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Method For Producing Lithium Metal Negative Electrode Structure And Lithium Metal Negative Electrode Structure

Abstract: The present invention provides a lithium metal anode structure manufacturing method and a lithium metal anode structure the method comprising the steps of: (a) forming a lithium metal layer-coated portion on one surface or both surfaces of a current collector to manufacture a laminate one side of the current collector including an uncoated portion on which a map is to be formed; (b) applying a photocurable material to stepped portions of the uncoated portion and the lithium metal layer-coated portion to cure the material or attaching an insulating tape to the stepped portions; and (c) cutting the laminate into unit electrodes in order to manufacture a lithium metal anode structure.

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Patent Information

Application #
Filing Date
24 October 2019
Publication Number
11/2020
Publication Type
INA
Invention Field
ELECTRICAL
Status
Email
mahua.ray@remfry.com
Parent Application
Patent Number
Legal Status
Grant Date
2023-12-27
Renewal Date

Applicants

LG CHEM, LTD.
128, Yeoui-daero, Yeongdeungpo-gu, Seoul 07336

Inventors

1. LEE, Sangkyun
LG Chem Research Park, 188, Munji-ro, Yuseong-gu, Daejeon 34122
2. CHOI, Baeck Boem
LG Chem Research Park, 188, Munji-ro, Yuseong-gu, Daejeon 34122
3. KU, Cha Hun
LG Chem Research Park, 188, Munji-ro, Yuseong-gu, Daejeon 34122
4. KIM, Minwook
LG Chem Research Park, 188, Munji-ro, Yuseong-gu, Daejeon 34122

Specification

The present invention relates to a method for producing a lithium metal negative electrode structure and a lithium metal negative electrode structures.

[Background Art]

Recently, increasing interest in energy storage technology. Mobile phones, camcorders and notebook PC, furthermore there is a commitment to research and development of electrochemical devices embodied as applications are increasingly extended to the electric vehicle energy. The electrochemical device is a field that receives the most attention in this respect. Particularly, development of secondary electrons that can be charged and discharged is new to improve capacity density and specific energy of as has been the focus of attention, in recent years, the development of these cells it is proceeding with research and development for the design of electrodes and batteries.

The Lyrium secondary battery, Ni-MH, Ni-Cd, sulfuric acid using an aqueous electrolyte solution developed in the early 1990's from the secondary batteries that are currently being applied - as compared to conventional batteries such as lead batteries with high operating voltage, the energy density significantly greater advantages as it has been highlighted.

In general, the lithium secondary battery is an electrode assembly including a separator interposed between the positive electrode, a negative electrode and the positive electrode and the negative electrode incorporated in the battery case in a stacked or wound structure, is configured by being a non-aqueous electrolytic solution is injected therein.

The lithium metal is used as the negative electrode has a low density (0.54g / cm3), a further material, the most attention as a negative electrode material with high energy density batteries due to the standard reduction potential (-3.045V SHE) is very low. Furthermore, because even chemically to the problem of activity is very high, generating, and recent mobile communication and high depending on the continued growth and rapid development of the use of portable electronic devices are required for the development of energy-density secondary battery continues to increase, is a need for a lithium metal anode using continues to rise.

At this time, have been using the negative electrode case of using lithium metal as the electrode, typically a lithium metal negative electrode structure formed by attaching a lithium foil on the collector in the plane.

1 is a diagram showing a plan view and a vertical cross-sectional view of the cathode structure is prepared by attaching the foil Lyrium on the entire surface of the conventional house plane, Fig. 2 is a diagram illustrating a method of manufacturing such a cathode structure. Fig.

1 and 2, the current collector metal foil 11, a lithium metal 13 is Lyrium metal anode sheet 10 is rolled or deposition at the same time as the punching in the unit electrodes for the electrode manufacture, the current collector metal foil 11 is also cut at the same time to form a tab (12).

At this time, the lithium metal 13 is lithium metal 13 is namgeona residue, burr (burr) remaining lithium metal 14 of the type that is formed during the punching in a mold punching bring the loose property is present in the lithium metal negative electrode there is a problem of safety and hindrance of fairness eu Further, as should be cut punching when the collector metal foil is also in a unit electrode, the current collector metal night are cut tap forming unit, and a lithium metal and the collector metal foil is at the same time the breaking strength between the unit electrode portion to be cut changes, and a knife (knife) cutting strength of the punching mold to be considered, the problem of metal lithium loose fitting characteristics of the male and female molds is also generated.

So be performed in such prior art reulring (rolling) to perform a laser (laser) punching in the punching process of the lithium metal electrode sheets, or flat the remaining lithium metal in the member form after the punching in order to solve this problem, the cost and it is an inefficient process the issue.

Thus, while the improved process of this nature, high is a need for a lithium metal negative electrode structures to address the problem situation.

[Detailed Description of the Invention]

[SUMMARY]

An object of the present invention is to solve the technical problem, which has been requested from the problems, and of the prior art.

The inventors of the present application are at the end of extensive research and various experiments in depth, in the manufacturing method of the lithium metal negative electrode structures, to apply the photo-curable material to the whole of the coated portion and the coating portion stepped portion of the lithium metal house and cured, or after attaching the insulating tape, when subjected to the electrode punching process, as well as to solve the conventional above-described problems, the thus prepared Lyrium metal cathode structure is isolated consisting of a photo-curable material in the step part coated portion of the tab, and a lithium metal layer or isolated confirmed that in the bar, since a secondary battery including a tape Lyrium metal layer can be obtained further effects that can prevent a short circuit between the positive electrode material according to the exposure to the tab, thus completing the present invention.

[Technical Solution]

Production method of the lithium metal negative electrode structures of the present invention for achieving these objects,

(A) throughout one or both sides of a house, the process for producing a laminate by, forming a coating of a metal layer to cover the entire Lyrium side portion plain house the tab is formed;

(B) as to the process of applying and curing the photocurable material in the step part of the coated portion and the uncoated portion of lithium metal or, attaching the insulating tape; And

(C) for the production of a lithium metal negative electrode structures, which emits another process the laminate to the unit electrodes;

It characterized in that it comprises a.

The manufacturing process according to the invention, process (c), and at the same time, after including the step of emitted other parts of solid to form a tab, or the process (c), by issuing other parts of (d) solid to the process of forming the tab, It can be included.

That is, the inventors of the present application have had repeated in-depth study in order to solve the problems above indicated that may occur in the case of producing a lithium electrode by rolling the lithium metal on the current collector, or evaporation because of fragile nature of lithium metal to an existing, in the case of attaching the coated portion to form a photo-curable material on a stepped portion or an insulating tape of the current collector of the solid portion and the lithium metal layer prior to the punching, it was confirmed that can solve the conventional problems occurring in the punching process for forming the tab.

At this time, the stepped portion up and down based on the entire perimeter of the uncoated portion and a lithium metal layer is formed is coated portion house the vertical width of 2 mm to 5 mm in the area

it means. That is, it comprises a border, and on this basis in the vertical direction part having a width of 2 mm to 5 mm, particularly, refers to a portion having a width of 2 mm to 4 mm.

Here, the photo-curable material to be coated, cured in the step portion is not limited one, particularly, cross-linking takes place by the UV light, that is, may be a UV curable material is cured by irradiation with ultraviolet rays.

The UV curable material can be added after the polymer in the form of an oligomer or low molecular weight having a viscosity of 10 cps to 100 cps, which can be polymerized with the material to be cured by irradiation with ultraviolet rays.

Specifically, the viscosity of the polymer of the oligomer or low molecular weight may be 30 cps to about 100 cps, more particularly, 50 cps to 100 cps.

The viscosity is meant the viscosity measured according to the Brookfield viscometer, and was used as a HAAKE's visco tester 550.

Since a typical UV curable material is a monomer (monomer) or the materials or the materials in a liquid state with low viscosity consisting of oligomers (oligomer) is injected into the affected area of ​​a polymer in the form of oligomers, or low molecular weight having a viscosity in the above range, it applied a little easier and the flow after coating can achieve optimal sealing performance improvement.

Dimmer hitting the above, for example, epoxy-based, urethane-based, acrylate-based, and may have one or more selected from the group consisting of silicone, a hydroxyl silgye and acrylic acid derivatives, polymers of the low molecular weight unsaturated polyester-based material, and polyacrylate, and one or more can be selected from the group consisting of acrylate-based materials, for example, it may be a poly-ester acrylate, epoxy acrylates, urethane acrylates or polyurethane, and the like.

Specifically, TMPTA (Trimethylolpropane Triacrylate), or

Acrylate-based materials, such as ETPTA (ethoxylated trimethylopropane triacrylate).

These ultraviolet-curing material, a polymer of the oligomer or low molecular weight can be applied to common compounds of the type heunhap and the cross-linking agent, and a photoinitiator for polymerization.

The cross-linking agent, there may be employed a conventionally known crosslinking agent, not limited, for example, an isocyanate compound, an epoxy compound, an aziridine compound, TMSPA (3- (trimethoxysilyl) propylacrylate) acrylate-based compound and a metal, such as least one member selected from the group from the group consisting of a chelate compound may be.

The photoinitiator is, there is a conventionally known photoinitiator may be used, not limited, for example, benzophenone, acetophenone, chloro acetophenone, diethoxyacetophenone of (Diethoxy Acetophenone) (DEAP), benzoin, benzoin methyl ether, benzoin ethyl ether, benzoin isopropyl ether, benzoin isobutyl ether, benzoin benzoic acid, benzoin methyl benzoate, benzoin dimethyl ketal, 2,4-diethyl thioxanthone, benzyl diphenyl sulfide, tetramethyl wooram mono sulfide, nitrile azo bis isobutyronitrile, benzyl, dibenzyl, diacetyl, beta-chloro-anthraquinone, 2-benzyl-1- (4-Dimorpholino Reno phenyl) butane {-1 2-benzyl-1- (4-polrion phenyl) -1-butanone}, 2,4,6-trimethylbenzoyldiphenylphosphine oxide, 1-hydroxycyclohexyl phenyl ketone haeksil, 2 hydroxy-2-methyl-1-phenylpropan-1-one, 1- [4- (2-hydroxyethoxy) - Carbonyl] -2-methyl-1-propan-1-circle, phenyl bis (2,4,6-trimethylbenzoyl) phosphine oxide, 1-phenyl-2-hydroxy-2-methyl-propanone (1 -phenyl-2-hydroxy-2-methyl propaneone) (HMPP), alpha-amino acetophenone (a- amino acetophenone), thioxanthone (thioxanthone) and 2-ethylanthraquinone (2-ethyl anthraquinone) (2 a -ETAQ) it may be at least one member selected from the group consisting of.

In some cases, it is as a monomer the UV curable material may be added to the area in a state in which the predetermined thickening agent added.

Thickening agent that can increase the viscosity of such materials, as carboxymethyl selreul agarose (carboxymethyl cellulose), hydroxyethyl selreul to agarose (Hydroxyethyl cellulose), polyvinyl alcohol (Polyvinyl Alcohol), polyvinyl acetate (Polyvinylacrylate) or the like have.

The ultraviolet curable material having a viscosity can be curing the ultraviolet (UV) range of 3 to 20 seconds after the addition to the step portion is irradiated.

On the other hand, the step portion has a Instead, a simpler method of applying and curing the photo-curable material, may be attached to the insulating tape, at this time, the

An insulating tape may be a polyethylene terephthalate (Polyethylene terephthalate), or polyimide (Polyimide) material.

Such the optical path is the thickness or coating thickness of the insulating tape of the chemical substance 10 nm to 1 卿, details may be lOOnm to 500nm.

If out of the range, is too thick thickness, and the punching process is inefficient due to hard on the strength of the punching process, when the knife for the punching process and the tab formation of the electrode, when too thin, a sufficient degree to which the present invention desired bar can not exert an effect, which is not preferable.

On the other hand, the current collector which the lithium-metal layer is formed, may be formed of a thickness of 3 to 200. This collector, so long as it has suitable conductivity without causing chemical changes in the fabricated battery is not particularly limited, for example, copper, copper alloy, stainless steel, aluminum, nickel, titanium, sintered carbon, copper or aluminum, surface-treated with carbon, nickel, titanium or silver, on the surface of stainless steel, aluminum - is the cadmium alloy, or the like may be used, and particularly, copper, copper alloy, stainless steel, aluminum, nickel, and more specifically , and copper may be used. Collector may be processed to form fine irregularities on its surface to increase the adhesion of the electrode active material, films, sheets, foils, nets, porous structures, foams : it is possible in various forms such as a nonwoven fabric material.

In addition, the Lyrium metal layer may have a thickness of 20 to 150 卿, may be more particularly from 20 to 100.

Out of the range, when the too small thickness of the lithium metal, the smaller the amount of lithium metal which acts as the active material compared to the current collector, it can not exhibit a sufficient capacity, and if it is too thick, poor output characteristic, or loose passage of the lithium metal to avoid problems due to the characteristics undesirable hard bar.

On the other hand, in the step (a), a method of forming a lithium metal layer to the current collector is one not being limited, may be carried out by evaporation or rolled lithium metal, specifically, the shape is deformed by the fragile nature of the Lyrium metal bar with a problem such as that may be, it may be formed by rolling.

Here, the size of the rolling may be appropriately selected in view of the thickness of the lithium metal.

The invention also provides the thus prepared lithium metal cathode structure, wherein the lithium metal negative electrode structures,

Full House;

A vertically extending tab from the current collector; And

Lithium metal layer formed on the entire one side or both sides of a house other than the tab;

And including,

Or the insulating layer made of a photo-curable material in the step part of the map and a lithium metal layer is formed, or may be insulating tape is attached.

Lithium metal negative electrode structures as described above, forming an insulating layer on the step portion of the tab and the lithium metal layer prior to the punching of the unit electrodes to achieve the effect as described above, or a bar for attaching the insulating tape after the manufacturing process of the electrode since no additional process to obtain an additional effect of preventing a short circuit between the positive electrode material according to the exposure on the lithium metal tab on the secondary battery.

Therefore, the lithium metal negative electrode structures according to the present invention, burr (burr) caused this to be minimized bar, as well as to solve the safety problems that can be caused by the residual lithium in the member form present in the negative electrode structure, a lithium metal layer is a tab sikineunde there can also be prevented since the short circuit which may occur in contact with the positive electrode material, resulting in localized heat generation and explosion bar, improves the safety of the battery by which a very effective.

At this time, the tab may be formed as an integral whole with the house. That is, the tap can be emitted the other parts of the solid lithium metal layer uncoated form, as described above.

The insulating layer or insulating part the difference in level of the map and a lithium metal layer tape is formed, the same effect as the above-described manufacturing method, is the same as the insulating layer or insulation tape is formed at the production process, the width of the border of the lithium metal layer and the tab, based on the vertical direction it may be 2 mm to 5 mm, particularly, specifically, the 2 mm to 4 mm, and the thickness may be 10 nm to 1, particularly lOOnm to 500nm.

Here, the thickness means the length in the stacking direction of the current collector and the lithium metal.

In addition, the insulating layer or insulating tape is so cut together in the punching process of the unit electrode, and the width may be the same as for system wide, or the unit is slightly extended to the outside edges of electrode 1mm to 5mm range than the tab width as may be desired way.

On the other hand, the cathode structure may be used for secondary batteries will be described in the following specific structure of the secondary battery.

The secondary battery is that its type is not particularly limited, as a specific example, high energy density, discharge voltage, the lithium ion (Li-ion) with the advantages of an output reliability secondary batteries, lithium polymer (Li-polymer) secondary battery, or a lithium ion polymer (Li-ion polymer) lithium secondary batteries such as secondary battery may be a.

In general, Lyrium secondary battery is composed of positive electrode, a negative electrode, a separator, and a lithium salt-containing non-aqueous electrolyte.

The cathode is, for example, after applying a common compound of the positive electrode active material, conductive material and a binder on a positive electrode collector and dried to manufacture, as necessary, may be further added to the layer jinje common compound.

The cathode current collector and / or the extended collector is generally fabricated to have a thickness of 3 to 500 micrometers. All of the cathode current collector and an extended house, so long as having a high conductivity without causing chemical changes in the fabricated battery is not particularly limited, for example, stainless steel, aluminum, nickel, titanium, sintered carbon, or aluminum, carbon, nickel or titanium on the surface of stainless steel, can be used as such as to a surface treatment or the like. Positive electrode current collector and the current collector extension may also improve the adhesion of the positive electrode active material to form fine irregularities on its surface, it is possible to form various films, sheets, foils, nets, porous structures, foams and non-woven fabrics and the like. '

The positive electrode active material is lithium cobalt oxide (LiCo0 2 ), lithium nickel oxide (LiNi0 2 ) layered compounds or one or more transition metal compounds, such as substituted; Formula Li 1 + x Mn 2-x 0 4 (wherein, X is 0 to 0.33), LiMn0 3 , LiMn 2 0 3 , LiMn0 2 such as lithium manganese oxides; Lithium copper oxide (Li 2 Cu0 2 ); LiV 3 0 8 , LiFe 3 0 4 , V 2 0 5 , Cu 2 V 2 0 7 of vanadium oxide and the like; Formula LiNi 1-x M x 0 2 (Here, M = Co, Mn, Al, Cu, Fe, Mg, B or Ga, x = 0.01 ~ 0.3 Im) Ni site type lithium nickel oxide which is represented by;

Formula LiMn 2-x M x 0 2 (where, M = Co, Ni, Fe , Cr, and Zn, or Ta, x = 0.01 ~ 0.1 Im) or Li 2 Mn 3 M0 8 (where, M = Fe, Co, lithium manganese composite oxide represented by Ni, Cu or Zn); Some of the formula LiMn Li is substituted with alkaline earth metal ion 2 0 4 ; Disulfide compounds; Fe 2 (Mo0 4 ) 3 and the like, but is not limited to these.

The conductive material is commonly added in a common compound in the total weight including the cathode active material with 1 to 30% by weight. This conductive material so long as it has suitable conductivity without causing chemical changes in the fabricated battery is not particularly limited, for example, hokyeon such as natural or artificial hokyeon hokyeon; Carbon black, acetylene black, Ketjen black, channel black, furnace black, lamp black, carbon black and thermal black; The conductive fiber of the carbon fibers and metallic fibers round; Metal such as carbon fluoride, aluminum, nickel powder, powder; Conductive whiskers such as zinc oxide and potassium titanate; Conductive metal oxides such as titanium oxide; Poly is a conductive material such as phenylene derivative may be used. '

The binder is a component assisting in binding to the total binding and the home, such as the active material and the conductive material is commonly added in a common compound total weight including the cathode active material with 1 to 30% by weight. Examples of the binder include polyvinylidene fluoride, polyvinyl alcohol, carboxymethyl selreul by Woods (CMC), starch, hydroxypropylcellulose, an ethylene a saelreul Woods, polyvinyl into Woods, playing saelreul as a pyrrolidone, tetrafluoroethylene, polyethylene , polypropylene, ethylene-propylene-diene terpolymer (EPDM), sulfonated EPDM, styrene beuti butylene rubber, fluoro rubber and various copolymers and the like.

The filler is selectively used as a component of suppressing the expansion of the positive electrode, if the standing fibrous materials without causing chemical changes in the fabricated battery is not particularly limited, for example, up pingye polymers such as polyethylene and polypropylene; And fibrous materials such as glass fiber and carbon fiber.

The negative electrode may be formed of a metal Lyrium cathode is formed, a lithium metal chungyi to the current collector as described above.

The separator is interposed between the positive electrode and the negative electrode, an insulating thin film having high ion permeability and mechanical strength is used. Pore ​​size of the membrane is

Generally 0.01 - 10 microns, and the thickness is generally 5 to 300 micrometers, the eu As the separator, for example, olefin polymers such as chemically resistant and hydrophobic polypropylene; A sheet or non-woven fabrics made of glass fiber or polyethylene, etc. are used. When a solid electrolyte polymer Dung is employed as the electrolyte, the solid electrolyte may also serve as both the separator.

The electrolyte may be a non-aqueous liquid electrolyte containing a lithium salt, a non-aqueous electrolyte and a lithium salt consists of a. The non-aqueous electrolyte is used as the non-aqueous liquid such as organic solvent, an organic solid electrolyte, inorganic solid electrolytes, but are not limited to these. In the non-aqueous organic solvents, e.g., N- methyl-piperidinyl a rice field, propylene carbonate, ethylene carbonate, butylene carbonate, dimethyl carbonate, diethyl carbonate, gamma-lactone, butyl, hydroxy-1,2-dimethoxy ethane, tetrahydroxy Franc (franc), 2- methyl tetrahydrofuran, dimethylsulfoxide, 1,3-dioxolane, formamide, dimethylformamide, dioxo run, acetonitrile, nitromethane, methyl formate, methyl acetate, phosphoric acid triester, trimethoxy hydroxy methane, dioxolane derivatives, sulfolane, methyl sulfolane, l, 3 eu-dimethyl-2-imidazolidinone, propylene carbonate carbonate derivatives, may be used an aprotic organic solvent such as tetrahydrofuran derivatives, ether, fatigue propionic acid methyl, propionic acid ethyl.

As the organic solid electrolyte, for example, polyethylene derivatives, polyethylene oxide derivatives, polypropylene oxide derivatives, phosphoric acid ester polymers, poly-edge presentation lysine (agitation lysine), polyester sulfide, polyvinyl alcohol, polyvinylidene fluoride, the polymers containing ionic dissociation groups may be used.

The inorganic solid electrolyte is, for example, Li 3 N, Lil, Li 5 NI 2 , Li 3 N-LiI-LiOH, LiSi0 4 , LiSi0 4 -LiI-LiOH, Li 2 SiS 3 , Li 4 Si0 4 , Li 4 Si0 4 -LiI-LiOH, Li 3 P0 4 -Li 2 S-SiS 2 has a nitride, halide, sulfate of Li such as such can be used.

The lithium salt is a material that is readily soluble in the non-aqueous electrolyte, for example, LiCl, LiBr, Lil, LiC10 4 , LiBF 4 , LiB 10 Cl 10 , LiPF 6 , LiCF 3 S0 3 , LiCF 3 C0 2 , LiAsF 6 , LiSbF 6 , LiAlCl 4 , CH 3 S0 3 Li, CF 3 S0 3 Li, (CF 3 S0 2 ) 2 NLi, chloroborane lithium, lower aliphatic carboxylic acid lithium, lithium tetraphenyl borate and imide have.

In addition, the non-aqueous electrolyte is in order to improve layer discharge characteristics and flame retardancy, for example, pyridine, triethylphosphite, triethanolamine, cyclic ether, ethylene

Diamine, n- glyme (glyme), hex phosphate tree amide, nitrobenzene derivatives, sulfur, quinone imine dyes, N- substituted oxazolidinone, Ν, Ν- substituted imidazolidine, ethylene glycol dialkyl ether, ammonium salts, Therefore, the blood, the case 2 may be added during meteuk ethanol, aluminum trichloride, etc. eu, in order to impart incombustibility, and also possible to further include a halogen-containing solvent such as carbon tetrachloride and ethylene trifluoride, a high-temperature storability may be further comprising a carbon dioxide gas in order to improve, it is possible to further include a FEC (Fluoro-Ethylene carbonate), PRS (Propene sultone).

In one specific example, LiPF 6 , LiC10 4 , LiBF 4 , LiN (S0 2 CF 3 ) 2 , such as a lithium salt, a highly dielectric solvent of DEC, DMC or EMC Fig solvent cyclic carbonate and a low viscosity of the EC or PC of heunhap added to the solvent of a linear carbonate can be prepared a lithium salt-containing non-aqueous electrolyte.

[Brief description of drawings]

Figure 1 is a schematic view of a cathode structure according to the prior art;

Figure 2 is a schematic diagram of a process for manufacturing a cathode structure of Figure 1;

3 is a schematic diagram of a process for preparing a, a cathode structure according to an embodiment of the invention;

Figure 4 is a picture of the die after punching for producing the prior art cathode structure; 5 is a photograph of the punching and then the negative electrode structure for the production of a conventional cathode structure;

Figure 6 is a photograph of a punching and then the negative electrode structure for the manufacture of a cathode structure according to the first embodiment of the present invention;

Figure 7 is a photograph of a punching and then the negative electrode structure for the manufacture of a cathode structure according to another embodiment of the present invention.

[Mode for Carrying out the invention]

In the following description, explained with reference to the drawings according to an embodiment of the present invention, which are for a more easy understanding of the invention, the scope of the present invention is not intended to be limited by it.

It has been shown to extraneous parts and described in order to clarify the description, and to attach the same reference numerals for the same or similar elements throughout the specification. In addition, the size of each component shown in the drawings and

The thickness is therefore showed arbitrarily for convenience of explanation, the substrate is not necessarily limited to the illustrated bar.

Figure 3 shows a schematic diagram of a process for producing a cathode structure according to one embodiment of the invention.

3, the first, including the entire one side or both sides of a house, and a coating unit 130, a lithium metal layer formed, the uncoated portion 110 to be without lithium metal layer is not formed, the tab formed by the subsequent punching step that is applied to or rolled Lyrium metal.

Then, applying the photo-curable material 140 to the step portion of the coated portion 110 and a lithium metal layer coating unit 130, the hardening or isolated attach the tape 140, and performs a process of emitting the other by the unit electrodes It is prepared. In this case, the lithium metal negative electrode structures 100 as soon as the punching unit for electrode electrode manufactured at the same time, solid portions 110 are also prepared is punched at the same time to form a tab (120).

When preparing a lithium metal negative electrode structures 100 in this manner, it is possible to solve the lithium burr (burr) caused problems in the punching process, which was the conventional problem. In addition, this lithium metal negative electrode structures 100, prepared as is isolated by the above production process, consisting of a photocurable material between the step portion of the map 120 and the lithium metal coating 130 of the extending from the current collector layer 140 has a structure that is attached to or is formed, or an insulating tape (140).

Therefore, lithium metal in a secondary battery after it is possible to prevent a short circuit between the positive electrode material according to the exposure to the tab.

In the following description, explained with reference to embodiments according to the invention, which are for a more easy understanding of the invention, the scope of the present invention is not intended to be limited by it.

Entire glass house made of copper (thickness: 30 m ): to prepare a negative electrode sheet (40加thickness), except for one side portion plain for the formation of the tab to remain in the deposition of lithium metal.

Then, as prepared in the unit electrodes was subjected to the punching process for forming a wrap. The mold and photos after the punching step, the front and back of the unit electrode shown in FIGS. 4 and 5, the optical picture.

Referring to Figure 4 if, the mold is when there is a remainder of Lyrium metal from members of the lithium metal to generate interrupts, to Figure 5, the unit electrodes was confirmed that as seen from the back of photo generated surface defects electrode outer portions pushed can.

House consisting of a copper body (thickness: 30) onto the deposited portion to leave except for the one side, and a lithium metal solid for the formation of a tab (thickness: 40) to prepare a negative electrode sheet, and coating the lithium metal is formed and the solid parts of the step isolated in section tape (thickness:

500nm) a taping (width, including the coated portion and the solid portion borders: 3 mm, length was the same taping) to the length of the tab to be formed later.

Then, as prepared in the unit electrodes was subjected to the punching process for forming the tab. The front and back of the electrode unit after the punching process shown in Figure 6 the optical picture.

6, the electrode units can be found that the smoothly without as seen from the rear of the photo milryeonam electrode outer portions punching.

House consisting of a copper body (thickness: 30), the additional solid for the formation of the lap to leave the deposited lithium metal, except for one side to (the thickness: 40) to prepare a negative electrode sheet, and coating the lithium metal is formed and the solid parts of the step in part, as a photo-curable material, ETPTA: as (ethoxylated trimethylopropane triacrylate, viscosity 60 cps) and a cross-linking agent, TMSPA (3- (trimethoxysilyl) propylacrylate), and a photoinitiator, the weight ratio of 2-hydiOxy-2-methylpropiophenone) 10: 0.5: cured by, and UV curing method applied to common compounds mixed with 0.5 (3 mm, length of the same, applied to the length of the to be formed after the tab thickness:: 500nm, including the coated portion and the solid portion border width).

Then, as prepared in the unit electrodes was subjected to the punching process for forming a wrap. The front and back of the electrode unit after the punching process, the optical picture is shown in Fig.

Referring to FIG. 7, the electrode unit may determine that the smoother without As you can see in the picture milryeonam rear portion of the outer electrode punching.

As a cathode active material, the positive electrode active material (LiCo0 2 ), 90 parts by weight 0 / 0 , Super-P (conductive material) 5 parts by weight 0 / 0 , and PVDF (a binder) in NMP (N-methyl solvent a positive electrode material mixture of 5% by weight of composition after producing the positive electrode slurry was added to the -2- pyrrolidone), to thereby prepare a positive electrode was coated on an aluminum whole house.

Comparative Example 1 and Example 1 In the production unit electrode as a cathode and as the anode, a separator polyethylene film: the (Celgard, thickness 20 μίΐ), and ethylene carbonate, dimethylene carbonate, diethyl carbonate, 1: 2 : on the solvent to heunhap 1 LiPF 6 using a liquid electrolyte with dissolved in 1M, were prepared secondary battery 10 by one.

It said secondary battery 2.5V - to the layer subjected to discharging with 1.0 C for 10 cycles at 4.35 V interval measuring the number of the short circuit, ignition occurred battery are shown in Table 1 below.

[Table 1]

As shown in Table 1, it can be confirmed that the of the secondary battery using a negative electrode according to the invention is higher than the safety.

Above has been described with reference to the drawings and embodiments in accordance with the present invention, those skilled in the art that the invention would be possible that various ungyong and modifications within the scope of the invention as disclosed in the accompanying claims.

[Industrial Applicability]

As described above, the lithium metal negative electrode structures according to the present invention, a photo-curable material to the whole of the coated portion and the coating portion of the step portion of lithium metal home

So prepared by coating, and is cured to, or attached to insulating tape perform emits another process, it is possible to solve the lithium burr (burr) caused problems in the punching process, which was the conventional problem, or perform laser (laser) the punching, the punching then do not need to add a separate process such as rolling (rolling) to make flat the remaining lithium metal in the form member, it is effective in terms of cost and process.

Further, the thus prepared lithium metal negative electrode structure is in the coating portion stepped portion of the tab, and a lithium metal, a bar, a lithium metal layer from the secondary battery after that an insulating layer or an insulating tape consisting of a photo-curable material according to the process tab additional effect of preventing a short circuit between the positive electrode material according to the exposure can be obtained.

Claims

A method for producing a lithium metal cathode structure,

(A) throughout one or both sides of a house, the process of manufacturing the enemy worms to, form a coating of a lithium metal layer to cover the entire side portion plain house the tab is formed;

(B) as to the process of applying and curing the photocurable material in the step part of the coated portion and the uncoated portion of lithium metal or, attaching the insulating tape; And

(C) for the production of a lithium metal negative electrode structures, which emits another process the laminate to the unit electrodes;

Lyrium method for producing a metallic cathode structure comprising a.

[Claim 2]

The method of claim 1, wherein the process (c), and at the same time, process for producing the lithium metal anode structure including the step of emitted other parts of solid to form a tab.

[Claim 3]

The method of claim 1, wherein after the process (c),

And (d) other parts of emitted solid prepared lithium metal anode structure including the step of forming the tab.

[Claim 4]

The method of claim 1, wherein the step portion of the method of manufacturing the collector coated portion and the lithium metal layer down to the coating based on the boundary portion is formed in the vertical direction width of 2 mm to 5 mm portion of the lithium metal negative electrode structures.

[5.]

The method of claim 1, wherein the photo-curable material, a UV curable material, method for producing the lithium metal negative electrode structures is cured by irradiation with ultraviolet rays.

[6.]

The method of claim 5 wherein the UV curable material is 10 cps to 100 cps viscosity of the oligomer with or after the addition in the form of a polymer of low molecular weight method of producing a lithium metal negative electrode structures is cured by irradiation with ultraviolet rays.

[7.]

Of claim 5, wherein the dimmer epoxy-based, urethane-based, acrylate-based, silicone-modified, hydroxyl silgye, and one or more selected from the group consisting of acrylic acid derivatives hitting the above, the polymers of low molecular weight, unsaturated polyester-based material, The method and the polyacrylate based material, one or more of lithium metal negative electrode structures is selected from the group consisting of.

[8.]

The method of claim 1, wherein the coating thickness or the thickness of the insulating tape of the photocurable substance is, 10 nm to l / mi The method of producing a lithium metal negative electrode structures.

[9.]

The method of claim 1, wherein producing the current collector include copper, copper alloy, stainless steel, aluminum, nickel or a lithium metal negative electrode structures.

[10.]

The method of claim 1, wherein the lithium metal layer,

Method for producing a lithium metal cathode structure having a thickness of 20 to 100 / m.

[Claim 111

The method of claim 1, wherein the process (a) is a method for producing a lithium metal negative electrode structures is carried out by vapor deposition or a rolling Lyrium metal in the current collector.

[12.]

Full House;

A vertically extending tab from the current collector; And

Lithium metal layer formed on the entire one side or both sides of a house other than the tab;

And including,

Or the insulating layer made of a photo-curable material on a step portion of the wrap with the lithium metal layer is formed, or an insulating structure in which a lithium metal negative electrode tape is attached. [13.]

The method of claim 12, wherein the tab is a lithium metal negative electrode structures are formed as an integral whole with the house.

[14.]

The method of claim 12, wherein the insulating layer or insulating tape is a lithium metal negative electrode structures is formed of a shape covering an end portion of the lithium metal caterpillars end and the tab.

[15.]

The method of claim 12, wherein the insulating layer or insulating width of the tape, based on the boundary of the lithium metal layer and the tab in the vertical direction 2 mm to 5 mm of the lithium metal negative electrode structures.

[16.]

The method of claim 12, wherein the insulating layer or the width of the insulating tape is the same lithium metal negative electrode structures and the width of the tab.

[Claim 17]

The method of claim 12, wherein the thickness of the insulating layer or insulating tape, 10 nm to m of the lithium metal negative electrode structures.

[Claim 18]

A secondary battery including a lithium metal cathode structure according to claim 12.

Documents

Orders

Section Controller Decision Date

Application Documents

# Name Date
1 201917043261-IntimationOfGrant27-12-2023.pdf 2023-12-27
1 201917043261.pdf 2019-10-24
2 201917043261-PatentCertificate27-12-2023.pdf 2023-12-27
2 201917043261-TRANSLATIOIN OF PRIOIRTY DOCUMENTS ETC. [24-10-2019(online)].pdf 2019-10-24
3 201917043261-STATEMENT OF UNDERTAKING (FORM 3) [24-10-2019(online)].pdf 2019-10-24
3 201917043261-Response to office action [25-10-2023(online)].pdf 2023-10-25
4 201917043261-Response to office action [02-05-2023(online)].pdf 2023-05-02
4 201917043261-PROOF OF RIGHT [24-10-2019(online)].pdf 2019-10-24
5 201917043261-Response to office action [21-12-2022(online)].pdf 2022-12-21
5 201917043261-PRIORITY DOCUMENTS [24-10-2019(online)].pdf 2019-10-24
6 201917043261-FORM 1 [24-10-2019(online)].pdf 2019-10-24
6 201917043261-8(i)-Substitution-Change Of Applicant - Form 6 [28-11-2022(online)].pdf 2022-11-28
7 201917043261-DRAWINGS [24-10-2019(online)].pdf 2019-10-24
7 201917043261-ASSIGNMENT DOCUMENTS [28-11-2022(online)].pdf 2022-11-28
8 201917043261-PA [28-11-2022(online)].pdf 2022-11-28
8 201917043261-DECLARATION OF INVENTORSHIP (FORM 5) [24-10-2019(online)].pdf 2019-10-24
9 201917043261-COMPLETE SPECIFICATION [24-10-2019(online)].pdf 2019-10-24
9 201917043261-Response to office action [01-11-2022(online)].pdf 2022-11-01
10 201917043261-ABSTRACT [10-02-2022(online)].pdf 2022-02-10
10 abstract.jpg 2019-10-25
11 201917043261-CLAIMS [10-02-2022(online)].pdf 2022-02-10
11 201917043261-FORM-26 [29-10-2019(online)].pdf 2019-10-29
12 201917043261-COMPLETE SPECIFICATION [10-02-2022(online)].pdf 2022-02-10
12 201917043261-Power of Attorney-311019.pdf 2019-11-05
13 201917043261-Correspondence-311019.pdf 2019-11-05
13 201917043261-DRAWING [10-02-2022(online)].pdf 2022-02-10
14 201917043261-FER_SER_REPLY [10-02-2022(online)].pdf 2022-02-10
14 201917043261-FORM 3 [24-03-2020(online)].pdf 2020-03-24
15 201917043261-FORM 18 [13-07-2021(online)].pdf 2021-07-13
15 201917043261-OTHERS [10-02-2022(online)].pdf 2022-02-10
16 201917043261-FER.pdf 2021-10-18
17 201917043261-OTHERS [10-02-2022(online)].pdf 2022-02-10
17 201917043261-FORM 18 [13-07-2021(online)].pdf 2021-07-13
18 201917043261-FORM 3 [24-03-2020(online)].pdf 2020-03-24
18 201917043261-FER_SER_REPLY [10-02-2022(online)].pdf 2022-02-10
19 201917043261-Correspondence-311019.pdf 2019-11-05
19 201917043261-DRAWING [10-02-2022(online)].pdf 2022-02-10
20 201917043261-COMPLETE SPECIFICATION [10-02-2022(online)].pdf 2022-02-10
20 201917043261-Power of Attorney-311019.pdf 2019-11-05
21 201917043261-CLAIMS [10-02-2022(online)].pdf 2022-02-10
21 201917043261-FORM-26 [29-10-2019(online)].pdf 2019-10-29
22 201917043261-ABSTRACT [10-02-2022(online)].pdf 2022-02-10
22 abstract.jpg 2019-10-25
23 201917043261-COMPLETE SPECIFICATION [24-10-2019(online)].pdf 2019-10-24
23 201917043261-Response to office action [01-11-2022(online)].pdf 2022-11-01
24 201917043261-PA [28-11-2022(online)].pdf 2022-11-28
24 201917043261-DECLARATION OF INVENTORSHIP (FORM 5) [24-10-2019(online)].pdf 2019-10-24
25 201917043261-DRAWINGS [24-10-2019(online)].pdf 2019-10-24
25 201917043261-ASSIGNMENT DOCUMENTS [28-11-2022(online)].pdf 2022-11-28
26 201917043261-FORM 1 [24-10-2019(online)].pdf 2019-10-24
26 201917043261-8(i)-Substitution-Change Of Applicant - Form 6 [28-11-2022(online)].pdf 2022-11-28
27 201917043261-Response to office action [21-12-2022(online)].pdf 2022-12-21
27 201917043261-PRIORITY DOCUMENTS [24-10-2019(online)].pdf 2019-10-24
28 201917043261-Response to office action [02-05-2023(online)].pdf 2023-05-02
28 201917043261-PROOF OF RIGHT [24-10-2019(online)].pdf 2019-10-24
29 201917043261-STATEMENT OF UNDERTAKING (FORM 3) [24-10-2019(online)].pdf 2019-10-24
29 201917043261-Response to office action [25-10-2023(online)].pdf 2023-10-25
30 201917043261-TRANSLATIOIN OF PRIOIRTY DOCUMENTS ETC. [24-10-2019(online)].pdf 2019-10-24
30 201917043261-PatentCertificate27-12-2023.pdf 2023-12-27
31 201917043261-IntimationOfGrant27-12-2023.pdf 2023-12-27
31 201917043261.pdf 2019-10-24

Search Strategy

1 201917043261_search_uploadanotherE_13-08-2021.pdf

ERegister / Renewals

3rd: 15 Feb 2024

From 06/09/2020 - To 06/09/2021

4th: 15 Feb 2024

From 06/09/2021 - To 06/09/2022

5th: 15 Feb 2024

From 06/09/2022 - To 06/09/2023

6th: 15 Feb 2024

From 06/09/2023 - To 06/09/2024

7th: 30 Aug 2024

From 06/09/2024 - To 06/09/2025

8th: 25 Aug 2025

From 06/09/2025 - To 06/09/2026