CN114147388A - A kind of yttria-stabilized zirconia solid-state phase change composite brazing filler metal and preparation method thereof - Google Patents
A kind of yttria-stabilized zirconia solid-state phase change composite brazing filler metal and preparation method thereof Download PDFInfo
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- 229910052751 metal Inorganic materials 0.000 title claims abstract description 82
- 239000002184 metal Substances 0.000 title claims abstract description 82
- 239000002131 composite material Substances 0.000 title claims abstract description 71
- 229910001233 yttria-stabilized zirconia Inorganic materials 0.000 title claims abstract description 65
- 238000005219 brazing Methods 0.000 title claims abstract description 63
- 239000000945 filler Substances 0.000 title claims abstract description 44
- 230000008859 change Effects 0.000 title claims abstract description 20
- 238000002360 preparation method Methods 0.000 title claims abstract description 20
- 238000006263 metalation reaction Methods 0.000 title 1
- 239000000919 ceramic Substances 0.000 claims abstract description 86
- 239000002245 particle Substances 0.000 claims abstract description 62
- 239000000843 powder Substances 0.000 claims abstract description 40
- 230000007704 transition Effects 0.000 claims abstract description 10
- 239000011159 matrix material Substances 0.000 claims abstract description 9
- 238000005728 strengthening Methods 0.000 claims abstract description 6
- 229910000679 solder Inorganic materials 0.000 claims description 47
- 239000010949 copper Substances 0.000 claims description 18
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 14
- 229910052802 copper Inorganic materials 0.000 claims description 14
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 13
- 238000000034 method Methods 0.000 claims description 13
- 239000000463 material Substances 0.000 claims description 12
- 238000000498 ball milling Methods 0.000 claims description 10
- 230000008569 process Effects 0.000 claims description 8
- 239000011248 coating agent Substances 0.000 claims description 4
- 238000000576 coating method Methods 0.000 claims description 4
- 230000004907 flux Effects 0.000 claims description 4
- 239000000203 mixture Substances 0.000 claims description 4
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 3
- 238000001816 cooling Methods 0.000 claims description 3
- 238000000227 grinding Methods 0.000 claims description 3
- 238000010438 heat treatment Methods 0.000 claims description 3
- 239000007769 metal material Substances 0.000 claims description 3
- 238000003980 solgel method Methods 0.000 claims description 3
- 238000005303 weighing Methods 0.000 claims description 3
- 238000007664 blowing Methods 0.000 claims 1
- 238000003466 welding Methods 0.000 abstract description 4
- 239000012071 phase Substances 0.000 description 38
- MCMNRKCIXSYSNV-UHFFFAOYSA-N ZrO2 Inorganic materials O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 description 20
- 239000007790 solid phase Substances 0.000 description 11
- 230000009466 transformation Effects 0.000 description 9
- 229910017945 Cu—Ti Inorganic materials 0.000 description 7
- 239000010410 layer Substances 0.000 description 7
- RUDFQVOCFDJEEF-UHFFFAOYSA-N yttrium(III) oxide Inorganic materials [O-2].[O-2].[O-2].[Y+3].[Y+3] RUDFQVOCFDJEEF-UHFFFAOYSA-N 0.000 description 7
- 229910009817 Ti3SiC2 Inorganic materials 0.000 description 6
- 238000006243 chemical reaction Methods 0.000 description 6
- 238000005476 soldering Methods 0.000 description 5
- 238000012360 testing method Methods 0.000 description 5
- 239000010953 base metal Substances 0.000 description 4
- 239000010936 titanium Substances 0.000 description 4
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- 239000011148 porous material Substances 0.000 description 3
- 239000002994 raw material Substances 0.000 description 3
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- 238000013329 compounding Methods 0.000 description 2
- 150000001875 compounds Chemical class 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- SIWVEOZUMHYXCS-UHFFFAOYSA-N oxo(oxoyttriooxy)yttrium Chemical compound O=[Y]O[Y]=O SIWVEOZUMHYXCS-UHFFFAOYSA-N 0.000 description 2
- 238000010587 phase diagram Methods 0.000 description 2
- 238000012545 processing Methods 0.000 description 2
- 238000011946 reduction process Methods 0.000 description 2
- 239000007787 solid Substances 0.000 description 2
- 238000003756 stirring Methods 0.000 description 2
- 229910017693 AgCuTi Inorganic materials 0.000 description 1
- 241001279686 Allium moly Species 0.000 description 1
- DXZIFGZIQQRESB-UHFFFAOYSA-N [C].[Ti].[Si] Chemical compound [C].[Ti].[Si] DXZIFGZIQQRESB-UHFFFAOYSA-N 0.000 description 1
- 238000000861 blow drying Methods 0.000 description 1
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- 238000010008 shearing Methods 0.000 description 1
- 229910052709 silver Inorganic materials 0.000 description 1
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Classifications
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B23—MACHINE TOOLS; METAL-WORKING NOT OTHERWISE PROVIDED FOR
- B23K—SOLDERING OR UNSOLDERING; WELDING; CLADDING OR PLATING BY SOLDERING OR WELDING; CUTTING BY APPLYING HEAT LOCALLY, e.g. FLAME CUTTING; WORKING BY LASER BEAM
- B23K35/00—Rods, electrodes, materials, or media, for use in soldering, welding, or cutting
- B23K35/22—Rods, electrodes, materials, or media, for use in soldering, welding, or cutting characterised by the composition or nature of the material
- B23K35/36—Selection of non-metallic compositions, e.g. coatings, fluxes; Selection of soldering or welding materials, conjoint with selection of non-metallic compositions, both selections being of interest
- B23K35/3601—Selection of non-metallic compositions, e.g. coatings, fluxes; Selection of soldering or welding materials, conjoint with selection of non-metallic compositions, both selections being of interest with inorganic compounds as principal constituents
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B23—MACHINE TOOLS; METAL-WORKING NOT OTHERWISE PROVIDED FOR
- B23K—SOLDERING OR UNSOLDERING; WELDING; CLADDING OR PLATING BY SOLDERING OR WELDING; CUTTING BY APPLYING HEAT LOCALLY, e.g. FLAME CUTTING; WORKING BY LASER BEAM
- B23K1/00—Soldering, e.g. brazing, or unsoldering
- B23K1/0008—Soldering, e.g. brazing, or unsoldering specially adapted for particular articles or work
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B23—MACHINE TOOLS; METAL-WORKING NOT OTHERWISE PROVIDED FOR
- B23K—SOLDERING OR UNSOLDERING; WELDING; CLADDING OR PLATING BY SOLDERING OR WELDING; CUTTING BY APPLYING HEAT LOCALLY, e.g. FLAME CUTTING; WORKING BY LASER BEAM
- B23K35/00—Rods, electrodes, materials, or media, for use in soldering, welding, or cutting
- B23K35/02—Rods, electrodes, materials, or media, for use in soldering, welding, or cutting characterised by mechanical features, e.g. shape
- B23K35/0222—Rods, electrodes, materials, or media, for use in soldering, welding, or cutting characterised by mechanical features, e.g. shape for use in soldering, brazing
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B23—MACHINE TOOLS; METAL-WORKING NOT OTHERWISE PROVIDED FOR
- B23K—SOLDERING OR UNSOLDERING; WELDING; CLADDING OR PLATING BY SOLDERING OR WELDING; CUTTING BY APPLYING HEAT LOCALLY, e.g. FLAME CUTTING; WORKING BY LASER BEAM
- B23K35/00—Rods, electrodes, materials, or media, for use in soldering, welding, or cutting
- B23K35/22—Rods, electrodes, materials, or media, for use in soldering, welding, or cutting characterised by the composition or nature of the material
- B23K35/36—Selection of non-metallic compositions, e.g. coatings, fluxes; Selection of soldering or welding materials, conjoint with selection of non-metallic compositions, both selections being of interest
- B23K35/3601—Selection of non-metallic compositions, e.g. coatings, fluxes; Selection of soldering or welding materials, conjoint with selection of non-metallic compositions, both selections being of interest with inorganic compounds as principal constituents
- B23K35/3602—Carbonates, basic oxides or hydroxides
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B23—MACHINE TOOLS; METAL-WORKING NOT OTHERWISE PROVIDED FOR
- B23K—SOLDERING OR UNSOLDERING; WELDING; CLADDING OR PLATING BY SOLDERING OR WELDING; CUTTING BY APPLYING HEAT LOCALLY, e.g. FLAME CUTTING; WORKING BY LASER BEAM
- B23K35/00—Rods, electrodes, materials, or media, for use in soldering, welding, or cutting
- B23K35/22—Rods, electrodes, materials, or media, for use in soldering, welding, or cutting characterised by the composition or nature of the material
- B23K35/36—Selection of non-metallic compositions, e.g. coatings, fluxes; Selection of soldering or welding materials, conjoint with selection of non-metallic compositions, both selections being of interest
- B23K35/362—Selection of compositions of fluxes
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B23—MACHINE TOOLS; METAL-WORKING NOT OTHERWISE PROVIDED FOR
- B23K—SOLDERING OR UNSOLDERING; WELDING; CLADDING OR PLATING BY SOLDERING OR WELDING; CUTTING BY APPLYING HEAT LOCALLY, e.g. FLAME CUTTING; WORKING BY LASER BEAM
- B23K2103/00—Materials to be soldered, welded or cut
- B23K2103/50—Inorganic material, e.g. metals, not provided for in B23K2103/02 – B23K2103/26
- B23K2103/52—Ceramics
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- Engineering & Computer Science (AREA)
- Mechanical Engineering (AREA)
- Chemical & Material Sciences (AREA)
- Inorganic Chemistry (AREA)
- Ceramic Products (AREA)
Abstract
本发明提供了一种基于氧化钇稳定氧化锆固态相变新型复合钎料及其制备方法，解决了传统复合钎料在针对大尺寸陶瓷/金属构件的钎焊连接时无法满足焊缝区域较低宏观残余应力和较高断裂韧性的要求这一技术问题。本发明选用具有固态相变性质的氧化钇稳定氧化锆陶瓷颗粒作为金属基复合钎料的强化相，并以Ag‑Cu‑2Ti粉末作为复合钎料的金属基体，随后在制备得到的复合钎料表面添加多孔金属网，最终实现YSZ、Ag‑Cu‑2Ti和多孔金属网的复合。
The invention provides a new type of composite brazing filler metal based on yttria-stabilized zirconia solid-state phase transition and a preparation method thereof, which solves the problem that the traditional composite brazing filler metal cannot meet the requirements of low macroscopical welding seam area when brazing connection of large-sized ceramic/metal components. Residual stress and higher fracture toughness requirements are technical issues. In the present invention, yttria-stabilized zirconia ceramic particles with solid-state phase change properties are selected as the strengthening phase of the metal-based composite brazing filler metal, and Ag-Cu-2Ti powder is used as the metal matrix of the composite brazing filler metal. The porous metal mesh is added to the surface, and finally the composite of YSZ, Ag‑Cu‑2Ti and porous metal mesh is realized.
Description
Technical Field
The invention belongs to the technical field of ceramic/metal brazing, and particularly relates to a novel solid-state phase change composite brazing filler metal based on yttria-stabilized zirconia and a preparation method thereof.
Background
The composite member of ceramic and metal materials has the advantages of high strength, corrosion resistance, wear resistance and good high-temperature stability of ceramic, easy processing, high toughness and excellent heat and electric conductivity of metal, and can meet the use requirements of harsh environments or higher technical indexes. The brazing connection is an important method for obtaining the ceramic/metal joint, and has the advantages of simple operation, strong repeatability, easy industrial production and the like. The residual stress is an important factor influencing the service performance of the ceramic/metal soldered joint, and aiming at the problem, methods including an intermediate layer, surface processing, composite solder and the like are proposed to regulate and control the residual stress in the process of preparing the soldered joint.
Compared with the other two methods, the composite brazing filler metal method has the advantages of relatively simple preparation process, convenient regulation and control of mechanical properties and the like. However, the conventional composite brazing filler metal still has obvious defects in the brazing connection of large-size ceramic/metal components, and cannot meet the requirements of a lower macroscopic residual stress and higher fracture toughness of a welding seam area.
Disclosure of Invention
The invention aims to solve the technical problem that the traditional composite solder can not meet the requirements of lower macroscopic residual stress and higher fracture toughness of a welding line region when the traditional composite solder is used for the braze welding connection of large-size ceramic/metal components, and provides a novel solid-state phase-change composite solder based on yttria stabilized zirconia and a preparation method thereof.
In order to achieve the purpose, the technical solution provided by the invention is as follows:
the novel composite brazing filler metal based on the solid-state phase change of the yttria-stabilized zirconia is characterized in that: comprises Ag-Cu-2Ti powder, yttria-stabilized zirconia ceramic particles with solid phase change property, a soldering paste and a porous metal mesh;
preparing composite solder powder by taking Ag-Cu-2Ti powder as a metal matrix and yttria-stabilized zirconia ceramic particles with solid phase change property as a strengthening phase;
the composite brazing filler metal powder is prepared into a paste brazing filler metal through a flux paste, then the paste brazing filler metal is uniformly coated on a ceramic base metal to be welded, and the porous metal mesh is compounded on the surface of the base metal, which is in contact with a joint to be welded, so that a novel composite brazing filler metal is formed;
y in the yttria-stabilized zirconia ceramic particles2O3The mole fraction of the raw materials is 0.6 +/-0.05 mol percent, and the specific raw material ratio is according to Y2O3-ZrO2The phase diagram of the compound is determined, and the main component phase of the yttria-stabilized zirconia ceramic particles at room temperature is t-ZrO2Phase sum m-ZrO2Phase, t-ZrO in the course of heating to 400-600 ℃2Phase transformation into m-ZrO2Phase (1); during cooling, m-ZrO2Phase transformation to t-ZrO2And (4) phase(s).
Further, the mass fraction of the yttria-stabilized zirconia ceramic particles in the composite solder powder is 6 +/-0.5 wt%;
the particle size of the yttria-stabilized zirconia ceramic particles is 1 mu m, and the purity is not lower than 99.9%; in order to ensure that the yttria-stabilized zirconia ceramic particles are not consumed in the brazing filler metal due to over reaction with the brazing filler metal and ensure that the yttria-stabilized zirconia ceramic particles can be uniformly mixed in Ag-Cu-Ti powder (the particle size of the powder is 300 meshes), yttria-stabilized zirconia ceramic particles with excessively small particle size (reaching the size of nanometer level) are not selected.
Further, the coating thickness of the paste solder is 100-200 μm.
Further, the ceramic base material to be welded is Ti3SiC2A ceramic; the expanded metal is an expanded copper mesh in view of performance and cost.
The invention provides a preparation method of a novel solid phase change composite solder based on yttria stabilized zirconia, which is characterized by comprising the following steps:
1) preparation of composite solder powder
Weighing Ag-Cu-2Ti powder and yttria-stabilized zirconia ceramic particles with solid phase change property, and performing ball milling to obtain composite solder powder;
2) preparation of novel composite solder
Uniformly mixing and stirring the soldering paste and the composite brazing filler metal powder prepared in the step 1) to prepare a paste brazing filler metal, uniformly coating the paste brazing filler metal on the surface of a ceramic base metal to be welded, and then coating a layer of porous metal mesh subjected to ultrasonic cleaning and blow-drying to obtain the novel composite brazing filler metal.
Further, the step 1) is specifically as follows:
weighing Ag-Cu-2Ti powder and yttria-stabilized zirconia ceramic particles with solid phase change property, putting the Ag-Cu-2Ti powder and the yttria-stabilized zirconia ceramic particles into an agate tank, and putting alumina grinding balls into the agate tank; and covering the agate tank, putting the agate tank into a ball mill for ball milling, and obtaining the composite solder powder after the ball milling is finished.
Further, in the step 1), the ball-to-material ratio in the agate tank is 8: 1-12: 1;
the technological parameters of the ball milling are as follows: the rotating speed is 180-220 r/min, and the time is 8 +/-0.5 h;
the ball mill is a planetary ball mill.
Further, in step 2), the expanded metal is ultrasonically cleaned for at least 10 minutes before use and is dried by a blower.
Further, in step 1), the yttria-stabilized zirconia ceramic particles are formed by Y2O3Particles and ZrO2The particles are prepared by a sol-gel method.
A composite member of ceramic and metal materials is characterized in that: the novel composite brazing filler metal is adopted for brazing.
The mechanism of the invention is as follows:
considering that solid-state phase transformation occurs in the temperature reduction process of zirconia, the solid-state phase transformation causes volume abnormal expansion phenomenon different from most substances, but the phase transformation temperature is generally high, the yttrium oxide is added to reduce the phase transformation temperature point, so that the yttrium oxide can be applied to brazing. The method comprises the steps of analyzing the solid phase transition characteristics of yttria-stabilized zirconia to determine the content of yttria in YSZ ceramic particles and the content of YSZ ceramic particles in a composite solder, then doping and mixing YSZ ceramic particles and Ag-Cu-2Ti powder to obtain composite solder powder with uniform components, uniformly stirring the composite solder powder with a soldering paste to obtain a paste solder, and finally compounding the paste solder powder with a porous copper mesh to obtain the required composite solder; the invention adopts YSZ ceramic particles as a strengthening phase of the composite solder, absorbs the residual strain energy by utilizing solid phase change caused by temperature reduction and residual stress in the temperature reduction process of YSZ, and hinders crack propagation by utilizing the characteristic of volume abnormal expansion in the phase change process so as to realize the effects of reducing the residual stress of the joint and improving the toughness of the joint.
The invention has the advantages that:
1. the invention selects Yttria Stabilized Zirconia (YSZ) ceramic particles with solid phase change property as a strengthening phase of the metal-based composite solder, uses Ag-Cu-2Ti powder as a metal matrix of the composite solder, and then adds a porous metal net (such as a porous copper net) on the surface of the prepared composite solder to finally realize the compounding of YSZ, Ag-Cu-2Ti and the porous metal net.
2. The preparation process of the composite solder is simple and can be finished by adopting conventional equipment. Compared with the joint obtained by brazing with the traditional Ag-Cu-Ti brazing filler metal, the strength and plasticity of the joint can be obviously improved by adding YSZ and using the porous copper mesh, and the shear strength of the joint obtained by brazing with the brazing filler metal with the optimal proportion is improved by 45 percent compared with that of the joint obtained by brazing without stabilizing zirconia ceramic particles by using yttria, and reaches 86 +/-2.0 MPa; therefore, the composite solder of the invention has a great promoting effect on the development of the regulation and control of the residual stress of the ceramic/metal soldered joint, can successfully realize the soldered connection of ceramic and metal, reduces the residual stress of the ceramic/metal soldered joint and improves the mechanical property and the service reliability of the ceramic/metal soldered joint.
Drawings
FIG. 1 shows 0.6% molY at room temperature2O3The added amounts of YSZ ceramic particles are analyzed by XRD phase and DSC test results, wherein (a) is analyzed by XRD phase and (b) is tested by DSC.
FIG. 2 is an XRD phase analysis diagram of the AgCuTi + YSZ ceramic particles.
FIG. 3 is a schematic view of the assembly of a brazing sample.
FIG. 4 is the temperature of 900 ℃ for 10min, Ti3SiC2The typical interface structure of ceramic/Ag-Cu-Ti +6 wt% YSZ ceramic particle composite solder + porous metal interlayer Cu net/red copper soldered joint.
FIG. 5 is a graph of YSZ ceramic particle content versus Ti at 900 deg.C for 10min3SiC2Influence rule of the shearing strength of the ceramic/red copper brazing connecting joint.
Detailed Description
The invention provides a novel composite solder, which can effectively reduce the residual stress of a ceramic/metal soldered joint and has mechanical property and service reliability. The invention is described in further detail below with reference to the following figures and specific examples:
example 1
The preparation method of the novel composite solder comprises the following steps:
1) preparation of YSZ ceramic particles
YSZ ceramic particles with Y2O3Particles and ZrO2The particles are prepared by a sol-gel method, and the raw material proportion is according to Y2O3-ZrO2Phase diagram of a compound, wherein Y2O3The mole fraction is 0.6 mol%, the granularity of the ceramic particles is 1 mu m, and the purity is not lower than 99.9%. The XRD phase analysis diagram and DSC curve of the prepared YSZ ceramic particles are shown in figure 1, and the phase composition and the phase transition bursting point are combined with the expected requirements.
From the results of the XED analysis, 0.6 wt% molY2O3The added YSZ ceramic particles have t-ZrO as main phase composition at room temperature2Phase sum m-ZrO2Consistent with the expected results. DSC test analysis shows that during heating, t-ZrO2Phase transformation into m-ZrO2The phase explosion temperature point is about 500 ℃, the whole phase transition temperature interval is about 400 ℃ to 600 ℃, and the volume expansion of the phase transition process is about 8 percent due to the t-ZrO2 phase and the m-ZrO2The phase-to-phase transition is reversible and therefore the same phase change occurs during cooling.
2) Mixing of YSZ ceramic particles with metallic brazing filler metal powder (i.e. preparing composite brazing filler metal powder)
Ag-Cu-2Ti metal solder powder and YSZ ceramic particle powder accounting for 6 wt% of YSZ ceramic particle powder are weighed, then placed into an agate tank, and placed into an alumina grinding ball according to the ball-to-material ratio within the range of 10: 1). And covering the agate tank, putting the agate tank into a planetary ball mill, and setting the rotating speed at 200r/min for 8 hours. And after the ball milling time is over, taking out the milling balls in the agate tank, and bagging the mixed composite solder for later use.
XRD detection and analysis of the composite solder uniformly mixed by ball milling are shown in figure 2, and the phase composition of the composite solder after ball milling is Ag, Cu and m-ZrO2Phase sum t-ZrO2The phases show that the doping process of the YSZ ceramic particles and the Ag-Cu-Ti powder brazing filler metal does not have any reaction, and the phases of the ceramic particles serving as a strengthening phase and the metal powder serving as a matrix do not have any change.
3) Final preparation of novel composite solder
Commercial soldering paste and a proper amount of ball-milled composite solder powder are mixed and stirred uniformly to prepare paste solder, and the paste solder is uniformly coated on Ti to be welded3SiC2The surface of the ceramic base material can be 100-200 mu m, and then a layer of porous copper mesh which is ultrasonically cleaned for 10min and dried by a blower is coated on the surface of the ceramic base material to obtain the novel composite brazing filler metal (not including Ti to be welded)3SiC2A ceramic base material).
In order to verify whether the novel composite brazing filler metal prepared in the embodiment 1 meets the requirements during brazing connection, a ceramic metal brazing test is further performed in the embodiment, specifically as follows:
pressing pure copper base materials to be welded on the basis of the step 3), and realizing final assembly of the brazing sample as shown in figure 3. Then, a brazing test is carried out, the brazing process parameter is 900 ℃, the temperature is kept for 10min, the obtained joint interface structure morphology is shown in figure 4, and the obtained joint interface morphology is Ti3SiC2The typical interface structure of ceramic/Ag-Cu-Ti +6 wt% YSZ ceramic particle composite solder + porous metal interlayer Cu net/red copper soldered joint can be seen that the interface is tightly combined without obvious defects of cracks or holes, the leftmost and rightmost sides are respectively titanium silicon carbon ceramic and red copper base metal, the middle area 1 and the area 2 are respectively a solder and ceramic diffusion reaction area and composite solder, the area 1 is composite solder and Ti3SiC2A reactive layer between the ceramic substrates, having a width of about 130 μm, consisting essentially of grey platelet structuresThe structure is a porous metal interlayer Cu net clad solder and Ti3SiC2The ceramic matrix reaction product fills the lamellar structure formed by pores, and a large number of black pores are formed on the interface of the ceramic matrix reaction product, wherein the black pores are Ti3SiC2The defect of the ceramic matrix is not a brazing connection reaction product, the area 2 is a reaction layer between the Ag-Cu-Ti composite brazing filler metal and the red copper matrix, the width of the reaction layer is about 100 mu m, the reaction layer is mainly composed of a gray network (Ag-based solid solution structure) and a small amount of white point-shaped particles (Cu-based solid solution structure) which are dispersedly distributed, and in addition, the gray network (Ag-based solid solution structure) is uniformly adhered with a small amount of black point-shaped particles (yttria-stabilized zirconia ceramic particles) which are dispersedly distributed; while the joint shear strength was tested to reach about 80MPa as shown by the 6 wt% panel in fig. 5.
Example 2
This example is a set of examples, and differs from example 1 in that the addition amounts of YSZ ceramic particles in the Ag-Cu-Ti solder in step 2) are 0 wt%, 2 wt%, 4 wt%, 8 wt%, and 10 wt%, respectively. Ti brazing to composite brazing filler metals prepared in various examples3SiC2The ceramic/red copper soldered joints were all tested for shear strength, the results are shown in fig. 5, and the soldering parameters were all maintained at 900 ℃ for 10 min. The 6 wt% YSZ is example 1, the remaining variables are example 2.
The result shows that in a certain range, along with the increase of the content of YSZ ceramic particles, more ceramic particles capable of generating solid phase transformation exist on the interface, the residual compressive stress generated by the solid phase transformation can relieve the residual stress generated by the mismatch of the expansion coefficients of the base materials, and meanwhile, the solid residual compressive stress can also inhibit the crack expansion on the joint interface, improve the interface structure and improve the performance of the joint; however, when the content of YSZ ceramic particles is too high, the wettability of the solder is drastically reduced, resulting in poor metallurgical bonding at the joint interface and reduced shear strength.
When the mass fraction of the yttria-stabilized zirconia ceramic particles in the composite solder powder is 4-8%, the performance of the joint is improved compared with that of the existing joint, and particularly the ratio of the yttria-stabilized zirconia in the solder is 6 wt% at best.
Example 3
The mole fraction of yttria in the yttria-stabilized zirconia of this example was tested in the preferred range; it has been found that the molar fraction of yttria should not fluctuate beyond 0.05 mol%, 0.6 mol% being the amount of zirconia in each set of examples which undergoes a solid state phase transition at the optimum temperature point.
In addition, corresponding tests are also carried out on other process parameter ranges (such as a ball-material ratio of 8: 1-12: 1, a rotating speed of 180-220 r/min and time of 8 +/-0.5 h), and the results show that the influence of the change of the parameters on the performance is small.
While the invention has been described with reference to specific embodiments, the invention is not limited thereto, and various equivalent modifications and substitutions can be easily made by those skilled in the art within the technical scope of the present disclosure.
Claims (10)
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN116100188A (en) * | 2023-03-01 | 2023-05-12 | 内蒙金属材料研究所 | A kind of aluminum alloy flux-cored welding wire modified by micro-nano particles and its preparation method and application |
| CN116551241A (en) * | 2023-05-10 | 2023-08-08 | 华中科技大学 | A kind of crackless aluminum alloy flux-cored welding wire and its preparation method and application |
Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US4624897A (en) * | 1983-06-17 | 1986-11-25 | Ngk Spark Plug Co., Ltd. | Clad brazing filler for bonding ceramic to metal, glass, or other ceramic and composites using such filler |
| CN1544196A (en) * | 2003-11-17 | 2004-11-10 | 哈尔滨工业大学 | Mechanical alloying preparation method of ceramic particle reinforced composite solder |
| CN101288928A (en) * | 2008-05-09 | 2008-10-22 | 中国科学技术大学 | Ceramic Particle Reinforced Composite Solder |
| CN102513720A (en) * | 2011-12-23 | 2012-06-27 | 哈尔滨工业大学深圳研究生院 | High-performance tin-based solder alloy and preparation method thereof |
-
2021
- 2021-11-15 CN CN202111345011.XA patent/CN114147388A/en active Pending
Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US4624897A (en) * | 1983-06-17 | 1986-11-25 | Ngk Spark Plug Co., Ltd. | Clad brazing filler for bonding ceramic to metal, glass, or other ceramic and composites using such filler |
| CN1544196A (en) * | 2003-11-17 | 2004-11-10 | 哈尔滨工业大学 | Mechanical alloying preparation method of ceramic particle reinforced composite solder |
| CN101288928A (en) * | 2008-05-09 | 2008-10-22 | 中国科学技术大学 | Ceramic Particle Reinforced Composite Solder |
| CN102513720A (en) * | 2011-12-23 | 2012-06-27 | 哈尔滨工业大学深圳研究生院 | High-performance tin-based solder alloy and preparation method thereof |
Non-Patent Citations (4)
| Title |
|---|
| H.Y.CHEN ET AL.: "Effects of surface microstructure on the active element content and wetting behavior of brazing filler metal during brazing Ti3SiC2 ceramic and Cu", 《VACUUM》 * |
| HAIYAN CHEN ET AL.: "Improvement for Interfacial Microstructure and Mechanical Properties of Ti3SiC2-Cu Joint Brazed by Ag-Cu-Ti Filler with Copper Mesh", 《CRYSTALS》 * |
| 杨鹏飞等: "平板式SOFC封接的实验研究", 《中国科学技术大学学报》 * |
| 马伟民: "《氧化物陶瓷刀具与仿真切削》", 31 October 2014 * |
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN116100188A (en) * | 2023-03-01 | 2023-05-12 | 内蒙金属材料研究所 | A kind of aluminum alloy flux-cored welding wire modified by micro-nano particles and its preparation method and application |
| CN116100188B (en) * | 2023-03-01 | 2025-02-28 | 内蒙金属材料研究所 | Aluminum alloy flux-cored welding wire modified by micro-nano particles and preparation method and application thereof |
| CN116551241A (en) * | 2023-05-10 | 2023-08-08 | 华中科技大学 | A kind of crackless aluminum alloy flux-cored welding wire and its preparation method and application |
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