LIQUID COLD WELDING METHODS AND APPARATUS
20230330783 · 2023-10-19
Assignee
Inventors
- Vladimir Yufit (London, GB)
- Le Sheng Nicholas YIU (London, GB)
- Belen BELLO RODRIGUEZ (London, GB)
- Farid TARIQ (London, GB)
- Moshiel BITON (Tel-Aviv Yaffo, IL)
- Nir HALUP (Tel-Aviv Yaffo, IL)
Cpc classification
International classification
Abstract
The application discloses a method of liquid cold welding (LCW) including: (a) engaging two or more porous conductive substrate layers between perforated non-conductive frames so that the substrate layers contact one another; (b) immersing the substrate layers in an electrolyte solution; and (c) applying electric current and/or voltage and/or electric power to the electrolyte solution. Apparatus suitable for performance of some embodiments of the method are also disclosed.
Claims
1. A method of electrochemical deposition comprising: (a) engaging two or more porous conductive substrate layers between perforated non-conductive frames so that said substrate layers contact one another; (b) immersing said substrate layers in an electrolyte solution that contains dissolved metal ions; and (c) applying electric current and/or voltage and/or electric power to said electrolyte solution to effect metal or metal composite deposition from said ions in said electrolyte solution onto said substrate layers, thereby joining said two or more porous conductive substrate layers.
2. The method of claim 1, wherein said applying includes applying an electric current flowing from counter electrodes, through said porous conductive substrate layers between perforated non-conductive frames to working electrodes.
3. The method of claim 1, wherein said applying includes applying a constant voltage using a reference electrode.
4. The method of claim 1, wherein said applying includes applying a constant power.
5. The method of claim 1, comprising: folding a single porous conductive substrate layer to form two or more porous conductive substrate layers.
6. The method of claim 1, comprising: feeding two or more porous conductive substrate layers concurrently between said perforated non-conductive frames; and withdrawing said two or more porous conductive substrate layers after said joining as a bonded substrate.
7. The method of claim 6, comprising: Increasing a distance between said perforated non-conductive frames to facilitate insertion and/or removal of said two or more porous conductive substrate layers.
8. The method of claim 7, comprising: decreasing a distance between said perforated non-conductive frames so that the substrate layers contact one another.
9. The method of claim 1, comprising: pumping said electrolyte solution through said perforated non-conductive frames and said substrate layers during said applying.
10. An electrochemical deposition apparatus comprising: (a) a container with two counter electrodes, or an active electrode and a reference electrode, positioned opposite one another within the container; and (b) at least two perforated non-conductive frames adapted to engage and retain a multilayer substrate so the layers remain in contact with one another; said frames positioned between said counter electrodes.
11. (canceled)
12. The apparatus according to claim 10, comprising: two or more feed rollers adapted to feed two or more porous conductive substrate layers concurrently between said perforated non-conductive frames; and an uptake roller adapted to spool said two or more porous conductive substrate layers after joining said two or more porous conductive substrate layers as a bonded substrate.
13. The apparatus according to claim 10, comprising: a distance regulation mechanism adapted to adjust a distance between said perforated non-conductive frames.
14. The apparatus according to claim 10 comprising a folding mechanism configured to fold a single porous conductive substrate layer to produce a stack of porous conductive substrate layers.
15. The apparatus according to claim 10, comprising: a pump positioned to pump said electrolyte solution through said perforated non-conductive frames and said substrate layers during operation.
Description
BRIEF DESCRIPTION OF THE DRAWINGS
[0017] In order to understand the invention and to see how it may be carried out in practice, embodiments will now be described, by way of non-limiting example only, with reference to the accompanying figures. In the figures, identical and similar structures, elements or parts thereof that appear in more than one figure are generally labeled with the same or similar references in the figures in which they appear. Dimensions of components and features shown in the figures are chosen primarily for convenience and clarity of presentation and are not necessarily to scale. The attached figures are:
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DETAILED DESCRIPTION OF EMBODIMENTS
[0047] Embodiments of the invention relate to electrochemical bonding methods and apparatus.
[0048] Specifically, some embodiments of the invention can be used to produce porous 3D metal structures. According to various exemplary embodiments of the invention these porous 3D metal structures are engineered for use in a variety of electrochemical and non-electrochemical application. Electrochemical applications include, but are not limited to batteries, fuel cells and electrolyzers. Non-electrochemical applications include, but are not limited to miniaturized heat exchangers, catalyst support and others.
[0049] The principles and operation of method and/or apparatus according to exemplary embodiments of the invention may be better understood with reference to the drawings and accompanying descriptions.
[0050] Before explaining at least one embodiment of the invention in detail, it is to be understood that the invention is not limited in its application to the details set forth in the following description or exemplified by the Examples. The invention is capable of other embodiments or of being practiced or carried out in various ways. Also, it is to be understood that the phraseology and terminology employed herein is for the purpose of description and should not be regarded as limiting.
[0051] Overview
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[0053] According to various exemplary embodiments of the invention WEs are fully or partially immersed in the electrolyte 2. In some embodiments contact between WE 5 and electrolyte 2 is minimized yet a good contact between it and substrates in WEA is ensured. By applying negative current, voltage or power on WE and positive current, voltage or power on CEs a metal ions in the electrolyte 2 begin to deposit on every substrate that is in electrical contact with WE. As a metal or metal alloy layer grows on different substrates 4 the metal or metal alloy forms a bonding layer between substrates 4.
[0054] According to various exemplary embodiments of the invention the thickness and morphology of this bonding layer is controlled by varying electrolyte composition (optionally including one or more different additives) and/or metal ion type and/or metal ion concentrations and/or pH and/or temperature and/or flow rate of electrolyte and/or stirring of electrolyte and/or current density and/or voltage and/or power. According to various exemplary embodiments of the invention the electrolyte is aqueous or non-aqueous contains dissolved metal ions such as, for example, copper, nickel, zinc and others.
[0055] In the depicted embodiment, reference electrode RE 6 controls voltage between WE 5 and RE 6 by adjusting current between CEs 1A and 1B and WE 5. Examples of aqueous REs include, but are not limited to, Ag/AgCl, Hg/Hg.sub.2Cl.sub.2, Hg/HgO.
[0056] Exemplary Materials According to various exemplary embodiments of the invention WEs 5 are constructed of any electronically conductive material provided it is stable in the electrolyte and the bonded 3D electrode can be easily detached from it. For example, stainless steel, titanium, niobium, carbon and composite carbon-polymer conductive materials are suitable for use in the context of various embodiments of the invention.
[0057] There are two types of CEs (e.g. 1A and 1B in
[0058] The second type of CEs is made of, or covered with, materials that do not dissolve during the LCW process but rather catalyze the reaction of electrolyte oxidation. Examples of such materials include but are not limited to TI, Nb, W, Mo and V coated by a few micron thick layer of Au, Pt, Ir, Ru or any other noble metal capable of electro-catalytically oxidizing the solvent in electrolyte 2 (water or any other solvent). With the second type of CEs, processes associated with metal deposition are sensitive to changes in pH (in the case of an aqueous electrolyte 2) of the electrolyte. In some embodiments, addition of a sufficient amount of metal ions that are reduced to form a bonding layer between porous substrates is required. Alternatively or additionally, in some embodiments pH adjustment is required.
[0059] Exemplary Working Electrodes (WE) and Conductive Frames
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[0061] According to various exemplary embodiments of the invention holes in frames 3 are placed to: produce uniform attachment across the porous substrate; or only in specific areas so the substrates will only be attached at pre-defined locations.
[0062] Alternatively or additionally, in some embodiments a shape of frame 3 is tailored in accordance with the shape of the substrate. Alternatively or additionally, in some embodiments the number of the holes per unit area in frame 3 is adjusted to change bonding forces. Alternatively or additionally, in some embodiments frames 3 are made from machined dielectric material somehow or from metal coated with dielectric material.
[0063] Exemplary Electrolyte Flow Considerations
[0064] In some embodiments, in order to improve permeation of electrolyte 2 in stacked porous layers (4 in
First Exemplary Device
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Second Exemplary Device
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Third Exemplary Device
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[0072] In the depicted embodiment, the device includes two or more feed rollers 21 adapted to feed two or more porous conductive substrate layers concurrently between perforated non-conductive frames 16A; and an uptake roller 22 adapted to spool said two or more porous conductive substrate layers after LCW as a bonded substrate.
[0073] In the depicted embodiment, the device includes a distance regulation mechanism (not depicted) adapted to adjust a distance between perforated non-conductive frames 16A. In some embodiments increasing the distance between frames 16A facilitates insertion and/or removal of the two or more porous conductive substrate layers. Alternatively or additionally, in some embodiments decreasing the distance between perforated non-conductive frames 16A causes the substrate layers to contact one another during welding.
[0074] Fourth Exemplary Device
[0075] In the depicted embodiment, the deposition rollers include counter electrodes 24 inside porous non-conductive cylinders 23 surrounded by covers 25. Pores in cylinders 23 vary in the size between 50 um and 10 cm depending on the size of cylinder 23.
[0076] During use electrolyte solution is pumped to cylinders 23 and exits via the pores. The current/voltage/power is applied between electrodes 24 and the 2D substrates to cause metal deposition in the area between 24 and the substrates. Covers 25 prevent spilling of electrolyte solution electrolyte. As rollers 21 and/or 22 rotate the next portion of 2D substrate is electrochemically bonded with the resulting 3D film winding on receiving roller 22. LCW of substrate layers is regulated by electrolyte composition and/or current/voltage/power and/or temperature and/or pore sizes in cylinders 23 and/or number of pores in cylinders 23 and/or pumping rate of the electrolyte and/or rotational speed of cylinders 23. In some embodiments, this device operates continuously, as opposed to in discrete increments. In some exemplary embodiments more than two rollers having features 23, 24 and 24 are installed.
[0077] Exemplary Method
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[0079] In the depicted embodiment, method 500 includes, engaging 510 two or more porous conductive substrate layers between perforated non-conductive frames so that the substrate layers contact one another. In some embodiments a single layer is folded as in
[0080] According to various exemplary embodiments of the invention the substrate layers are of the same or different material. Alternatively or additionally, the substrate layers are of the same or different thickness.
[0081] Depicted method 500 also includes immersing 520 the substrate layers in an electrolyte solution and applying 530 electric current and/or voltage and/or electric power to said electrolyte solution. According to various exemplary embodiments of the invention method 500 is performed using a device as depicted in
[0082] In some embodiments applying 530 includes applying an electric current flowing from one CE (e.g. 15A), to said porous metal substrate layers 17A acting as WE between perforated non-conductive frames.
[0083] According to various exemplary embodiments of the invention the current is constant or pulsed. According to various exemplary embodiments of the invention different pulse sequences are employed including, but not limited to pulse reversal.
[0084] In some embodiments applying 530 includes applying a voltage using a reference electrode (e.g. 6). In some embodiments, the applied voltage is constant.
[0085] In some embodiments applying 530 includes applying power. In some embodiments, the applied power is constant.
[0086] In some embodiments, method 500 includes feeding two or more porous conductive substrate layers concurrently between perforated non-conductive frames; and withdrawing the two or more porous conductive substrate layers after LCW as a bonded substrate as depicted in
[0087] Alternatively or additionally, in some embodiments method 500 includes folding 540 a single porous conductive substrate layer to form two or more porous conductive substrate layers. In some embodiments, perforated isolators are inserted between the folded layers. In some embodiments, the perforated isolators contribute to an ability to separate layers from the folded stack after LCW.
[0088] It is expected that during the life of this patent many new electrode types and/or electrolyte solutions will be developed and the scope of the invention is intended to include all such new technologies a priori.
[0089] As used herein the term “about” refers to ±10%.
[0090] Although the invention has been described in conjunction with specific embodiments thereof, it is evident that many alternatives, modifications and variations will be apparent to those skilled in the art. Accordingly, it is intended to embrace all such alternatives, modifications and variations that fall within the spirit and broad scope of the appended claims.
[0091] Specifically, a variety of numerical indicators have been utilized. It should be understood that these numerical indicators could vary even further based upon a variety of engineering principles, materials, intended use and designs incorporated into the various embodiments of the invention. Additionally, components and/or actions ascribed to exemplary embodiments of the invention and depicted as a single unit may be divided into subunits. Conversely, components and/or actions ascribed to exemplary embodiments of the invention and depicted as sub-units/individual actions may be combined into a single unit/action with the described/depicted function.
[0092] Alternatively, or additionally, features used to describe a method can be used to characterize an apparatus and features used to describe an apparatus can be used to characterize a method.
[0093] It should be further understood that the individual features described hereinabove can be combined in all possible combinations and sub-combinations to produce additional embodiments of the invention. The examples given above are exemplary in nature and are not intended to limit the scope of the invention which is defined solely by the following claims.
[0094] Each recitation of an embodiment of the invention that includes a specific feature, part, component, module or process is an explicit statement that additional embodiments of the invention not including the recited feature, part, component, module or process exist.
[0095] Alternatively or additionally, various exemplary embodiments of the invention exclude any specific feature, part, component, module, process or element which is not specifically disclosed herein.
[0096] Specifically, the invention has been described in the context of manufacturing of 3D porous substrates but might also be used in preparation of jewelry or other decorative items.
[0097] All publications, references, patents and patent applications mentioned in this specification are herein incorporated in their entirety by reference into the specification, to the same extent as if each individual publication, patent or patent application was specifically and individually indicated to be incorporated herein by reference. In addition, citation or identification of any reference in this application shall not be construed as an admission that such reference is available as prior art to the present invention.
[0098] The terms “include”, and “have” and their conjugates as used herein mean “including but not necessarily limited to”.
[0099] Additional objects, advantages, and novel features of various embodiments of the invention will become apparent to one ordinarily skilled in the art upon examination of the following examples, which are not intended to be limiting. Additionally, each of the various embodiments and aspects of the present invention as delineated hereinabove and as claimed in the claims section below finds experimental support in the following examples.
EXAMPLES
[0100] Reference is now made to the following examples, which together with the above descriptions; illustrate the invention in a non-limiting fashion.
Example 1
Effect of Current on Porosity in LCW Fabrication
[0101] In order to examine the effect of applied current on the porosity of a porous 3D metal structures produced according to various embodiments of the invention 3 pieces of porous nickel films each 50 um thick were subjected to LCW in a device as depicted in
[0102] In one case constant current density of 300 mA/cm.sup.2 was applied for 2 hours. Final porosity was 70% (
[0103] In another case constant current density of 600 mA/cm.sup.2 was applied for 2 hours. Final porosity was 46% (
[0104] % Porosity was estimated based on weight and volume of samples before deposition and after.
[0105] This example illustrates that increasing applied current contributes to a decrease porosity of the resultant product. Alternatively or additionally, this example illustrates that that 3D substrates with at least 150 um thickness and unique morphology can be produced via LCW and that porosity and morphology can be controlled via current.
Example 2
Exemplary Use of a Reference Electrode in LCW Fabrication
[0106] In order to evaluate the possibility of using a reference electrode to control the porosity of a porous 3D metal structures produced according to various embodiments of the invention five pieces of porous nickel films each 50 um thick were subjected to LCW in a device as depicted in
[0107] In one case constant current density of 400 mA/cm.sup.2 was applied for 2 hour and final porosity was 85% (
[0108] In another case constant voltage of −4 V vs Ag/AgCl reference electrode was applied for 2 hours duration (
[0109] This example illustrates that 3D structures formed via LCW can also be created under potential-controlled regime using a reference electrode. Alternatively or additionally, this example illustrates that 3D substrates with at least 250 um thickness and unique morphology can be produced and that their porosity and morphology can be controlled using a reference electrode.
Example 3
Exemplary Use of Layers with Different Properties in LCW Fabrication
[0110] In order to evaluate the effect of using layers with different properties on a resultant porous 3D metal structure produced according to an embodiment of the invention a 500 um thick layer of nickel foam was sandwiched between 2 pieces of porous nickel films each 50 um thick and subjected to LCW in a device as depicted in
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[0112] This example illustrates that thick (at least 600 um) 3D substrates can be formed via LCW method. Alternatively or additionally, this example illustrates that 2D and 3D porous metal films can be bonded together to produce porous 3D substrates with unique morphology.
Example 4
Effect of Duration of Current Application on the Resultant Product
[0113] In order to evaluate the effect of varying the amount of time that current is applied on a resultant porous 3D metal structure produced according to an embodiment of the invention 2 pieces of porous copper films each 50 um thick subjected to LCW in a device as depicted in
[0114] This example illustrates that increasing fabrication time can lead to thicker but less porous samples.
[0115] Alternatively or additionally, this example illustrates that 3D substrates with at least 100 um thickness and unique morphology can be produced and that their porosity and morphology can be controlled through the duration of deposition.
Example 5
Fabrication of Multimetallic Nickel Aluminum Substrates
[0116] In order to evaluate the possibility of using porous aluminum films to produce a porous 3D metal structures according to an embodiment of the invention 3 pieces of porous aluminum films each 50 um thick were subjected to LCW in a device as depicted in
[0117] Constant current density of 200 mA/cm2 was applied for 2 hour
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[0119] Alternatively or additionally, this example illustrates that 3D porous Ni—Cu multimetallic structures with unique morphology and physical properties can be fabricated via LCW and that their morphology and properties can be controlled via current.
Example 6
Fabrication of Multimetallic Nickel Copper Substrates
[0120] In order to evaluate the possibility of using porous copper films to produce a porous 3D metal structures according to an embodiment of the invention 5 pieces of porous copper films each 50 um thick were subjected to LCW in a device as depicted in
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[0122] This example illustrates that it is possible to fabricate 3D copper substrates in Nickel electrolyte and using nickel as a bonding material. This another example showing that different metals can bonded with different materials.
Example 7
Fabrication of 3D Substrates Via Localized/Selective LCW
[0123] In order to investigate the influence of pore size, plate porosity and current conditions on LCW quality and quantity, a series of experiments was conducted using a porous copper substrate and a copper electrolyte solution as in example 4.
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[0130] This example illustrates that LCW can be carried out using pulse deposition methods as well as constant current. The pulse parameters such as amplitude, duration, the rest step or even reversing of pulse current/voltage/power direction can be adjusted to produce various morphologies of metal deposits or to regulate amount of deposited metal. Variations of the pulse parameters are tailored for a wide variety of applications and the pulse parameters given above do not limit the scope of the claimed invention.