Method for producing molded body for electrodes

Abstract

Disclosed is a method for producing a molded body for electrodes, the method including: a step for transporting a collector foil; a step for supplying an electrode material onto the collector foil, the electrode material containing an electrode active material, a conductive assistant, and an electrolyte solution and having a solid content concentration of 40 vol% to 70 vol%; a step for forming a first electrode material film by leveling the electrode material supplied onto the collector foil with use of a first film forming member; and a step for forming a second electrode material film by leveling the first electrode material film with use of a second film forming member. If W1 is the width of the first electrode material film and W2 is the width of the second electrode material film, W1 / W2 is more than 0.86 and less than 0.96, and if H1 is the thickness of the first electrode material film and H2 is the thickness of the second electrode material film, H2 / H1 is more than 0.3 and less than 0.9.

Description

Method for manufacturing electrode molded body

[0001] The present disclosure relates to a method for producing a molded body for an electrode.

[0002] In recent years, from the viewpoint of safety, quasi-solid-state batteries in which a part of the electrolytic solution is replaced with a solid electrolyte have been studied. The production of a battery electrode using a powder containing an electrode active material generally includes a step of coating a support with an electrode material containing the powder electrode active material.

[0003] For example, JP 2017-533548 A discloses a method for manufacturing an electrochemical cell, which includes the steps of coating a semi-solid anode on a first surface of a negative current collector, the step of placing a frame defining an opening on the first surface of the negative current collector, the step of placing the semi-solid anode in the opening of the frame, and the step of removing excess semi-solid anode material from the opening, wherein the excess semi-solid anode material is removed with a vibrating doctor blade. JP 2021-530829 A discloses a method comprising continuously distributing a semi-solid electrode slurry on a current collector, separating the semi-solid electrode slurry into separate portions, and cutting the current collector to form a completed electrode.

[0004] The manufacturing of an electrode molded body for use in a semi-solid or all-solid-state battery includes a step of forming an electrode material film on a current collector foil using an electrode material containing an electrode active material, the thickness of which corresponds to the electrode molded body. In this step, the width of the formed electrode material film sometimes does not match the width of the current collector foil. Specifically, the width of the electrode material film sometimes is too short compared to the width of the current collector foil, or the electrode material film sometimes protrudes from the current collector foil.

[0005] The present disclosure has been made in view of the above circumstances, and an object of one embodiment of the present disclosure is to provide a method for manufacturing an electrode molded body that is capable of forming an electrode material film with a width appropriate for the width of a current collector foil.

[0006] The present disclosure includes the following aspects: <1> A method for producing an electrode molded body, comprising: a step of transporting a current collector foil; a step of supplying, onto the current collector foil, an electrode material containing an electrode active material, a conductive additive, and an electrolyte solution and having a solids concentration of 40% by volume to 70% by volume; a step of leveling the electrode material supplied onto the current collector foil using a first film-forming member to form a first electrode material film; and a step of leveling the first electrode material film using a second film-forming member to form a second electrode material film, wherein, when the width of the first electrode material film is W1 and the width of the second electrode material film is W2, W1 / W2 is greater than 0.86 and less than 0.96, and when the thickness of the first electrode material film is H1 and the thickness of the second electrode material film is H2, H2 / H1 is greater than 0.3 and less than 0.9. <2> A method for producing an electrode molded body according to <1>, wherein the first film-forming member vibrates at a frequency of 10 kHz or greater and less than 100 kHz. <3> The method for producing an electrode molded body according to <1> or <2>, wherein WN1 / WN2 is greater than 0.8 and less than 1, where WN1 is the width of the first film-forming member and WN2 is the width of the second film-forming member. <4> The method for producing an electrode molded body according to any one of <1> to <3>, wherein a first restricting member that restricts the width of the first electrode material film is provided between the first film-forming member and the current collecting foil. <5> The method for producing an electrode molded body according to <4>, wherein the first restricting member is not in contact with the first film-forming member or the current collecting foil. <6> The method for producing an electrode molded body according to <4> or <5>, wherein the downstream end of the first film-forming member in the conveying direction of the current collecting foil is closer to the current collecting foil than the upstream end of the first film-forming member in the conveying direction of the current collecting foil, and the first film-forming member is provided at an angle with respect to the current collecting foil. <7> The method for producing an electrode molded body according to <6>, wherein the first restricting member has a shape that decreases in height in the conveying direction of the current collecting foil. <8> The method for manufacturing a molded article for an electrode according to <7>, wherein the shortest distance between the lower surface of the first film forming member and the upper surface of the first restricting member is more than 0 mm and not more than 0.5 mm. <9> The method for manufacturing a molded article for an electrode according to <7> or <8>, wherein the shortest distance between the lower surface of the first restricting member and the upper surface of the current collecting foil is more than 0 mm and not more than 0.5 mm. <10> The method for manufacturing a molded article for an electrode according to any one of <7> to <9>, wherein the shortest distance between the downstream end of the first restricting member in the conveying direction of the current collecting foil and the downstream end of the first film forming member in the conveying direction of the current collecting foil is more than 0 mm and not more than 5 mm.<11> The method for manufacturing an electrode molded body according to any one of <1> to <10>, further comprising a step of leveling the second electrode material film using a third film-forming member to form a third electrode material film. <12> The method for manufacturing an electrode molded body according to any one of <1> to <11>, further comprising a second restricting member that restricts the width of the second electrode material film between the second film-forming member and the current collector foil. <13> The method for manufacturing an electrode molded body according to any one of <1> to <11>, further comprising a step of leveling the electrode material supplied onto the current collector foil using N film-forming members in turn (N is 2 or more) to form an electrode material film, wherein the vibration frequency of the (N-1)th film-forming member is Hz. Ｎ－１ , the vibration frequency of the Nth film forming member is Hz Ｎ In this case, Hz Ｎ / Hz Ｎ－１ <14> The method for producing an electrode molded body according to any one of <1> to <12>, wherein the value of Wh is 0.001 to 0.1. <14> The method for producing an electrode molded body according to any one of <1> to <12>, wherein the value of Wh is 0.001 to 0.1. <14> The method for producing an electrode molded body according to any one of <1> to <12>, Ｎ－１ , the vibration amplitude of the Nth film forming member is Wh Ｎ In this case, Wh Ｎ / Wh Ｎ－１ <14> The method for producing a molded body for an electrode according to any one of <1> to <13>, wherein the value is 0.005 to 0.5.

[0007] According to one embodiment of the present disclosure, there is provided a method for manufacturing an electrode molded body that is capable of forming an electrode material film with a width appropriate for the width of a current collector foil.

[0008] Fig. 1 is a schematic side view showing an example of a manufacturing process of an electrode molded body. Fig. 2 is a schematic plan view showing an example of a manufacturing process of an electrode molded body.

[0009] Hereinafter, a method for producing an electrode molded body according to the present disclosure will be described. However, the present disclosure is not limited to the following embodiments and can be implemented with appropriate modifications within the scope of the object of the present disclosure.

[0010] When describing embodiments of the present disclosure with reference to the drawings, descriptions of overlapping components and reference numerals may be omitted. Components indicated by the same reference numerals in the drawings are the same components. The dimensional ratios in the drawings do not necessarily represent the actual dimensional ratios.

[0011] In the present disclosure, a numerical range expressed using "to" means a range that includes the numerical values ​​described before and after "to" as the lower and upper limits. In numerical ranges described in stages in the present disclosure, the upper limit value described in a certain numerical range may be replaced with the upper limit value of another numerical range described in stages, and the lower limit value described in a certain numerical range may be replaced with the lower limit value of another numerical range described in stages. In numerical ranges described in stages in the present disclosure, the upper or lower limit value described in a certain numerical range may be replaced with a value shown in the examples.

[0012] In the present disclosure, a combination of two or more preferred embodiments is a more preferred embodiment. Furthermore, when a plurality of substances corresponding to each component are present in the composition, the amount of each component in the composition in this specification means the total amount of the corresponding plurality of substances present in the composition, unless otherwise specified.

[0013] In this specification, the term "process" includes not only an independent process but also a process that cannot be clearly distinguished from other processes as long as the intended purpose of the process is achieved.

[0014] In this specification, "mass %" and "wt %" are synonymous, and "parts by mass" and "parts by weight" are synonymous. Furthermore, "total solid content" refers to the total mass of the components excluding the solvent from the entire composition. The "solid content" may be solid or liquid at 25°C.

[0015] [Method for manufacturing an electrode molded body] A method for manufacturing an electrode molded body according to the present disclosure includes the steps of: conveying a current collector foil; supplying an electrode material onto the current collector foil, the electrode material including an electrode active material, a conductive additive, and an electrolyte solution, and having a solids concentration of 40% by volume to 70% by volume; leveling the electrode material supplied onto the current collector foil using a first film-forming member to form a first electrode material film; and leveling the first electrode material film using a second film-forming member to form a second electrode material film. When the width of the first electrode material film is W1 and the width of the second electrode material film is W2, W1 / W2 is greater than 0.8 and less than 1. When the thickness of the first electrode material film is H1 and the thickness of the second electrode material film is H2, H2 / H1 is greater than 0.3 and less than 0.9.

[0016] Conventionally, when manufacturing an electrode molded body using an electrode material with a high solid content (40% to 70% by volume), the widthwise edges of the formed electrode material film may be thicker than the remaining portions. This is thought to be because, when supplying and forming the electrode material, the pressure applied to the widthwise center is relatively high and the pressure applied to the widthwise edges is relatively low, which causes the fluidized electrode material to easily collect at the widthwise edges. When the electrode material film is thickened only at the widthwise edges, electric field concentration is likely to occur when electrodes are stacked. In response to this problem, the inventors have discovered a method in which the electrode material is supplied so as to be narrower than the desired width and thicker than the desired thickness, and then the formed electrode material film is gradually compressed and expanded, thereby gradually adjusting the width and thickness while supplying the electrode material. Specifically, the method for manufacturing an electrode molded body according to the present disclosure includes at least two steps of leveling the electrode material. Furthermore, W1 / W2 is greater than 0.86 but less than 0.96, and H2 / H1 is greater than 0.3 but less than 0.9. By forming the electrode material film under such conditions, it is possible to obtain an electrode molded article having excellent uniformity in thickness at the widthwise end portions.

[0017] Japanese Patent Publication Nos. 2017-533548 and 2021-530829 do not describe a method of forming a film in stages using a first film forming member and a second film forming member.

[0018] The method for manufacturing an electrode molded body according to the present disclosure will be described below with reference to the drawings. Fig. 1 is a schematic side view showing the manufacturing process of an electrode molded body. Fig. 2 is a schematic plan view showing the manufacturing process of an electrode molded body.

[0019] <Step of transporting current collector foil> In the method for manufacturing an electrode molded body according to the present disclosure, the current collector foil is transported. The current collector foil 11 is placed, for example, on a moving stage (not shown) provided in the manufacturing apparatus. The current collector foil 11 is transported in the transport direction indicated by the arrow in FIG. 1 by moving the moving stage in the transport direction. The transport speed of the current collector foil is not particularly limited, and is, for example, 1 m / min to 20 m / min.

[0020] (Current Collector Foil) From the viewpoint of transportability, etc., the average thickness of the current collector foil is preferably 3 μm or more, more preferably 5 μm or more, and particularly preferably 10 μm or more. From the viewpoint of flexibility and lightness, the average thickness is preferably 100 μm or less, more preferably 70 μm or less, and particularly preferably 50 μm or less. The average thickness of the current collector foil is the arithmetic mean of the thicknesses measured at three locations by cross-sectional observation. A known microscope (e.g., a scanning electron microscope) can be used for cross-sectional observation.

[0021] The size of the current collector foil is not particularly limited, but from the viewpoint of forming an electrode material film continuously, it is preferably long.

[0022] The current collector foil includes a current collector foil used as a positive electrode current collector or a negative electrode current collector. Examples of the positive electrode current collector include aluminum, aluminum alloy, stainless steel, nickel, and titanium. The positive electrode current collector is preferably aluminum or an aluminum alloy. The positive electrode current collector may be aluminum having a coating layer on its surface containing one or more of carbon, nickel, titanium, silver, gold, platinum, and vanadium oxide.

[0023] Examples of the negative electrode current collector include aluminum, copper, a copper alloy, stainless steel, nickel, and titanium. The negative electrode current collector is preferably aluminum, copper, a copper alloy, or stainless steel, and more preferably copper or a copper alloy. The negative electrode current collector may be copper or stainless steel having a coating layer on its surface containing one or more of carbon, nickel, titanium, silver, and lithium.

[0024] The current collector foil is preferably an aluminum foil (including an aluminum foil having the above-described coating layer on its surface) or a copper foil (including a copper foil having the above-described coating layer on its surface). Aluminum foil is usually used as a positive electrode current collector. Copper foil is usually used as a negative electrode current collector.

[0025] The current collecting foil may also be provided with a resin film as a support material. Examples of the support material include a resin film. Examples of the resin film include polyethylene terephthalate (PET) film, polypropylene (PP) film, polyethylene (PE) film, cyclic olefin polymer (COP, COC) film, triacetyl cellulose (TAC) film, polyimide (PI) film, and polyamide (PA) film. Another example of the support material is a release material. Examples of the release material include release paper (e.g., release paper manufactured by Lintec Corporation), a film having a release layer, and paper having a release layer, with release paper being preferred.

[0026] <Step of supplying electrode material onto current collector foil> The method for producing an electrode molded body according to the present disclosure includes a step of supplying an electrode material, which contains an electrode active material, a conductive additive, and an electrolyte solution and has a solids concentration of 40% by volume to 70% by volume, onto a current collector foil.

[0027] The method for supplying the electrode material onto the current collector foil is not particularly limited. For example, the electrode material may be continuously or intermittently supplied from a tank storing the electrode material to the upstream side of the current collector foil in the conveying direction. The amount of electrode material supplied to the current collector foil can be appropriately selected depending on the size, thickness, etc. of the electrode material film to be produced.

[0028] (Electrode Material) The electrode material contains at least an electrode active material, a conductive additive, and an electrolyte solution, and may contain other components as necessary.

[0029] - Electrode active material - An electrode active material is a material capable of inserting and releasing ions of a metal element belonging to Group 1 or Group 2 of the periodic table. The electrode active material is contained in a solid component. Examples of the electrode active material include a positive electrode active material and a negative electrode active material.

[0030] The positive electrode active material is not limited and may be any known electrode active material used for positive electrodes. The positive electrode active material is preferably a positive electrode active material that can reversibly insert and release lithium ions.

[0031] Specific examples of the positive electrode active material include transition metal oxides and elements that can be composited with lithium (e.g., sulfur). Among the above, the positive electrode active material is preferably a transition metal oxide.

[0032] The transition metal oxide is preferably a transition metal oxide containing at least one transition metal element (hereinafter referred to as "element Ma") selected from the group consisting of Co (cobalt), Ni (nickel), Fe (iron), Mn (manganese), Cu (copper), and V (vanadium).

[0033] When the transition metal oxide contains Li and the element Ma, the molar ratio of Li to Ma (Li / Ma) is preferably 0.3 to 2.2.

[0034] The transition metal oxide may also contain at least one transition metal element (hereinafter referred to as "element Mb") selected from the group consisting of Group 1 elements other than lithium, Group 2 elements, Al (aluminum), Ga (gallium), In (indium), Ge (germanium), Sn (tin), Pb (lead), Sb (antimony), Bi (bismuth), Si (silicon), P (phosphorus), and B (boron). The content of element Mb is preferably 0 mol % to 30 mol % relative to the amount of element Ma.

[0035] Examples of transition metal oxides include transition metal oxides having a layered rock salt structure, transition metal oxides having a spinel structure, lithium-containing transition metal phosphate compounds, lithium-containing transition metal halide phosphate compounds, and lithium-containing transition metal silicate compounds.

[0036] Examples of transition metal oxides having a layered rock salt structure include LiCoO ２ (Lithium cobalt oxide [LCO]), LiNi ２ O ２ (lithium nickel oxide), LiNi ０．８５ Co ０．１０ Al ０．０５ O ２ (nickel cobalt lithium aluminum oxide [NCA]), LiNi １／３ Co １／３ Mn １／３ O ２ (lithium nickel manganese cobalt oxide [NMC]), and LiNi ０．５ Mn ０．５ O ２ (lithium manganese nickel oxide).

[0037] Examples of transition metal oxides having a spinel structure include LiCoMnO ４ , Li ２ FeMn ３ O ８ , Li ２ CuMn ３ O ８ , Li ２ CrMn ３ O ８ , and Li ２ NiMn ３ O ８ Examples include:

[0038] Examples of lithium-containing transition metal phosphate compounds include olivine-type iron phosphate salts (e.g., LiFePO ４ , and Li ３ Fe ２ (P.O. ４ ) ３ ), iron pyrophosphate (e.g., LiFeP ２ O ７ ), cobalt phosphate salts (e.g., LiCoPO ４), monoclinic Nasicon-type vanadium phosphate salts (e.g., Li ３ V ２ (P.O. ４ ) ３ (Lithium vanadium phosphate)).

[0039] Examples of lithium-containing transition metal halophosphate compounds include iron fluorophosphates (e.g., Li ２ FePO ４ F), manganese fluorophosphate salts (e.g., Li ２ MnPO ４ F), and cobalt fluorophosphate salts (e.g., Li ２ CoPO ４ F).

[0040] Examples of lithium-containing transition metal silicate compounds include Li ２ FeSiO ４ , Li ２ MnSiO ４ , and Li ２ CoSiO ４ Examples include:

[0041] The transition metal oxide is preferably a transition metal oxide having a layered rock salt structure, such as LiCoO ２ (Lithium cobalt oxide [LCO]), LiNi ０．８５ Co ０．１０ Al ０．０５ O ２ (nickel cobalt lithium aluminum oxide [NCA]), and LiNi １／３ Co １／３ Mn １／３ O ２ (nickel manganese cobalt oxide [NMC]) and more preferably at least one compound selected from the group consisting of:

[0042] The positive electrode active material may be a commercially available product or a synthetic product produced by a known method (e.g., a calcination method). For example, the positive electrode active material obtained by the calcination method may be washed with water, an acidic aqueous solution, an alkaline aqueous solution, or an organic solvent. The positive electrode active material may also have a carbon coating on its surface.

[0043] The shape of the positive electrode active material is not limited, but from the viewpoint of ease of handling, it is preferably in the form of particles.

[0044] The volume average particle size of the positive electrode active material is not limited and can be, for example, 0.1 μm to 50 μm. The volume average particle size of the positive electrode active material is preferably 0.3 μm to 40 μm, and more preferably 0.5 μm to 30 μm. When the volume average particle size of the positive electrode active material is 0.3 μm or more, scattering of the positive electrode active material during handling can be suppressed. When the volume average particle size of the positive electrode active material is 40 μm or less, the thickness of the electrode layer can be easily adjusted and the occurrence of voids during the molding process can be suppressed.

[0045] The volume average particle size of the positive electrode active material is measured by the following method. A dispersion containing 0.1 mass % or less of the positive electrode active material is prepared by mixing the positive electrode active material with a solvent (e.g., pure water, ethanol, heptane, octane, toluene, or xylene). The dispersion is irradiated with 1 kHz ultrasound for 10 minutes and used as a measurement sample. Using a laser diffraction / scattering particle size distribution measurement device (e.g., LA-960 manufactured by Horiba, Ltd.), data is acquired 50 times at a temperature of 25°C, and the volume average particle size is determined from the volume frequency particle size distribution. A quartz cell is used as the measurement cell. The above measurement is performed using five samples, and the average of the measured values ​​is used as the volume average particle size of the positive electrode active material. For other detailed conditions, refer to "JIS Z 8828:2013" as necessary.

[0046] Examples of methods for adjusting the particle size of the positive electrode active material include methods using a pulverizer, a crusher, or a classifier. Alternatively, a known milling method may be used to adjust the particle size of the positive electrode active material.

[0047] The positive electrode active material may be used alone or in combination of two or more. Even when one type of positive electrode active material is used, positive electrode active materials having different particle sizes may be used in combination.

[0048] The content of the positive electrode active material relative to the total volume of the electrode material is preferably 30 to 60% by volume, more preferably 35 to 55% by volume, and even more preferably 40 to 50% by volume.

[0049] The negative electrode active material is not limited and may be any known negative electrode active material used for negative electrodes. The negative electrode active material is preferably a negative electrode active material that can reversibly insert and release lithium ions.

[0050] Examples of the negative electrode active material include carbonaceous materials, metal oxides (e.g., tin oxide), silicon oxide, metal composite oxides, lithium alone, lithium alloys (e.g., lithium-aluminum alloys), and metals capable of forming alloys with lithium (e.g., Sn, Si, and In). Among these, the negative electrode active material is preferably a carbonaceous material or a lithium composite oxide from the viewpoint of reliability.

[0051] Carbonaceous materials are materials consisting essentially of carbon. Examples of carbonaceous materials include petroleum pitch, carbon black (e.g., acetylene black), graphite (e.g., natural graphite and artificial graphite (e.g., vapor-grown graphite)), hard carbon, and carbonaceous materials obtained by calcining synthetic resins (e.g., polyacrylonitrile (PAN) and furfuryl alcohol resin). Examples of carbonaceous materials include carbon fibers (e.g., polyacrylonitrile-based carbon fibers, cellulose-based carbon fibers, pitch-based carbon fibers, vapor-grown carbon fibers, dehydrated PVA (polyvinyl alcohol)-based carbon fibers, lignin carbon fibers, glassy carbon fibers, and activated carbon fibers). Examples of graphite include mesophase microspheres, graphite whiskers, and tabular graphite. In this disclosure, "tabular" refers to a shape having two major planes facing in opposite directions.

[0052] The metal composite oxide is preferably a metal composite oxide capable of absorbing and desorbing lithium. From the viewpoint of high current density charge / discharge characteristics, the metal composite oxide capable of absorbing and desorbing lithium preferably contains at least one element selected from the group consisting of titanium and lithium.

[0053] The metal oxide and metal composite oxide are particularly preferably amorphous oxides.

[0054] The metal oxides and metal composite oxides are also preferably chalcogenides, which are reaction products of metal elements and elements of Group 16 of the periodic table.

[0055] Among the compound group consisting of amorphous oxides and chalcogenides, amorphous oxides and chalcogenides of metalloid elements are preferred, and oxides and chalcogenides containing at least one element selected from the group consisting of elements of Groups 13 to 15 in the periodic table, Al, Ga, Si, Sn, Ge, Pb, Sb, and Bi are more preferred.

[0056] It is also preferable that the negative electrode active material further contains titanium. From the viewpoint that the volume change during the absorption and desorption of lithium ions is small, and thus rapid charge and discharge characteristics are excellent, and that deterioration of the electrode is suppressed, thereby enabling an improvement in the life of the lithium ion secondary battery, the negative electrode active material containing titanium is preferably Li ４ Ti ５ O １２ (lithium titanate [LTO]) is preferred.

[0057] The negative electrode active material may be a commercially available product or a synthetic product produced by a known method (e.g., a calcination method). For example, the negative electrode active material obtained by the calcination method may be washed with water, an acidic aqueous solution, an alkaline aqueous solution, or an organic solvent.

[0058] The negative electrode active material is available, for example, as CGB20 (Nippon Graphite Industries Co., Ltd.).

[0059] The composition of the negative electrode active material is measured using inductively coupled plasma (ICP) emission spectroscopy.

[0060] The shape of the negative electrode active material is not limited, but is preferably particulate from the viewpoints of ease of handling and ease of control of uniformity during mass production.

[0061] The volume average particle size of the negative electrode active material is preferably 0.1 μm to 60 μm, more preferably 0.3 μm to 50 μm, and particularly preferably 0.5 μm to 40 μm. The volume average particle size of the negative electrode active material is measured by a method similar to the method for measuring the volume average particle size of the positive electrode active material.

[0062] The particle size of the negative electrode active material can be adjusted, for example, by using a pulverizer or a classifier.

[0063] The negative electrode active material may be used alone or in combination of two or more. Even when one type of negative electrode active material is used, negative electrode active materials having different particle sizes may be used in combination.

[0064] The content of the negative electrode active material relative to the total volume of the electrode material is preferably 30 to 60% by volume, more preferably 35 to 57% by volume, and even more preferably 45 to 55% by volume.

[0065] The surfaces of the positive electrode active material and the negative electrode active material may each be coated with a surface coating agent. Examples of the surface coating agent include metal oxides containing Ti, Nb, Ta, W, Zr, Si, or Li. Examples of the metal oxide include titanate spinel, tantalum-based oxides, niobium-based oxides, and lithium niobate-based compounds.

[0066] Conductive additives: The electrode material contains a conductive additive from the viewpoint of improving the electronic conductivity of the electrode active material. There are no limitations on the conductive additive, and known conductive additives can be used. The conductive additive is contained in the solid component.

[0067] Examples of conductive additives include graphite (e.g., natural graphite and artificial graphite), carbon black (e.g., acetylene black, ketjen black, and furnace black), amorphous carbon (e.g., needle coke), carbon fibers (e.g., vapor-grown carbon fibers and carbon nanotubes), other carbonaceous materials (e.g., graphene and fullerene), metal powders (e.g., copper powder and nickel powder), metal fibers (e.g., copper fibers and nickel fibers), and conductive polymers (e.g., polyaniline, polypyrrole, polythiophene, polyacetylene, and polyphenylene derivatives).

[0068] The conductive additive may be used alone or in combination of two or more. The content of the conductive additive relative to the total volume of the electrode material is preferably 0.05% by volume to 5% by volume, more preferably 0.1% by volume to 4% by volume, and even more preferably 0.5% by volume to 3% by volume. In the method for producing an electrode layer according to the present disclosure, the amount of the conductive additive used is preferably determined so that the content in the electrode layer falls within the above-mentioned range.

[0069] -Electrolyte Solution- The electrode material contains an electrolyte solution. There are no particular limitations on the electrolyte solution, and any known electrolyte solution can be used. Examples of the electrolyte solution include an electrolyte solution containing an electrolyte and a solvent. Specific examples of the electrolyte solution include an electrolyte solution containing a lithium salt compound as the electrolyte and a carbonate compound as the solvent.

[0070] An example of the lithium salt compound is lithium hexafluorophosphate. The electrolyte solution may contain one kind of lithium salt compound alone, or may contain two or more kinds of lithium salt compounds.

[0071] Examples of carbonate compounds include linear carbonate compounds such as ethyl methyl carbonate (also referred to as EMC), dimethyl carbonate (also referred to as DMC), and diethyl carbonate (DEC), and cyclic carbonate compounds such as ethylene carbonate (also referred to as EC) and propylene carbonate (also referred to as PC). The electrolyte may contain one type of carbonate compound alone, or may contain two or more types of carbonate compounds, or may use one or more linear carbonate compounds and one or more cyclic carbonate compounds in combination.

[0072] As the electrolyte contained in the electrolytic solution, for example, a known inorganic solid electrolyte can be used.

[0073] An ionic liquid may be used as a component of the electrolytic solution, for example. The ionic liquid may be used as either an electrolyte or a solvent.

[0074] The content of the electrolyte solution relative to the total volume of the electrode material is preferably 70% by volume or less, and may be 50% by volume or less, or 40% by volume or less. The lower limit of the content of the electrolyte solution relative to the total volume of the electrode material is not limited, and may be 20% by volume or more, or 30% by volume or more. The content of the electrolyte solution relative to the total volume of the electrode material is preferably, for example, 30% by volume to 50% by volume.

[0075] The electrode material may contain, as a liquid component, a solvent (hereinafter simply referred to as "solvent") other than the solvent contained as a component of the electrolyte. Examples of the solvent include alcohol compound solvents, ether compound solvents, amide compound solvents, amino compound solvents, ketone compound solvents, aromatic compound solvents, aliphatic compound solvents, and nitrile compound solvents.

[0076] The boiling point of the solvent at normal pressure (i.e., 1 atmosphere) is preferably 50° C. or higher, and more preferably 70° C. or higher. The upper limit of the boiling point of the solvent at normal pressure (i.e., 1 atmosphere) is preferably 250° C. or lower, and more preferably 220° C. or lower.

[0077] The solvent may be used alone or in combination of two or more. The content of the liquid components (i.e., the electrolyte solution and the solvent) relative to the total volume of the electrode material is preferably 70% by volume or less, and may be 50% by volume or less, or may be 40% by volume or less. The lower limit of the content of the liquid components relative to the total volume of the electrode material is not limited, and may be 20% by volume or more, or may be 30% by volume or more. The content of the liquid components relative to the total volume of the electrode material is preferably 30% by volume to 50% by volume.

[0078] Note that the liquid components contained in the electrode material, i.e., the components in the electrode layer that are liquid at 25° C., are preferably liquid even at −10° C., and are preferably liquid even at −20° C. In other words, the components in the electrode layer that are liquid at 25° C. are preferably components that do not solidify even at −10° C., and are preferably components that do not solidify even at −20° C.

[0079] Other Components: In addition to the above components, the electrode material may contain inorganic solid electrolytes, binders, dispersants, other additives, and the like. From the viewpoint of improving energy density, the electrode material preferably has a low binder (also referred to as a resin component) content, preferably 1% by mass or less, and particularly preferably no binder (0% by mass). In addition to the resin component, the binder includes components called rheology modifiers and dispersants, and examples of such binders include fluorine-containing resins, hydrocarbon-based thermoplastic resins, acrylic resins, and urethane resins. Examples of dispersants include known dispersants capable of dispersing substances to be dispersed. As other additives, known additives added to electrodes can be used.

[0080] The electrode material can be prepared by mixing, for example, an electrode active material, a conductive additive, an electrolytic solution, and, if necessary, an inorganic solid electrolyte and other components. Examples of the mixing method include methods using a ball mill, a bead mill, a planetary mixer, a blade mixer, a roll mill, a kneader, or a disk mill.

[0081] The electrode material has a solid content concentration of 40% to 70% by volume. The solid content concentration means the content rate of solid components relative to the total volume of the electrode material. From the viewpoint of battery performance, the solid content concentration is preferably 46% to 63% by volume. The solid content concentration is calculated from the composition ratio of each component contained in the electrode material and the specific gravity of those components.

[0082] <Process for forming first electrode material film and second electrode material film> The method for manufacturing an electrode molded body according to the present disclosure includes a process for leveling an electrode material supplied onto a current collector foil using a first film-forming member to form a first electrode material film, and a process for leveling the first electrode material film using a second film-forming member to form a second electrode material film.

[0083] 1 and 2 , a first film forming member 21 and a second film forming member 22 are provided on the current collector foil 11 in this order from the upstream side to the downstream side in the conveyance direction of the current collector foil. The current collector foil 11 moves in the direction of the arrow, and electrode material 30 supplied onto the current collector foil 11 passes through the first film forming member 21 and is formed into a layer, thereby forming a first electrode material film 31. Furthermore, as the first electrode material film 31 passes through the second film forming member 22, the thickness and width of the first electrode material film 31 are adjusted, and a second electrode material film 32 is formed.

[0084] Specifically, when the width of the first electrode material film 31 is W1 and the width of the second electrode material film 32 is W2, W1 / W2 is greater than 0.86 and less than 0.96, and when the thickness of the first electrode material film 31 is H1 and the thickness of the second electrode material film 32 is H2, H2 / H1 is greater than 0.3 and less than 0.9. W1 / W2 is preferably 0.89 or greater and less than 0.96, and more preferably 0.92 or greater and less than 0.96. H2 / H1 is preferably 0.5 or greater and less than 0.9, and more preferably 0.7 or greater and less than 0.9.

[0085] The widths of the first electrode material film 31 and the second electrode material film 32 are measured using an image captured from the top surface of the electrode. The thicknesses of the first electrode material film 31 and the second electrode material film 32 are measured using a non-contact displacement meter, for example, a laser displacement meter.

[0086] By gradually leveling the electrode material 30 and adjusting the thickness and width of the electrode material film, an electrode molded body can be obtained that has excellent thickness uniformity at the widthwise ends of the electrode material film that is finally formed.

[0087] First Film-Depositing Member and Second Film-Depositing Member The first film-depositing member 21 and the second film-depositing member 22 are not particularly limited as long as they are members that can level the electrode material, and examples thereof include regulating members such as blades and rollers.

[0088] The blade is a flat, plate-like member. The shape, size, material, etc. of the contact portion that comes into contact with the electrode material may be appropriately selected depending on the type of electrode material (type of electrode active material, solids concentration, composition of the electrolyte (viscosity, surface tension), etc.), the size, thickness, etc. of the intended electrode material film.

[0089] The contact portion of the blade with the electrode material preferably does not easily adhere to the electrode material. For example, it is preferable that at least the contact portion of the blade exhibits releasability. The blade may be, for example, a resin blade (e.g., a fluororesin such as polytetrafluoroethylene (PTFE) or polyether ether ketone (PEEK)), a metal blade (e.g., stainless steel, aluminum, iron, or cemented carbide), or a ceramic blade. Furthermore, in order to impart releasability to the surface of the contact portion of the blade, the blade may have a surface layer that exhibits releasability (e.g., a surface layer containing a fluororesin, or a surface layer containing silicon-based particles and a resin). Furthermore, in order to enhance the wear resistance of the blade, the metal or ceramic blade body may have a high-hardness coating such as titanium oxide, titanium nitride (TiN), or tungsten carbide.

[0090] When leveling the electrode material 30, the first film forming member 21 is preferably vibrated at a frequency of 10 kHz or more and less than 100 kHz.

[0091] There are no particular limitations on the vibration direction of the first film deposition member 21. The vibration amplitude of the first film deposition member 21 is preferably 1 μm to 100 μm.

[0092] The vibration can be applied by, for example, a vibrator. The vibration propagates to the electrode material and applies shear force, which can reduce the viscosity and improve the fluidity of at least the electrode material 30 at the contact portion with the first film-forming member 21. This allows the surface shape of the formed first electrode material film 31 to be uniform, and a first electrode material film 31 with little thickness variation can be obtained.

[0093] Similarly, it is preferable that the second film deposition member 22 also vibrates when leveling the first electrode material film 31. From the viewpoint of improving the uniformity of the thickness of the width direction end portions of the finally formed electrode material film, it is preferable that the vibration frequency of the second film deposition member 22 is smaller than the vibration frequency of the first film deposition member 21. Specifically, it is preferable that the ratio of the vibration frequency of the second film deposition member 22 to the vibration frequency of the first film deposition member 21 is 0.001 to 0.1. Furthermore, from the viewpoint of improving the uniformity of the thickness of the width direction end portions of the finally formed electrode material film, it is preferable that the vibration amplitude of the second film deposition member 22 is smaller than the vibration amplitude of the first film deposition member 21. Specifically, it is preferable that the ratio of the vibration amplitude of the second film deposition member 22 to the vibration amplitude of the first film deposition member 21 is 0.005 to 0.5.

[0094] In the method for manufacturing an electrode molded body according to the present disclosure, the electrode material film may be formed using two or more film-forming members. That is, the method for manufacturing an electrode molded body according to the present disclosure may further include a step of leveling the second electrode material film 32 using a third film-forming member to form a third electrode material film. By gradually leveling the electrode material using three or more film-forming members, it is possible to improve the uniformity of the thickness of the width direction end portions of the electrode material film that is finally formed.

[0095] That is, the method may include a step of forming an electrode material film by successively leveling the electrode material supplied onto the current collector foil using N film-forming members (where N is 2 or more). Ｎ－１ , the vibration frequency of the Nth film forming member is Hz Ｎ In this case, Hz Ｎ / Hz Ｎ－１ is preferably 0.001 to 0.1. In addition, the vibration amplitude of the (N-1)th film-forming member is set to Wh Ｎ－１, the vibration amplitude of the Nth film forming member is Wh Ｎ In this case, Wh Ｎ / Wh Ｎ－１ is preferably 0.005 to 0.5.

[0096] That is, in the manufacturing method of the electrode molded body according to the present disclosure, the vibration frequency and vibration amplitude of the film-forming member are reduced in the final stage of forming the electrode material film, thereby improving the uniformity of the thickness of the widthwise ends of the electrode material film that is finally formed.

[0097] In order to set W1 / W2 to 0.7 or more and less than 1, when the width of the first film forming member 21 is WN1 and the width of the second film forming member 22 is WN2, it is preferable that WN1 / WN2 be 0.7 or more and less than 1. The width here means the length in the direction perpendicular to the conveyance direction of the current collecting foil.

[0098] It is preferable that the downstream end 21a of the first film forming member 21 in the conveying direction of the current collecting foil 11 is closer to the current collecting foil 11 than the upstream end 21b in the conveying direction of the current collecting foil 11, and that the first film forming member 21 is arranged at an incline with respect to the current collecting foil 11.

[0099] The distance here means the shortest distance between the downstream tip 21 a or the upstream tip 21 b and the upper surface of the current collecting foil 11 .

[0100] By providing the first film forming member 21 at an angle relative to the current collecting foil 11, the supply amount of the electrode material 30 can be adjusted, and a more uniform first electrode material film can be formed.

[0101] 1 and 2, first restricting members 41, 42 that restrict the width of the first electrode material film 31 are preferably provided between the first film forming member 21 and the current collector foil 11. The first restricting members 41, 42 are preferably provided spaced apart from each other in the width direction of the current collector foil. The width of the first electrode material film 31 is controlled by supplying the electrode material 30 between the first restricting members 41, 42. As a result, the uniformity of the thickness of the width direction end portions of the electrode material film that is finally formed is improved.

[0102] In addition, a second regulating member (not shown) that regulates the width of the second electrode material film 32 may be provided between the second film forming member 22 and the current collecting foil 11, similar to the first regulating members 41, 42.

[0103] As shown in Figures 1 and 2, the first restricting members 41, 42 preferably do not contact the first film forming member 21 and the current collecting foil 11. By providing the first restricting members 41, 42 independently and without contacting the first film forming member 21 and the current collecting foil 11, the first restricting members themselves do not transmit vibrations, thereby suppressing the flow of the electrode material on their surfaces. Furthermore, if the first restricting members do not contact the current collecting foil, defects such as wrinkles and scratches on the current collecting foil can be suppressed. Furthermore, the first restricting members 41, 42 are preferably located upstream of the first film forming member 21 in the conveying direction of the current collecting foil. This allows the amount of electrode material 30 in contact with the first film forming member 21 to be adjusted before the electrode material 30 is leveled by the first film forming member 21.

[0104] The shape of the first restricting members 41, 42 is not particularly limited, but it is preferable that the first restricting members 41, 42 have a shape that decreases in height in the conveyance direction of the current collector foil 11. This shape can prevent the electrode material from entering the gap between the first restricting members and the film-forming member or current collector foil, causing the edge shape of the electrode to become unstable. The shape that decreases in height in the conveyance direction of the current collector foil 11 may be a shape that decreases in steps or a shape that decreases continuously. The shape of the first restricting members 41, 42 may be a triangle in side view so that the height decreases continuously, but it is preferable that the tip of the first restricting members 41, 42 on the downstream side in the conveyance direction be notched.

[0105] The shortest distance between the lower surface 211 of the first film-forming member 21 and the upper surface 411 of the first restricting member 41 is preferably short, and more preferably longer than 0 mm and equal to or less than 0.5 mm. A short distance between the two can prevent the electrode material from penetrating into the gap between the first restricting member and the film-forming member or current collecting foil, thereby preventing the end shape of the electrode from becoming unstable.

[0106] The shortest distance between the lower surface 412 of the first restricting member 41 and the upper surface 111 of the current collector foil 11 is preferably short, and more preferably longer than 0 mm and equal to or less than 0.5 mm. A short distance between the two can prevent the electrode material from entering the gap between the first restricting member and the film-forming member or current collector foil, thereby preventing the end shape of the electrode from becoming unstable.

[0107] The shortest distance between the downstream tip 41 a of the first restricting member 41 in the conveyance direction of the current collector foil 11 and the downstream tip 21 a of the first film forming member 21 in the conveyance direction of the current collector foil 11 is preferably short, and more preferably longer than 0 mm and equal to or less than 5 mm. If the distance between the two is short, it is possible to prevent the electrode material from adhering to the tip of the first restricting member, thereby preventing the end shape of the electrode from becoming unstable.

[0108] The thickness of the electrode material film in the electrode molded article is preferably 100 μm to 1000 μm, more preferably 200 μm to 600 μm. The thickness of the electrode material film is the arithmetic average of thicknesses measured at any three locations by cross-sectional observation. A known microscope (e.g., a scanning electron microscope) can be used for cross-sectional observation.

[0109] The method for producing an electrode molded body according to the present disclosure may include other steps in addition to those described above, such as a step of pressurizing the electrode material film.

[0110] (Step of Pressurizing Electrode Material Film) The method for producing an electrode molded body according to the present disclosure may include a step of pressurizing the electrode material film obtained in the above-described steps. By including the pressurizing step in the method for producing an electrode molded body according to the present disclosure, it is possible to increase the density of the electrode material and achieve in-plane uniformity of the density and thickness.

[0111] Examples of the pressure means used in this step include a pair of pressure rolls and a press.

[0112] When the electrode material film is pressurized, the pressure is preferably 0.01 MPa to 100 MPa, more preferably 0.1 MPa to 50 MPa, and particularly preferably 0.2 MPa to 10 MPa.

[0113] In this step, the electrode material film may be pressurized in stages using a plurality of pressurizing means (for example, pairs of pressurizing rolls). By pressurizing the electrode material film in stages using a plurality of pressurizing means, the density and thickness of the electrode material can be made more uniform. For example, the electrode material film can be pressurized in stages by using a plurality of pairs of pressurizing rolls in which the gap between the rolls is adjusted to be narrower in stages.

[0114] This step is preferably performed by moving the pressure applying means and the electrode material film (specifically, the support on which the electrode material film is formed) relative to each other. In the present disclosure, "moving the pressure applying means and the electrode material film relative to each other" includes moving the pressure applying means in one direction relative to the electrode material film, moving the electrode material film in one direction relative to the pressure applying means, and moving both the pressure applying means and the electrode material film in one direction, but it is preferable to move the electrode material film in one direction relative to the pressure applying means.

[0115] The means for moving the electrode material film (specifically, the support on which the electrode material film is formed) is not limited, and any known conveying means can be used, such as a belt conveyor, a linear motion guide, and a cross roller table.

[0116] In this step, from the viewpoint of improving formability, the electrode material film heated at, for example, 30° C. to 100° C. may be pressurized.

[0117] The electrode molded article obtained by the method for producing an electrode molded article according to the present disclosure has excellent in-plane thickness uniformity and can be used as various electrodes. The electrode molded article is preferably an electrode molded article for an all-solid-state secondary battery.

[0118] From the viewpoint of improving battery performance (e.g., discharge capacity and output characteristics), the average thickness of the electrode molded body is preferably 0.01 mm to 2 mm, more preferably 0.05 mm to 1.5 mm, and particularly preferably 0.1 mm to 1 mm. The average thickness of the electrode molded body is measured in the same manner as the average thickness of the current collector foil.

[0119] The present disclosure will be described in more detail below with reference to examples, but the present disclosure is not limited to the following examples as long as they do not depart from the gist of the disclosure.

[0120] Examples 1 to 3 and Comparative Examples 1 to 5: A mixture of ethylene carbonate, propylene carbonate, and diethylene carbonate was mixed with LiPF as an electrolyte. ６ After mixing, vinylene carbonate was further mixed. 64 g of the resulting mixture was taken out and designated as electrolyte solution X1. 2 g of Ketjen black as a conductive additive and 174 g of lithium iron phosphate as a positive electrode active material were stirred for 30 seconds at 1500 rpm (revolutions per minute) in a mixer (Thinky Mixer ARE-310, manufactured by Thinky Corporation) to prepare a kneaded material Y1 (176 g). 64 g of electrolyte solution X1 was added to 176 g of the kneaded material Y1, and the mixture was stirred for 120 seconds at 1500 rpm in a mixer (Thinky Mixer ARE-310, manufactured by Thinky Corporation) to obtain a positive electrode material P1. The volume ratio of the solid component to the liquid component of the resulting positive electrode material P1 was 48:52.

[0121] As shown in Figures 1 and 2, two film-forming members (a first film-forming member and a second film-forming member) were arranged, and a positive electrode material P1 was supplied onto the current collecting foil to produce an electrode molded body. The widths, vibration frequencies, and vibration amplitudes of the first and second film-forming members were adjusted to the values ​​shown in Table 1. A first restricting member was provided between the first film-forming member and the current collecting foil to restrict the width of the first electrode material film. The first restricting member was not in contact with the first film-forming member or the current collecting foil. The shortest distance between the lower surface of the first film-forming member and the upper surface of the first restricting member was 0.1 mm. The shortest distance between the lower surface of the first restricting member and the upper surface of the current collecting foil was 0.3 mm. The shortest distance between the downstream end of the first restricting member in the current collecting foil conveyance direction and the downstream end of the first film-forming member in the current collecting foil conveyance direction was 2 mm.

[0122] The electrode material supplied onto the current collecting foil was leveled using a first film-forming member to form a first electrode material film so that the width W1 and thickness H1 were the values ​​shown in Table 1. The first electrode material film was leveled using a second film-forming member to form a second electrode material film so that the width W2 and thickness H2 were the values ​​shown in Table 1.

[0123] The obtained electrode molded body was evaluated to determine whether the second electrode material film was formed on the current collector foil without excess or deficiency. Specifically, the evaluation was based on the distance between the widthwise end of the second electrode material film and the widthwise end of the current collector foil. The evaluation criteria are as follows: "A" is a level that is acceptable for practical use. A: The average value of the distance between the widthwise end of the second electrode material film and the widthwise end of the current collector foil is within 1 mm. B1: The width of the second electrode material film is shorter than the width of the current collector foil, and the average value of the distance between the widthwise end of the second electrode material film and the widthwise end of the current collector foil exceeds 1 mm. B2: The width of the second electrode material film is longer than the width of the current collector foil, and the average value of the distance between the widthwise end of the second electrode material film and the widthwise end of the current collector foil exceeds 1 mm.

[0124]

[0125] In Examples 1 and 2, W1 / W2 was greater than 0.86 and less than 0.96, and H2 / H1 was greater than 0.3 and less than 0.9, so it was found that an electrode material film was formed with a width appropriate for the width of the current collecting foil. In Comparative Examples 1 and 4, W1 / W2 was 0.86 or less, so an electrode material film was not sufficiently formed on the current collecting foil. In Comparative Example 2, W1 / W2 was 0.96 or more, so the electrode material film significantly protruded from the current collecting foil. In Comparative Example 3, H2 / H1 was 0.3 or less, so the electrode material film significantly protruded from the current collecting foil. In Comparative Example 5, H2 / H1 was 0.9 or more, so an electrode material film was not sufficiently formed on the current collecting foil.

[0126] Example 100 In Example 100, a positive electrode material P1 was supplied onto a current collector foil in the same manner as in Example 2, except that a third film-forming member was further disposed, to produce an electrode molded body. The width, vibration frequency, and vibration amplitude of the first and second film-forming members were adjusted to be the same as those in Example 2. The width of the third film-forming member was adjusted to 208 mm, the vibration frequency of the third film-forming member was adjusted to 0.3 kHz, and the vibration amplitude of the third film-forming member was adjusted to 1 μm.

[0127] The electrode material supplied onto the current collecting foil was leveled using a first film forming member to form a first electrode material film so that the width W1 and thickness H1 were the same as those in Example 2. The first electrode material film was leveled using a second film forming member to form a second electrode material film so that the width W2 and thickness H2 were the same as those in Example 2. The second electrode material film was leveled using a third film forming member to form a third electrode material film so that the width W3 and thickness H3 were the same as those in Width W2 and thickness H2 (Width: 204 mm, Thickness: 0.4 mm).

[0128] The obtained electrode molded body was evaluated in the same manner as in Example 2 to determine whether the third electrode material film was formed on the current collector foil without excess or deficiency. The evaluation result was A. Furthermore, the surface of the third electrode material film in Example 100 was smoother than the surface of the second electrode material film.

[0129] In this example, except that only one film-forming member was disposed, a positive electrode material P1 was supplied onto a current collector foil to produce an electrode molded body in the same manner as in Example 2. The width, vibration frequency, and vibration amplitude of one film-forming member were adjusted to be the same as those of the second film-forming member in Example 2.

[0130] The obtained electrode molded article was evaluated in the same manner as in Example 2 to determine whether the first electrode material film was formed on the current collector foil without excess or deficiency. It was found that there were both portions where the width of the first electrode material film was shorter than the width of the current collector foil and portions where the width of the first electrode material film was longer than the width of the current collector foil. The evaluation results were both B1 and B2.

[0131] The disclosure of Japanese Patent Application No. 2023-218611, filed on December 25, 2023, is incorporated herein by reference in its entirety. In addition, all documents, patent applications, and technical standards described herein are incorporated herein by reference to the same extent as if each individual document, patent application, and technical standard were specifically and individually indicated to be incorporated by reference.

Claims

1. A method for manufacturing a shaped body for an electrode, comprising: a step of conveying a current collector foil; a step of supplying an electrode material containing an electrode active material, a conductive assistant, and an electrolytic solution and having a solid content concentration of 40% to 70% by volume onto the current collector foil; a step of leveling the electrode material supplied onto the current collector foil using a first film-forming member to form a first electrode material film; and a step of leveling the first electrode material film using a second film-forming member to form a second electrode material film, wherein when the width of the first electrode material film is W1 and the width of the second electrode material film is W2, W1 / W2 is greater than 0.86 and less than 0.96, and when the thickness of the first electrode material film is H1 and the thickness of the second electrode material film is H2, H2 / H1 is greater than 0.3 and less than 0.

9.

2. The method for manufacturing a shaped body for an electrode according to claim 1, wherein the first film-forming member vibrates at a frequency of 10 kHz or more and less than 100 kHz.

3. The method for manufacturing a shaped body for an electrode according to claim 1 or 2, wherein when the width of the first film-forming member is WN1 and the width of the second film-forming member is WN2, WN1 / WN2 is greater than 0.8 and less than 1.

4. The method for manufacturing a shaped body for an electrode according to claim 1 or 2, wherein a first restricting member for restricting the width of the first electrode material film is provided between the first film-forming member and the current collector foil.

5. The method for manufacturing a shaped body for an electrode according to claim 4, wherein the first restricting member is not in contact with the first film-forming member and the current collector foil.

6. The method for manufacturing a shaped body for an electrode according to claim 4, wherein the downstream end of the first film-forming member in the conveying direction of the current collector foil is closer to the current collector foil than the upstream end of the current collector foil in the conveying direction, and the first film-forming member is provided inclined with respect to the current collector foil.

7. The method for manufacturing a shaped body for an electrode according to claim 6, wherein the first restricting member has a shape in which the height decreases in the conveying direction of the current collector foil.

8. The method for manufacturing a shaped body for an electrode according to claim 7, wherein the shortest distance between the lower surface of the first film-forming member and the upper surface of the first restricting member is greater than 0 mm and less than or equal to 0.5 mm.

9. The method for manufacturing a shaped body for an electrode according to claim 7, wherein the shortest distance between the lower surface of the first restricting member and the upper surface of the current collector foil is greater than 0 mm and less than or equal to 0.5 mm.

10. The method for manufacturing a molded body for an electrode according to claim 7, wherein the shortest distance between the downstream end of the current collector foil in the transport direction of the first regulating member and the downstream end of the current collector foil in the transport direction of the first film forming member is more than 0 mm and 5 mm or less.

11. The method for manufacturing a molded body for an electrode according to claim 1 or 2, further comprising a step of leveling the second electrode material film using a third film forming member to form a third electrode material film.

12. The method for manufacturing a molded body for an electrode according to claim 1 or 2, wherein a second regulating member for regulating the width of the second electrode material film is provided between the second film forming member and the current collector foil.

13. A step of forming an electrode material film by leveling the electrode material supplied onto the current collector foil in order using N (where N is 2 or more) film-forming members, and the vibration frequency of the (N - 1)th film-forming member is Hz Ｎ－１ , and the vibration frequency of the Nth film-forming member is Hz Ｎ When it is set as Hz Ｎ / Hz Ｎ－１ is 0.001 to 0.

1. The method for manufacturing a molded body for an electrode according to claim 1 or claim 2.

14. A step of forming an electrode material film by leveling the electrode material supplied onto the current collector foil in order using N (where N is 2 or more) film forming members, and the vibration amplitude of the (N - 1)th film forming member is Wh Ｎ－１ , and the vibration amplitude of the Nth film forming member is Wh Ｎ When it is set as, Wh Ｎ / Wh Ｎ－１ is 0.005 to 0.5, The manufacturing method of the molded object for electrodes of Claim 1 or Claim 2.

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