Method for producing a layer composite as a pre-product for an electrode assembly of a battery cell; method for producing an electrode assembly, and layer composite

Abstract

The invention relates to a method for producing a layer composite which is a pre-product for an electrode assembly of a battery cell, wherein the layer composite has at least one separator layer embedded on both sides, wherein the separator layer is embedded in a structure A-S-K or K-S-Cx, where A is an anode layer, K is a cathode layer, S is a separator layer, and Cx is a current-conducting layer for a bipolar battery cell, an anodic current-collecting layer or a cathodic current-collecting layer, wherein the layer composite contains a maximum of two separator layers S, and a maximum of one Cx layer, the method comprising: producing the structure A-S-K or K-S-Cx by joining and / or depositing the layers A, S, K or K, S, Cx simultaneously or in any order, wherein i) production takes place under the action of pressure and / or heat in order to bond at least the layers A and S and / or the layers K and S to one another under the influence of the pressure and / or the heat, and / or ii) during production, the layer K and / or A is formed by deposition on the layer S.

Description

[0001] Description

[0002] Method for producing a layered composite as a precursor for an electrode assembly of a battery cell; method for producing an electrode assembly and layered composite

[0003] The invention relates to a method for producing a layered composite that is a precursor for an electrode assembly of a battery cell, a method for producing an electrode assembly for a battery cell and a layered composite for use as a precursor for an electrode assembly for a battery cell.

[0004] Due to the rapid market development of electric vehicles and grid-based energy storage, high-performance, cost-effective lithium-ion batteries are currently one of the most promising options for large-scale energy storage. Solid-state batteries offer many advantages for use in electric cars. Compared to conventional lithium-ion batteries, they offer a higher energy density, allowing for smaller batteries or, for the same size, more powerful designs. They also offer greater safety and faster charging. However, the production of solid-state separators for solid-state batteries is particularly time-consuming, energy-intensive, and expensive.

[0005] In solid-state batteries, it is difficult to achieve good ion conduction between the separator and the anode or cathode, because Li +Ions must overcome solid-to-solid interfaces. This applies both in the electrode coating and between the individual layers. Solid-state cells with multiple solid electrolytes optimized for their respective electrode potentials are particularly suitable, but this creates additional interfaces that must be optimized for ion conductivity. Good interfaces could be achieved for relatively soft solid electrolytes by applying very high pressure (during operation), but this is not cost-effective for use in a vehicle. Automotive battery cells are usually quite large (>50Ah) because a larger form factor allows for greater energy density. (Cylindrical cells are also becoming increasingly larger.) This further exacerbates the problem of generating high, large-area pressure if this approach were to be used.

[0006] WO 2022 / 261332 discloses a continuous roll-to-roll process for the fabrication of large-volume, dimensionally stable, large-format, high-performance solid-state batteries using a polymer matrix electrolyte (PME) with high lithium-ion conductivity. The batteries can comprise a cathode layer sandwich with a thin, continuous PME layer over the anode and highly conductive PME in both the anode and cathode structures. The batteries can also retain a thin PME layer acting as a solid electrolyte between the cathode and anode, thus maintaining continuity between the layers, resulting in minimal interfacial resistance and enhanced structural integrity.

[0007] The object of the invention is to improve the production of solid-state cells in such a way that high conductivity and thus good fast charging and discharging capability can be achieved between a separator layer and an adjacent layer of solid electrolyte.

[0008] The problem is solved by a method for producing a layered composite that is a precursor for an electrode assembly of a battery cell, according to claim 1, and a method for producing an electrode assembly for a battery cell and a layered composite according to the further independent claims.

[0009] According to the invention, a layered composite is first produced as a precursor in which improved mechanical and electrical contact is established between a separator layer and an adjacent conductive layer made of solid electrolyte or metal. The adjacent layer can be an anode layer, a cathode layer, or a current collector layer. In the resulting layered composite as a precursor, the separator is already embedded in and contacted by the adjacent layers. During the production of the layered composite as a precursor, the manufacturing conditions, in particular pressure and / or temperature, can be selected to achieve good contact and conductivity at the interface between the separator layer and the adjacent layers.Since the precursor has fewer layers than the final electrode assembly of a battery cell, it is simpler and more economical to establish the contacts and conductivity. This is because, for example, less pressure and / or temperature is required than when applying pressure and temperature to the final layered assembly of the battery cell, which contains more layers. The electrode assembly in the battery cell is also referred to as a stack.

[0010] According to another aspect of the invention, the layered composite or the aforementioned precursor can be continuously manufactured on a roll. According to yet another aspect of the invention, the interface where several layered composites are joined to produce an electrode assembly for the battery cell is a current collector layer. It has been shown that contacting a current collector layer is simple and achievable without harsh conditions.

[0011] The battery cell is preferably an accumulator, in particular a solid-state battery cell or solid-state accumulator.

[0012] The invention discloses a method for producing a layered composite that is a precursor for an electrode assembly of a battery cell, wherein the layered composite has at least one structure selected from ASK or KS-Cx, wherein

[0013] A is an anode layer,

[0014] K is a cathode layer,

[0015] S is a separator layer, and

[0016] Cx is a conductive layer for a bipolar battery cell, an anodic current collector layer or a cathodic current collector layer, wherein the separator layer S is incorporated into the structure ASK or KSC. x is embedded on both sides, wherein the layered composite contains a maximum of two such embedded separator layers S, and a maximum of one layer C xcontains, the method having:

[0017] Establishing one or more of the ASK and / or KSC structures x by combining and / or layering the layers A, S, K or K, S, C x simultaneously or in any sequence, wherein i) the manufacturing is carried out under the influence of pressure and / or heat in order to bond at least the layers A and S and / or the layers K and S together under the influence of pressure and / or heat, and / or ii) during the manufacturing process the layer K and / or A is formed on the layer S, or the layer S is formed on the layer K, A and / or C x is formed.

[0018] Preferably the structure is ASK or KSC x in the layered structure, present a maximum of two times.

[0019] The invention further relates to a method for producing an electrode assembly for a battery cell by joining several such layered composites, which may be included in the method but are not necessarily required to be.

[0020] The layered composite according to the invention exists as an isolated product and can be stored as such, for example on a roll or as layers, particularly for later use. The layered composite is specifically not a composite that occurs temporarily in a continuous process, i.e., as an intermediate product. The layered composite according to the invention can exist as a self-contained product and can be stored as such.

[0021] In one embodiment, the invention relates to a method for producing a layered composite that is a precursor for an electrode assembly of a battery cell, wherein the layered composite is selected from: a) ASK-Ck-KSA b) KSA-Ca-ASK c) Cx -ASK c1) C x -SK d) C x -KSA e) KS-Ca-SK where

[0022] A is an anode layer,

[0023] K is a cathode layer,

[0024] S is a separator layer,

[0025] Ck is a cathodic current collecting layer,

[0026] C a an anodic current collector layer is and

[0027] C x a conductive layer for a bipolar battery cell, an anodic current collection layer, or a cathodic current collection layer, such that C x in the special case a layer Ck or C a may be, especially if it is not a conductive layer for a bipolar battery cell, the method having:

[0028] Producing a layered composite a), b), c), c1), d) or e) by joining and / or forming the layers of a composite a), b), c), c1), d) or e) simultaneously or in any sequence, wherein i) the production is carried out under the influence of pressure and / or heat in order to bond at least the layers A and S and / or the layers K and S together under the influence of pressure and / or heat, and / or ii) during the production the layer K and / or A is formed on the layer S, or the layer S on the layer K, A, C a and / or C x is formed.

[0029] In the above-mentioned layer combinations a) - e) (including c1), there are no further layers A, K, S, Ck, C at the beginning, at the end or within the layer combination. a or C x , present. That is, the aforementioned layers A, K, S, Ck, C a or C xThe following layers are definitive for each layer composite type: carrier layers or separating materials that do not include layers A, K, S, Ck, C a or C x These products, or those that can serve as such, may be combined with a layered composite. This also applies to other methods and products of the invention.

[0030] The layered composites a) - e) (including c1) exist as isolated products and can be stored as such, for example on rolls or as layers, particularly for later use. The layered composites a) - e) (including c1) are not, in particular, composites that occur temporarily in a continuous process. The layered composites a) - e) (including c1) can exist as a self-contained product and can be stored as such.

[0031] The aforementioned layers, a layer composite produced according to the invention, an extended layer composite produced according to the invention mentioned below, and an electrode assembly produced according to the invention are such that they are solvent- or liquid-free. The methods mentioned according to the invention are intended for the production of products for solid-state battery cells. The dashes in the above illustrations of the layer composites, and further illustrations of layer composites and electrode assemblies in this description, denote mechanical and / or electrical contact. Specifically, the dashes denote direct contact of layers at an interface.

[0032] In one embodiment of the method, the layer composite is produced in a continuous process. Examples of this are continuous forming processes on a roll.

[0033] In one embodiment of the method, the layered composite is wound onto a roll or assembled into individual stacks, each stack containing exactly one layered composite. Such a wound or assembled layered composite is storable and can be provided as a semi-finished product for further use, in particular for the manufacture of an electrode assembly.

[0034] The terms "anode layer," "cathode layer," "separator layer," "cathodical current collector layer," "anodic current collector layer," and "current-conducting layer for a bipolar battery cell" denote a functional purpose and suitability for the stated objective. In a layered composite that is a precursor, particularly an isolated layered composite that is a precursor, the stated function need not yet be fulfilled.

[0035] The materials listed below for different layers are to be understood as examples and not as limiting.

[0036] The anode layer, the cathode layer and the separator layer are preferably made of a solid, in particular a solid electrolyte.

[0037] Materials for an anode layer are not particularly limited and can be materials known and suitable for lithium or sodium batteries. All solid electrolytes are suitable, especially those with conductivity for lithium or sodium.

[0038] A material for the anode layer, also referred to as anode active material, may, for example, be selected from the group consisting of intercalation material for lithium and / or sodium, conversion material for lithium and / or sodium, alloying material for lithium and / or sodium, metallic lithium, metallic sodium and combinations thereof, wherein the anode active material is particularly preferably selected from the group consisting of metallic lithium, metallic sodium, lithium titanium oxide, lithium titanium phosphate, silicon, prelithiated silicon, silicon-containing zinc phase, graphite, hard carbon and combinations thereof.

[0039] Materials for a cathode layer are not particularly limited and are well-known and suitable for lithium or sodium batteries. For example, all solid electrolytes are suitable, especially those with conductivity for lithium or sodium.

[0040] A material for the cathode layer, also referred to as cathode active material, may, for example, be selected from the group consisting of intercalation material for lithium and / or sodium, conversion material for lithium and / or sodium, alloying material for lithium and / or sodium, and combinations thereof, wherein the cathode active material is particularly preferably selected from the group consisting of layered oxide, spinel, olivine, cation-disordered rock salt, conversion material, and combinations thereof, wherein the cathode active material is particularly preferably selected from the group consisting of NCM, LMO, LNMO, LFP, DRX, sulfur, lithium vanadium phosphate, Prussian blue, Prussian white, sodium vanadium phosphate, and combinations thereof.

[0041] Materials for a separator layer can be selected without restriction and for all aspects of the invention from any of the following:

[0042] - Lithium-conducting polymer and / or a sodium-conducting polymer, wherein the polymer is selected, for example, from the group consisting of poly[bis(2-[2-methoxyethoxy)ethoxy) phosphazene), polyethylene oxide, nether, succinonitrile, polyacrylonitrile, and combinations thereof;

[0043] - Lithium-conducting oxide and / or a sodium-conducting oxide, wherein the oxide is selected, for example, from the group consisting of Li7La3Zr20i2, Lie^LasZr^Tao.eO^, LLZO, LLTO and combinations thereof;

[0044] - Lithium-conducting phosphate and / or a sodium-conducting phosphate, wherein the phosphate is selected, for example, from the group consisting of Lii,3Alo,3Tii,7(P04)3, LATP, NaSICON compound and combinations thereof;

[0045] - a lithium-conducting sulfide and / or a sodium-conducting sulfide, wherein the sulfide is selected, for example, from the group consisting of U2-P2S5, Li9,54Sii,74Pi,44Sn,7Clo,3, LiePSsCl, LiePSsBr, LiySiPSs, Li GeP2Si2, Li SnP2Si2 and combinations thereof;

[0046] - Lithium-conducting halide and / or a sodium-conducting halide, preferably selected from the group consisting of LisInCl, LisYCk and combinations thereof. Materials for a cathodic current-collecting layer may, without limitation and for all aspects of the invention, be selected from aluminum or aluminum-coated polymer film.

[0047] Materials for an anodic current collecting layer can be selected without restriction and for all aspects of the invention from copper, nickel, or metal-coated polymer film.

[0048] Materials for a conductive layer for a bipolar battery cell can be selected without restriction and for all aspects of the invention from bimetallic foil (e.g. copper / aluminium), nickel, or stainless steel.

[0049] The application of pressure preferably means a line pressure in the range of 100 N / mm to 1000 N / mm.

[0050] The application of pressure is preferably carried out using the following device: press or calender.

[0051] The application of heat preferably means heating to a temperature in the range of 50°C to 700°C, preferably 50°C to 300°C.

[0052] In the invention, the separator layer preferably consists of at least 95 wt.%, at least 98 wt.%, at least 99 wt.%, at least 99.5 wt.%, or most preferably at least 99.8 wt.% or at least 99.9 wt.% of an inorganic solid electrolyte. The remainder can be a binder. In another preferred embodiment, the separator layer consists of 100 wt.% of an inorganic solid electrolyte. The solid electrolyte can be an oxide or sulfide solid electrolyte, preferably an oxide solid electrolyte.

[0053] Methods for joining or forming layers are not specifically restricted.

[0054] When joining layers, the layers to be joined are already formed beforehand, meaning they exist as finished layers. Examples of methods for joining previously formed layers include pressing processes, for example with sheets (sheet pressing), or roll-to-roll processes using a calender. Generally, lamination processes can be used, in which one layer is laminated to another, e.g., from a roll. The formation of one layer on top of another can be achieved by application or deposition.

[0055] Application refers in particular to a liquid process or a dry process. A liquid process is preferably a casting process, for example, film casting. A dry process is preferably film formation with particles and fibrillating binders under shear forces. After film formation, a sintering step, for example, may be added.

[0056] Deposition is understood in particular to be a process in which the layer to be formed is created from a gas phase or from an aerosol, preferably by spray deposition, aerosol deposition, in particular powder aerosol deposition, physical vapor deposition (PVD), chemical vapor deposition.

[0057] In one embodiment, the method for producing a layer composite comprises: applying to layer composite a) b) or e) a further current-collecting layer to form an extended layer composite a1), b1) or e1), which is selected from a1). In the case of layer composite a)

[0058] ASK-Ck-KSA-Ca where C a the further current collection layer is b1) In the case of the combination b) KSA-Ca-ASKC k where Ck is the further current collection layer e1) In the case of the compound e) KS-Ca-SK-Ck where Ck is the further current collection layer

[0059] The advantage of the extended layer assemblies is that electrode assemblies can be fabricated directly from them without the need for additional current-collecting layers. This means that simply joining several extended layer assemblies is sufficient. In the aforementioned extended layer assemblies a1), b1), and e1), there are no additional layers A, K, S, Ck, C at the beginning, end, or within the layer assembly. a or C x , present. That is, the aforementioned layers A, K, S, Ck, C a or C x The following layers are definitive for each extended layer composite type: carrier layers or separating materials that do not include layers A, K, S, Ck, C a or C x These products, or those that can serve as such, may be combined with a layered composite. This also applies to other methods and products of the invention.

[0060] The extended layer composites a1), b1) and e1) exist as isolated products and are storable as such, for example on reels or as layers, particularly for later use. The extended layer composites a1), b1) and e1) are specifically not composites that occur temporarily in a continuous process, i.e., they are not intermediate products of a process.

[0061] In a further aspect, the invention relates to a method for manufacturing an electrode assembly for a battery cell, comprising the joining of a plurality of layered composites a) ASK-Ck-KSA b) KSAC a -ASK c) C x -ASK c1) C x -SK d) C x -KSA, and / or e) KSC a -SK where A, K, S, Ck, C a , and C x as defined above, and if required, further current collection layers to an electrode assembly selected from

[0062] In the case of a large number of layered structures a)

[0063] (especially for a monopole battery cell):

[0064] (-ASK-Ck-KSAC a ) n where C a the further current collection layers are, In the case of a multitude of layered assemblies b) (especially for a monopole battery cell): (-KSAC a -ASKC k )n where Ck are the further current collection layers,

[0065] In the case of a large number of layered structures c)

[0066] (especially for a bipolar battery cell):

[0067] (-Cx-ASK) n

[0068] In the case of a large number of layer clusters c1)

[0069] (especially for a bipolar battery cell):

[0070] (-Cx-SK) n

[0071] In the case of a large number of layer groups d)

[0072] (especially for a bipolar battery cell):

[0073] (-Cx-KSA)n

[0074] In the case of a combination of c) and d) (especially for a monopole battery cell) [(-Cx-ASK)(-Cx-KSA)] n

[0075] In the case of a multitude of layered arrangements e) (especially for a monopole battery cell):

[0076] (-KS-Ca-SK-Ck)n where C x C a and Ck are the further current collection layers, where n is in each case an integer greater than or equal to 2, preferably greater than or equal to 3, and even more preferably greater than or equal to 4, 5, or 6. The upper limit of n is, in principle, unlimited. A suitable upper limit of n that can be combined with all the aforementioned lower limits is 1000, 500, 300, 200, 250, or 125.

[0077] The expressions in parentheses represent repetition units, and the number n is the number of repetitions.

[0078] It is evident that the electrode assemblies formed from layered composites a) and b) have an identical sequence of layers despite the different definition of the repeating unit. Only the precursor, layered composite a) or b), differs, as do the current-collecting layers C added during assembly. a or Ck.

[0079] The assembly can be done step by step. For example, two layered composites can first be joined together, inserting a current collector layer in between if necessary. Then another layered composite can be added, again inserting a current collector layer if necessary, and so on.

[0080] The joining process can be carried out in a press, preferably an isostatic press.

[0081] Preferably, a multitude of layered composites are joined without pressure and / or heat. Alternatively, joining can be carried out under pressure and / or heat, preferably using low pressures and / or temperatures. Suitable pressures are in the range of 0.01 to 600 MPa, preferably 0.01 to 300 MPa, and even more preferably 0.01 to 50 MPa. Suitable temperatures are in the range of 20°C to 300°C, 20°C to 200°C, or 20°C to 100°C.

[0082] When one or more additional current collector layers are inserted, a distinction can be made between an anode or cathode and the additional current collector layer Ck or C. aA primer layer is inserted to improve contact. A primer layer preferably contains or consists of an electrically conductive material and a binder, wherein the electrically conductive material is particularly preferably selected from the group consisting of amorphous carbon, graphitic carbon and combinations thereof, and / or the binder is particularly preferably selected from the group consisting of CMC, PDVF, and combinations thereof.

[0083] In one embodiment of the method for manufacturing an electrode assembly, the layered composites a)-e) (including c1) are manufactured according to a method according to the invention for manufacturing a layered composite; reference is made to the structures and conditions mentioned above, such as pressure and temperature. However, the layered composites a)-e) (including c1) need not be manufactured according to a method according to the invention. In yet another aspect, the invention relates to a method for manufacturing an electrode assembly for a battery cell, comprising the joining of a plurality of layered composites a1), b1) or e1) a1) ASK-Ck-KSA-Ca b1) KSA-Ca-ASKC k e1) KS-Ca-SKC k where A, K, S, C k , and C a , as defined above, to an electrode assembly that is selected from

[0084] In the case of a multitude of layer combinations a1): (-ASK-Ck-KSA-Ca)n

[0085] In the case of a multitude of layer combinations b1): (-KSA-Ca-ASK-Ck)n

[0086] In the case of a large number of layer groups e1):

[0087] (-KS-Ca-SK-Ck)n where n is an integer greater than or equal to 2, preferably greater than or equal to 3, and even more preferably greater than or equal to 4, 5, or 6. The upper limit of n is, in principle, unlimited. A suitable upper limit of n that can be combined with all the aforementioned lower limits is 1000, 500, 300, 200, 250, or 125.

[0088] The layered arrays a1), b1), e1) used in this process were previously also referred to as extended layered arrays. With the extended layered arrays, the insertion of further current collector layers is not necessary because all current collector layers are already present in the extended layered arrays.

[0089] It is evident that the electrode assemblies formed from the layered composites a1) and b1) have an identical sequence of layers despite the different definition of the repeating unit. Only the precursor, layered composite a1) or b1), differs. Preferably, a plurality of extended layered composites are joined without pressure and / or heat. Alternatively, the joining can be carried out under pressure and / or heat, with suitable pressures and temperatures already mentioned above, when joining a plurality of (non-extended) layered composites.

[0090] In one embodiment of the method for manufacturing an electrode assembly, the extended layer composites a1), b1) and e1) are manufactured according to a method for manufacturing an extended layer composite as described above. Reference is made to the conditions mentioned above, such as pressure and temperature. However, the extended layer composites a1), b1) and e1) need not be manufactured according to a method according to the invention.

[0091] In a further aspect, the invention relates to a layered composite for use as a precursor for an electrode assembly for a battery cell, wherein the layered composite is selected from a) ASK-Ck-KSA a1) ASK-Ck-KSA-Ca b) KSA-Ca-ASK b1) KSA-Ca-ASK-Ck c) Cx-ASK c1) Cx-SK d) Cx-KSA, e) KS-Ca-SK, and / or e1) KS-Ca-SK-Ck wherein

[0092] A is an anode layer,

[0093] K is a cathode layer,

[0094] S is a separator layer,

[0095] Ck is a cathodic current collecting layer,

[0096] C a an anodic current collector layer is and

[0097] Cx is a conductive layer for a bipolar battery cell, an anodic current collector layer or a cathodic current collector layer, wherein the layer assembly does not include any further layers A, K, S, Ck, C a or C x exhibits. The layered structures a1), b1) and e1) can also be referred to as extended layered structures, as above.

[0098] Methods according to the invention for producing the layered composite are disclosed above. However, these methods do not necessarily have to be used to produce a layered composite. Features mentioned in the methods can apply analogously and in any combination to the intermediate product.

[0099] Preferably, the layered composite is wound onto a roll or assembled in a single stack.

[0100] The invention also discloses a battery cell comprising an electrode assembly as disclosed above, preferably manufactured specifically using a method according to the invention.

[0101] The invention is described below with reference to exemplary embodiments. The figures shown are:

[0102] Fig. 1 shows an electrode assembly as it is obtainable according to a method according to the invention;

[0103] Fig. 2a, b layer composites not according to the invention and methods for producing a

[0104] Electrode assembly according to Fig. 1 thereof;

[0105] Fig. 3a, b shows a layer composite according to the invention and an extended layer composite according to the invention, as well as a method for producing a

[0106] Electrode assembly according to Fig. 1 thereof;

[0107] Fig. 4 shows the production of a layer composite according to the invention;

[0108] Fig. 5a, b shows a further layer composite according to the invention and its operating principle as a zero-excess anode;

[0109] Fig. 6a, b shows a further extended layer composite according to the invention and its operating principle as a zero-excess anode;

[0110] Fig. 7a, b Method for producing an electrode assembly from the further layer composite according to the invention or the further extended layer composite according to the invention of Fig. 4a, b and 5a, b; Fig. 8 a further layer composite according to the invention for producing a bipolar cell and the method for producing an electrode assembly.

[0111] Fig. 1 shows the general case of an electrode assembly as a stack with a periodic sequence after stack formation, from top to bottom:

[0112] C a -ASKC k -KSAC a -ASKC k -KSA-Ca where

[0113] K is a cathode layer,

[0114] S is a separator layer,

[0115] C k a cathodic current collecting layer,

[0116] C a an anodic current collector layer is and

[0117] The repetition unit, viewed from below, is a unit C. a -ASKC k -KSA. However, the boundaries of the repetition unit can also be set differently. The repetition can be continued as often as desired, which, as in other figures, is indicated by dots above and below.

[0118] Arrow P1 shows the ion flow between cathode K and anode A through the separator S, the direction depending on whether the battery cell containing the electrode assembly is being discharged or charged.

[0119] Arrow P2 shows the electron flow between anode A and anodic current collector layer C a, the direction of which depends on whether the battery cell containing the electrode assembly is being discharged or charged.

[0120] Arrow P3 shows the electron flow between cathode K or cathode and cathodic current collector layer C k , the direction of which depends on whether the battery cell containing the electrode assembly is being discharged or charged.

[0121] Figures 2a and 2b do not show a method according to the invention for producing the electrode assembly according to Figure 1. The electrode assembly shown is not exactly that of Figure 1, but the layer sequence is identical. In the formation principle of Figure 2a, layer composites K-Ck-K and AC are used. a -A is used as a precursor and joined together with additional, individually present separator layers S. The joining points are designated F.

[0122] In the formation principle of Fig. 2b, layer combinations SK-Ck-KS and AC are used. a-A are used as precursors and joined together. The joining points are also designated F. Since the separator layers S are already contained in a layered composite, there are fewer joining points than with the formation principle of Fig. 2a. Alternatively, layered composites K-Ck-K and SAC could be used. a -AS can be used.

[0123] The formation principles of Fig. 2a and Fig. 2b have in common that joining occurs at the separator layers S. This results in more difficult contacting, and usually the entire electrode assembly is pressed together at the end, after formation of the complete stack. Harsh conditions, high pressures and high temperatures are required to achieve good contacting and ion conductivity.

[0124] Fig. 3a shows a method according to the invention for producing an electrode assembly from a layered composite KSAC. a-ASK, which is shown in its entirety in the center of Fig. 3a. Above and below it are further layered composites KSA-C. a -ASK is used, which are shown incompletely, with only KS at the top and bottom, so that the AC part is shown in each case. a -ASK is missing, indicated by dots. The layer assemblies KSAC are formed at the joints F. a -ASK with additional current-collecting layers Ck joined together. In a modification of Fig. 3a, it would be possible to assemble an electrode assembly from layered composites ASK-Ck-KSA with additional current-collecting layers C. a to put together.

[0125] Unlike in Figs. 2a and 2b, the joining points for manufacturing the electrode assembly are not on one of the separator layers S but on current collecting layers Ck.

[0126] An improved ion-conducting contact can already be incorporated in the precursor, the layer composite KSAC. a-ASK, between S and A and between S and K, are produced analogously in a pre-product / layer composite ASK-Ck-KSA, as will be explained below with reference to Fig. 4. The joining of the layer composites KSAC a -ASK with the additional current collection layers Ck can be performed under mild conditions, e.g. low pressure, because contacting the additional current collection layers Ck, which are usually made of metal, is easy.

[0127] Fig. 3b shows a modification of the principle of Fig. 3a. Here, the KSAC a -ASK already before final assembly to the electrode assembly with each an additional current collection layer Ck to form an extended layer composite KSAC a -ASK-Ck have been connected, so that the electrode assembly consists solely of the extended layer composite KSAC. a -ASK-Ck can be formed.

[0128] Fig. 4 shows the production of a layered composite KSAC. a -ASK, which is a precursor for the electrode assembly of a battery cell, and from which the electrode assembly can be produced according to Fig. 3a. The individual layers are joined together under pressure p and / or heat (temperature ?). In this specific example, an existing layer C is used. a The starting point is a layer A, which is deposited, applied, or laminated to both sides of the substrate. A layer S is deposited, applied, or optionally laminated to each of the two layers A. A layer K is deposited or applied to each of the two layers S. The joining points are marked F. Primer layers (not shown here) can be applied between the layers. The joining of layers K, S, A, and C aAlternatively, the joining of the layers can occur simultaneously or stepwise in any desired sequence. Pressure and / or heat can, generally according to the invention and specifically also with other layered composites, be applied intermittently if the layers are joined stepwise.

[0129] The layers can be joined together, for example, using a roll-to-roll process.

[0130] Pressure and / or heat application preferably, but at least, occurs after all layers have been joined to form the KSAC layer composite. a -ASK. This approach allows lower pressures or temperatures to be used to establish good mechanical and electrical contact between the separator layer S and the anode layer A or cathode layer K than when applying pressure and / or temperature to the entire electrode assembly of Fig. 1, which consists of significantly more layers. Fig. 5a shows a layered composite KSC.a -SK. This is a so-called "zero-excess anode" or also referred to as an "anode-free design", in which the separator layer S is directly on the current collector layer C. a The anode layer A is applied during charging, as shown by arrow L, as depicted in Fig. 5b. During discharging, as shown by arrow E, this anode layer A is removed. The anode layer A is preferably formed from the active metal lithium or sodium.

[0131] The production of the layered composite KSC a -SK can be done in a specific example as follows:

[0132] Formation of a separator layer S as a solid separator layer on the anodic current collector layer C aDouble-sided. The separator layer S is, for example, an ion-conducting oxide layer (solid electrolyte separator). It is formed by deposition, e.g., by aerosol deposition including post-annealing or sintering, or alternatively by film-forming sintering, casting, or in a dry process.

[0133] Then a cathode layer K (at least one active material, at least one solid electrolyte (catholyte)) is produced on a transfer film or freestanding and laminated roll-to-roll onto the separator layer S (under pressure and possibly also heat).

[0134] Alternatively and preferably, the C network is used. a -S a cathode layer K directly coated, preferably as a dry process without the use of solvents.

[0135] Fig. 6a shows an extended layer composite KSC a -SK-Ck, which relies on the KSC shift system a-SK of Fig. 5a a cathodic current collecting layer Ck is applied

[0136] To produce the extended layer composite, the cathode layer K can be produced on the cathodic current collector layer Ck, and the separator layer S can then be deposited on top, e.g., using powder aerosol deposition. Selective heat treatment is optional.

[0137] Alternatively, to produce the extended layer composite shown in Fig. 6a, a layer composite KSC can be used. a Under pressure and heat, the current collection layer Ck is rolled onto one side of the SK. Fig. 6b shows, analogously to Fig. 5b, the structure after the charging process with the anode formed.

[0138] Layered composites produced according to the invention, such as those shown in Figures 3a, 3b, 5a, and 6a, can be prefabricated so that layers are available for stacking, or they can be wound directly (e.g., for use in cylindrical cells). Missing current collector layers can be added as an additional component in a stacking process. Depending on the choice of roll manufacturing method (single-sided vs. double-sided coating on the current collector) and the type of stacking, it is possible to construct monopolar or bipolar cells. Liquid (or liquid electrolyte) can be sprayed on after lamination, if desired and necessary.

[0139] Fig. 7a shows the fabrication of an electrode assembly from layered composites KSC a -S- K (according to Fig. 5a), where only one of the layer composites in the center of Fig. 7a is fully shown. Joining points are designated F.

[0140] Fig. 7b shows the fabrication of an extended electrode assembly made of layered composites KSC a -SK-Ck (according to Fig. 6a), where only one of the layer composites in the center of Fig. 7b is fully shown. Joining points are designated F.

[0141] Fig. 8 shows layered composites C x -ASK and the assembly into an electrode assembly for a bipolar cell at the connection points F, which is constructed as an internal series circuit. All shown internal layers Cx are current-conducting layers of the bipolar battery cell. Bottom or top terminating layers Cx are anodic or cathodic current-collecting layers Ck or C. a For example, layer C shown at the very bottom. x not located inside but at the end, it would be a current collector layer C. a , since it is adjacent to an anode.

[0142] Reference symbol list

[0143] A anode layer

[0144] K Cathode layer

[0145] S separator layer

[0146] Ck cathodic current collecting layer

[0147] C a anodic current collector layer

[0148] Cx conductive layer for a bipolar battery cell, anodic current collection layer or cathodic current collection layer

[0149] P1 ion flow between cathode K and anode A through the separator S

[0150] P2 Electron flow between anode A and anodic current collector layer C a

[0151] P3 Electron flow between cathode K or cathode and cathodic

[0152] Current collection layer Ck

[0153] F joint

[0154] L store

[0155] E Unloading p Pressure

[0156] T Temperature / Heat

Claims

- 22 - Patent claims 1. Method for producing a layered composite that is a precursor for an electrode assembly of a battery cell, wherein the layered composite has at least one structure selected from ASK or KS-Cx, wherein A is an anode layer, K is a cathode layer, S is a separator layer, and Cx is a conductive layer for a bipolar battery cell, an anodic current collector layer or a cathodic current collector layer, wherein the separator layer S is incorporated into the structure ASK or KSC. x is embedded on both sides, wherein the layered composite contains a maximum of two such embedded separator layers S, and a maximum of one layer C x contains, the method having: Establishing one or more of the ASK and / or KSC structures x by combining and / or layering the layers A, S, K or K, S, Cx simultaneously or in any sequence, wherein i) the manufacturing is carried out under the influence of pressure and / or heat in order to bond at least the layers A and S and / or the layers K and S together under the influence of pressure and / or heat, and / or ii) during the manufacturing process the layer K and / or A is formed on the layer S, or the layer S is formed on the layer K, A, and / or C x is formed.

2. A method for producing a layer composite according to claim 1, wherein the layer composite is selected from: a) ASK-Ck-KSA b) KSA-Ca-ASK c) Cx-ASK c1) Cx-SK d) Cx-KSA, and / or e) KS-Ca-SK wherein Ck is a cathodic current collector layer, as a special case of a layer C x , C a an anodic current collector layer is, as a special case of layer C x , and the layered composite has no further layers A, S, K, Ck, C a or C xexhibits, and wherein the method exhibits: Forming a layered composite a), b), c), c1), d) or e) by joining and / or forming the layers of a composite a), b), c), c1), d) or e) simultaneously or in any order.

3. Method according to claim 2, comprising Applying to the layer composite a) b) or e) a further current collection layer to obtain an extended layer composite a1), b1) or e1), which is selected from a1). In the case of layer composite a) ASK-Ck-KSA-Ca where C a the further current collection layer is b1) In the case of the combination b) KSA-Ca-ASK-Ck where Ck is the further current collection layer e1) In the case of the compound e) KS-Ca-SK-Ck where Ck is the further current collection layer.

4. Method according to one of claims 2 or 3, wherein the layer composite obtained as product does not contain any further layers A, K, S, Ck, C a or Cx exhibits.

5. Method according to any of the preceding claims, wherein the production of the layer composite takes place in a continuous process.

6. Method according to any of the preceding claims, wherein the layer composite is wound onto a roll or is assembled into individual stacks, each stack containing exactly one layer composite.

7. A method for manufacturing an electrode assembly for a battery cell comprising the joining of a plurality of layer assemblies, each of the layer assemblies having at least one separator layer embedded on both sides, wherein the separator layer is formed into a structure ASK or KSC. x is embedded, where A is an anode layer, K is a cathode layer, S is a separator layer, and C xa conductive layer for a bipolar battery cell, an anodic current collection layer or a cathodic current collection layer, wherein the layer assembly contains a maximum of two such embedded separator layers S, and a maximum of one layer C x contains.

8. Method for manufacturing an electrode assembly for a battery cell, comprising joining a plurality of layered assemblies a) ASKC k -KSA b) KSA-Ca-ASK c) C x -ASK c1) C x -SK d) C x -KSA, and / or e) KS-Ca-SK where A is an anode layer, K is a cathode layer, - 25 - S is a separator layer, Ck is a cathodic current collecting layer, C a an anodic current collector layer is and Cx is a conductive layer for a bipolar battery cell, an anodic current collector layer, or a cathodic current collector layer, and, if required, further current collector layers to an electrode assembly selected from In the case of a large number of layer groups a): (-ASK-Ck-KSA-Ca)n where C a the other current collection layers are, In the case of a large number of layer groups b): (-KSA-Ca-ASK-Ck)n where Ck are the further current collector layers, In the case of a large number of layered networks c): (-Cx-ASK) n In the case of a large number of layer clusters c1): (-Cx-SK) n In the case of a large number of layer groups d): (-Cx-KSA)n In the case of a combination of layered structures c) and d) [(-Cx-ASK)(-Cx-KSA)] n In the case of a large number of layer groups e): (-KS-Ca-SK-Ck)n where Ck are the further current collection layers, where n is an integer greater than or equal to 2 in each case. - 26 - 9. Method for manufacturing an electrode assembly for a battery cell, comprising joining a plurality of layered assemblies a1), b1) or e1) a1) ASK-Ck-KSA-Ca b1) KSA-Ca-ASKC k e1) KS-Ca-SKC k where A is an anode layer, K is a cathode layer, S is a separator layer, C k a cathodic current collecting layer, Approximately one anodic current collector layer is selected for an electrode assembly made of In the case of a large number of layer groups a1): (-ASK-Ck-KSA-Ca)n In the case of a large number of layer groups b1): (-KSA-Ca-ASK-Ck)n In the case of a large number of layer groups e1): (-KS-Ca-SK-Ck)n where n is an integer greater than or equal to 2.

10. Layer composite, for use as a precursor for an electrode assembly for a battery cell, wherein the layer composite is selected from a) ASKC k -KSA a1) ASK-Ck-KSA-Ca b) KSA-Ca-ASK b1) KSA-Ca-ASK-Ck c) Cx-ASK c1) Cx-SK - 27 - d) Cx-KSA, e) KS-Ca-SK, and / or e1) KS-Ca-SK-Ck where A is an anode layer, K is a cathode layer, S is a separator layer, Ck is a cathodic current collecting layer, C a an anodic current collector layer is and Cx is a conductive layer for a bipolar battery cell, an anodic current collector layer or a cathodic current collector layer, wherein the layer assembly does not include any further layers A, K, S, Ck, C a or C x exhibits.

11. Layer composite according to claim 10, wherein the layer composite is wound onto a roll or is assembled in a single stack.

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