Method for producing an electrode layer with a separator layer, an electrode layer with a separator layer, an electrode layer-separator layer-counter electrode layer stack, as well as an electrochemical cell, an electrostatic cell or a combination thereof, and use thereof

Abstract

A method for producing an electrode layer with a separator layer, an electrode layer with a separator layer, and an electrode layer-separator layer-counter electrode layer stack is provided. Furthermore, an electrochemical cell, an electrostatic cell, or a combination thereof is provided, and its use is proposed. These products can be produced in a simple, fast, and cost-effective manner. The ionic conductivity between the electrode layer and the separator layer, and where applicable, also to the counter electrode layer, is excellent. The provided products can be manufactured easily and quickly and are characterized by high electrical performance, high cycle stability, low safety risk, and low risk of irreparable damage.

Description

[0001] A method for producing an electrode layer with a separator layer, an electrode layer with a separator layer, and an electrode layer-separator layer-counterelectrode layer stack are provided. Furthermore, an electrochemical cell, an electrostatic cell, or a combination thereof is provided, and the use thereof is proposed. These products can be produced in a simple, rapid, and cost-effective manner. The ionic conductivity between the electrode layer and the separator layer, and if applicable, also to the counterelectrode layer, is excellent. The provided products can be produced simply and quickly and are characterized by high electrical performance, high cycle stability, low safety risk, and a low risk of irreparable damage.

[0002] In the manufacture of galvanic and electrostatic energy storage cells, filling them with a liquid electrolyte represents a complex, technically demanding process step (Kwade, A. et al., Nature Energy, Vol. 3, pp. 290-300). The presence of a liquid electrolyte, which is flammable and has a low boiling point, also poses a safety risk, as the liquid electrolyte can easily evaporate and form an explosive mixture. A further safety risk can arise from electrically conductive contact between the anode and cathode in such batteries (e.g., due to mechanical stress on the batteries), which could cause a short circuit, leading to battery overheating and the risk of burns. Furthermore, such a situation could cause irreparable damage to the battery.

[0003] To circumvent this problem, it has been proposed, on the one hand, to use batteries without a liquid electrolyte (i.e., solid-state batteries) (Ates, T. et al., Energy Storage Materials, Vol. 17, pp. 204-210). On the other hand, it has been proposed to equip batteries with a gel electrolyte instead of a liquid electrolyte (Liang, Y.F. et al., Electrochimica Acta, Vol. 296, pp. 1064-1069). However, these batteries have the disadvantage of being complex and time-consuming to manufacture, and their cycle life and electrical performance require improvement.

[0004] Based on this, the object of the present invention was to provide a method by which an electrode layer can be equipped with a separator layer in a simple and rapid manner, wherein excellent ionic conductivity exists between the electrode layer and the separator layer, and the provided electrode layer with the separator layer has high cycle stability, a low safety risk, and a low risk of irreparable damage. Furthermore, an electrode layer with a separator layer and also an electrode layer-separator layer-counter electrode layer stack should be provided, which has said advantages. Furthermore, an electrochemical cell, electrostatic cell, or combination thereof should be provided, which has the aforementioned advantages. Furthermore, a use of the electrochemical cell and / or electrostatic cell should be proposed.

[0005] The object is achieved by the method according to claim 1, the method according to claim 9, the electrode layer with separator layer according to claim 12, the electrode layer-separator layer-counter electrode layer stack according to claim 13, the electrochemical cell, electrostatic cell or combination thereof according to claim 14 and the use according to claim 15. The dependent claims show advantageous developments.

[0006] According to the invention, a method for producing an electrode layer with a separator layer is provided, comprising or consisting of the steps: a) providing a planar electrode layer, wherein the planar electrode layer has a planar top side and a planar bottom side; and b) forming a separator layer on the flat upper side of the electrode layer by applying a liquid containing a liquid electrolyte and a polymer, i) onto the top side of the flat electrode layer and allowing it to react, whereby a gel is formed from the liquid electrolyte and the polymer and the gel forms a separator layer; or ii) at least on one side of a porous membrane, wherein the pores of the porous membrane are filled with the liquid and allowed to react, wherein a gel is formed from the liquid electrolyte and the polymer and the porous membrane and the gel together form a separator layer, wherein the separator layer is subsequently applied to the upper side of the flat electrode layer; characterized in that the polymer i) is a liquid, cross-linking polymer and is cross-linked by reacting in step b); or ii) a non-crosslinking polymer is present in the liquid together with an organic solvent having a boiling point of <70°C at atmospheric pressure in order to dissolve the non-crosslinking polymer in the liquid before step b), wherein during the reaction in step b) said organic solvent evaporates.

[0007] The method according to the invention makes it possible to provide an electrode layer equipped with a separator layer in a simple, rapid and cost-effective manner, wherein the ionic conductivity between the electrode layer and the separator layer is excellent and the electrode layer with separator layer is characterized by high cycle stability, a low safety risk and a low risk of irreparable damage.

[0008] The simplicity and speed result from the process steps of the method according to the invention, which can be carried out quickly and easily. The production of an electrochemical cell and / or electrostatic cell is also easier with the electrode layer according to the invention with a separator layer, since this already contains the separator on the one hand and the liquid electrolyte (bound in the gel) on the other. In addition, assembly with other components is easier (e.g. during a coating process) because the liquid electrolyte is in the form of a gel and not a liquid and is therefore already physically bonded to the electrode layer. In short, the liquid electrolyte is easier to process due to its physically bonded form (gel form). Furthermore, the electrolyte filling otherwise required during cell assembly can be omitted because the electrolyte (in gel form) is already a component of the electrode layer.When manufacturing an electrochemical cell and / or electrostatic cell, this results in in-situ electrolyte filling of the electrodes during compression of the cell stack.

[0009] Low costs can be achieved because the method according to the invention allows an optimal adjustment of the amount of electrolyte when providing the electrode layer with separator layer, ie the amount of electrolyte can be saved.

[0010] The excellent ionic conductivity between the electrode layer and the separator layer is achieved by wetting the electrode layer (or, alternatively, the porous membrane) with the liquid electrolyte contained in the gel of the separator layer. The gel acts like an open reservoir that absorbs and releases the liquid electrolyte (similar to a liquid-soaked sponge). The gel of the separator layer is mechanically flexible and, through a "sponge effect," ensures excellent contact between the electrode layer and the liquid electrolyte in the separator layer.

[0011] The high cycle stability compared to solid-state batteries is achieved on the one hand by improved ion-conducting contact at the interface between the electrode layer and the separator layer (alternatively also the porous membrane) (sponge function of the gel) and on the other hand by improved mechanical properties (support function of the gel).

[0012] The low safety risk is achieved by the liquid electrolyte being in gel form, i.e. the separator layer is gelled. On the one hand, this means that the gel provides mechanical support, which reduces or completely prevents the risk of possible contact between the anode and cathode in an assembled battery (e.g. due to mechanical stress). On the other hand, the gel significantly reduces the risk of leakage and / or evaporation of the liquid electrolyte, thereby reducing the risk of damage and also of possible explosion. Safety can be further increased by using a high-boiling liquid electrolyte to form the gel. A further advantage of the process is that liquid electrolytes can be used which are otherwise often unsuitable for conventional electrolyte dosing due to their rheological properties.

[0013] In the process according to the invention, the liquid, crosslinking polymer may contain or consist of a plastic selected from the group consisting of one-component addition polymer, two-component addition polymer and combinations thereof, wherein the plastic is in particular silicone rubber.

[0014] Furthermore, the liquid crosslinking polymer may be present in the liquid in a concentration of 10 to 90 vol.%, preferably 40 to 60 vol.%, based on the total volume of the liquid.

[0015] In the process, the non-crosslinking polymer may contain or consist of a fluorinated plastic, wherein the fluorinated plastic in particular contains or consists of PVDF-HFP.

[0016] Furthermore, the non-crosslinking polymer may be present in the liquid in a concentration of 3 to 30 wt%, preferably 4 to 6 wt%, based on the total weight of the organic solvent.

[0017] Apart from that, the non-crosslinking polymer may be present together with the organic solvent in a concentration of 10 to 90 vol%, preferably 40 to 60 vol%, with respect to the total volume of the liquid.

[0018] In the method, the liquid may be applied by a method selected from the group consisting of doctor blades, pipetting, and combinations thereof.

[0019] Furthermore, the liquid can be applied at a height in the range of up to 300 µm, preferably in the range of up to 50 µm, wherein the height refers to an extension of the liquid in a direction perpendicular to the top and / or bottom of the planar electrode layer.

[0020] The liquid electrolyte may contain or consist of an organic solvent having a boiling point of ≥ 80°C, preferably > 200°C, at atmospheric pressure, and a conducting salt.

[0021] The organic solvent can be selected from the group consisting of PC, FEC, EC, DMC, EMC, DEC, VEC, VC, TBAC (acetyltributylcitrate), GTB (glycerol tributyrate), GTA (glycerol triacetate), γ-buthyrolactone and combinations thereof, wherein the organic solvent is preferably selected from the group consisting of PC, FEC, EC and combinations thereof.

[0022] The conducting salt in the organic solvent can be a lithium conducting salt or a sodium conducting salt. The lithium conducting salt is preferably selected from the group consisting of LiPF6, LiClO4, LiNO3, and C6H 18LiNSi2, F2LiNO4S2, C2F6LiNO4S2, LiB[C2O4]2, LiBF4, and combinations thereof. The sodium conducting salt is preferably selected from the group consisting of NaPF6, NaBF4, NaTF, NaTFSI, NaClO4, and combinations thereof. The conducting salt is optionally present in a concentration of 0.5 M to 2 M, preferably 1 M, in the liquid containing a liquid electrolyte and a polymer.

[0023] Furthermore, the liquid electrolyte may contain or consist of an ionic liquid.

[0024] The ionic liquid can be selected from the group consisting of pyrrolidinium-based ionic liquids, imidazolium-based ionic liquids, triliquid acid derivative-based ionic liquids, and combinations thereof. Preferably, the ionic liquid is selected from the group consisting of 1-methyl-1-propylpyrrolidinium bis(trifluoromethylsulfonyl)imide, 1-methyl-1-propylpyrrolidinium bis(fluorosulfonyl)imide, 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide, 1-ethyl-3-methylimidazolium bis(fluorosulfonyl)imide, and combinations thereof.

[0025] The conducting salt in the ionic liquid can be a lithium conducting salt or a sodium conducting salt. The lithium conducting salt is preferably selected from the group consisting of LiPF6, LiClO4, LiNO3, and C6H 18LiNSi2, F2LiNO4S2, C2F6LiNO4S2, LiB[C2O4]2, LiBF4, and combinations thereof. The sodium conducting salt is preferably selected from the group consisting of NaPF6, NaBF4, NaTF, NaTFSI, NaClO4, and combinations thereof. The conducting salt is optionally present in a concentration of 0.5 M to 2 M, preferably 1 M, in the liquid containing a liquid electrolyte and a polymer.

[0026] In the process, the reaction can be carried out at a temperature in the range of 20 to 150°C, preferably at a temperature in the range of 30 to 60°C. The reaction can comprise heating the liquid. This temperature can refer to step b), subsection i) of the process, step b), subsection ii) of the process, or to both variants of the process mentioned in subsections i) and ii).

[0027] Furthermore, the reaction can be allowed to continue for a period of 30 seconds to 24 hours, preferably 30 seconds to 3 hours. This period can refer to step b), subsection i) of the process, step b), subsection ii) of the process, or to both variants of the process mentioned in subsections i) and ii).

[0028] The porous membrane used in the alternative method can consist of at least one layer, optionally also at least one additional layer. The following features of the porous membrane can refer to all layers of the porous membrane.

[0029] The porous membrane may contain or consist of an electrically insulating material, wherein the material preferably has a specific electrical resistance of ≥ 10 10 Ω mm 2 / m, particularly preferably ≥ 10 11 Ω mm 2 / m, has.

[0030] Furthermore, the porous membrane can contain or consist of an organic material, preferably a polymeric plastic. The polymeric plastic is particularly preferably selected from the group consisting of polyolefin, fluoropolymer, polyamide, polyimide, cellulose, and combinations thereof. In particular, the polymeric plastic is selected from the group consisting of polyethylene, polypropylene, polytetrafluoroethylene, polyamide, para-aramid, polyimide, and combinations thereof.

[0031] In addition, the porous membrane may contain or consist of an inorganic material, preferably a ceramic material. The ceramic material is in particular selected from the group consisting of oxide ceramics, carbide ceramics, nitride ceramics, and phosphate ceramics.

[0032] In addition, the porous membrane may contain or consist of an ion-conductive material,

[0033] Apart from that, the porous membrane may have a thickness, in a direction perpendicular to one side of the porous membrane, in the range of 1 µm to 300 µm, preferably in the range of 1 µm to 70 µm, wherein the thickness is optionally a total thickness of all layers of the porous membrane.

[0034] In addition, the porous membrane may have a porosity in the range of 30% to 70%, preferably in the range of 40% to 60%, particularly preferably in the range of 45% to 50%.

[0035] According to the invention, a method for producing an electrode layer-separator layer-counter electrode layer stack is further provided, comprising the steps a) carrying out the method according to the invention; b) applying a bottom side of a counter electrode layer on the separator layer; c) Pressing the electrode layer, separator layer and counterelectrode layer together at a pressure sufficiently high to allow the liquid electrolyte bound in the gel to at least partially escape from the gel and thus to wet the top side of the electrode layer and the bottom side of the counterelectrode layer with liquid electrolyte and, if the electrode layer and / or counterelectrode layer have pores, to allow it to penetrate into said pores.

[0036] This process can be used to produce an electrode layer-separator layer-counter electrode layer stack in a simple, fast and cost-effective manner, with excellent ionic conductivity between the electrode layer, the separator layer and the counter electrode layer, and which is characterized by high cycle stability, low safety risk and low risk of irreparable damage.

[0037] The electrode layer and / or counterelectrode layer used in the process may contain or consist of an alkali metal, wherein the alkali metal is optionally applied to a metal selected from the group consisting of stainless steel, nickel, copper, indium, aluminum, and combinations thereof. The alkali metal is preferably selected from the group consisting of lithium, sodium, and combinations thereof.

[0038] Furthermore, the electrode layer and / or counterelectrode layer used in the process may contain or consist of carbon, preferably a carbon selected from the group consisting of graphite, graphene, activated carbon and combinations thereof.

[0039] In addition, the electrode layer and / or counterelectrode layer used in the process may contain or consist of silicon, a silicon alloy and / or a silicon composite.

[0040] Apart from that, the electrode layer and / or counterelectrode layer used in the process can contain or consist of a metal selected from the group consisting of stainless steel, nickel, copper, indium, and aluminum, preferably aluminum, wherein the aluminum is optionally alloyed, preferably with at least one element selected from main group II of the periodic table, main group III of the periodic table, main group IV of the periodic table, a subgroup of the periodic table, and combinations thereof. The at least one element is preferably selected from the group consisting of magnesium, indium, zinc, tin, silicon, manganese, and combinations thereof.

[0041] In addition, the electrode layer and / or counterelectrode layer used in the process may contain or consist of a material selected from the group consisting of nickel-manganese-cobalt oxide, lithium iron phosphate, lithium manganese oxide, lithium nickel-manganese oxide, lithium nickel oxide, lithium cobalt oxide, lithium aluminum nickel oxide, lithium manganese phosphate, lithium iron manganese phosphate, sodium phosphates (e.g. NaFePO4, Na2Co2Fe(PO4)3, Na3V2(PO4)3, Na2MnP2O7), sodium metal oxides (e.g. NaM x O y , M = V, Fe, Mn, Cr, Co, Ti, Ni), Prussian blue analogs (e.g. Na 2-x MnFe(CN)6)) and combinations thereof.

[0042] Furthermore, the electrode layer and / or counterelectrode layer used in the process can have a thickness, in a direction perpendicular to the surface of the electrode layer and / or counterelectrode layer, in the range of 10 to 100 µm, preferably 50 to 70 µm.

[0043] In addition, the electrode layer and / or counterelectrode layer used in the process can have a surface structure, wherein the surface structure is present on its upper side in the case of the electrode layer and on its underside in the case of the counterelectrode layer. The surface structure preferably has a structure depth in the range of 1 nm to 100 µm. Particularly preferably, the surface structure is selected from the group consisting of embossed surface structure, brushed surface structure, patterned surface structure, grooved surface structure, etched surface structure, lasered surface structure, and combinations thereof.

[0044] In the method, the pressing may comprise or consist of exerting mechanical pressure on the electrode layer-separator layer-counter electrode layer stack.

[0045] The mechanical pressure is preferably in the range of 0.1 to 1000 kg / cm 2 .

[0046] Furthermore, the mechanical pressure can be applied by winding the electrode layer-separator layer-counter electrode layer stack with a tensile stress.

[0047] In addition, the mechanical pressure can be applied by stacking the electrode layer-separator layer-counter electrode layer stack.

[0048] Apart from that, the mechanical pressure can be applied for a duration of 5 seconds to 24 hours, preferably 10 seconds.

[0049] In addition, the mechanical pressure can be applied at a temperature in the range of 20 to 60 °C, preferably 20 °C.

[0050] According to the invention, an electrode layer with a separator layer is further provided, containing or consisting of: a) a planar electrode layer, wherein the planar electrode layer has a planar top side and a planar bottom side; and b) a separator layer, wherein the separator layer consists of a gel containing or consisting of a polymer and a liquid electrolyte, wherein the gel contacts the upper side of the planar electrode layer, or consisting of a gel containing or consisting of a polymer and a liquid electrolyte, and a porous membrane, wherein the gel is applied to at least one side of the porous membrane and the gel the top side of the flat electrode layer; characterized in that the polymer i) is a cross-linked polymer; or ii) is a non-crosslinked polymer.

[0051] The electrode layer with separator layer according to the invention has excellent ionic conductivity between the electrode layer and the separator layer and is characterized by high cycle stability, low safety risk and low risk of irreparable damage.

[0052] The electrode layer with separator layer according to the invention is preferably produced by the method according to the invention.

[0053] Furthermore, according to the invention, an electrode layer-separator layer-counter electrode layer stack is provided, containing or consisting of: a) an electrode layer according to the invention with a separator layer; b) a counter electrode layer on top of the electrode layer.

[0054] The cathode layer-separator layer-anode layer stack according to the invention has excellent ionic conductivity between the electrode layer, the separator layer and the counter electrode layer and is characterized by high cycle stability, low safety risk and low risk of irreparable damage.

[0055] The cathode layer-separator layer-anode layer stack is preferably produced by the method according to the invention.

[0056] Furthermore, according to the invention, an electrochemical cell, electrostatic cell or a combination thereof is provided which contains an electrode layer-separator layer-counter electrode layer stack according to the invention.

[0057] The electrochemical cell is characterized by high electrical performance, high cycle stability, low safety risk and low risk of irreparable damage.

[0058] The electrochemical cell can be a lithium-ion battery. The electrostatic cell can be a double-layer capacitor.

[0059] The use of the electrochemical cell according to the invention, the electrostatic cell according to the invention or the combination thereof for energy supply i) a mobile device, preferably a mobile phone, a headset, a hearing aid, a vehicle, an aircraft and / or a ship; and / or ii) a stationary device, preferably a building; and / or (iii) a medical device, preferably a hearing aid; proposed.

[0060] The subject matter of the invention will be explained in more detail with reference to the following figures, without wishing to restrict it to the specific embodiments shown here.

[0061] Fig. 1 shows a first variant of the method according to the invention. First, a liquid 4 is produced which contains a liquid electrolyte and a polymer. For this purpose, for example, PVDF-HFP or silicone rubber is mixed with propylene carbonate or fluoroethylene carbonate and with a lithium conductive salt or an ionic liquid. This is followed by application 9 of the liquid 4 onto the upper side 2 of a planar electrode layer 1 (e.g., anode layer). The liquid 4 is then heated, whereby a gel 4' is formed from the liquid electrolyte and the polymer, which forms a separator layer 11 on the upper side 2 of the planar electrode layer 1. The liquid electrolyte is physically bound by the formed gel 4'. The gel 4' therefore serves as a reservoir of liquid electrolyte. In an assembly with a planar counterelectrode layer (e.g.,Cathode layer) the gel 4' is positioned between the flat electrode layer and the flat counter electrode layer and the layers are pressed together (see . Fig. 4A). As a result, a portion of the liquid electrolyte physically bound in the gel 4' is released to the flat electrode layer 1 and to the flat counterelectrode layer (so-called in-situ electrolyte filling), resulting in excellent wetting of their surfaces with liquid electrolyte (not shown).

[0062] Fig. Figure 2 shows a second variant of the method according to the invention. First, the method described in the figure description Fig. 1 is prepared. This is followed by application 10 of the liquid 4 to the upper side 6 of a flat, porous membrane 5, whereby the liquid penetrates into the pores of the flat, porous membrane 5. The reaction is then continued until the liquid 4 has formed a gel 4'. This creates a flat, porous membrane 5' which has the gel 4' on its upper side 6 and whose pores are filled with the gel 4'. The upper side 6 of the flat, porous membrane 5' is then applied 12 to the upper side 2 of the flat electrode layer 1, which has the gel 4', so that the gel 4' is thereby applied to the upper side 2 of the flat electrode layer 1. The liquid electrolyte is physically bound by the formed gel 4'. The gel 4' therefore serves as a reservoir of liquid electrolyte. When assembled with a flat counter electrode layer (e.g.Cathode layer), the flat counter electrode layer is positioned on the flat, porous membrane 5' and the layers are pressed together (see . Fig. 4B). As a result, a portion of the liquid electrolyte physically bound in the gel 4' is released to the flat electrode layer 1 and (through the pores of the flat, porous membrane 6) also to the flat counterelectrode layer, resulting in excellent wetting of their surfaces with liquid electrolyte (not shown).

[0063] Fig. Figure 3 shows a third variant of the method according to the invention. First, the Fig. 1 is prepared. This is followed by application 10 of the liquid 4 to both the top side 6 and the bottom side 7 of a flat, porous membrane 5. The mixture is then allowed to react until the liquid 4 has formed a gel 4'. This creates a flat, porous membrane 5' which has the gel 4' on its top side 6 and on the bottom side 7 and whose pores are filled with the gel 4'. The top side 6 of the flat, porous membrane 5', which contains the gel 4', is then applied 12 to the top side 2 of the flat electrode layer 1, so that the gel 4' is thereby applied to the top side 2 of the flat electrode layer 1. The liquid electrolyte is physically bound by the formed gel 4'. The gel 4' therefore serves as a reservoir of liquid electrolyte. When assembled with a flat counter electrode layer (e.g.Cathode layer), the flat counter electrode layer is positioned on the flat, porous membrane 5' and the layers are pressed together (see . Fig. 4C). As a result, part of the liquid electrolyte physically bound in the gel 4' is released to the flat electrode layer and to the flat counterelectrode layer (also through the pores of the flat membrane), resulting in excellent wetting of their surfaces with liquid electrolyte (not shown).

[0064] Fig. 4 shows various embodiments of electrode layer-separator layer-counter electrode layer stacks according to the invention. Fig. 4A shows an electrode layer-separator layer-counterelectrode layer stack comprising a planar electrode layer 1 and a planar counterelectrode layer 8. A gel 4' containing the polymer and the liquid electrolyte is arranged between the planar electrode layer 1 and the planar counterelectrode layer 8. Here, the gel 4' forms the separator layer 11. Fig. 4B shows an electrode layer-separator layer-counterelectrode layer stack comprising a planar electrode layer 1 and a planar counterelectrode layer 8. A planar, porous membrane 5' is arranged between the planar electrode layer 1 and the planar counterelectrode layer 8. The porous membrane 5' has a gel 4' containing the polymer and the liquid electrolyte on a top side 6 and in its pores. Said planar porous membrane 5', together with the gel 4', forms the separator layer 11. Fig.4C shows an electrode layer-separator layer-counterelectrode layer stack comprising a planar electrode layer 1 and a planar counterelectrode layer 8. A planar, porous membrane 5' is arranged between the planar electrode layer 1 and the planar counterelectrode layer 8. The membrane 5' has the gel 4' containing the polymer and the liquid electrolyte on its top side 6, on its bottom side 7, and in its pores. Said planar, porous membrane 5', together with the gel 4', forms the separator layer 11. List of reference symbols 1 flat electrode layer (e.g. anode layer); 2 Top side of the electrode layer; 3 Underside of the electrode layer; 4 Liquid containing a liquid electrolyte and a polymer; 4' Gel containing the liquid electrolyte and the polymer (forms the separator layer 11 or a part thereof); 5 flat membrane with pores; 5' flat membrane whose pores are filled with gel 4' (forms the separator layer 11); 6 Top side of the flat, porous membrane; 7 Underside of the flat, porous membrane; 8 flat counter electrode layer (e.g. cathode layer); 9 Applying the liquid to the top of the flat electrode layer; 10 Applying the liquid to the top and / or bottom of the flat, porous membrane; 11 Separator layer, which consists of the gel 4' alone, or the gel 4' and the flat membrane 5'; 12 Applying the separator layer to the top of the flat electrode layer. QUOTES CONTAINED IN THE DESCRIPTION

[0000] This list of documents submitted by the applicant was generated automatically and is included solely for the convenience of the reader. This list is not part of the German patent or utility model application. The DPMA assumes no liability for any errors or omissions. Cited non-patent literature

[0000] Kwade, A. et al., Nature Energy, Vol. 3, pp. 290-300

[0002] Ates, T. et al., Energy Storage Materials, Vol. 17, pp. 204-210

[0003] Liang, YF et al., Electrochimica Acta, Vol. 296, pp. 1064-1069

[0003]

Claims

[1] A method for producing an electrode layer with a separator layer, comprising or consisting of the steps: a) providing a planar electrode layer, wherein the planar electrode layer has a planar top side and a planar bottom side; and b) forming a separator layer on the flat upper side of the electrode layer by applying a liquid containing a liquid electrolyte and a polymer, i) onto the top side of the flat electrode layer and allowing it to react, whereby a gel is formed from the liquid electrolyte and the polymer and the gel forms a separator layer; or ii) at least on one side of a porous membrane, wherein the pores of the porous membrane are filled with the liquid and allowed to react, wherein a gel is formed from the liquid electrolyte and the polymer and the porous membrane and the gel together form a separator layer, wherein the separator layer is then applied to the upper side of the planar electrode layer; characterized by that the polymer - is a liquid, crosslinking polymer and is crosslinked by reacting in step b); or - a non-crosslinking polymer is present in the liquid together with an organic solvent having a boiling point of <100°C at atmospheric pressure, in order to dissolve the non-crosslinking polymer in the liquid before step b), wherein said organic solvent evaporates during the reaction in step b). [2] Method according to the preceding claim, characterized bythat the liquid, cross-linking polymer i) contains or consists of a plastic selected from the group consisting of one-component addition polymer, two-component addition polymer and combinations thereof, wherein the plastic is in particular silicone rubber; and / or ii) in a concentration of 10 to 90 vol%, preferably 40 to 60 vol%, based on the total volume of the liquid. [3] Method according to one of the preceding claims, characterized by that the non-crosslinking polymer (i) contains or consists of a fluorinated plastic, wherein the fluorinated plastic contains or consists in particular of PVDF-HFP; and / or ii) is present in the liquid in a concentration of 3 to 30% by weight, preferably 4 to 6% by weight, based on the total weight of the organic solvent; and / or iii) together with the organic solvent in a concentration of 10 to 90 vol%, preferably 40 to 60 vol%, based on the total volume of the liquid. [4] Method according to one of the preceding claims, characterized by that the liquid i) is applied by a method selected from the group consisting of doctor blade coating, pipetting and combinations thereof; and / or ii) is applied at a height in the range of up to 300 µm, preferably in the range of up to 50 µm, wherein the height refers to an extension of the liquid in a direction perpendicular to the top and / or bottom of the planar electrode layer. [5] Method according to one of the preceding claims, characterized bythat the liquid electrolyte contains or consists of an organic solvent which has a boiling point of ≥ 80°C, preferably > 200°C, at atmospheric pressure, and a conducting salt, wherein preferably i) the organic solvent is selected from the group consisting of PC, FEC, EC, DMC, EMC, DEC, VEC, VC, TBAC (acetyltributylcitrate), GTB (glycerol tributyrate), GTA (glycerol triacetate), γ-buthyrolactone and combinations thereof, wherein the organic solvent is preferably selected from the group consisting of PC, FEC, EC and combinations thereof; and / or ii) the conducting salt is a lithium conducting salt or a sodium conducting salt, wherein the lithium conducting salt is preferably selected from the group consisting of LiPF6, LiClO4, LiNO3, C6H 18LiNSi2, F2LiNO4S2, C2F6LiNO4S2, LiB[C2O4]2, LiBF4 and combinations thereof and / or the sodium conducting salt is preferably selected from the group consisting of NaPF6, NaBF4, NaTF, NaTFSI, NaClO4 and combinations thereof, wherein the conducting salt is optionally present in a concentration of 0.5 M to 2 M, preferably 1 M, in the liquid. [6] Method according to one of the preceding claims, characterized by that the liquid electrolyte contains or consists of an ionic liquid, wherein the ionic liquid is preferably i) is selected from the group consisting of pyrrolidinium-based ionic liquids, imidazolium-based ionic liquids, triliquid acid derivative-based ionic liquids, and combinations thereof, wherein the ionic liquid is preferably selected from the group consisting of 1-methyl-1-propylpyrrolidinium bis(trifluoromethylsulfonyl)imide, 1-methyl-1-propylpyrrolidinium bis(fluorosulfonyl)imide, 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide, 1-ethyl-3-methylimidazolium bis(fluorosulfonyl)imide, and combinations thereof; and / or ii) contains a conducting salt, wherein the conducting salt is particularly preferably a lithium conducting salt or a sodium conducting salt, wherein the lithium conducting salt is very preferably selected from the group consisting of LiPF6, LiClO4, LiNO3, C6H 18LiNSi2, F2LiNO4S2, C2F6LiNO4S2, LiB[C2O4]2, LiBF4 and combinations thereof and / or the sodium conducting salt is very preferably selected from the group consisting of NaPF6, NaBF4, NaTF, NaTFSI, NaClO4 and combinations thereof, wherein the conducting salt is optionally present in a concentration of 0.5 M to 2 M, preferably 1 M, in the ionic liquid. [7] Method according to one of the preceding claims, characterized by that in the proceedings i) is allowed to react at a temperature in the range of 20 to 150 °C, preferably at a temperature in the range of 30 to 60 °C; and / or (ii) is allowed to react for a period of 30 seconds to 24 hours, preferably 30 seconds to 3 hours. [8] Method according to one of the preceding claims, characterized by that the porous membrane i) consists of at least one layer, optionally also at least one further layer; and / or ii) contains or consists of an electrically insulating material, wherein the material preferably has a specific electrical resistance of ≥ 10 10 Ω mm 2 / m, particularly preferably ≥ 10 11 Ω mm 2 / m, and / or iii) contains or consists of an organic material, preferably contains or consists of a polymeric plastic, wherein the polymeric plastic is particularly preferably selected from the group consisting of polyolefin, fluoropolymer, polyamide, polyimide, cellulose, and combinations thereof, wherein the polymeric plastic is particularly selected from the group consisting of polyethylene, polypropylene, polytetrafluoroethylene, polyamide, para-aramid, polyimide and combinations thereof; and / or iv) contains or consists of an inorganic material, preferably contains or consists of a ceramic material, wherein the ceramic material is in particular selected from the group consisting of oxide ceramic, carbide ceramic, nitride ceramic and phosphate ceramic; and / or (v) contains or consists of an ion-conductive material; and / or vi) has a thickness, in a direction perpendicular to one side of the porous membrane, in the range from 1 µm to 300 µm, preferably in the range from 1 µm to 70 µm, wherein the thickness is optionally a total thickness of all layers of the porous membrane; and / or vii) has a porosity in the range of 30% to 70%, preferably in the range of 40% to 60%, particularly preferably in the range of 45% to 50%. [9] Method for producing an electrode layer-separator layer-counter electrode layer stack, comprising the steps a) carrying out a method according to one of the preceding claims; b) applying a bottom side of a counter electrode layer on the separator layer; c) Pressing the electrode layer, separator layer and counterelectrode layer together at a pressure sufficiently high to allow the liquid electrolyte bound in the gel to at least partially escape from the gel and thus to wet the upper side of the electrode layer and the lower side of the counterelectrode layer with liquid electrolyte and, if the electrode layer and / or counterelectrode layer have pores, to allow it to penetrate into said pores. [10] Method according to claim 9, characterized by that the electrode layer and / or counter electrode layer i) contains or consists of an alkali metal, wherein the alkali metal is optionally applied to a metal selected from the group consisting of stainless steel, nickel, copper, indium, aluminum and combinations thereof, and wherein the alkali metal is preferably selected from the group consisting of lithium, sodium and combinations thereof; and / or ii) contains or consists of carbon, preferably a carbon selected from the group consisting of graphite, graphene, activated carbon and combinations thereof; and / or iii) contains or consists of silicon, a silicon alloy and / or a silicon composite; and / or iv) contains or consists of a metal selected from the group consisting of stainless steel, nickel, copper, indium, aluminum, preferably aluminum, wherein the aluminum is optionally alloyed, preferably with at least one element selected from the II. main group of the periodic table, the III. main group of the periodic table, the IV. main group of the periodic table, a subgroup of the periodic table and combinations thereof, wherein the at least one element is preferably selected from the group consisting of magnesium, indium, zinc, tin, silicon, manganese and combinations thereof; and / or v) contains or consists of a material selected from the group consisting of nickel manganese cobalt oxide, lithium iron phosphate, lithium manganese oxide, lithium nickel manganese oxide, lithium nickel oxide, lithium cobalt oxide, lithium aluminum nickel oxide, lithium manganese phosphate, lithium iron manganese phosphate, sodium phosphates, sodium metal oxides, Prussian blue analogues and combinations thereof; and / or vi) has a thickness, in a direction perpendicular to the surface of the electrode layer and / or counterelectrode layer, in the range of 10 to 100 µm, preferably 50 to 70 µm; and / or vii) has a surface structuring, wherein the surface structuring is present on its upper side in the case of the electrode layer and is present on its underside in the case of the counterelectrode layer, wherein the surface structuring preferably has a structure depth in the range from 1 nm to 100 µm, wherein the surface structuring is particularly preferably selected from the group consisting of embossed surface structuring, brushed surface structuring, patterned surface structuring, grooved surface structuring, etched surface structuring, lasered surface structuring and combinations thereof. [11] Method according to one of claims 9 or 10, characterized by that the pressing comprises or consists of exerting a mechanical pressure on the electrode layer-separator layer-counter electrode layer stack, wherein the mechanical pressure is preferably i) in the range of 0.1 to 1000 kg / cm2 lies; and / or ii) by winding the electrode layer-separator layer-counter electrode layer stack with a tensile stress; and / or iii) is applied by stacking the electrode layer-separator layer-counter electrode layer stack; and / or iv) is applied for a duration of 5 seconds to 24 hours, preferably 10 seconds; and / or v) is applied at a temperature in the range of 20 to 60 °C, preferably 20 °C. [12] Electrode layer with separator layer, containing or consisting of: a) a planar electrode layer, wherein the planar electrode layer has a planar top side and a planar bottom side; and b) a separator layer, wherein the separator layer consists of a gel containing or consisting of a polymer and a liquid electrolyte, wherein the gel contacts the upper side of the planar electrode layer, or consists of a gel containing or consisting of a polymer and a liquid electrolyte and a porous membrane, wherein the gel is applied to at least one side of the porous membrane and the gel contacts the upper side of the planar electrode layer; characterized by that the polymer i) is a cross-linked polymer; or ii) is a non-crosslinked polymer; wherein the electrode layer with separator layer is preferably produced by a process according to any one of claims 1 to 8. [13] Electrode layer-separator layer-counter electrode layer stack, containing or consisting of: a) an electrode layer with a separator layer according to one of claims 1 to 8; b) a counter electrode layer on top of the electrode layer; wherein the cathode layer-separator layer-anode layer stack is preferably produced by a method according to one of claims 9 to 11. [14] An electrochemical cell, electrostatic cell or combination thereof, comprising an electrode layer-separator layer-counter electrode layer stack according to claim 13. [15] Use of the electrochemical cell, electrostatic cell or combination thereof according to claim 14 for energy supply i) a mobile device, preferably a mobile phone, a headset, a hearing aid, a vehicle, an aircraft and / or a ship; and / or ii) a stationary device, preferably a building; and / or iii) a medical device, preferably a hearing aid.

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