CN115383343B - Sn-based lead-free composite solder based on core-shell structure reinforced phase reinforcement - Google Patents
Sn-based lead-free composite solder based on core-shell structure reinforced phase reinforcement Download PDFInfo
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- 229910000679 solder Inorganic materials 0.000 title claims abstract description 61
- 239000011258 core-shell material Substances 0.000 title claims abstract description 39
- 239000002131 composite material Substances 0.000 title claims abstract description 34
- 230000002787 reinforcement Effects 0.000 title claims abstract description 17
- 239000002245 particle Substances 0.000 claims abstract description 42
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- 238000000034 method Methods 0.000 claims abstract description 20
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- 239000011812 mixed powder Substances 0.000 claims abstract description 15
- 230000008569 process Effects 0.000 claims abstract description 15
- 230000003014 reinforcing effect Effects 0.000 claims abstract description 9
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims abstract description 6
- 239000000463 material Substances 0.000 claims abstract description 5
- 238000005476 soldering Methods 0.000 claims abstract description 5
- 238000009792 diffusion process Methods 0.000 claims abstract description 4
- 238000001914 filtration Methods 0.000 claims abstract description 4
- 230000004907 flux Effects 0.000 claims abstract description 4
- 238000003756 stirring Methods 0.000 claims abstract description 4
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 14
- 239000000377 silicon dioxide Substances 0.000 claims description 7
- 229910052681 coesite Inorganic materials 0.000 claims description 5
- 229910052906 cristobalite Inorganic materials 0.000 claims description 5
- 229910052682 stishovite Inorganic materials 0.000 claims description 5
- 229910052905 tridymite Inorganic materials 0.000 claims description 5
- 238000001291 vacuum drying Methods 0.000 claims description 5
- 229910052802 copper Inorganic materials 0.000 claims description 4
- 229910052581 Si3N4 Inorganic materials 0.000 claims description 3
- 229910052709 silver Inorganic materials 0.000 claims description 3
- 229910017944 Ag—Cu Inorganic materials 0.000 claims description 2
- 229910052725 zinc Inorganic materials 0.000 claims description 2
- 229910001245 Sb alloy Inorganic materials 0.000 claims 1
- 229910052797 bismuth Inorganic materials 0.000 claims 1
- 239000002184 metal Substances 0.000 abstract description 18
- 229910052751 metal Inorganic materials 0.000 abstract description 18
- 239000002210 silicon-based material Substances 0.000 abstract description 9
- 229910052759 nickel Inorganic materials 0.000 abstract description 7
- 238000002360 preparation method Methods 0.000 abstract description 6
- 229910052718 tin Inorganic materials 0.000 abstract description 6
- 150000002739 metals Chemical class 0.000 abstract description 5
- 229910000765 intermetallic Inorganic materials 0.000 abstract description 4
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- 229910021389 graphene Inorganic materials 0.000 description 6
- PXHVJJICTQNCMI-UHFFFAOYSA-N nickel Substances [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 6
- 239000010949 copper Substances 0.000 description 5
- 238000009826 distribution Methods 0.000 description 5
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- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 description 2
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 2
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 2
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 2
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 description 2
- 238000005054 agglomeration Methods 0.000 description 2
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- 239000010703 silicon Substances 0.000 description 2
- 235000012239 silicon dioxide Nutrition 0.000 description 2
- 239000004332 silver Substances 0.000 description 2
- 238000005728 strengthening Methods 0.000 description 2
- 229910000838 Al alloy Inorganic materials 0.000 description 1
- 229920000049 Carbon (fiber) Polymers 0.000 description 1
- 239000005751 Copper oxide Substances 0.000 description 1
- 229910000861 Mg alloy Inorganic materials 0.000 description 1
- 229910004298 SiO 2 Inorganic materials 0.000 description 1
- 229910020888 Sn-Cu Inorganic materials 0.000 description 1
- 229910007116 SnPb Inorganic materials 0.000 description 1
- 229910019204 Sn—Cu Inorganic materials 0.000 description 1
- 229910001069 Ti alloy Inorganic materials 0.000 description 1
- 238000004220 aggregation Methods 0.000 description 1
- 238000000498 ball milling Methods 0.000 description 1
- 230000004888 barrier function Effects 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000004917 carbon fiber Substances 0.000 description 1
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- 230000008859 change Effects 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 238000000748 compression moulding Methods 0.000 description 1
- 229910000431 copper oxide Inorganic materials 0.000 description 1
- 239000012792 core layer Substances 0.000 description 1
- 229960004643 cupric oxide Drugs 0.000 description 1
- 125000004122 cyclic group Chemical group 0.000 description 1
- 230000005611 electricity Effects 0.000 description 1
- 238000007772 electroless plating Methods 0.000 description 1
- 238000009713 electroplating Methods 0.000 description 1
- 238000004134 energy conservation Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
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- 238000005303 weighing Methods 0.000 description 1
Classifications
-
- 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
- B23K35/24—Selection of soldering or welding materials proper
- B23K35/28—Selection of soldering or welding materials proper with the principal constituent melting at less than 950 degrees C
- B23K35/282—Zn as the principal constituent
-
- 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
- B23K35/40—Making wire or rods for soldering or welding
Landscapes
- Engineering & Computer Science (AREA)
- Mechanical Engineering (AREA)
- Electric Connection Of Electric Components To Printed Circuits (AREA)
- Powder Metallurgy (AREA)
Abstract
The invention discloses a Sn-based lead-free composite solder based on core-shell structure reinforcement phase reinforcement and a preparation method thereof, and relates to the technical field of manufacturing of electronic packaging connecting materials. The composite solder consists of 95 to 99.9 weight percent of Sn-based lead-free solder alloy powder and 0.1 to 5 weight percent of core-shell structure reinforcing particles. The core of the core-shell structure particle adopts Si and Si-based compounds, and adopts metals such as Ni, ag, cu and the like which can react with Sn in situ to generate intermetallic compounds as the shell. The invention obtains mixed powder by mechanically stirring reinforcing particles and Sn-based lead-free solder alloy powder in absolute ethyl alcohol for 10-30 min according to the content of the components, filtering and drying. The mixed powder can be added with soldering flux to prepare paste, or directly pressed into sheet/block in a mould for different subsequent welding processes, such as reflow welding, diffusion welding and the like. The invention is used for preparing Sn-based lead-free composite solder, can lead the reinforced particles to be uniformly distributed, improves the mechanical property of the solder, and has simple and reliable process and low cost.
Description
Technical Field
The invention relates to the technical field of manufacturing of electronic packaging connecting materials, in particular to a Sn-based lead-free composite solder based on core-shell structure reinforcement phase reinforcement.
Background
Along with the development demands of miniaturization, multifunctionality, low cost and the like of electronic products, the density of the packaging body is higher and higher, the size of welding spots is smaller and the number of the welding spots is larger and larger, and the material thermal expansion coefficient mismatch enables the welding spots with a connecting function to bear the cyclic change of stress and strain in the service process of the device, so that the thermal fatigue damage of the welding spots is caused, and the whole packaging device is disabled. Therefore, the development of lead-free solder with higher service reliability has become a subject to be studied urgently in the field of electronic packaging.
In the last 80 s, since the solder developed toward leadless, scientists have been working on developing various leadless solders, including Sn-Cu, sn-Ag-Cu, sn-Zn, sn-Bi, and other series alloys, instead of SnPb solders. In order to further improve the mechanical, thermal, electrical and other properties of the solder, researchers adopt a composite material technology to add nanoscale or microscale reinforcing particles, including metal particles, ceramic particles, graphene nano-sheets and the like, into the traditional solder.
The following requirements should generally be met for the strengthening phase to be added to the braze: (1) Proper density and ideal size, so that the solder is uniformly dispersed in the solder matrix; (2) The composite property is excellent, and the wettability, strength and reliability of the solder are improved or not obviously reduced after the composite property is added; (3) The preparation process can be applied to large-scale industrial production and has lower cost.
At present, most of reinforced particles used for preparing the composite brazing filler metal are carbon-based materials, such as graphene powder, graphene nano sheets, carbon fibers, multi-wall carbon nano tubes and the like, but the density of the carbon-based materials is much smaller than that of Sn-based brazing filler metal, and the smaller particle size enables the specific surface area to be large, so that the problems of particle aggregation, floating, weak bonding strength and the like can be generated. At present, some patents adopt metal plating on the surface of a carbon-based material to solve the problem, for example, a tin-based silver graphene lead-free composite solder is prepared by using a nano-silver modified graphene nano-sheet in the patent of application number 201510624582.5, a nickel-plated graphene reinforced tin-based composite lead-free solder is disclosed in the patent of application number 201710892272.0, and a high-strength Sn-Ag-Cu-RE composite solder is prepared by copper plating of graphene in the patent of application number 201810795284.6.
Silicon and silicon compounds have the advantages of low cost, abundant reserves, simple preparation and the like, have better hardness, stability and thermal conductivity, and are widely applied to the fields of improving the performances of Mg, al and Ti alloys, semiconductor materials and the like at present by adding Si and Si 3N4、SiC、SiO2. However, because the conductivity is far less than that of metal and the density is less than that of the Sn-based solder matrix, the Sn-based solder matrix is easy to float and agglomerate in the welding process, and the application of the Sn-based solder matrix in the field of Sn-based composite solder is limited.
Disclosure of Invention
The invention aims to provide a Sn-based lead-free composite solder based on core-shell structure reinforced phase reinforcement, which solves the problem of the prior Sn-based lead-free composite solder based on core-shell structure reinforced phase reinforcement in the prior art.
In order to achieve the above purpose, the present invention provides the following technical solutions:
The Sn-based lead-free composite solder based on the core-shell structure reinforced phase reinforcement consists of 95-99.9 wt.% of Sn-based lead-free solder alloy powder and 0.1-5 wt.% of mixed powder of core-shell structure reinforced particles.
As a further scheme of the invention: the reinforced particles are spherical, long cylindrical, flat and the like, and the size range is 20nm-10 mu m.
As still further aspects of the invention: the reinforced particle components are Si@Ni, siC@Ni, siO2@Ni and Si3N4@Ni; si@Cu, siC@Cu, siO2@Cu, si3N4@Cu; si@Ag, siC@Ag, siO2@Ag, si3N4@Ag.
As still further aspects of the invention: the Sn-based lead-free solder alloy powder comprises: the size of the alloy powder is 25-50 μm.
The preparation method of the Sn-based lead-free composite solder based on the reinforced phase of the core-shell structure comprises the following steps:
s1: placing the reinforced particles and Sn-based lead-free solder alloy powder into absolute ethyl alcohol, mechanically stirring for 10-30 min, and filtering;
S2: vacuum drying at a constant temperature of 40 ℃ for 12-24 hours to obtain Sn-based lead-free alloy powder and core-shell structure reinforced phase particles which are fully mixed;
S3: the mixed powder can be added with soldering flux to prepare paste, or directly pressed into sheet/block in a mould for different subsequent welding processes, such as reflow welding, diffusion welding and the like.
The core-shell structure reinforced phase particles used in the invention can react with the solder matrix to generate intermetallic compounds in the welding process, and Si or Si-based compounds in the core part of the particles do not react with the solder matrix, so that the particles can not coarsen and grow in the service process to form a reinforced phase with stable dispersion distribution, thereby improving the mechanical property of the composite solder and the reliability in the service process
Compared with the prior art, the invention has the beneficial effects that:
1. The invention uses Si and Si-based compound with excellent mechanical and thermal properties as the core part of the reinforced phase particles, adopts Ni, ag, cu and other metals which can react with Sn to generate IMC as the shell, and relieves the problems of agglomeration, floating and the like of micro-or nano-particles in liquid metal, thereby ensuring that the reinforced phase particles of the core part can be more uniformly distributed in the brazing filler metal matrix.
2. According to the invention, the IMC generated by the reaction of metals such as Ni, ag, cu and the like and Sn can improve the mechanical property of the solder to a certain extent, for example, ni and Sn can be generated near a Cu substrate (Cu, ni) 6Sn5 to serve as a diffusion barrier to prevent the generation of an interfacial Cu 3 Sn brittle phase of a composite welding spot in the service process;
3. The invention adopts a physical method to mix powder, avoids the damage and the destruction of the grinding medium to the reinforced phase particles with the core-shell structure in the ball milling process, thereby keeping the reinforcing effect of the reinforced phase particles on the brazing filler metal;
4. The composite brazing filler metal has the advantages of low preparation cost, energy conservation and environmental protection, and can be used for industrial production.
Drawings
FIG. 1 is a scanning electron microscope microstructure morphology of a core-shell structure reinforcing particle;
FIG. 2 is a scanning electron microscope microstructure topography of Sn-based solder alloy powder;
FIG. 3 is a microscopic morphology and elemental distribution of core-shell structured particles distributed in Sn-based solders;
FIG. 4 is a schematic diagram showing the distribution of (a) general particles in Sn-based solder;
(b) Schematic diagram of the uniform distribution of core-shell structured particles in Sn-based solders.
Detailed Description
The following description of the embodiments of the present invention will be made clearly and completely with reference to the accompanying drawings, in which it is apparent that the embodiments described are only some embodiments of the present invention, but not all embodiments. All other embodiments, which can be made by those skilled in the art based on the embodiments of the invention without making any inventive effort, are intended to be within the scope of the invention.
Referring to fig. 1 to 4, in the embodiment of the present invention, a Sn-based leadless composite solder based on core-shell structure reinforcement phase enhancement may be obtained by ultrasonic cleaning of solder paste in acetone and then filtration and drying, or may be purchased directly from the market, and the core-shell structure reinforcement phase particles may be prepared by electroless plating, electroplating, vapor deposition, mechanical coating, etc. the present invention directly uses commercially available Sn-based solder alloy powder and core-shell structure reinforcement phase particles as raw materials. As in patent application No. 200510105456.5.0, a low-cost, room-temperature and rapid chemical plating method and process for preparing silicon carbide-nickel core-shell structure are disclosed, application No. 200910157002.0 discloses a method for preparing silicon dioxide/silver core-shell structure particles with the assistance of PVP, and application No. 201710190255.2 discloses a method for preparing copper/silicon dioxide core-shell structure nano particles. Spherical particles with a core-shell structure, wherein the shell layer is made of Ni, ag and Cu metals, and the core layer is made of Si and Si 3N4、SiC、SiO2 can be used as reinforcing particles of the composite solder.
The following is a non-limiting example of a Sn-based lead-free composite solder based on core-shell structure reinforcement phase reinforcement and a preparation method thereof, which are only some of the examples of the present invention, but not all of the examples. All other embodiments, which can be made by those skilled in the art based on the embodiments of the invention without making any inventive effort, are intended to be within the scope of the invention. Table 1 shows the composition, dimensions and subsequent methods of use of the core-shell structure reinforcing particles and Sn-based lead-free alloy powders.
Table 1 technical conditions in examples
Example 1:
8.82g of Sn-3.0Ag-0.5Cu alloy powder with the size of 30-35 mu m and 0.18g of Si 3N4 @Ni core-shell structure spherical particles with the average size of 1.5 mu m are weighed, placed into 50mL of absolute ethyl alcohol together, mechanically stirred for 20min, filtered out of solution, and the mixed powder is placed into a vacuum drying box and dried for 24h at the constant temperature of 40 ℃ to obtain 9g of mixed powder with good micro-dispersity and macro-compactness.
1.0G of lead-free halogen-free non-conductive soldering paste with the model KL-558 is weighed and mechanically and fully stirred and mixed with the dried mixed powder for more than 30 minutes to prepare the Sn-based lead-free composite solder paste, and the Sn-based lead-free composite solder paste can be heated and remelted for subsequent performance tests such as mechanics, thermal, electricity and the like or refrigerated storage for standby.
Example 2:
8.712g of Sn-0.7Cu alloy powder with the size of 35-40 mu m and 0.088g of SiO 2 @Ag core-shell structure spherical particles with the average size of 1 mu m are weighed, placed into 50mL of absolute ethyl alcohol together, mechanically stirred for 15min, filtered out of solution, and the mixed powder is placed into a vacuum drying box and dried for 24h at the constant temperature of 40 ℃ to obtain 8.8g of mixed powder with good micro-dispersity and macroscopic compactness.
Pouring the mixed powder into a graphite mould with the thickness of 10 multiplied by 10mm for compression molding to prepare the Sn-based lead-free composite solder sheet which can be used for the subsequent mounting process.
Example 3:
8.82g of Sn-3.5Ag alloy powder with the size of 30-40 mu m and 0.18g of SiC@Cu core-shell structure spherical particles with the size of 75nm are weighed, placed in 50mL of absolute ethyl alcohol together, mechanically stirred for 10min, filtered out of solution, and the mixed powder is placed in a vacuum drying box and dried for 24h at the constant temperature of 40 ℃ to obtain 9g of mixed powder with good micro-dispersity and macroscopic compactness.
Weighing 1.0g of lead-free environment-friendly soldering paste with the model of RMA-223-TPF, mechanically and fully stirring and mixing with the dried mixed powder for more than 30min to prepare the Sn-based lead-free composite solder paste, and carrying out subsequent mechanical, thermal, electrical and other performance tests or refrigerating and preserving for later use.
Fig. 1 is a scanning electron microscope microstructure morphology diagram of a single core-shell structure reinforced particle, and fig. 2 is a Sn-based lead-free solder alloy powder with good sphericity and dispersibility. After the core-shell structure reinforcing phase particles are added into the brazing filler metal, the stable structure formed in the brazing filler metal is shown in fig. 3, and from the distribution of Sn, ni and Si elements in fig. 3, it can be seen that Ni and Sn form intermetallic compounds, and Si-based compound particles are well pinned in a brazing filler metal matrix. The general Si and Si-based compounds may float up in the liquid Sn matrix due to the density difference and the flux discharge, as shown in fig. 4 (a), while the core-shell particles may form IMCs in the liquid Sn matrix to be uniformly distributed, as shown in fig. 4 (b). The excellent mechanical and thermal properties of Si and Si-based compounds are utilized to make the Si and Si-based compounds serve as the core part of the reinforced phase particles, and metals such as Ni, ag, cu and the like which can be wetted with Sn and react to generate IMC serve as the shell plating layer, so that the problems of agglomeration, floating and the like of micro-particles or nano-particles are relieved when the Si and Si-based compounds are compounded with a matrix material, and the reinforced phase particles of the core part can be more uniformly distributed in a brazing filler metal matrix. Meanwhile, the shell metal can react with the solder matrix to generate intermetallic compounds, and Si or Si-based compounds in the core part of the particles do not react with the solder matrix, so that the shell metal does not coarsen and grow up in the service process to form a strengthening phase with stable dispersion distribution, and the mechanical property of the composite solder and the reliability in the service process are improved.
Although the present invention has been described with reference to the foregoing embodiments, it will be apparent to those skilled in the art that modifications may be made to the embodiments described, or equivalents may be substituted for elements thereof, and any modifications, equivalents, improvements and changes may be made without departing from the spirit and principles of the present invention.
Claims (4)
1. The Sn-based lead-free composite solder based on core-shell structure reinforced phase reinforcement is characterized in that: the Sn-based lead-free composite solder based on core-shell structure reinforced phase reinforcement consists of 95-99.9wt.% of Sn-based lead-free solder alloy powder and 0.1-5wt.% of mixed powder of core-shell structure reinforced particles;
The reinforcing particle component is Si@Ni、SiC@Ni、SiO2@Ni、Si3N4@Ni、Si@Cu、SiC@Cu、SiO2@Cu、Si3N4@Cu、Si@Ag、SiC@Ag、SiO2@Ag or Si 3N4 @Ag.
2. The Sn-based lead-free composite solder reinforced based on the reinforced phase of the core-shell structure according to claim 1, wherein: the reinforced particles are spherical, long cylindrical and flat, and the size range is 20nm-10 mu m.
3. The Sn-based lead-free composite solder reinforced based on the reinforced phase of the core-shell structure according to claim 1, wherein: the Sn-based lead-free solder alloy powder comprises: sn-Cu, sn-Ag-Cu, sn-Zn, sn-Bi, sn-Sb alloy powder, and the size range is 25-50 mu m.
4. A method for preparing the Sn-based lead-free composite solder based on reinforced core-shell structure reinforcement phase as claimed in any one of claims 1 to 3, comprising the following steps:
s1: placing the reinforced particles and Sn-based lead-free solder alloy powder into absolute ethyl alcohol, mechanically stirring for 10-30 min, and filtering;
S2: vacuum drying at the constant temperature of 40 ℃ for 12-24 hours to obtain Sn-based lead-free alloy powder and core-shell structure reinforced phase particles which are fully mixed;
s3: the mixed powder can be added with soldering flux to prepare paste, or can be directly pressed into sheet-shaped/block-shaped materials in a mould for different subsequent welding processes, wherein the welding processes are reflow welding or diffusion welding.
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CN114769934A (en) * | 2022-05-20 | 2022-07-22 | 哈尔滨理工大学 | High-retention-rate multi-size particle reinforced low-temperature composite brazing filler metal and preparation method thereof |
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CN114131237A (en) * | 2021-12-14 | 2022-03-04 | 浙江亚通焊材有限公司 | Foam soldering tin and preparation method thereof |
CN114227059A (en) * | 2022-01-06 | 2022-03-25 | 南京工程学院 | Bi @ MAX core-shell structure, high-reliability lead-free solder and preparation method thereof |
CN114769934A (en) * | 2022-05-20 | 2022-07-22 | 哈尔滨理工大学 | High-retention-rate multi-size particle reinforced low-temperature composite brazing filler metal and preparation method thereof |
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