium alloy parent metal perform eutectic reaction at a lower temperature, a low-melting-point eutectic Cu-Zr liquid phase is generated between interfaces, and a transient liquid phase connection (TLP) joint with a dendritic structure is formed on the zirconium alloy side after isothermal solidification; on the MAX phase ceramic side, al in the Ti-Al-C system MAX phase ceramic is very active at high temperature and can be separated along the basal plane because of weak bonding of Ti-Al bonds, and is diffused to the eutectic liquid phase and the zirconium alloy side. The Ti-Al-C ceramic is decomposed to generate TiC when Al is removed; and finally, performing displacement reaction on Zr and TiC in the Zr-Cu low-melting eutectic liquid phase, so that ZrC is generated on the connecting surface, and the generation of a brittle Zr-Al phase is fundamentally avoided. Since the difference between the thermal expansion coefficient of ZrC and the Ti-Al-C based ceramics and zirconium alloy base materials is small, the residual stress generated in the cooling process at the connecting temperature is minimized, and thus, relatively high joint strength can be obtained.
Compared with the prior Ti-Al-C system MAX phase ceramic and zirconium alloy connection technology, the method for connecting the Ti-Al-C system MAX phase ceramic and the zirconium alloy has the following beneficial effects:
1. the joint strength is high: because the generation of a Zr-Al brittle phase is avoided in the joint, a ZrC ceramic phase matched with the thermal expansion coefficient of a base material is generated instead, and the joint strength is remarkably improved.
2. The welding temperature is relatively low: the connection temperature can be achieved only by preserving heat for a short time under the condition of obtaining a low-melting-point eutectic liquid phase, and the damage of high temperature to the performance of the zirconium alloy base material can be reduced to the greatest extent.
3. The welding pressure is small: during connection, the assembly is only carried out under a small pressure, and the problem that the joint is formed poorly because the zirconium alloy base metal is embedded into the zirconium alloy base metal under the action of pressure because the surface of the base metal is subjected to plastic deformation under a large pressure (more than 10 MPa) to promote the close contact of the materials and accelerate the diffusion of atoms between interfaces is avoided because the zirconium alloy base metal is subjected to severe plastic deformation under a high temperature as in the traditional diffusion welding.
4. The invention has simple and easy operation, enriches the technical variety of connecting Ti-Al-C series MAX phase ceramic and zirconium alloy, and has wide application prospect and great practical value.
Drawings
FIG. 1 is a graph showing Ti obtained under the conditions of 900 ℃/30min/10kPa using a 30 μm copper metal foil in example one 3 AlC 2 Low-power back-scattering electron photograph of interface structure of ceramic/Zr-4 alloy joint;
FIG. 2 is a graph showing Ti obtained at 900 ℃/30min/10kPa using a 30 μm copper metal foil in example one 3 AlC 2 High-power back scattering electron photograph of interface structure of ceramic/Zr-4 alloy joint;
FIG. 3 is a graph showing Ti obtained at 900 ℃/30min/10kPa using a 30 μm copper metal foil in example one 3 AlC 2 ceramic/Zr-4 alloyBack-scattered electron pictures of the joint near the ceramic side;
FIG. 4 is a high angle annular dark field photograph of a transmission electron microscope sample prepared using a focused plasma beam in example one;
FIG. 5 is a photograph of selected area electron diffraction spots of ZrC phase generated between the interfaces of the joints in the first embodiment.
Detailed Description
The first embodiment is as follows: the method for connecting the Ti-Al-C system MAX phase ceramic and the zirconium alloy according to the embodiment is implemented according to the following steps:
1. pure copper is used as an intermediate layer;
2. mechanically polishing and polishing surfaces to be connected of Ti-Al-C system MAX phase ceramic and zirconium alloy to be welded respectively, and then ultrasonically cleaning to obtain Ti-Al-C system MAX phase ceramic and zirconium alloy to be welded;
3. sequentially stacking the middle layer in the first step and the to-be-welded Ti-Al-C system MAX phase ceramic and the to-be-welded zirconium alloy in the sequence of the Ti-Al-C system MAX phase ceramic/middle layer/zirconium alloy, and applying certain pressure to obtain a to-be-welded assembly;
4. and (3) placing the assembly to be welded into a high-temperature vacuum furnace, preserving heat for 5-45 min at 885-950 ℃, and cooling to room temperature to finish the connection of the Ti-Al-C series MAX phase ceramic and the zirconium alloy.
In this embodiment, pure copper is used to join the Ti-Al-C-based MAX phase ceramic and the zirconium alloy at a temperature lower than the melting point of copper (1083 ℃).
The second embodiment is as follows: the first difference between the present embodiment and the specific embodiment is that the intermediate layer in the first step adopts a high-purity copper metal foil with purity greater than 99%, or a high-purity copper metal layer is electroplated or vapor deposited on the zirconium alloy to be welded as the intermediate layer.
And a third specific embodiment: the present embodiment differs from the first or second embodiment in that the thickness of the intermediate layer described in the first step is 5 to 100 μm.
The specific embodiment IV is as follows: the difference between the present embodiment and one to three embodiments is that the to-be-welded Ti-Al-C system MAX phase ceramic in the second step is Ti 2 AlC、Ti 3 AlC 2 Or Ti 4 AlC 3 And (3) ceramics.
Fifth embodiment: the difference between the present embodiment and one to three embodiments is that the to-be-welded Ti-Al-C system MAX phase ceramic in the second step is Ti 2 (Al 1-x Si x )C、Ti 3 (Al 1-x Si x )C 2 Or Ti 4 (Al 1-x Si x )C 3 Solid solution ceramics.
The Ti-Al-C system MAX phase ceramic to be welded in the embodiment is a solid solution ceramic obtained by partially replacing Al element in the Ti-Al-C system MAX phase ceramic by a plurality of main group elements such as Si.
Specific embodiment six: the difference between the present embodiment and one to fifth embodiments is that the zirconium alloy to be welded in the second step is a nuclear grade Zr-4 alloy, zr-2 alloy, zr-2.5Nb alloy, N18 alloy or N36 alloy having Zr content exceeding 95% by weight.
Seventh embodiment: the present embodiment differs from one to six of the embodiments in that the mechanical polishing described in step two is sequentially performed with 400# SiC sandpaper, 800# SiC sandpaper, 1500# SiC sandpaper, 2000# SiC sandpaper and 3000# SiC sandpaper, and the polishing is performed with 0.05 μm SiO 2 And (5) polishing the suspension.
SiO of the present embodiment 2 SiO in suspension 2 The particle size of (2) was 0.05. Mu.m.
Eighth embodiment: the present embodiment differs from one of the first to seventh embodiments in that the pressure applied in the third step is 0.005 to 0.5MPa.
Detailed description nine: the difference between the present embodiment and one to eighth embodiments is that the temperature rising speed is controlled to be 10-25 ℃/min in the fourth step.
Detailed description ten: the difference between the embodiment and one of the embodiments one to nine is that the cooling rate in the fourth step is 5-25 ℃/min.
Embodiment one: the method for connecting the Ti-Al-C system MAX phase ceramic and the zirconium alloy is implemented according to the following steps:
1. a high-purity copper metal foil with the purity of 99.99 percent and the thickness of 30 mu m is adopted as an intermediate layer;
2. respectively treat welded Ti 3 AlC 2 The surface to be connected of the ceramics and the Zr-4 alloy is mechanically ground and polished, wherein the mechanical grinding is sequentially carried out by using 400# SiC sand paper, 800# SiC sand paper, 1500# SiC sand paper, 2000# SiC sand paper and 3000# SiC sand paper, and the ground surface to be welded is Ti 3 AlC 2 The surface to be welded of the ceramic is made of SiO with the thickness of 0.05 mu m 2 Polishing the suspension, and then sequentially carrying out ultrasonic cleaning in soapy water, deionized water and absolute ethyl alcohol for 5min to obtain Ti to be welded 3 AlC 2 Ceramic and Zr-4 alloy to be welded;
3. the intermediate layer of the first step and the Ti to be welded of the second step are subjected to 3 AlC 2 The ceramic and the Zr-4 alloy to be welded are according to Ti 3 AlC 2 Sequentially stacking ceramic/high-purity copper metal foil/Zr-4 alloy, and applying pressure of 10kPa to obtain a fitting to be welded;
4. placing the assembly to be welded into a high-temperature vacuum furnace, controlling the heating rate to be 25 ℃/min, preserving the heat for 30min at 900 ℃, controlling the cooling rate to be 15 ℃/min, and cooling to room temperature to finish Ti 3 AlC 2 And connecting the ceramic with Zr-4 alloy.
Ti obtained in the present example 3 AlC 2 The shear strength of the ceramic and Zr-4 alloy joint is about 153.5MPa, which is far higher than that of Ti reported at present 3 AlC 2 Strength of ceramic and Zr-4 alloy joint<10 MPa), indicating that high quality Ti can be obtained by the method of this example 3 AlC 2 The ceramic is connected with Zr-4 alloy.
In this example, ti obtained at 900 ℃/30min/10kPa using a 30 μm copper interlayer 3 AlC 2 Low-power and high-power back-scattered electron photographs of the interface structure of the ceramic/Zr-4 alloy joint are shown in fig. 1 and 2, respectively.
It can be seen from FIGS. 1 and 2 that the joint obtained by the method of this example was dense and free of any defects such as cracks, and the joint connection quality was high, and the Zr-4 alloy did not undergo plastic deformation. The Cu metal foil and Zr-4 alloy in the connection completely react, no copper residue is observed between interfaces, a diffusion reaction zone with the thickness of about 60 mu m is observed in the center of a welding line, the elements in the layer still occupy most of Zr, only a certain change in microstructure is generated, and the performance is shownIs dendritic in structure, which is a typical structure obtained after isothermal solidification of the weld. Further observation of the ceramic side in magnification, as shown in FIG. 3, it can be seen that the ceramic side is close to Ti 3 AlC 2 A grey compound layer is formed on the side and the layer thickness is not uniform. In order to determine that the ZrC phase is generated in the joint, the joint is precisely cut by adopting a focused plasma beam (FIB) technology, and a transmission electron microscope sample is prepared, wherein the cutting position corresponds to the position shown by a black rectangular frame in fig. 3. Fig. 4 gives a high angle annular dark field photograph of a transmitted sample from which it can also be seen that the joint connection is dense. The diffraction pattern photo shown in FIG. 5 was obtained by performing selective electron diffraction operation using the phase in the transmission electron microscope joint, and ZrC was confirmed to be generated in the joint by calibrating the diffraction spots, with the crystallographic band axis of [0-11 ]]. ZrC is generated mainly due to Ti 3 AlC 2 Al has higher activity at high temperature, and is derived from Ti 3 AlC 2 The TiC is generated by the medium-out, and further the substitution reaction of the Cu-Zr low-melting eutectic liquid phase and the TiC is carried out: tiC+ [ Zr ]]→ZrC+[Ti]Thereby generating ZrC between the connection interfaces, due to ZrC and Ti 3 AlC 2 The difference between the thermal expansion coefficients of the metal and Zr-4 is small, so that the joint has higher strength.
Claims (8)
- A method for connecting Ti-Al-C series MAX phase ceramic and zirconium alloy is characterized in that the connecting method is realized according to the following steps:1. pure copper is used as an intermediate layer;2. mechanically polishing and polishing surfaces to be connected of Ti-Al-C system MAX phase ceramic and zirconium alloy to be welded respectively, and then ultrasonically cleaning to obtain Ti-Al-C system MAX phase ceramic and zirconium alloy to be welded;3. sequentially stacking the middle layer of the first step and the to-be-welded Ti-Al-C system MAX phase ceramic and the to-be-welded zirconium alloy according to the sequence of the Ti-Al-C system MAX phase ceramic/middle layer/zirconium alloy, and applying pressure of 0.005-0.5 MPa to obtain a to-be-welded assembly;4. placing the assembly to be welded into a high-temperature vacuum furnace, preserving heat for 5-45 min at 885-950 ℃, and cooling to room temperature to finish the connection of the Ti-Al-C series MAX phase ceramic and the zirconium alloy;the thickness of the intermediate layer in the first step is 5-100 μm.
- 2. The method for joining a Ti-Al-C MAX phase ceramic and a zirconium alloy according to claim 1, wherein the intermediate layer in the first step is a high purity copper metal foil having a purity of more than 99%, or a high purity copper metal layer is plated or vapor deposited on the zirconium alloy to be welded as the intermediate layer.
- 3. The method for joining a Ti-Al-C system MAX phase ceramic and a zirconium alloy according to claim 1, wherein the Ti-Al-C system MAX phase ceramic to be welded in the second step is Ti 2 AlC、Ti 3 AlC 2 Or Ti 4 AlC 3 And (3) ceramics.
- 4. The method for joining a Ti-Al-C system MAX phase ceramic and a zirconium alloy according to claim 1, wherein the Ti-Al-C system MAX phase ceramic to be welded in the second step is Ti 2 (Al 1-x Si x )C、Ti 3 (Al 1-x Si x )C 2 Or Ti 4 (Al 1-x Si x )C 3 Solid solution ceramics.
- 5. The method for joining a Ti-Al-C MAX phase ceramic and a zirconium alloy according to claim 1, wherein the zirconium alloy to be welded in the second step is a nuclear grade Zr-4 alloy, zr-2 alloy, zr-2.5Nb alloy, N18 alloy or N36 alloy having Zr content exceeding 95% by weight.
- 6. The method for joining a Ti-Al-C system MAX phase ceramic and a zirconium alloy according to claim 1, wherein the mechanical polishing in the second step is polishing with 400# SiC sand paper, 800# SiC sand paper, 1500# SiC sand paper, 2000# SiC sand paper and 3000# SiC sand paper in this order, and the polishing is performed with 0.05 μm SiO 2 And (5) polishing the suspension.
- 7. The method for joining a Ti-Al-C MAX phase ceramic and a zirconium alloy according to claim 1, wherein the heating rate is controlled to be 10 to 25 ℃/min in the fourth step.
- 8. The method for connecting Ti-Al-C system MAX phase ceramic and zirconium alloy according to claim 1, which is characterized in that the cooling rate in the fourth step is 5-25 ℃/min.
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