premix molded body

Abstract

A pre-mix form includes a base metal and a plurality of types of solid particles dispersed in the base metal. The base metal includes one of a liquid base metal and a solid base metal. The plurality of types of solid particles includes at least non-reactive magnetic particles that are responsive to a magnetic field to controllably disperse the plurality of types of solid particles in the base metal, and reactive particles that are reactive with the base metal under the magnetic field.

Description

[0001] Priority

[0002] This PCT application claims priority to U.S. Patent Application No. 17 / 365,811 filed July 1, 2021, which is a continuation-in-part of U.S. Patent Application No. 17 / 073,370 filed October 18, 2020, the entire contents of which are incorporated herein by reference. TECHNICAL FIELD

[0003] The present disclosure relates generally to the field of bonding and joining, and more particularly, to a pre-mixed shaped body and a method of making / using the pre-mixed shaped body.

[0004] BACKGROUND

[0005] Conventional bonding and joining techniques employing soldering or brazing require the addition of heat energy and flux. In soldering or brazing, heat energy is required to melt the joining or filler material to flow, contact the surfaces, and form a bond. Flux is required to remove oxides and contaminants from the mating surfaces and filler material, and to protect the filler material from environmental oxidation. Typically, the surface of the filler material develops an oxide layer that is detrimental to the formation of a bond. Therefore, the prevention and removal of the oxide layer from the filler material is required during the bonding process. SUMMARY

[0006] One aspect of the present disclosure provides a pre-mixed shaped body. The pre-mixed shaped body includes a base metal and a plurality of types of solid particles dispersed in the base metal. The base metal includes one of a liquid base metal and a solid base metal. The plurality of solid particles includes at least: non-reactive magnetic particles that are responsive to a magnetic field to controllably disperse the plurality of solid particles in the base metal, and reactive particles that are reactive with the base metal under the magnetic field.

[0007] Another aspect of the present disclosure provides a method of making a pre-mixed shaped body. The invention provides a particle-liquid mixture containing a plurality of solid particles and a liquid base metal. The plurality of types of solid particles includes at least reactive particles that are reactive with the base metal and non-reactive magnetic particles. A magnetic field is applied to the particle-liquid mixture to magnetically disperse the plurality of types of solid particles in the liquid base metal to form a particle-liquid dispersion without substantially causing a reaction between the reactive particles and the liquid base metal. A putty-like pre-mixed shaped body is prepared based on the particle-liquid dispersion without solidifying the liquid base metal.

[0008] Another aspect of the present disclosure provides a method of manufacturing a premix compact. The present invention provides a particle-liquid mixture containing a plurality of solid particles and a liquid base metal. The plurality of types of solid particles includes at least reactive particles that are reactive with the base metal and non-reactive magnetic particles. A magnetic field is applied to the particle-liquid mixture to magnetically disperse the plurality of types of solid particles in the liquid base metal without substantially causing a reaction between the reactive particles and the liquid base metal to form a particle-liquid dispersion. The liquid base metal is solidified to disperse the plurality of types of solid particles in the solidified base metal without substantially causing a reaction between the reactive particles and the solid base metal. A solid premix compact is produced that includes the plurality of types of solid particles and the solidified base metal.

[0009] Another aspect of the present disclosure provides a method of using a premix compact. Matching bonding surfaces are provided and a particle-liquid mixture corresponding to the consolidated premix compact is disposed between the matching bonding surfaces. The particle-liquid mixture includes a plurality of types of solid particles and a base metal in a liquid state. The plurality of types of solid particles includes at least reactive particles and non-reactive magnetic particles. A first magnetic field is applied to the particle-liquid mixture to magnetically disperse the plurality of types of solid particles in the liquid base metal to form a particle-liquid dispersion. A second magnetic field is applied to solidify the particle-liquid dispersion to allow a reaction between the reactive particles and the base metal.

[0010] Another aspect of the present disclosure provides a method of using a premix compact. Matching bonding surfaces are provided and a particle-liquid mixture corresponding to the consolidated premix compact is disposed between the matching bonding surfaces. The particle-liquid mixture includes a plurality of types of solid particles and a base metal in a liquid state. The plurality of types of solid particles includes at least reactive particles and non-reactive magnetic particles. A first magnetic field is applied to the particle-liquid mixture to magnetically disperse the plurality of types of solid particles in the liquid base metal to form a particle-liquid dispersion. A second magnetic field is applied to solidify the particle-liquid dispersion to allow a reaction between the reactive particles and the base metal.

[0011] Other aspects of the present disclosure will become apparent to those of ordinary skill in the art upon review of the description, claims, and drawings in this disclosure. BRIEF DESCRIPTION OF DRAWINGS

[0012] The following drawings are included as examples only to illustrate various disclosed embodiments and are not intended to limit the scope of the present disclosure.

[0013] Figure 1Ais an exemplary method of manufacturing a premix form provided by embodiments of the present disclosure.

[0014] Figure 1B is another exemplary method of manufacturing a fusion preform provided by embodiments of the present disclosure.

[0015] Figure 2 is an exemplary particle-liquid mixture in a container provided by embodiments of the present disclosure.

[0016] Figure 3 is an exemplary apparatus provided by embodiments of the present disclosure comprising a magnetic processing device for processing a particle-liquid mixture.

[0017] Figures 4-7 is a controllable application of a magnetic field to a particle-liquid mixture in a container provided by embodiments of the present disclosure.

[0018] Figure 8 is an exemplary solidified particle-liquid dispersion in a container provided by embodiments of the present disclosure.

[0019] Figure 9A is an exemplary method for using a premix form provided by embodiments of the present disclosure.

[0020] Figure 9B is another exemplary method for using a premix form provided by embodiments of the present disclosure.

[0021] Figure 10 is an exemplary apparatus provided by embodiments of the present disclosure comprising a magnetic processing device for processing a solid premix form.

[0022] Figures 11-15 is exemplary mixing and dispersion of a liquefied premix form under modulated application of a magnetic field provided by embodiments of the present disclosure.

[0023] Figure 16 is an exemplary solid alloy corresponding to a premix form provided by embodiments of the present disclosure. DETAILED DESCRIPTION

[0024] Reference will now be made in detail to exemplary embodiments of the present disclosure, which are illustrated in the accompanying drawings. Wherever possible, the same reference numbers will be used throughout the drawings to refer to the same or like parts.

[0025] Figures 1A-1B is an exemplary method of manufacturing a premix form provided by embodiments of the present disclosure.

[0026] In Figures 1A-1BAt 102, e.g., in a container, a particle-liquid mixture is provided that includes a plurality of types of solid particles and a liquid base metal (i.e., the base metal in liquid form).

[0027] In one embodiment, to provide the particle-liquid mixture, the plurality of types of solid particles can be mixed with the base metal in solid form (e.g., solid particles of the base metal or base metal particles) in a container. The base metal particles and / or the plurality of types of solid particles can be in the form of metal powder, pellets, wires, fibers, ingots, or any combination thereof. The base metal particles and the plurality of types of solid particles can be mixed, e.g., at room temperature. The base metal particles can then be melted into liquid form along with the mixed plurality of types of solid particles, e.g., by any suitable heating process, to form the particle-liquid mixture. For example, the base metal particles can be melted by induced convection or induction heating caused by an applied magnetic field. The magnetic field can be controlled / modulated to heat the base metal without destroying the structure of other particles in the mixture.

[0028] Alternatively, to form the particle-liquid mixture, the base metal particles can be melted in a container to form the liquid base metal. The plurality of types of solid particles can then be injected into the liquid base metal to form the particle-liquid mixture.

[0029] The base metal can include a metal and / or a metal alloy having a low melting point. For example, the base metal can have a melting point of less than about 200 °C. The base metal can include, e.g., Ga, In, Sn, Bi, Pb, Cd, Hg, Rb, Zn, Bi, or any combination / alloy thereof. In certain embodiments, the base metal can include Ga, GaInSn, and / or InSnBi.

[0030] In the particle-liquid mixture, the weight ratio of the liquid base metal to the plurality of types of solid particles can be in the range of about 4: 1 to about 1:4, e.g., in the range of 4: 1 to 1:2, such that the plurality of types of solid particles are easily handled in liquid form in a quantity and have sufficient mechanical properties. The average size of the plurality of types of solid particles can be in the range from about 100 nanometers to about 100 micrometers.

[0031] Various types of solid particles can be mixed with the base metal. For example, the plurality of types of solid particles can include reactive particles, non-reactive magnetic particles, and / or any suitable additives for providing desired characteristics to the particle-liquid mixture and / or the subsequently formed pre-mixed shaped body.

[0032] As used herein, the terms "reactive" and "non-reactive" are relative terms used to indicate the degree of reactivity or reaction capability between the solid particles and the base metal. For example, under certain conditions, "reactive" particles can react with the base metal in liquid form (i.e., liquid base metal) for binding / solidifying / alloying the solid particles with the base metal, corresponding to a pre-mixed shaped body. "Non-reactive" particles can refer to solid particles that are unable to bind / solidify / form an alloy with the liquid base metal under the same particular conditions. For example, the solid particles can be considered non-reactive when they "react" with the liquid base metal at a very slow kinetics such that they are unable to bind / solidify / alloy after a predetermined period of time. As an extreme example, a material that does not react at all with the liquid base metal can include a ceramic or a covalently bonded organic material.

[0033] The reactive particles can react with the base metal. The reactive particles can include at least a reactive metal material. The reactive metal material can include Fe, Ni, Cu, Ag, Au, In, Cu, Sn, Bi, Zn, Ti, V, Cr, Mo, Nb, Zr, Hf, Pt, Ir, and / or any combination thereof (e.g., an alloy).

[0034] The reactive particles can have an average size ranging from about 100 nanometers to about 50 micrometers, for example, ranging from about 100 nanometers to about 25 micrometers. To obtain desirable reactivity, the reactive particles can be selected to be neither too large nor too small. Too large reactive particles can take a long time to react with the base metal, while too small particles can react too fast. The inventors have found that when the size of the reactive particles is less than 100 nanometers, the reaction between the reactive particles and the base metal can be too fast for the alloying.

[0035] The reactive particles can be magnetic and / or non-magnetic. For example, reactive magnetic particles can include Fi, Ni, and / or alloys thereof. Reactive non-magnetic particles can include Cu, Ag, Au, In, Cu, Sn, Bi, Zn, Ti, V, Cr, Mo, Nb, Zr, Hf, Pt, Ir, or any combination thereof (e.g., an alloy). In addition to being reactive with the base metal, in some embodiments, the reactive magnetic particles can also be capable of responding to a magnetic signal.

[0036] The magnetic or non-magnetic reactive particles can include a core-shell structure. The core-shell structure can include a core material and a shell material that is different from the core material and at least partially surrounds the core material. The core material can have a reaction rate with the base metal that is greater than the shell material, or vice versa.

[0037] In some embodiments, the core-shell structure of the reactive particles can include an oxide shell material at least partially covering a reactive metal material as the core material. The oxide shell material can include an oxide material of the reactive metal material. The oxide shell material can be a native oxide material or can be intentionally formed by oxidation reaction with the reactive metal material, such as thermal oxidation. For example, when the reactive metal material is one or more of Fe and Ni as the core material, the shell material can be an oxide of one or more of Fe and Ni. Unlike conventional preform materials that must remove the oxide shell layer to form and use the pre-mixed preform, the disclosed oxide shell layer is needed to control the reaction kinetics / rate of forming and using the pre-mixed preform.

[0038] In other embodiments, the core-shell structure of the reactive particles can include a non-oxide shell material. For example, the core-shell structure can include one or more of: a core-shell structure having the shell material including Cu and the core material including Au; a core-shell structure having the shell material including steel and the core material including Cu; a core-shell structure having the shell material including ZnO or TiO2and the core material including Cu, Ag, Ni, or combinations thereof; and / or a core-shell structure having the shell material including Cu and at least partially covering the Cu with copper oxide and the core material including Co, ceramic materials including AIN, SiC, SiO2, TiO2, ZrO2, AI2O3, BeO, Si3N4, B4C, WC, and / or diamond, or combinations thereof.

[0039] In various embodiments, the core material in the core-shell structure can be multi-layered, such as formed from at least one material that reacts with the matrix material and at least another material to provide desired properties to the subsequently formed pre-mixed preform (e.g., to provide improved mechanical strength). In some embodiments, the shell material can also be multi-layered. For example, when the shell material includes Cu, such as to react with the matrix metal, the copper shell material can include an additional copper oxide shell layer at least partially covering the copper shell material.

[0040] In various embodiments, the particle-liquid mixture can be magnetically dispersed to form a particle-liquid dispersion (e.g., as shown in FIG. 1). For example, the particle-liquid mixture can be magnetically dispersed in a magnetic field to form a particle-liquid dispersion. Figures 1A-1BThe reactive particles can be formed into a liquid dispersion (e.g., as shown in operation 104 in FIG. 1A), which can be a uniform dispersion that does not substantially cause any reaction (e.g., alloying reaction) between the reactive particles and the base metal. The particle-liquid dispersion can be used to form a preform as disclosed herein, including a dough-like preform (e.g., as shown in operation 106 in FIG. 1A) and a solid preform (e.g., as shown in operations 108 and 109 in FIGS. 1A-1B). The preform can then be used directly for bonding / curing / alloying or stored / transported for later / future use.

[0041] In an embodiment disclosed herein, the shell material of the reactive particles can be used to control the kinetics and dissolution rate of the core material, thereby controlling, for example, the shelf life and / or reaction rate of the formed preform.

[0042] The core-shell structure of the reactive particles can at least further extend the shelf life of the formed mixed preform. For example, the shell material can be thick enough to largely prevent solid-state alloying between the reactive particles and the solid base metal. The shell material can be thin enough at the same time so that the shell can break during reflow to allow such a reaction. The shell material can have a thickness ranging from the thickness of an atomic layer to about 100 nanometers. For example, the shell material can have a thickness of a few atomic layers. The thickness of the shell material can be controlled depending on the selection of the base metal and the reactive particles and / or the target shelf life of the formed preform.

[0043] In an example preform including the reactive particles having the core material of one or more of Fe and Ni and the shell material of an oxide of one or more of Fe and Ni, the dissolution or ingress rate of the example base metal Ga material through the shell material depends on the thickness of the shell material. In an example of forming a dough-like preform for quick use, the shell material can be relatively thin for quick solidification and can be increased in thickness to extend the handling and solidification time of the material. To form a solid preform, the shell material can be thick enough, for example, at least a few nanometers, so that there is no reaction (e.g., for a few minutes) during initial mixing and subsequent solidification. The liquid base metal can have a reaction and ingress rate through the shell material that increases with temperature, not solidifying at temperatures close to room temperature to achieve a long shelf life, but quickly solidifying at processing temperatures.

[0044] According to various embodiments, in addition to controlling the shell thickness, other mechanisms can be applied to the core-shell structure of the reactive particles to control the shelf life, reaction kinetics / rate of the formed preform.

[0045] For example, one premix preform can contain a reactive particle that includes a shell material. The shell material reacts slower than the core material with the base metal to provide a longer processing time for the preform. For example, the shell material can be copper, the core material can be gold, and the base metal can be liquid gallium, which reacts faster with gold than with copper.

[0046] Another example premix preform can contain a reactive particle that includes a reactive shell material (e.g., copper) and a non-reactive core material (e.g., Co, and / or a ceramic material including AlN, SiC, SiO2, TiO2, ZrO2, Al2O3, BeO, Si3N4, B4C, WC, and / or diamond). In some cases, the reactive shell material can include multiple layers having at least an oxide layer that partially covers the reactive shell material. In one example, the shell material can be Cu, the core material can be Co, and the shell material can further include copper oxide that covers the copper shell material. The magnetic properties of Co can be used for heating, mixing, and / or wetting, while the shell material can allow for a coherent interface and strong bonding of the premix preform to a bonding surface. In another example, the shell material can be Cu, the core material can be a ceramic material such as AlN, and the shell material can further include copper oxide that covers the copper shell material. Such a reactive particle can provide a slow reaction rate and provide an extended shelf life for the premix preform formed.

[0047] In various embodiments, the shell material can be selected to combine to support and strengthen the matrix / block of the premix preform.

[0048] In an example premix preform, the shell material of the reactive particle can be non-reactive and / or can partially cover an interior particle of a reactive core material (e.g., as a flaky shell). When the interior particle is dissolved by the Ga liquid, the shell material can remain in the preform material to provide mechanical strength and form a composite. Such a shell material can include a ductile material that includes steel, and the core material can be Cu. In another example, the shell material can be a brittle oxide such as ZnO and / or TiO2 that will crack due to thermal expansion mismatch with Cu, Ag, and / or Ni metals used as core materials within the shell material. The hard and brittle shell material can strengthen the matrix / block of the premix preform during processing.

[0049] In various embodiments, the shell material can be broken during the preform processing. For example, the shell material of the reactive particles can be overcome by, for example, dissolving the base metal due to the application of a magnetic field. For example, under the control of a magnetic field, the oxide shell material can break to allow its core material Fe or Cu to interact / react with the liquid base metal.

[0050] The plurality of types of solid particles can also include non-reactive magnetic particles. The non-reactive magnetic particles can not be reactive with the base metal, but can correspond to a magnetic signal, for example, to facilitate / drive the heating, mixing, and / or wetting of the particle-liquid mixture (e.g., operation 104 as shown in FIGS. 1A-1B). For example, the non-reactive magnetic particles can include Co-containing particles, Nd-containing particles, and / or Cr-containing particles.

[0051] The non-reactive magnetic particles can have an average size in the range of about 1 micron to about 100 microns, for example, in the range of about 5 microns to about 100 microns. For example, the non-reactive magnetic particles can include large size magnetic particles having at least one dimension greater than 5 microns. Such large size magnetic particles can include micro-wires, micro-fibers, or combinations thereof.

[0052] In some cases, large size magnetic particles, for example, micro-wires and / or micro-fibers, can be added as solid particles to further facilitate the heating, mixing, and / or wetting characteristics of the particle-liquid mixture in the container or disposed between the bonding surfaces to further provide the desired characteristics. The large size magnetic particles can be reactive or non-reactive. For example, large size (e.g., greater than about 50 microns) reactive and magnetic Fe and / or Ni particles can be added to the particle-liquid mixture to provide ideal mixing and wetting for dispersion and at least partially participate in the bonding / curing reaction.

[0053] In some embodiments, the plurality of types of solid particles can include any other particles to provide desired characteristics / features to the subsequently formed pre-mixed form. For example, semiconductor particles and / or metal-doped semiconductor particles (e.g., SiC, AIN, Si02, and / or diamond, with or without dopants) can be added as additive particles to provide improved thermal conductivity to the formed pre-mixed form while reducing the electrical conductivity of the pre-mixed form. In some cases, the additive particles, whether reactive, non-reactive, magnetic, or non-magnetic, can be further added to the particle-liquid mixture to facilitate the heating, mixing, and / or wetting performance in forming or processing the pre-mixed form.

[0054] Figure 2This is an exemplary particulate-liquid mixture in a container provided in this disclosure embodiment. As disclosed, Figure 2 The particles described herein may be altered and / or omitted, and the exemplary particle-liquid mixture may contain more particles.

[0055] like Figure 2 As shown, the exemplary particle-liquid mixture 220 includes a liquid matrix metal 20A, which is mixed with various particles disclosed herein, such as reactive particles 201 / 203 (e.g., at least reactive magnetic particles 201 and reactive nonmagnetic particles 203), non-reactive magnetic particles 206, and / or any other suitable solid additive 208.

[0056] The particulate-liquid mixture 220 is contained in the container 210. The container 210 can be used for mixing, dispersing, and / or solidifying. The container 210 may be polymeric and may or may not have filler to minimize the adhesion strength between the contained mixture and the interior surface of the container. For example, the container 210 may at least include a plastic surface for contacting the particulate-liquid mixture. The plastic surface is made of a material including polytetrafluoroethylene (PTFE or Teflon), high-density polyethylene (HDPE), or low-density polyethylene (LDPE), which has low surface energy to prevent wetting. Of course, the container can be made of any other suitable material, including metals, ceramics, or non-polymer materials, with or without the plastic surface.

[0057] exist Figures 1A-1B At position 104, a magnetic field is applied to the particle-liquid mixture to magnetically disperse the various types of solid particles in the liquid matrix metal to form a particle-liquid dispersion. The magnetic field can be applied in a manner that substantially does not cause any reaction between the solid particles and the liquid substrate metal.

[0058] As disclosed herein, the particle-liquid dispersion may refer to a magnetically dispersed particle-liquid mixture, wherein the various types of solid particles can be controllably dispersed by applying a magnetic field, for example, substantially uniformly dispersed in the liquid matrix metal.

[0059] Figures 3-7 An exemplary particle-liquid mixture 220 is shown in which a magnetic field is controllably applied to the container 210 to magnetically disperse the various types of solid particles (e.g., particles 201, 203, 206 and / or 208) in the liquid matrix metal 20A to form a particle-liquid dispersion.

[0060] although Figures 2-7 The container shown is configured to have an opening on one side and in the length direction (e.g.)Figure 3 The container can be positioned in any manner or at any angle according to various needs of embodiments of the present disclosure. Additionally, the particle-liquid mixture in the container can be located at a distance having a thickness from the inner wall of the container. The thickness covers a portion of the width / diameter or the entire width / diameter of the container.

[0061] Referring to Figure 3 The container 210 containing the particle-liquid mixture 220 can be placed in a magnetic field, for example, generated by a magnetic processing device 330.

[0062] In one embodiment, the magnetic processing device 330 can include a coil wound around the container 210. The shape and / or size of the wire for the coil winding can be determined based on the specific application of the magnetic field. For example, the coil winding can have, for example, a uniform shape and size, and can be uniformly or non-uniformly distributed and wound along the length direction of the container 210.

[0063] The magnetic processing device 330 can be connected to or include a controller (not shown), for example, a computer controller, to control the current and / or current change of the coil winding, thereby controlling, for example, the polarity, intensity, positioning, movement, orientation, rotation, spin, etc. of the magnetic field. For example, the controller can select a length of the coil to selectively apply the magnetic field to a partial amount of the particle-liquid mixture to locally disperse solid particles in the particle-liquid mixture. In another example, the magnetic field can be controlled and changed in a specific direction, for example, the length direction of the container. In yet another example, the controller can control the coil winding to repeatedly provide a rotating field and / or a translating field, for example, back and forth along a specific direction. In yet another example, the controller can control the coil winding to move the particle-liquid mixture between different positions, from one position to another, along the inner wall of the container, or move the particle-liquid material out of the container without physically processing the material.

[0064] The magnetic field can be applied in any suitable manner. Other suitable magnetic processing devices can include electromagnets and / or physical permanent magnets. For example, near the particle-liquid mixture contained in the container, electronic control of electromagnets and / or control of moving physical permanent magnets can be performed to provide the magnetic field.

[0065] In some embodiments, the container in FIGS. 3-7 can be positioned in the magnetic processing device.

[0066] In one embodiment, the magnetic field can be applied and calibrated such that the solid particles in the liquid matrix metal can be pulled and moved towards the interface with the container, for example, as shown in Figure 4 Meanwhile, the magnetic field can be used to heat and keep the matrix metal in liquid state without further heating the reaction.

[0067] The magnetic field can be moved at various angles to drag the solid particles across the surface of the container, for example, to move across the cross-section of the particle-liquid mixture in any suitable shape or motion path, for example, as shown in Figure 5 The solid particles dragged on the container surface can scrape, remove and / or destroy the natural oxide layer at the outermost layer 505 of the particle-liquid mixture at the mixture-container interface, thereby enabling surface wetting at the bond. In some embodiments, large size particles can be applied with greater force compared to the viscous force experienced in the particle-liquid mixture, and can have a better chance of moving the solid particles to the mixture-container interface, for example, as shown in Figure 6 As such, the motion of the magnetic particles can be controlled to improve surface wetting and reduce voids and gaps often produced in conventional welding materials.

[0068] The applied magnetic field can allow movement and dispersion of all solid particles in the particle-liquid mixture. Unlike the driving mode by mechanical force that often compresses the particles and drives out the liquid component, the disclosed particle-liquid mixture / dispersion can move as a mass from one location to another and does not squeeze out the liquid component. In addition, the magnetic field can also be used to smoothen the particle-liquid mixture after the particle-liquid mixture is dispersed as a large "mass", as shown in Figure 7

[0069] Thus, the non-reactive solid particles can be used to drive, spread, mix and / or heat the particle-liquid mixture to form a uniform particle-liquid dispersion and thus a pre-mix form with high quality. When processing the pre-mix form, the non-reactive solid particles can be used to drive the solidification and / or strengthen the corresponding particle-liquid mixture / dispersion to proceed with bonding.

[0070] In one embodiment, a gradient magnetostatic field can be used to align the magnetic fibers or wires within the particle-liquid mixture to provide preferred and anisotropic properties, for example, as shown in Figure 6 ​As shown. For example, large-sized magnetic particles of Fe, Ni, Co, Cr, Nb and / or alloys thereof can be incorporated into the particle-liquid mixture to form the premixed molded body or for bonding / curing / alloying during the processing of the premixed molded body. Magnetic caliber can be modified to produce various properties, such as anisotropic thermal conductivity and / or mechanical strength.

[0071] Unlike traditional mechanical mixing methods, the disclosed magnetic mixing / dispersion can be carried out under a magnetic field, allowing various particles to be oriented, moved, and / or aligned along the entire cross-section of the particle-liquid mixture.

[0072] For example, under a dynamic or helical magnetic field, the solid magnetic particles (with or without large-sized reactive or non-reactive properties) can be driven to move through the liquid matrix metal. The shape of the mixture can be designed, for example, to mimic the premixed molded body in the target. The disclosed magnetic mixing / dispersion can be random or ordered and can be performed simultaneously with magnetic heating.

[0073] The disclosed magnetic mixing / dispersion allows the subsequently formed premixed molded body to have sufficiently separated reactive materials / particles, significantly increasing the shelf life of the formed premixed molded body. When the premixed molded body is ready for bonding, the separated materials in the premixed molded body can be reflowed and redispersed before being placed on the bonding surface or after the bonding surfaces are brought into contact. In some cases, in the premixed molded body, the materials can be coarsely mixed into granular blocks or can comprise layers of different materials.

[0074] In some embodiments, the particulate-liquid mixture / dispersion can be dispersed and flattened on a surface, such as... Figure 7 As shown. The flattened particle-liquid mixture / dispersion may have a thickness of, for example, about 1 mm or less.

[0075] refer to Figure 1A In operation 106, the particulate-liquid dispersion is then processed, for example, by rolling, pressing, extruding, casting, etc., to form a clay-like premixed body without solidifying the liquid matrix metal. The clay-like premixed body can be formed in the form of strips, sheets, ingots, filaments, or any suitable shape. For example, the clay-like premixed body can be rolled to have a thickness ranging from about 5 micrometers to about 500 micrometers.

[0076] The clay-like premixed molding body can then be used directly or cured at 108 in Figure 1A. The solid premixed molding body may have a shape / size corresponding to the clay-like premixed molding body.

[0077] At Figure 1A At 108, the dough-like premix form can be cooled, for example, by liquid cooling, Peltier cooling, or immersion in a cooling liquid such as water or LN2. The cooling process can quench the dough-like premix form without substantially causing any reaction, thereby producing a corresponding solid premix form.

[0078] In some embodiments, as Figure 1B indicated, after forming the particle-liquid dispersion at operation 104, a solidification process at 107 can be performed so that the solid particles are uniformly dispersed in the solidified matrix metal without substantially causing reactions between them, as Figure 8 indicated.

[0079] When solidifying the particle-liquid dispersion, the entire assembly, for example, including the container and the particle-liquid dispersion contained therein, can be cooled, for example, by liquid cooling, Peltier cooling, or immersion in a cooling liquid such as water. The cooling process can quench the particle-liquid dispersion without substantially causing any reaction, for example, without destroying the shell material of the reactive nuclear material.

[0080] With continued reference to Figure 1B At 109, the solidified particle-liquid dispersion can be processed by rolling, drawing, forging, stamping, milling, turning, or the like to form a solid premix form. For example, the solidified particle-liquid dispersion can be rolled to have a thickness of about 25 microns to about 10 millimeters, or in some cases, the solidified particle-liquid dispersion can be drawn into a wire. In other cases, the solidified particle-liquid dispersion can be ground or cryogenically ground into a powder formulation at room temperature, thereby forming the solid premix form.

[0081] In this way, the dough-like premix form prepared at operation 106 in FIG. 1A, or the solid premix form prepared at 108 in Figure 1A , and / or the solid premix form at 109 in Figure 1B may be ready for use in an application.

[0082] It should be noted that when the exemplary methods shown in Figures 1A and 1B are performed, there is essentially no reaction between the base metal and the reactive particles. For example, the resulting clay-like premixed molded body may comprise various types of solid particles magnetically dispersed in the liquid base metal, and there is essentially no reaction between the reactive particles and the liquid base metal at temperatures near room temperature (e.g., about 25°C) or lower. The resulting solid premixed molded body may comprise various morphologies of solid particles magnetically dispersed in the solid base metal. At temperatures near room temperature (e.g., about 25°C) or lower, there is essentially no reaction between the reactive particles and the solid base metal.

[0083] Figures 9A-9B This is an exemplary method for using premixed molded articles provided in the embodiments of this disclosure.

[0084] exist Figures 9A-9B 902 in the middle provides a mating adhesive surface.

[0085] As used herein, the terms “mating surface,” “adhesive surface,” and “mating-adhesive surface” are used interchangeably in this disclosure. Therefore, the term “adhesive material” can refer to any material placed and treated between mating-adhesive surfaces, for example, for reflow, redispersing, and bonding / curing / alloying.

[0086] The adhesive material may therefore include, for example, a particle-liquid mixture (e.g., such as...) Figures 1A-1B As shown in 102), particulate-liquid dispersions (e.g., such as...) Figures 1A-1B (as shown in 104) and / or any premixed molding, including clay-like premixed molding (e.g., as shown in 104) Figure 1A As shown in 106), and / or solid premixed molded parts (e.g., as ...). Figure 1A 108 and Figure 1B (As shown in 109).

[0087] The mating adhesive surfaces can be provided by two mating substrates. In some cases, the mating adhesive surfaces can be opposing surfaces within a single substrate. The mating adhesive surfaces can be provided for placing particulate-liquid mixtures / dispersions and / or premixed molded bodies (e.g., clay-like premixed molded bodies and / or solid premixed molded bodies) between the mating adhesive surfaces for bonding / curing / alloying of the particulate-liquid mixture corresponding to the premixed molded body.

[0088] For ease of illustration, the exemplary method of using the pre-mixing form is described by using a pair of mating surfaces as an example, according to various embodiments of the present disclosure, the adhesive material can also be disposed on one adhesive surface or between adhesive surfaces of the same substrate in actual applications.

[0089] The adhesive surfaces can include engineered metals, such as steel with a gold coating, face-centered cubic (FCC) metals, such as in bulk or plated form, ceramics, such as silicon carbide, silicon dioxide, and / or aluminum nitride, and / or insulators, including glass, quartz, and / or sapphire. The insulators can or can not be metallized prior to bonding. The two adhesive surfaces can be made of the same or different materials.

[0090] In various embodiments, the adhesive surfaces can be pre-processed to provide a sufficiently clean and / or oxide-free adhesive surface.

[0091] For example, the adhesive surfaces can be solvent cleaned by immersion in a solvent containing acetone, alcohol, and / or deionized water at a temperature of 20°C or less. In other cases, the adhesive surfaces can be cleaned with acetone and alcohol first, and then rinsed with deionized water to clean the surfaces.

[0092] In another example, when the adhesive surfaces are made of metals, such as Cu or Ag, there can be excess oxides of copper or silver formed on the adhesive surfaces. The adhesive surfaces can be pre-processed to remove such excess oxides, such as by an etching process (including plasma etching, acid etching, and / or base etching) and / or mechanical abrasion (such as sandblasting, shot blasting, etc.). In one exemplary embodiment, the adhesive surfaces can be pre-processed by mechanical grinding using p2000 grit or 0000 steel wool to brighten the treated surfaces, and / or by chemical etching using NaOH followed by a deionized water rinse.

[0093] On the other hand, it should be understood that a certain amount (or small amount) of native oxides can remain on the adhesive surfaces without being completely removed. This can avoid possible alloying between the adhesive material and the adhesive surfaces.

[0094] In various embodiments, the treated adhesive surfaces can have a surface roughness ranging from 1 nanometer to 100 microns. Such roughness is desirable for providing adhesion to the adhesive material during subsequent reflow, re-dispersion, and / or curing. In contrast, while a too-smooth surface of the adhesive surfaces can be used in the adhesive / curing process, it can not facilitate re-mixing and curing of the adhesive material, and thus is less suitable.

[0095] In Figures 9A-9Bat 904, a particle-liquid mixture, e.g., which can correspond to a pre-mixed form, is disposed between the bonding surfaces. The particle-liquid mixture can include various types of solid particles and a base metal, similar to, the same as, or different from Figures 1A-1B those shown in FIGS. 2-8.

[0096] In some embodiments, the particle-liquid mixture for bonding / solidification / alloying can be obtained from Figures 1A-1B operation 102 in FIG. 1. In other embodiments, the particle-liquid mixture for bonding / solidification / alloying can be obtained from a pre-mixed form, e.g., a clay-like pre-mixed form (e.g., obtained at 106 in FIG. 1) and / or a solid pre-mixed form (e.g., obtained at 108 in FIG. 1 and 109 in FIG. 2) by a heating process, e.g., by convection / induction heating generated by a controlled magnetic field, and / or by any other suitable heating process. Figure 1A Figure 1A Figure 1B

[0097] At 906 in FIG. 9, a first magnetic field is applied to disperse the particle-liquid mixture to form a particle-liquid dispersion. Figure 9A

[0098] In various embodiments, the application of the first magnetic field at operation 906 in FIG. 9 can be similar to or the same as the magnetic field application at operation 104 in FIGS. 1 and 2. As shown in Figure 9A FIG. 9, the various types of solid particles in the particle-liquid mixture can be uniformly or otherwise controllably dispersed to form the particle-liquid dispersion. Figure 2 Figures 1A-1B

[0099] Figure 10 is an exemplary apparatus provided by embodiments of the present disclosure, which includes a magnetic processing device for processing a solid pre-mixed form.

[0100] In FIG. 10, as an example, a solid pre-mixed form 1040 is disposed between bonding surfaces 1055 of a mating substrate 1050. The bonding surfaces 1055 can have a disclosed surface roughness to better handle the bonding material at the interface therebetween. Then, as shown in FIG. 11, the solid pre-mixed form 1040 is heated using, e.g., a magnetic processing device / mechanism 1030 (or any other suitable heating device) to liquefy the solid base metal 1020B to form a corresponding particle-liquid mixture with a liquid base metal 1020A. Under the magnetic control at 1070 in FIG. 10, the solid particles in the particle-liquid mixture can be uniformly dispersed to form the particle-liquid dispersion. Figure 10 Figure 11 As shown in FIG. 11, the particle-liquid mixture can be uniformly dispersed to form a particle-liquid dispersion 1075.

[0101] As shown in FIG. 11, the particle-liquid mixture can be uniformly dispersed to form a particle-liquid dispersion 1075.​​​​​​​Figures 10-11 As shown, various particles disclosed herein can include, for example, reactive particles 1001 / 1003 and 1101 / 1103 (e.g., at least including reactive magnetic particles 1001 / 1101 and reactive non-magnetic particles 1003 / 1103), non-reactive magnetic particles 1006 / 1106, and / or any other possible solid additives 1008 / 1108.

[0102] Returning Figure 10 Each bonding surface 1055 can be disposed with a gap 1060 from the solid premix compact 1040. The gap 1060 can have an initial distance between the bonding surface 1055 and the solid premix compact 1040. Such an initial distance can allow the solid premix compact 1040 to contact each bonding surface 1055 without pressure or with less pressure (<1 MPa) applied to the solid premix compact 1040. In the undesirable case of large pressure application, the mating bonding surfaces can tend to compress each other and the constituents of the solid premix compact can be separated, resulting in undesirable effects of the solidification of the bonding material.

[0103] The initial distance of the gap 1060 can be maintained throughout the bonding / solidification / alloying process, for example, using a physical spacer or the spatial limitation of the two bonding surfaces 1050. For example, a clamp or robot hold can be used to maintain the initial thickness of the gap 1060. In various embodiments, the spacer can be removed after the bonding / solidification / alloying process of the solid premix compact 1040 is completed, or can be retained as an inactive portion of the mating substrate 1050 of the bonded structure after the bonding / solidification / alloying process is completed.

[0104] In various embodiments, the spacer can be made of a material selected to add toughness or strength to the formation of the bond of the solid premix compact to achieve the formed bond with air-tightness and electrical and thermal conductivity. For example, the spacer can include a solid core material and a low-melting binder material formed on the solid core material. In this case, the polymer can strengthen the formed bond and help to release stress from the solid premix compact.

[0105] In various embodiments, the solid core material for the spacer can be a metal or an organic polymer. The solid core material can be relatively ductile and capable of deforming to fill the adhesive void. The solid core material can have a melting point higher than the processing temperature for the adhesive such that the spacer remains solid. Examples of the solid core material can include ductile metals such as copper, gold, silver, or aluminum that do not form a negative oxidation pair with the substrate or the pre-mix alloy. Another example of the solid core material can include a polymer such as nylon (polyamide).

[0106] The low melting point adhesive material formed on the solid core material can include a polymer having a melting temperature equal to or lower than the pre-mix alloy solidification temperature and include, for example, a thermoplastic polyurethane, a styrene block copolymer, an ethylene vinyl acetate, a polyolefin, and / or a polylactic acid.

[0107] Figures 11-14 A first magnetic field is shown controllably applied to the exemplary particle-liquid mixture 1120 between the adhesive surfaces 1055 to magnetically disperse the plurality of types of solid particles (e.g., particles 1101, 1103, 1106, and / or 1108) in the liquid matrix metal 1020A to form a particle-liquid dispersion. During this process, the reactive particles 1101 / 1103 can or can not react with the liquid matrix metal 1020A. For example, the first magnetic field can be applied in a manner that does not disrupt the shell material to allow the reaction to occur.

[0108] In one embodiment, a magnetic processing device, such as the device 1030 in Figure 10 may be used to apply the first magnetic field. The magnetic processing device can include a coil wound around the adhesive substrate 1050. The shape and size of the wire used for the coil winding can be determined based on the specific application of the first magnetic field. For example, the coil winding can have a uniform shape and size and can be wound uniformly or non-uniformly along the length of the adhesive substrate.

[0109] The magnetic processing device may be connected to or include a controller (not shown), such as a computer controller, to control the current and / or current variations of the coil windings, and thus control, for example, the polarity, intensity, positioning, movement, rotation, spin, etc., of a first magnetic field. For example, the controller may select a coil of a certain length to selectively apply the first magnetic field to a portion of the particulate-liquid mixture. In another example, the first magnetic field may be controlled and varied along a specific direction, such as along the length of the adhesive substrate. In yet another example, the controller may control the coil windings to repeatedly provide a rotational field and / or a translational field, for example, back and forth along a specific direction. In yet another example, the controller may control the coil windings to move the particulate-liquid mixture / dispersion between different locations along the adhesive surface of the adhesive substrate, or to remove the particulate-liquid material from the adhesive substrate.

[0110] The first magnetic field can be applied in any suitable manner. Other suitable magnetic processing devices may include electromagnets and / or physical permanent magnets that can be controlled to heat, mix, disperse, etc. For example, electronic control of the electromagnet and / or control of the movement of the physical permanent magnet can be performed to provide the first magnetic field.

[0111] In one embodiment, such as Figure 12 As shown, the first magnetic field can be applied and calibrated such that solid particles in the liquid matrix metal can be pulled and moved toward the interface with the bonding surface. Simultaneously, the first magnetic field can be used to heat and maintain the matrix metal in a liquid state.

[0112] like Figure 13 As shown, the first magnetic field can be moved at various angles to drag the solid particles across the two adhesive surfaces, for example, moving them through the cross-section of the adhesive material in any suitable shape or path of motion. The solid particles dragged on the bonding surfaces may scrape, remove, and / or destroy the natural oxide layer formed at the outermost layer 1305 of the bonding material (e.g., a particle-liquid mixture) at the interface, thereby achieving dispersion and wetting. Figure 14 As shown. Compared to the adhesive forces in the bonding material, larger particles can be subjected to greater forces and have a better chance of moving the solid particles to the adhesive-bonded surface interface. Thus, the movement of magnetic particles can be controlled to improve surface wetting, eliminate the need for flux, and reduce voids and gaps often found in conventional welding materials.

[0113] Application of the first magnetic field can allow for movement and dispersion of all solid particles in the binding material. Unlike traditional mechanical force driven by pressing the particles and driving the liquid component out, the disclosed particle-liquid mixture / dispersion can move as a mass from one location to another and not squeeze out the liquid component. Furthermore, as shown in Figure 14 FIG. 2, the first magnetic field can also be used to smoothen the particle-liquid mixture after it is dispersed as a large "mass".

[0114] The non-reactive solid particles can be used to drive, disperse, mix, and / or heat the particle-liquid mixture to form a uniform particle-liquid dispersion, which can drive uniform reaction to solidify and can further strengthen the binding material.

[0115] In one embodiment, referring to Figure 15 A gradient static magnetic field can be used to align magnetic fibers or wires within the binding material to provide preferred and anisotropic properties. For example, large size magnetic particles of Fe, Ni, Co, Cr, Nb, and / or alloys thereof can be incorporated into the particle-liquid mixture for binding. The magnetic alignment can be varied to produce various properties, such as anisotropic thermal and / or mechanical strength.

[0116] Unlike traditional mechanical mixing, the disclosed magnetic mixing can be performed, such as by a dynamic magnetic field or a spiral magnetic field, to drive the motion of the solid magnetic particles (reactive or non-reactive, with or without large size) through the binding material. For example, under a dynamic magnetic field, the disclosed various types of solid particles can be attracted to move towards the interface between the binding material and the binding surface. Once at the interface, the solid particles can move in plane to scratch the interface to mix the native oxide of the base metal (e.g., at 1305 in FIG. 1) into the interior of the binding material (e.g., at the interface). Accordingly, the removal or disturbance of the oxide layer can cause metal alloying and increase the interface strength. Figure 13

[0117] The shape of the binding material can be designed according to the actual application, for example. The disclosed magnetic mixing / dispersion can be in a random or ordered manner and can be performed simultaneously with magnetic heating.

[0118] In Figure 9A ​at 908 to bond / solidify / alloy the particle-liquid dispersion to allow for reaction between the reactive particles and the base metal or solidification. During this solidification operation, the temperature can be controlled by the second magnetic field in combination with the controllable composition of the particle-liquid dispersion. For example, the use of the second magnetic field can allow for a solidification temperature of a particular particle-liquid dispersion to be different than the conventional use solidification temperature of the corresponding materials in the particle-liquid system.

[0119] In various embodiments, the solidification temperature can be about 250°C or less, such as about 150°C or less, or about 50°C or less (e.g., at room temperature). More particularly, the use of a particular / controlled composition of the particle-liquid dispersion in combination with the second magnetic field can allow for a lower solidification temperature, such as no higher than 150°C, and in some embodiments, no higher than 100°C, and in other embodiments, no higher than 50°C. Of course, by controlling the second magnetic field and / or the composition of the particle-liquid dispersion, a high solidification temperature, such as about 250°C, can also be controlled and used.

[0120] The second magnetic field can be applied in a different manner than the first magnetic field, such as in strength, polarity, duration, etc. The second magnetic field can be provided by the same magnetic processing device as the first magnetic field but modulated differently.

[0121] Under the second magnetic field, the bonding material can be heated at a temperature to activate the chemical reaction between the reactive particles and the base metal for solidification / alloying, such as at a temperature above the melting point of the liquid component (from the Figure 9A the bonding material obtained at operation 904. During these solidification / bonding / alloying processes, the temperature is no higher than 150°C, and in some embodiments, no higher than 100°C, and in other embodiments, no higher than 50°C.

[0122] In one embodiment, the first magnetic field can be dynamic in nature to drive the motion of the particles to disperse the particle-liquid mixture to form a particle-liquid dispersion. For example, as shown in FIG. 9, a stationary pole magnet can be moved within the entire space disposed. The resulting first magnetic field is controlled / applied in such a way that does not cause significant solidification or heating, thereby can prevent premature solidification. The second magnetic field can be controlled to have a similar effect as induction heating, where the motion of the particles is limited, and the pre-mixed shaped body is heated to drive solidification. Figure 10

[0123] ​As disclosed herein, the reactive particles can include a core-shell structure having a shell material at least partially covering a core material. In one embodiment, the shell material of the reactive particles can be used to control the kinetics and dissolution rate of the core material, thereby controlling the reaction rate between the reactive particles and the base metal used for solidification.

[0124] The shell material can range in thickness from one atomic layer to about 100 nanometers, such as a few atomic layers. The shell material can be thick enough to largely prevent solid state alloying between the reactive particles and the solid base metal for pre-mixing the shaped body. The shell material can also be thin enough so that the shell can rupture during solidification to allow such a reaction. The thickness of the shell material can be controlled depending on the selection of the base metal and the reactive particles.

[0125] In one exemplary embodiment, the core material is one or more of Fe and Ni, and the shell material is an oxide of one or more of Fe and Ni. The exemplary base metal Ga material reacts with the shell material by dissolution or interdiffusion at a rate that depends on the thickness of the shell material.

[0126] According to various embodiments, in addition to controlling the shell thickness, other mechanisms can be applied to the core-shell structure of the reactive particles to control the reaction kinetics / rate of solidification / alloying.

[0127] For example, the reactive particles can include a shell material that reacts slower than the core material with the base metal to provide a longer solidification time. For example, the shell material can be copper, the core material can be gold, and the base metal can be liquid gallium, which reacts faster with gold than with copper.

[0128] Another exemplary reactive particle can include a reactive shell material (e.g., Cu) and a non-reactive core material (e.g., Co, and / or a ceramic material including AlN, SiC, Si02, Ti02, Zr02, AI2O3, BeO, Si3N4, B4C, WC, and / or diamond). In some cases, the reactive shell material can include multiple layers having an oxide layer at least partially covering the reactive shell material. In one example, the shell material can be Cu, and the core material can be Co, while the shell material can also include copper oxide covering the copper shell material. The magnetic properties of Co can be used to heat, mix, or wet the bonding surface, while the shell material can enable a coherent interface and strong bonding of the adhesive material to the bonding surface. In another example, the shell material can be Cu, the core material can be AlN, and the shell material can also include copper oxide covering the copper shell material.

[0129] In various embodiments, the shell material can be selected to incorporate to support and strengthen the solid alloy. In one example, the shell material of the reactive particles can be non-reactive and / or can partially cover all of the interior particles of the core material (e.g., as a flaky shell). When the interior particles are dissolved by the Ga liquid, the shell material can remain in the preform material to provide mechanical strength and form a composite. Such shell material can include a ductile material, including steel, and the core material can be Cu. In another example, the shell material can be a brittle oxide, such as ZnO or TiO2, which can break due to thermal expansion mismatch with the Cu, Ag, or Ni metal used as the core material inside the shell material. The hard and brittle shell material can strengthen the solid alloy.

[0130] In various embodiments, the shell material can be broken during preform processing, such as solidification / bonding / alloying. For example, the shell material of the reactive particles can be overcome by dissolution of the base metal, which occurs due to, for example, application of the second magnetic field. For example, under control of the second magnetic field, the oxide shell material can be broken to allow its core material Fe or Cu to interact / react with the liquid base metal.

[0131] In various embodiments, the solidified material, i.e., the binder or the solid alloy, can be an all-metal solid. Figure 16 is an exemplary solid alloy that has at least added non-reactive magnetic particles, according to embodiments of the present disclosure. The solid alloy can have higher temperature stability than solidification temperature. As shown, the non-reactive particles can remain in the solid alloy and can be uniformly dispersed therein, for example, to provide desired properties, such as mechanical strength, high thermal and electrical conductivity. Figure 16 is an exemplary solid alloy that has at least added non-reactive magnetic particles, according to embodiments of the present disclosure. The solid alloy can have higher temperature stability than solidification temperature. As shown, the non-reactive particles can remain in the solid alloy and can be uniformly dispersed therein, for example, to provide desired properties, such as mechanical strength, high thermal and electrical conductivity.

[0132] Figure 9B is another exemplary method of using a pre-mixed preform, according to various embodiments of the present disclosure.

[0133] As shown in operation 904 in Figure 9B After operation 904 in which the particle-liquid mixture corresponding to the pre-mixed preform is disposed between the mating bonding surfaces, the particle-liquid mixture can be heated at a temperature higher than the low melting temperature of the base metal to re-flow the particle-liquid mixture, as shown in operation 907 in Figure 9B .

[0134] In Figure 9BThe heating process can include any heating means by conduction, convection, or radiation, etc. For example, a pulsed laser can be used to heat the particle-liquid mixture. The heating process can be arranged while applying a magnetic field to the particle-liquid mixture. In the heating process of operation 907 in FIG. 9B, the temperature is no higher than 150°C, and in some embodiments, no higher than 100°C, and in other embodiments, no higher than 50°C.

[0135] In Figure 9B At 909, a magnetic field is applied to the particle-liquid mixture while the particle-liquid mixture is heated to allow a reaction to occur between reactive particles and the base metal. During this reaction operation 909, the temperature is no higher than 150°C, and in some embodiments, no higher than 100°C, and in other embodiments, no higher than 50°C.

[0136] Under the magnetic field, the adhesive material can be dispersed and further heated at a temperature to activate a chemical reaction between the reactive particles and the base metal to solidify, for example, at a temperature higher than the melting point of the liquid component (from which the adhesive material obtained in operation 904). Figure 9A

[0137] For example, a magnetic processing device (e.g., as shown in FIG. 9A) can be used and controlled to modulate the magnetic field. For example, the magnetic processing device can include a coil wound around the matching adhesive substrate. The shape and size of the wire used in the coil winding can be determined according to the specific application of the magnetic field. Figure 10

[0138] The magnetic processing device can be connected to or include a controller, e.g., a computer controller, to control the current and / or current variation of the coil winding, and thus control, for example, the polarity, strength, positioning, motion, rotation, spin, etc. of the first magnetic field. For example, the controller can select a length of the coil to selectively apply the magnetic field to a partial amount of the particle-liquid mixture to locally disperse solid particles in the particle-liquid mixture. In another example, the magnetic field can be controlled and varied in a particular direction, e.g., the length direction of the adhesive substrate. In yet another example, the controller can control the coil winding to repeatedly provide a rotating field and / or a translating field back and forth in a particular direction. In yet another example, the controller can control the coil winding to move the particle-liquid mixture / dispersion between different positions along the adhesive surface of the adhesive substrate, or move the particle-liquid material out of the adhesive substrate.

[0139] ​​Other suitable magnetic processing devices can include electromagnets and / or physical permanent magnets that can be controlled for heating, mixing, dispersing, etc. For example, electronic control of electromagnets and / or control of moving physical permanent magnets can be performed to provide the first magnetic field.

[0140] The magnetic particles in the particle-liquid mixture can align, move, and disperse while being heated. The magnetic field can be modulated such that the orientation of the particles changes and the motion of the magnetic particles can provide mixing / dispersion within the cross-section of the particle-liquid mixture. The magnetic motion can be rotational, translational, or a mix of rotational and translational such that the particles move within the cross-section of the particle-liquid mixture. During this process, the adhesive surface can come into contact with some of the moving liquid. The moving liquid can then disrupt and disperse the native oxide layer of the outermost layer of the particle-liquid mixture, forming a new interface.

[0141] In addition to more uniformly dispersing particles in the particle-liquid mixture, the magnetic field can be adjusted to allow for a reaction between the reactive particles and the substrate to form a solid alloy.

[0142] Thus, under a magnetic field, various types of solid particles can be oriented, moved, and / or aligned along the entire cross-section of the adhesive material containing the particles. When under a dynamic magnetic field, the particles align and move along the motion of the magnetic field. Various motions of the particles can be induced under the action of the magnetic field. For example, under a rotating magnetic field, a radial motion of the particles can be generated, which can essentially scrape and mix the adhesive material at the interface between the adhesive material and the adhesive surface. The motion of the particles can cause agitation at the interface. By dynamically controlling / modulating the magnetic field, the concentration at different places can be controlled. The motion of the particles can fill voids in the adhesive material to redistribute the particles across the cross-section of the adhesive material. This distribution can provide a uniform chemical composition. Furthermore, the surface adhesion at the interface can be disrupted and changed due to the motion of the particles to provide wetting on the contact substrate, which can homogenize the compound and have a uniform distribution. Furthermore, fluctuating the magnetic field across the cross-section and heating can provide heating and local distribution of concentration.

[0143] Typically, fluxes are necessary for adhesion of solder / bonding materials to form a natural oxide layer. Typically, the fluxes are applied prior to the bonding process and used to clean and wet the bonding surfaces. However, the fluxes present several drawbacks. For example, the fluxes can bring corrosion and contamination to the bonded parts, and can cause adverse health effects due to the fumes and exhaust gases generated during bonding and processing. Flux materials are also often mixed in the metal powders in preforms to help the interface bond to the bonding surfaces. For example, the surface or exterior of the joint material can be mixed with flux, while the interior of the bonding material can be free of flux. However, without agitation at the traditional preform bonding interface to disrupt the natural oxide layer floating on the outer surface of the bonding material, the adhesion at the interface will not be ideal. The traditional preforms do not sufficiently adhere to most bonding surfaces.

[0144] The modulated magnetic field can allow various types of solid particles as disclosed to move towards the interface between the bonding material and the bonding surface, and further create scratches or scrapes at such interface to disrupt the natural oxide of the base metal on the outer surface of the bonding material (e.g., at 1305 in Figure 13 The natural oxide of the base metal scratched into the interior of the bonding material from the outer surface can then strengthen the mechanical properties of the resulting bonded material, and can further allow the base metal to directly interact with and wet the bonding surface.

[0145] Accordingly, according to various embodiments of the present disclosure, the need for pre-wetting of the bonding substrate and any fluxes in the bonding material is eliminated by applying the disclosed particle-liquid mixture in combination with the modulated magnetic field.

[0146] The resulting solidified bond of the brand new and more stable alloy state can now withstand higher temperatures than the bonding surface (and portions thereof) are subjected to. In one embodiment, the resulting solidified bond can withstand higher temperatures than the solidification temperature, for example, high temperatures of about 200 °C or higher, such as about 260 °C or higher.

[0147] The present disclosure is as described above, but the present disclosure is not limited to the disclosed embodiments. Various changes and modifications can be made by those skilled in the art without departing from the spirit and scope of the present disclosure. Accordingly, the scope of the present invention is to be limited only by the scope of the claims.

Claims

1. A premixed molded article, comprising: base metal, and Various types of solid particles dispersed in the matrix metal, wherein the matrix metal includes one of liquid matrix metal and solid matrix metal. The various types of solid particles include at least: Non-reactive magnetic particles, which respond to a magnetic field to controllably disperse the various types of solid particles in the matrix metal, and Reactive particles, which can react with the base metal under the action of the magnetic field, wherein one of the reactive particles includes a core-shell structure, wherein: The core-shell structure includes a core material and a shell material different from the core material and at least partially surrounding the core material. The reaction rate between the core material and the base metal is different from that of the shell material.

2. The premixed molded article according to claim 1, characterized in that, The base metal includes Ga, In, Sn, Bi, Pb, Cd, Hg, Rb, Zn, Bi, or combinations thereof.

3. The premixed molded article according to claim 1, characterized in that, The reactive particles comprise at least one reactive metallic material, which includes Fe, Ni, Cu, Ag, Au, In, Cu, Sn, Bi, Zn, Ti, V, Cr, Mo, Nb, Zr, Hf, Pt, Ir, or combinations thereof.

4. The premixed molded article according to claim 1, characterized in that, The thickness of the shell material ranges from atomic layer thickness to 100 nm.

5. The premixed molded article according to claim 1, characterized in that, The core material includes a reactive metallic material, and the shell material includes an oxide layer of the reactive metallic material.

6. The premixed molded article according to claim 1, characterized in that, The core-shell structure includes one or more of the following: A core-shell structure having a shell material comprising one or more oxides of Fe and Ni and a core material comprising one or more of Fe and Ni; A core-shell structure having a shell material comprising Cu and a core material comprising Au; A core-shell structure having a shell material comprising steel and a core material comprising copper; A core-shell structure having a shell material comprising ZnO or TiO2 and a core material comprising Cu, Ag, Ni or a combination thereof; and A core-shell structure having a shell material comprising Cu and copper oxide at least partially covering Cu, and a core material comprising Co, BeO, Si3N4, B4C, WC, diamond, AlN, SiC, SiO2, TiO2, ZrO2, Al2O3, or combinations thereof.

7. The premixed molded article according to claim 1, characterized in that, The reactive particles include reactive magnetic particles, reactive non-magnetic particles, or a combination thereof.

8. The premixed molded article according to claim 7, characterized in that, The reactive magnetic particles include one or more of Fe and Ni.

9. The premixed molded article according to claim 7, characterized in that, The reactive magnetic particles have an average size greater than 50 micrometers.

10. The premixed molded article according to claim 7, characterized in that, The reactive nonmagnetic particles include Cu, Ag, Au, In, Cu, Sn, Bi, Zn, Ti, V, Cr, Mo, Nb, Zr, Hf, Pt, Ir, or combinations thereof.

11. The premixed molded article according to claim 1, characterized in that, The weight ratio of the base metal to the various types of solid particles ranges from 4:1 to 1:

4.

12. The premixed molded article according to claim 1, characterized in that, The various types of solid particles have an average size ranging from 100 nanometers to 100 micrometers.

13. The premixed molded article according to claim 1, characterized in that, The reactive particles have an average size ranging from 100 nanometers to 50 micrometers.

14. The premixed molded article according to claim 1, characterized in that, The non-reactive magnetic particles have an average size ranging from 5 micrometers to 100 micrometers.

15. The premixed molded article according to claim 1, characterized in that, The non-reactive magnetic particles include Co-containing particles, Nd-containing particles, Cr-containing particles, or combinations thereof.

16. The premixed molded article according to claim 1, characterized in that, The non-reactive magnetic particles include at least one large magnetic particle with a size greater than 5 micrometers, and the large magnetic particle includes microwires, microfibers, or combinations thereof.

17. The premixed molded article according to claim 1, characterized in that, The various types of solid particles also include additives, which include semiconductor particles, metal-doped semiconductor particles, or combinations thereof, and the semiconductor particles include SiC particles, AlN particles, SiO2 particles, or combinations thereof.

18. The premixed molded article according to claim 1, further... include: A clay-like premixed molded body comprising the various types of solid particles magnetically dispersed in a liquid matrix metal, wherein the reactive particles do not substantially react with the liquid matrix metal at a temperature of 25°C or lower.

19. The premixed molded article according to claim 1, further comprising: A solid premixed molded body comprising the plurality of solid particles of the aforementioned types magnetically dispersed in a solid matrix metal, wherein the reactive particles do not substantially react with the solid matrix metal at a temperature of 25°C or lower.

20. A method for manufacturing the premixed molded article of claim 1, comprising: A particulate-liquid mixture is provided, comprising multiple types of solid particles and a liquid matrix metal, wherein the multiple types of solid particles include at least: Reactive particles that can react with the matrix metal; and Non-reactive magnetic particles; A magnetic field is applied to the particle-liquid mixture to magnetically disperse the various types of solid particles in the liquid matrix metal to form a particle-liquid dispersion, without substantially causing a reaction between the reactive particles and the liquid matrix metal; and A clay-like premixed molded body is prepared based on the particle-liquid dispersion without the need to solidify the liquid matrix metal.

21. The method according to claim 20, characterized in that, Providing the particle-liquid mixture includes: Mix the various types of solid particles with the matrix metal particles; and The matrix metal particles are melted into liquid matrix metal by applying a magnetic field to the matrix metal, wherein the liquid matrix metal is mixed with various types of solid particles.

22. The method according to claim 20, characterized in that, Providing the particle-liquid mixture includes: The solid substrate metal is liquefied by applying a magnetic field; and The various types of solid particles are added to the liquefied matrix metal to provide the particle-liquid mixture.

23. The method according to claim 20, characterized in that, The preparation of the clay-like premixed molding body based on the particle-liquid dispersion includes: The particle-liquid dispersion is processed by one or more of rolling, pressing, extrusion, and casting to form a putty-like premixed molded body.

24. The method of claim 20, further comprising: The clay-like premixed molded body is prepared by rolling the particle-liquid dispersion, wherein the thickness of the clay-like premixed molded body ranges from 5 micrometers to 500 micrometers.

25. The method of claim 20, further comprising: A solid premixed molded body is formed by curing the clay-like premixed molded body without substantially causing a reaction in the solid premixed molded body; and The solid premixed molded body is processed by one or more of rolling, pressing, extrusion and casting.

26. The method of claim 20, further comprising: The particulate-liquid mixture is provided in a container, wherein the container comprises a plastic surface made of a material including polytetrafluoroethylene, high-density polyethylene, low-density polyethylene, or a combination thereof.

27. The method according to claim 26, characterized in that, Applying the magnetic field to the particle-liquid mixture includes: A container containing the particulate-liquid mixture is placed in a magnetic processing device, wherein the magnetic processing device includes a coil wound around the container; and The controller controls the current or current variation in the coil to modulate one or more of the polarity, intensity, positioning, movement, direction, and rotation of the magnetic field applied to part or all of the particle-liquid mixture.

28. The method of claim 26, further comprising: During the formation of the particle-liquid dispersion, the particle-liquid mixture is moved from one location to another by applying the magnetic field along the inner wall of the container.

29. The method according to claim 20, characterized in that, Applying the magnetic field to the particle-liquid mixture by varying the magnetic field at one or more angles includes: The magnetic field, which varies at one or more angles, is modulated to move the various types of solid particles through the cross-section of the particle-liquid mixture and drag the various types of solid particles along the surface of the container containing the particle-liquid mixture.

30. The method according to claim 20, characterized in that, Applying the magnetic field to the particle-liquid mixture further includes: A gradient static magnetic field is applied to controllably align the various types of solid particles in the particle-liquid mixture to provide one or more of anisotropic thermal conductivity and anisotropic mechanical strength.

31. A method for manufacturing the premixed molded article of claim 1, comprising: A particulate-liquid mixture is provided, comprising multiple types of solid particles and a liquid matrix metal, wherein the multiple types of solid particles include at least: Reactive particles that can react with the matrix metal; and Non-reactive magnetic particles; A magnetic field is applied to the particle-liquid mixture to magnetically disperse the various types of solid particles in the liquid matrix metal without substantially causing a reaction between the reactive particles and the liquid matrix metal to form a particle-liquid dispersion. The liquid matrix metal is solidified to disperse the various types of solid particles within the solidified matrix metal without substantially causing a reaction between the reactive particles and the solid matrix metal; and Prepare a solid premixed molded body comprising the various types of solid particles and the cured matrix metal.

32. The method according to claim 31, characterized in that, The solidification of the liquid matrix metal includes: Rapid quenching processes include liquid cooling and Peltier cooling.

33. The method according to claim 31, characterized in that, The thickness of the solid premixed molded body ranges from 25 micrometers to 10 millimeters.

34. A method of using the premixed molded article of claim 1, comprising: Provides mating adhesive surfaces; A particle-liquid mixture corresponding to the premixed molded body is placed between the mating adhesive surfaces, wherein: The particle-liquid mixture comprises multiple types of solid particles and a liquid matrix metal, wherein the multiple types of solid particles include at least reactive particles that can react with the matrix metal and non-reactive magnetic particles. A first magnetic field is applied to the particle-liquid mixture to magnetically disperse the various types of solid particles in the liquid matrix metal to form a particle-liquid dispersion; and A second magnetic field is applied to solidify the particle-liquid dispersion to allow the reactive particles to react with the matrix metal.

35. The method according to claim 34, characterized in that, When setting the particle-liquid mixture, a gap is formed between each mating adhesive surface and the adjacent side of the particle-liquid mixture.

36. The method of claim 34, further comprising: A physical spacer is provided between the particle-liquid mixture and each mating adhesive surface to maintain a gap between the particle-liquid mixture and each mating adhesive surface.

37. The method according to claim 34, characterized in that, The mating bonding surface is provided by two mating substrates, and each of the two mating substrates includes one or more of engineering metals, face-centered cubic metals, ceramics, and insulators.

38. The method of claim 34, further comprising, before providing the mating adhesive surfaces: Solvent cleaning of the mating adhesive surfaces; and / or Remove excess oxides from one or more of the mating adhesive surfaces.

39. The method according to claim 34, characterized in that, One or more of the mating adhesive surfaces have a surface roughness ranging from 1 nanometer to 100 micrometers.

40. The method of claim 34, further comprising, before disposing the particulate-liquid mixture between the mating adhesive surfaces: The particulate-liquid mixture is provided by one or more of the following operations: Mixing various types of solid particles with the matrix metal particles, and melting the matrix metal particles into the liquid matrix metal; The matrix metal particles are liquefied to form the liquid matrix metal, and the various types of solid particles are added to the liquid matrix metal; and Liquefied clay-like premixed molding body and / or solid premixed molding body to provide the particle-liquid mixture.

41. The method according to claim 34, characterized in that, Setting the particle-liquid mixture between the mating adhesive surfaces includes: The premixed molded body is disposed between the mating adhesive surfaces, wherein the premixed molded body comprises a clay-like premixed molded body and / or a solid premixed molded body; and The particle-liquid mixture is formed by liquefying the premixed molded body disposed between the mating adhesive surfaces.

42. The method according to claim 34, characterized in that, Applying the first magnetic field and / or applying the second magnetic field includes: The mating adhesive surface is placed in a magnetic processing device, wherein the magnetic processing device includes a coil wound around the mating adhesive surface; and Controlling the current or current variation in the coil to modulate one or more of the polarity, intensity, positioning, movement, direction, and rotation of the magnetic field applied to part or all of the particle-liquid mixture or the particle-liquid dispersion.

43. The method of claim 34, further comprising: The particle-liquid mixture is moved from one location to another along one or more of the mating adhesive surfaces by applying the first magnetic field to form the particle-liquid dispersion.

44. The method according to claim 34, characterized in that, The first magnetic field is applied to cause the various types of solid particles to be drawn to move within the liquid matrix metal toward the interface with each mating adhesive surface, wherein: Under the action of the first magnetic field, the various types of solid particles destroy the oxide layer formed on the outermost layer of the particle-liquid mixture, improve the surface wettability of the mating and bonding surfaces, and thus eliminate the need for flux.

45. The method according to claim 34, characterized in that, The second magnetic field is applied to alloy the various types of solid particles with the matrix metal at a temperature of 250°C or lower.

46. ​​The method according to claim 34, characterized in that, Under the second magnetic field, the various types of solid particles are alloyed with the matrix metal at a temperature of 50°C or lower.

47. The method according to claim 34, characterized in that, Applying the first magnetic field includes: A gradient static magnetic field is applied to controllably align the various types of solid particles in the particle-liquid mixture to provide one or more of anisotropic thermal conductivity and anisotropic mechanical strength to the solidified particle-liquid dispersion.

48. A method of using the premixed molded article of claim 1, comprising: Provides mating adhesive surfaces; The premixed molded body is disposed between the mating adhesive surfaces, wherein: The premixed molded body comprises multiple types of solid particles and a matrix metal, wherein the multiple types of solid particles include at least reactive particles and non-reactive magnetic particles; The premixed molded body is heated at a temperature above the low melting temperature of the base metal to provide a particle-liquid mixture comprising the various types of solid particles in the liquid base metal; and A magnetic field is applied while heating to magnetically disperse the various types of solid particles in the liquid matrix metal, allowing the reactive particles to react with the matrix metal.

49. The method according to claim 48, characterized in that, The gap between the particle-liquid mixture and each mating bonding surface has a thickness that is maintained when the premixed molded body is heated.

50. The method according to claim 48, characterized in that, The premixed molded body includes a clay-like premixed molded body and / or a solid premixed molded body.

51. The method of claim 48, further comprising: Under the influence of the magnetic field, the particle-liquid mixture is moved from one location to another along one or more of the mating adhesive surfaces, thereby magnetically dispersing the various types of solid particles in the liquid matrix metal.

52. The method according to claim 48, characterized in that, When the magnetic field is applied, the various types of solid particles in the liquid matrix metal are drawn toward the interface with each mating bonding surface, wherein: The various types of solid particles disrupt the oxide layer formed on the outermost layer of the particle-liquid mixture to improve the surface wettability of the mating adhesive surfaces and eliminate the need for flux.

53. The method according to claim 48, characterized in that, The magnetic field is applied to allow the reactive particles to react with the base metal at a temperature of 150°C or lower.

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