The present invention relates to a process for producing a shaped organic charge storage unit, especially a secondary battery, the electrodes of which comprise an organic redox-active polymer, and which includes a polymeric solid electrolyte. The present invention additionally also relates to the shaped organic charge storage unit itself. By comparison with those from the prior art, the charge storage unit of the present invention shows greater resistance to deformation, which is manifested in a reduced tendency to fracture in the shaping process.

Background of the invention

Charge storage units, for example secondary batteries, find various uses in sectors in which they are exposed to high mechanical stresses.

For example, batteries are required in the field of patient-centred laboratory diagnostics, where they are applied to flexible substrates such as paper, textiles or bandage material.

There is also a need in the sports sector for electronic measuring devices that measure various body functions such as heartbeat, calories burnt etc., and are worn on the body by sportspeople. Such measuring devices and the batteries included therein require high mechanical stability and a small space requirement since they are worn on the body and, when they are applied to textiles, for example, are subjected to mechanical shear forces and impacts as a result of the movement of the wearer.

In addition, in the consumer goods and electrical industry, there is also a need for batteries that are applied to a flexible substrate and can be shaped without losing their ability to function. This is the case, for instance, for housings of electronic toys, electronic musical instruments or electronic joke articles.

The production of packaging material often entails the deformation of the articles by stretching or compressing, which also affects electrodes applied thereto if they do not have adequate mechanical durability. For these purposes, the prior art describes various durable and shapable charge storage units.

WO 2015/160944 A1 describes a metal-based battery applied to paper that can be used for wearable electronic devices. WO 2015/100414 A1 describes a shapable lithium ion battery that can be applied to packaging material, for example.

However, these batteries described in the prior art have the disadvantage that they do not have good resistance to the mechanical stresses associated with the applications described above. In addition, for example, the batteries described in WO 2015/160944 A1 are primary batteries that cannot be recharged. The batteries described in WO 2015/100414 A1 are difficult to produce and contain heavy metals and toxic liquid electrolytes that can escape easily. There is thus a need for flexible, durable charge storage units that do not have the aforementioned problems and feature high mechanical durability. There is also a need for efficient organic charge storage units having high capacities.

Detailed description of the invention

A process has now been found for producing a shaped organic charge storage unit that solves these problems.

It has namely been found that, surprisingly, organic redox-active polymers have high mechanical stability and are therefore of particularly good suitability for use in shaped, especially folded, organic charge storage units. Flexibility and mechanical durability is especially assisted by the combination with a polymer electrolyte. As a result, the charge storage units according to the invention are printable, rapidly producible, and by virtue of their shapability assure better utilization of the space provided.

Improved mechanical stability is observed especially with respect to folded metal-based charge storage units, which break more often in the production process compared to the batteries according to the invention that are based on organic redox polymers. In addition, the charge storage units according to the invention are organic and can thus be employed in fields of use that are closed to the prior art metal-based batteries, which are of concern in respect of health. The charge storage unit according to the invention also features a high capacity.

1. First aspect: Process for producing a shaped organic charge storage unit

In a first aspect, the present invention relates to a process for producing a shaped organic charge storage unit L _org , which is preferably a secondary battery, comprising the following steps: a) applying a mixture M ₁ comprising at least one organic redox-active polymer P _redox1 , at least one conductivity additive L ₁ , at least one solvent Solv ₁ , optionally at least one binder additive B ₁ and optionally at least one ionic liquid IL ₁ to a substrate S ₁ , b) at least partly removing the solvent Solv ₁ , to obtain an electrode E ₁ applied to the substrate S ₁ ; c) applying a polymer electrolyte P _el to the electrode E ₁ ; d) applying a mixture M ₂ comprising at least one organic redox-active polymer P _redox2 , at least one conductivity additive L ₂ , at least one solvent Solv ₂ , optionally at least one binder additive B2 and optionally at least one ionic liquid IL ₂ to the polymer electrolyte P _el , e) at least partly removing the solvent Solv ₂ , to obtain an electrode E ₂ applied to the polymer electrolyte P _el ; f) applying a substrate S2 to the electrode E ₂ ; to obtain an organic charge storage unit L _org ; characterized in that g) the substrate S ₁ is shaped in the region of the substrate S ₁ covered by the electrode E ₁ to obtain a shaped organic charge storage unit L _org .

The process according to the invention enables the production of organic charge storage units that have been shaped and are usable in a more versatile manner compared to conventional shaped charge storage units. This enables the use of the charge storage units produced by the process according to the invention on non-planar surfaces, for example when a battery has to be mounted on a corner or on concave or convex surfaces. The invention thus opens up new space-saving options for mounting a charge storage unit with high fracture resistance, for instance in packaging, toys, laboratory diagnostics, bandage material, cosmetics, clothing, especially sports clothing, aquarium equipment (filter, heating, electric thermometer for smaller aquaria), musical instruments. A further field of use in which space-saving solutions are being sought is that of smartphones or TV appliances, especially those having a flexible surface/display, which accordingly also require a charge storage unit that assures and tolerates corresponding flexibility. For these fields of use too, it is possible to use the charge storage unit L _org according to the present invention. 1.1 Step (a) of the process according to the invention

In step a) of the process according to the invention in the first aspect of the invention, a mixture M ₁ comprising at least one organic redox-active polymer P _redox1 , at least one conductivity additive L ₁ , at least one solvent Solv ₁ , optionally at least one binder additive B ₁ and optionally at least one ionic liquid IL ₁ is applied to a substrate S.

1.1.1 Substrate S ₁ The substrate S ₁ is especially selected from conductive materials, preferably from the group consisting of metals, carbon materials, oxide substances. These conductive materials may form the substrate S ₁ on their own or, as is preferred in the present invention, may have been applied to nonconductive materials such as, in particular, a material selected from the group consisting of plastics, which are especially polyethylene terephthalate (= PET) or polyurethane, textiles, cellulose, especially paper, wood. Useful substrates S ₁ include cellulose fibres coated with carbon nanotubes (CNTs) (production described in WO 2015/100414, paragraphs [0104], [0105]).

Further preferred substrates S ₁ are metal foils.

Metals that are preferentially suitable as substrate S ₁ and may also be used in the form of nanoparticles or foils are selected from silver, platinum, gold, iron, copper, aluminium, zinc or a combination of these metals. Preferred carbon materials suitable as substrate are selected from carbon black, glassy carbon, graphite foil, graphene, carbon skins, carbon nanotubes (CNTs). Preferred oxide substances suitable as substrate S ₁ are selected, for example, from the group consisting of indium tin oxide (ITO), indium zinc oxide (IZO), antimony zinc oxide (AZO), fluorine tin oxide (FTO) or antimony tin oxide (ATO), zinc oxide (ZO). Substrates S ₁ used may also be mixtures of the groups mentioned, for example mixtures of metals and carbon materials, for example silver with carbon.

The form of the substrate S ₁ in step (a) is not subject to further restriction. However, it is preferable that the substrate S ₁ is planar at least in the region in which the mixture M ₁ is applied in the subsequent step (b), which means that the surface of the substrate S ₁ on which the mixture M ₁ is applied in step (b) of the process according to the invention in the first aspect of the invention is in a plane. The use of a planar substrate S ₁ has the advantage that the application of uniform layers as described hereinafter is more easily possible. 1.1.2 Mixture M ₁

The mixture M ₁ used in step a) of the process according to the invention comprises at least one organic redox-active polymer P _redox1 , at least one conductivity additive L ₁ , at least one solvent Solv ₁ , optionally at least one binder additive B ₁ and optionally at least one ionic liquid IL ₁ .

The mixture M ₁ is especially an electrode slurry, especially a solution or suspension, with which the constituents of the electrode E ₁ obtained at a later stage are applied to the substrate S ₁ .

1.1.2.1 Organic redox-active polymer P _redox1

The polymers usable as organic redox-active polymer P _redox1 that are included in the mixture M ₁ are known to those skilled in the art and are described, for example, in US 2016/0233509 A1 , US 2017/01 14162 A1 , US 2017/0179525 A1 , US 2018/010891 1 A1 , US 2018/0102541 A1 , WO 2017/207325 A1 , WO 2015/032951 A1. An overview of further usable organic redox-active polymers is given by the article S. Muench, A. Wild, C. Friebe, B. Haupler, T. Janoschka, U.S. Schubert, Chem. Rev. 2016, 116, 9438-9484.

The polymers P _redox1 can be obtained by methods known to those skilled in the art.

The corresponding methods are summarized by S. Muench, A. Wild, C. Friebe, B. Haupler, T. Janoschka, U.S. Schubert, Chem. Rev. 2016, 116, 9438-9484.

In addition, the synthesis of the polymers P _redox1 comprising a redox-active aromatic imide function is described in WO 2015/003725 A1 and US 4,898,915 A.

In addition, polymers P _redox1 comprising a redox-active aromatic function comprising at least one stable oxygen radical and the synthesis of the corresponding polymers P _redox1 are also known to the person skilled in the art from WO 2017/207325 A1 , EP 1 752 474 A1 , WO 2015/032951 A1 , CN 104530424 A, ON 104530426 A, T. Suga, H. Ohshiro, S. Sugita, K. Oyaizu, H. Nishide, Adv. Mater. 2009, 21, 1627-1630 and T. Suga, S. Sugita, H. Ohshiro, K. Oyaizu, H. Nishide, Adv. Mater. 2011 , 3, 751-754.

In addition, the synthesis of polymers P _redox1 comprising a redox-active anthraquinone/carbazole function and the synthesis of the polymers P _redox1 comprising a redox-active benzoquinone function is also described in, or is possible as a matter of routine for the person skilled in the art on the basis of his knowledge in the art from, WO 2015/132374 A1 , WO 2015/144798 A1 , EP 3 279 223 A1 , WO 2018/024901 A1 , US 2017/0077518 A1 , US 2017/0077517 A1 , US 2017/0104214 A1 , D. Schmidt, B. Haupler, C. Stolze, M.D. Hager, U.S. Schubert, J. Polym. Sci., Part A: Polym. Chem. 2015, 53, 2517-2523, M.E. Speer, M. Kolek, J.J. Jassoy, J. Heine, M. Winter, P.M. Bieker, B.

Esser, Chem. Commun. 2015, 51, 15261-15264 and M. Baibarac, M. Lira-Cantú , J. Oro Sol, I. Baltog, N. Casah-Pastor, P. Gomez-Romero, Compos. Sci. Technol. 2007, 67, 2556-2563.

In addition, the synthesis of polymers P _redox1 comprising a redox-active dialkoxybenzene function is also described in WO 2017/032583 A1 , EP 3 136 410 A1 , EP 3 135 704 A1 , WO 2017/032582 A1 , P. Nesvadba, L. B. Folger, P. Maire, P. Novak, Synth. Met. 2011 , 161, 259-262; W. Weng, Z.C. Zhang, A. Abouimrane, P.C. Redfern, L.A. Curtiss, K. Amine, Adv. Funct. Mater. 2012, 22, 4485- 4492.

In addition, the synthesis of polymers P _redox1 comprising a redox-active triphenylamine function is also described in JP 2011-74316 A, JP 2011-74317 A.

In addition, the synthesis of polymers P _redox1 comprising a redox-active viologen function is also described in ON 1071 18332 A.

In addition, the synthesis of polymers P _redox1 comprising a redox-active ferrocene function is also described in K. Tamura, N. Akutagawa, M. Satoh, J. Wada, T. Masuda, Macromol. Rapid Commun. 2008, 29, 1944-1949.

The organic redox-active polymer P _redox1 is preferably selected from the group consisting of polyimides and polymers comprising m units of the general formula (III):

where m is an integer ³ 4, preferably an integer ³ 10, more preferably an integer ³ 100, even more preferably an integer in the range of 1000 to 10 ⁹ , yet more preferably an integer in the range of 2000 to 10 000, W is a repeat unit, Sp is an organic spacer and R ^x is an organic redox-active group, where the bond identified by (i) in a unit of the formula (III) binds to the bond identified by (ii) in the adjacent unit of the formula (III). R ^x in the structure (III) is preferably selected from the group consisting of compounds of the general formulae (lll-A), (lll-B), (lll-C), (lll-D), (lll-E), (lll-F) where

and where, in the structures (lll-A), (lll-B) and (lll-C), at least one aromatic carbon atom may be substituted by a group selected from alkyl group, halogen group, alkoxy group, hydroxyl group. Even more preferably, R ^x in the structure (III) is selected from the group consisting of compounds of the general formulae (lll-A), (lll-B), (lll-C), (lll-D), with (lll-D) being the very most preferred.

W in the structure (III) is a repeat unit, and the person skilled in the art is able to select this using his knowledge in the art. The spacer units Sp are connecting units between the redox-active units and the repeat units W that may especially likewise be selected by the person skilled in the art in a routine manner drawing on knowledge in the art.

Preferably, the W radical in the structure (III) is selected from the group consisting of the structures

where the bond identified by (i) in a unit of the formula (W1), (W2), (W3) binds in each case to the bond identified by (ii) in the adjacent unit of the formula (W1), (W2) or (W3), where the bond identified by (iii) in each case identifies the bond to Sp, and where R ^W1 , R ^W2 , R ^W3 , R ^W4 , R ^W5 , R ^W6 , R ^W7 are independently selected from the group consisting of hydrogen, alkyl group, haloalkyl group, -COOR ^W8 with R ^W8 = H or alkyl,

R ^W1 , R ^W2 , R ^W3 , R ^W4 , R ^W5 , R ^W6 , R ^W7 are preferably independently selected from the group consisting of hydrogen, methyl, -COOH, -COOCH3, and where, even more preferably, the W radical in the structure (III) has the structure (W1) in which one of R ^W1 , R ^W2 , R ^W3 is methyl and the other two are hydrogen or all of R ^W1 , R ^W2 , R ^W3 are hydrogen; and the Sp radical in the structure (III) is selected from the group consisting of direct bond, (Sp1), (Sp2):

where pA1 , pA2, pA3 are each 0 or 1 , excluding the case that“pA2 = 0, pA1 = pA3 = 1”, where qA1 , qA2, qA3 are each 0 or 1 , excluding the case that“qA2 = 0, qA1 = qA3 = 1”, where qA4, qA5, qA6 are each 0 or 1 , where at least one of qA4, qA5, qA6 = 1 and where the case that“qA5 = 0, qA4 = qA6 = 1” is excluded, where B ^Sp is selected from the group consisting of

divalent (hetero)aromatic radical, preferably phenyl,

divalent aliphatic radical, which is preferably alkylene, optionally substituted by at least one group selected from nitro group, -NH2, -CN, -SH, -OH, halogen and optionally having at least one group selected from ether, thioether, amino ether, carbonyl group, carboxylic ester, carboxamide group, sulfonic ester, phosphoric ester, and where in the cases in which Sp binds to a non-carbon atom in the R ^x radical, the structure (Sp1) is subject to the additional condition“qA3 = 0, qA2 = 1 , qA1 = 1 or qA3 = qA2 = qA1 = 0 or qA3 = 0, qA2 = 1 , qA1 = 0”, preferably the condition“qA3 = qA2 = qA1 = 0”, and the structure (Sp2) to the additional condition“qA6 = 0, qA5 = 1 , qA4 = 1 or qA6 = 0, qA5 = 1 , qA4 = 0”, and where denotes the bond pointing toward R ^x ,

and where denotes the bond pointing toward W.

It is pointed out that the condition“where at least one of qA4, qA5, qA6 = 1”, in respect of Sp2, relates solely to the definition of the respective variables qA4, qA5, qA6 and does not mean that the Sp radical in the structure (III) cannot also be a direct bond. More preferably, the Sp radical is selected from the group consisting of direct bond, (Sp2) with more preferably from the group consisting of direct bond, denotes the bond pointing toward R ^x , and where denotes the bond pointing toward W. If the polymer P _redox1 is a polyimide, it is preferably selected from the group consisting of the structures (IV-1), (IV-2), (IV-3), (IV-4), (IV-5), (IV-6), (IV-7), (IV-8), (IV-9):

where n is an integer ³ 4, preferably an integer ³ 10, more preferably an integer ³ 100, even more preferably an integer in the range of 1000 to 10 ⁹ , yet more preferably an integer in the range of 2000 to 10 000,

and the bond identified by (iv) in the structures (IV-1), (IV-2), (IV-3), (IV-4), (IV-5), (IV-6), (IV-7), (IV- 8), (IV-9) binds in each case to the bond identified by (v), and where in the structures (IV-1), (IV-2), (IV-3), (IV-4), (IV-5), (IV-6), (IV-7), (IV-8), (IV-9), at least one aromatic carbon atom may be substituted by a group selected from alkyl, halogen, alkoxy, OH, preferably halogen, OH, and where Ar ^I , Ar ^II are each independently a hydrocarbyl group having at least one aryl radical and especially having 6 to 30, preferably 6 to 15, more preferably 6 to 13, carbon atoms. If the polymer P _redox1 is a polyimide, this is more preferably selected from the group consisting of the structures (IV-1), (IV-2), (IV-3), (IV-4), (IV-5), (IV-6), (IV-7), (IV-8), (IV-9), where n is an integer ³ 4, preferably an integer ³ 10, more preferably an integer ³ 100, even more preferably an integer in the range of 1000 to 10 ⁹ , yet more preferably an integer in the range of 2000 to 10 000, and the bond identified by (iv) in the structures (IV-1), (IV-2), (IV-3), (IV-4), (IV-5), (IV-6), (IV-7), (IV-8), (IV- 9) binds in each case to the bond identified by (v), and where Ar ^I , Ar ^II are each independently a hydrocarbyl group having at least one aryl radical and especially having 6 to 30, preferably 6 to 15, more preferably 6 to 13, carbon atoms. More preferably, the polymer P _redox1 comprises t repeat units joined to one another, selected from the group consisting of the structures P1 , P2, P3, P4, P5, P6:

where t is an integer ³ 4, preferably an integer ³ 10, more preferably an integer ³ 100, even more preferably an integer in the range of 1000 to 10 ⁹ , yet more preferably an integer in the range of 2000 to 10 000, where R ^P5 , R ^P6 are each independently selected from the group consisting of hydrogen, methyl, and are especially each hydrogen, and the bond identified by (vi) in a unit of the formula P1 binds to the bond identified by (vii) in the adjacent unit of the formula P1 ,

and the bond identified by (viii) in a unit of the formula P2 binds to the bond identified by (ix) in the adjacent unit of the formula P2,

and the bond identified by (x) in a unit of the formula P3 binds to the bond identified by (xi) in the adjacent unit of the formula P3,

and the bond identified by (xii) in a unit of the formula P4 binds to the bond identified by (xiii) in the adjacent unit of the formula P4,

and the bond identified by (xiv) in a unit of the formula P5 binds to the bond identified by (xv) in the adjacent unit of the formula P5,

and the bond identified by (xvi) in a unit of the formula P6 binds to the bond identified by (xvii) in the adjacent unit of the formula P6. In a preferred embodiment of the process according to the invention for producing a charge storage unit, the polymer P1 is included as polymer P _redox1 in the electrode E ₁ used with preference as cathode, and at least one of the polymers P2, P3, preferably P2, is included as polymer P _redox2 in the electrode E ₂ used in particular as anode.

In a preferred embodiment of the process according to the invention for producing a charge storage unit, the polymer P4 is included as polymer P _redox1 in the electrode E ₁ used with preference as cathode, and at least one of the polymers P2, P3, preferably P2, is included as polymer P _redox2 in the electrode E ₂ used in particular as anode.

In a preferred embodiment of the process according to the invention for producing a charge storage unit, the polymer P5 with R ^P5 = H is included as polymer P _redox1 in the electrode E ₁ used with preference as cathode, and at least one of the polymers P2, P3, preferably P2, is included as polymer P _redox2 in the electrode E ₂ used in particular as anode.

In a preferred embodiment of the process according to the invention for producing a charge storage unit, the polymer P5 with R ^P5 = CH ₃ is included as polymer P _redox1 in the electrode E ₁ used with preference as cathode, and at least one of the polymers P2, P3, preferably P2, is included as polymer P _redox2 in the electrode E ₂ used in particular as anode.

In a preferred embodiment of the process according to the invention for producing a charge storage unit, the polymer P6 with R ^P6 = H is included as polymer P _redox1 in the electrode E ₁ used with preference as cathode, and at least one of the polymers P2, P3, preferably P2, is included as polymer P _redox2 in the electrode E ₂ used in particular as anode.

In a preferred embodiment of the process according to the invention for producing a charge storage unit, the polymer P6 with R ^P6 = CH ₃ is included as polymer P _redox1 in the electrode E ₁ used with preference as cathode, and at least one of the polymers P2, P3, preferably P2, is included as polymer P _redox2 in the electrode E ₂ used in particular as anode.

The end groups of the first repeat unit of the polymer P _redox which is present for these on the bonds defined by "(i)" in the chemical structure (III), and is present for these on the bonds defined by "(vi)" in the chemical structure P1 , and is present for these on the bonds defined by "(viii)" in the chemical structure P2, and is present for these on the bonds defined by "(x)" in the chemical structure P3, and is present for these on the bonds defined by "(xii)" in the chemical structure P4, and is present for these on the bonds defined by "(xiv)" in the chemical structure P5, and is present for these on the bonds defined by "(xvi)" in the chemical structure P6, and is present for these on the bonds defined in each case by "(iv)" in the chemical structures (IV-1), (IV-2), (IV-3), (IV-4), (IV- 5), (IV-6), (IV-7), (IV-8), (IV-9), and the end groups of the last repeat unit of the polymer P _redox according to the invention which is present for these on the bonds defined by "(ii)” in the chemical structure (III), and is present for these on the bonds defined by "(vii)" in the chemical structure P1 , and is present for these on the bonds defined by "(ix)" in the chemical structure P2, and is present for these on the bonds defined by "(xi)" in the chemical structure P3, and is present for these on the bonds defined by "(xiii)" in the chemical structure P4, and is present for these on the bonds defined by "(xv)" in the chemical structure P5, and is present for these on the bonds defined by "(xvii)" in the chemical structure P6, and is present for these on the bonds defined in each case by "(v)" in the chemical structures (IV- 1), (IV-2), (IV-3), (IV-4), (IV-5), (IV-6), (IV-7), (IV-8), (IV-9), are not particularly restricted and are apparent from the polymerization method used in the preparation method for the polymer P _redox1 · Thus, they may be termination fragments of an initiator or of a repeat unit. Preferably, these end groups are selected from hydrogen, halogen, hydroxyl, unsubstituted aliphatic radical or aliphatic radical substituted by -CN, -OH, halogen (which may especially be an unsubstituted or correspondingly substituted alkyl group), (hetero)aromatic radical, which is preferably a phenyl radical, benzyl radical or ohydroxybenzyl.

1.1.2.2 Conductivity additive L ₁

1.1.2.2.1 Preferred conductivity additive L ₁ The at least one conductivity additive L ₁ which is included in the mixture M ₁ which is used in step (a) of the process according to the first aspect of the invention is at least one electrically conductive material, especially selected from the group consisting of carbon materials, electrically conductive polymers, metals, semimetals, (semi)metal compounds, preferably selected from carbon materials, electrically conductive polymers.

According to the invention,“(semi)metals” are selected from the group consisting of metals, semimetals, and are preferably metals.

Metals are especially selected from the group consisting of zinc, iron, copper, silver, gold, chromium, nickel, tin, indium.

Semimetals are especially selected from silicon, germanium, gallium, arsenic, antimony, selenium, tellurium, polonium. The conductivity additive L ₁ is more preferably a carbon material. Carbon materials are especially selected from the group consisting of carbon fibres, carbon nanotubes, graphite, graphene, carbon black, fullerene. Electrically conductive polymers are especially selected from the group consisting of polypyrroles, polyanilines, polyphenylenes, polypyrenes, polyazulenes, polynaphthylenes, polycarbazoles, polyindoles, polyazepines, polyphenylene sulfides, polythiophenes, polyacetylenes, poly(3,4- ethylenedioxythiophene) polystyrenesulfonate (= PEDOT PSS), polyarcenes, poly-(p- phenylenevinylenes).

1.1.2.2.2 Preferred amount of the conductivity additive L ₁

The amount of the conductivity additive L ₁ included in the mixture M ₁ in step (a) of the process according to the first aspect of the invention is not subject to any further restriction. However, it is preferable that the total weight of all conductivity additives L ₁ included in the mixture M ₁ , based on the total weight of the redox polymers P _redox1 included in the mixture M ₁ , is in the range of 0.1 % to 1000% by weight, preferably in the range of 10% to 500% by weight, more preferably in the range of 30% to 100% by weight, yet more preferably in the range of 40% to 80% by weight, even more preferably in the range of 50% by weight to 60% by weight, most preferably 58.3% by weight.

1.1.2.3 Solvent Solv ₁

The at least one solvent Solv ₁ included in the mixture M ₁ is especially a solvent having a high boiling point, preferably selected from the group consisting of N-methyl-2-pyrrolidone, water, dimethyl sulfoxide, ethylene carbonate, propylene carbonate, dimethyl carbonate, methyl ethyl carbonate, y-butyrolactone, tetrahydrofuran, dioxolane, sulfolane, N,N'-dimethylformamide, N,N'- dimethylacetamide, more preferably dimethyl sulfoxide or water, even more preferably water.

More particularly, the mixture M ₁ comprises a sufficient amount of solvent Solv ₁ that the concentration of the organic redox-active polymer P _redox1 in the mixture M ₁ is between 1 and 100 mg/ml, preferably between 5 and 50 mg/ml.

1.1.2.4 Binder additive B ₁ More particularly, the mixture M ₁ also comprises at least one binder additive B ₁ .

Binder additives B ₁ are familiar to the person skilled in the art as materials having binding properties. Preference is given to polymers selected from the group consisting of poly(vinylidene fluoride-co-hexafluoropropylene) (PVdF-HFP), polytetrafluoroethylene, polyvinylidene fluoride, polyhexafluoropropylene, polyvinyl chloride, polycarbonate, polystyrene, polyacrylate,

polymethacrylate, polysulfone, cellulose derivatives, polyurethane, and the binder additive more preferably comprises cellulose derivatives, e.g. sodium carboxymethylcellulose or PVdF-HFP or polyvinylidene fluoride.

In the cases in which the mixture M ₁ comprises at least one binder additive B ₁ , the amount of all binder additives B ₁ included in the mixture M ₁ in step (a) of the process according to the invention in the first aspect of the invention is not subject to any further restriction.

However, it is preferable in these cases that the total weight of all binder additives B ₁ included in the mixture M ₁ , based on the total weight of the redox polymer P _redox1 included in the mixture M ₁ , is in the range of 0.001 % to 100% by weight, more preferably in the range of 0.1 % to 90% by weight, yet more preferably in the range of 3% to 70% by weight, still more preferably in the range of 5% to 50% by weight, even more preferably in the range of 7.5% by weight to 20% by weight, and is most preferably 16.6% by weight.

1.1.2.5 Ionic liquid IL ₁ More particularly, the mixture M ₁ also comprises at least one ionic liquid IL ₁ .

The at least one ionic liquid IL ₁ included in the mixture M ₁ is not particularly restricted and is described, for example, in WO 2004/016631 A1 , WO 2006/134015 A1 , US 201 1/0247494 A1 or US 2008/0251759 A1 .

More particularly, the at least one ionic liquid IL ₁ included in the mixture M ₁ in step (a) of the process according to the invention has the structure Q ⁺ A-.

1.1.2.5.1 Preferred cation Q+ of IL ₁ Q ⁺ therein is a cation selected from the group consisting of the following structures (Q1), (Q2),

(Q3), (Q4), (Q5): where R ^Q1 , R ^Q2 , R ^Q3 , R ^Q4 , R ^Q5 , R ^Q6 , R ^Q7 , R ^Q8 are each independently selected from the group consisting of alkyl group, haloalkyl group, cycloalkyl group, where R ^Q9 R ^Q10 R ^Q11 R ^Q12 R ^Q13 R ^Q14 R ^Q15 R ^Q16 R ^Q17 R ^Q"18 R ^Q19 p ^Q 2o R ^Q 2I R ^Q 22 R ^Q 23 R ^Q24 R ⁰²⁵ , R ^Q26 , R ^Q27 , R ^Q28 , R ^Q29 , R ^Q3 °, R ^Q31 , R ^Q32 , R ^Q33 , R ^Q34 , R ^Q35 are each independently selected from the group consisting of hydrogen, alkyl group, (poly)ether group, haloalkyl group, cycloalkyl group.

Preferably, Q ⁺ is a cation selected from the group consisting of the structures (Q1), (Q2), (Q3), (Q4), (Q5) where R ^Q1 , R ^Q2 , R ^Q3 , R ^Q4 , R ^Q5 , R ^Q6 , R ^Q7 , R ^Q8 are each independently selected from the group consisting of alkyl group having 6 to 40, more preferably 10 to 30, carbon atoms, cycloalkyl group having 6 to 40, more preferably 10 to 30, carbon atoms, where R ^Q9 R ^Q10 R ^Q11 R ^Q12 R ^Q13 R ^Q14 R ^Q15 R ^Q16, R ^Q17 R ^{Q 18} R ^Q19 p ^Q20 R ^Q21 R ^Q22 R ^Q23 R ^Q24

R ^Q25 , R ^Q26 , R ^Q27 , R ^Q28 , R ^Q29 , R ^Q30 , R ^Q3 , R ^Q32 , R ^Q33 , R ^{Q34 Q35} are each independently selected from the group consisting of hydrogen, alkyl group having 1 to 25, preferably 1 to 10, carbon atoms, (poly)ether group having 1 to 25, preferably 1 to 10, carbon atoms.

More preferably, Q ⁺ is a cation selected from the group consisting of the structures (Q1), (Q3) where R ^Q1 , R ^Q2 , R ^Q3 , R ^Q4 are each independently selected from the group consisting of alkyl group having 6 to 30, preferably 10 to 25, carbon atoms, where R ^Q9 , R ^Q10 , R ^Q11 , R ^Q12 , R ^Q13 are each independently selected from the group consisting of hydrogen, alkyl group having 1 to 25, preferably 1 to 10, carbon atoms and R ^Q10 , R ^Q11 , R ^Q13 are more preferably each hydrogen and R ^Q9 , R ^Q12 are each independently an alkyl radical having 1 to 6 carbon atoms. Even more preferably, Q ⁺ is a cation of the structure (Q3) where R ^Q10 , R ^Q11 , R ^Q13 are each hydrogen and R ^Q9 is selected from the group consisting of methyl, ethyl, n-propyl, iso-propyl, n- butyl, sec-butyl, tert- butyl, and R ^Q12 is selected from the group consisting of methyl, ethyl, n-propyl, iso-propyl, n-butyl, sec-butyl, tert- butyl. Even more preferably, Q ⁺ is a cation of the structure (Q3) where R ^Q10 , R ^Q11 , R ^Q13 are each hydrogen and R ^Q9 is selected from the group consisting of methyl, ethyl, n-butyl, preferably selected from the group consisting of ethyl, n-butyl, where R ^Q9 is most preferably ethyl, and R ^Q12 is selected from the group consisting of methyl, ethyl, where R ^Q12 is most preferably methyl.

Particularly preferred as Q ⁺ is the 1-ethyl-3-methylimidazolium cation.

1.1.2.5.2 Preferred anion A- of IL ₁

In the aforementioned formula Q ⁺ A-, A- is an anion, especially selected from the group consisting of phosphate, phosphonate, alkylphosphonate, monoalkylphosphate, dialkylphosphate,

bis[trifluoromethanesulfonyl]imide, alkylsulfonate, haloalkylsulfonate, alkylsulfate, haloalkylsulfate, bis[fluorosulfonyl]imide, halide, dicyanamide, hexafluorophosphate, sulfate, tetrafluoroborate, trifluoromethanesulfonate, perchlorate, hydrogensulfate, haloalkylcarboxylate, alkylcarboxylate, formate, bisoxalatoborate, tetrachloroaluminate, dihydrogenphosphate,

monoalkylhydrogenphosphate, nitrate.

In the aforementioned formula Q ⁺ A-, A- is preferably selected from the group consisting of phosphate, phosphonate, alkylphosphonate, monoalkylphosphate, dialkylphosphate,

bis[trifluoromethanesulfonyl]imide, alkylsulfonate, alkylsulfate, bis[fluorosulfonyl]imide, halide, dicyanamide, hexafluorophosphate, sulfate, tetrafluoroborate, trifluoromethanesulfonate, perchlorate, hydrogensulfate, alkylcarboxylate, formate, bisoxalatoborate, tetrachloroaluminate, dihydrogenphosphate, monoalkylhydrogenphosphate, nitrate, where the alkyl groups in alkylphosphonate, monoalkylphosphate, dialkylphosphate, alkylsulfonate, alkylsulfate,

alkylcarboxylate, monoalkylhydrogenphosphate each have 1 to 10, preferably 1 to 6, more preferably 1 to 4, carbon atoms.

In the aforementioned formula Q ⁺ A-, A- is more preferably selected from the group consisting of dialkylphosphate, bis[trifluoromethanesulfonyl]imide, alkylsulfonate, bis[fluorosulfonyl]imide, chloride, dicyanamide, hexafluorophosphate, tetrafluoroborate, trifluoromethanesulfonate, perchlorate, acetate, propionate, formate, tetrachloroaluminate, monoalkylhydrogenphosphate, nitrate, where the alkyl groups in dialkylphosphate, alkylsulfonate, monoalkylhydrogenphosphate each have 1 to 10, preferably 1 to 6, more preferably 1 to 4, carbon atoms.

In the aforementioned formula Q ⁺ A-, A- is even more preferably selected from the group consisting of diethylphosphate, bis[trifluoromethanesulfonyl]imide, methanesulfonate, bis[fluorosulfonyl]imide, chloride, dicyanamide, hexafluorophosphate, tetrafluoroborate, trifluoromethanesulfonate, perchlorate, acetate, propionate, formate, tetrachloroaluminate, monoethylhydrogenphosphate, nitrate.

In the aforementioned formula Q ⁺ A-, A- is even more preferably selected from the group consisting of trifluoromethanesulfonate, bis[trifluoromethanesulfonyl]imide, diethylphosphate, dicyanamide, most preferably from the group consisting of trifluoromethanesulfonate,

bis[trifluoromethanesulfonyl]imide, and is at the very most preferably

bis[trifluoromethanesulfonyl]imide.

1.1.2.5.3 Amount of IL ₁ used

In the cases in which the mixture M ₁ comprises at least one ionic liquid IL ₁ , the amount of the ionic liquid IL ₁ included in the mixture M ₁ in step (a) of the process according to the invention in the first aspect of the invention is not subject to any further restriction.

In the cases in which the mixture M ₁ comprises at least one ionic liquid IL ₁ , however, it is preferable that the total molar amount of all ionic liquids IL ₁ included in the mixture M ₁ in step (a) of the process according to the invention, based on the total molar amount of all organic redox-active polymers P _redox1 included in the mixture M ₁ , is in the range from 0.1 % to 1000% by weight, more preferably in the range of 1 % to 500% by weight, yet more preferably in the range of 5% to 200% by weight, still more preferably in the range of 40 to 160% by weight, even more preferably in the range of 80% to 120% by weight, and is most preferably 100% by weight.

1.1.3 Applying the mixture M ₁ to the substrate S ₁

The mixture M ₁ can be applied to the substrate S ₁ by methods familiar to the person skilled in the art.

Bar coating, slot die coating, screen printing or stencil printing are familiar to the person skilled in the art and are preferably used for the purpose.

1.2 Step (b) of the process according to the invention

After step (a) of the process according to the invention, the solvent Solv ₁ is at least partly removed in step (b). The removal from the mixture M ₁ that has been applied to the substrate S ₁ is effected by methods known to the person skilled in the art, for example by drying under air, in the presence of inert gas (preferably nitrogen or argon) or under reduced pressure, in each case especially at elevated temperature.

On conclusion of step (b), an electrode E ₁ applied to the substrate S ₁ is obtained.

1.3 Step (cl of the process according to the invention

In step (c) of the process according to the invention, a polymer electrolyte P _el is applied to the electrode E ₁ obtained after step (b) of the process according to the invention.

1.3.1 Polymer electrolyte P _el

Such polymer electrolytes P _el are familiar to the person skilled in the art and are described, for example, in the prior art documents that follow.

W. Huang, Z. Zhu, L. Wang, S. Wang, H. Li, Z. Tao, J. Shi, L. Guan, J. Chen, Angew. Chem. Int.

Ed. 2013, 52, 9162-9166 describe a battery including a polymer electrolyte composed of poly(methacrylate) and polyethylene glycol.

J. Kim, A. Matic, J. Ahn, P. Jacobsson, C. Song, RSC Adv. 2012, 2, 10394-10399 describe an ionic liquid-based microporous polymer electrolyte hosted in poly(vinylidene fluoride-co- hexafluoropropylene) (PVdF-HFP).

Z. Zhu, M. Hong, D. Guo, J. Shi, Z. Tao, J. Chen, J. Am. Chem. Soc. 2014, 136, 16461-16464 describe a polymer electrolyte composed of poly(methacrylate) and polyethylene glycol in combination with S1O ₂ .

M. Lecuyer, J. Gaubicher, A. Barres, F. Dolhem, M. Deschamps, D. Guyomard, P. Poizot, Electrochem. Commun. 2015, 55, 22-25 and W. Li, L. Chen, Y. Sun, C. Wang, Y. Wang, Y. Xia, Solid State Ionics 2017, 300, 1 14-1 19 describe polyethylene oxide as polymer electrolyte in a lithium battery.

A corresponding use of a matrix composed of PVdF-HFP with poly(2, 2,6,6- tetramethylpiperidinyloxy methacrylate) (PTMA) as polymeric linear active material is described by J. Kim, A. Matic, J. Ahn, P. Jacobsson, RSC Adv. 2012, 2, 9795-9797.

Use of similar polymer electrolytes for increasing the safety of organolithium batteries is described by J. Kim, G. Cheruvally, J. Choi, J. Ahn, D. Choi, C. Eui Song, J. Electrochem. Soc. 2007, 154, A839-A843. More particularly, the polymer electrolyte P _el is obtained by polymerizing a mixture M _pel comprising at least one compound selected from compounds of the formula (I), and compounds of the formula

(II):

where R ^A , R ^M are independently selected from the group consisting of hydrogen, alkyl group, (poly)ether group, aryl group, aralkyl group, alkaryl group, haloalkyl group,

and wherein the mixture M _pel optionally comprises at least one ionic liquid IL ₃ .

Preferably, the polymerizing of the mixture M _pel is conducted on the electrode E ₁ or the mixture M _pel is polymerized and the polymer electrolyte P _el thus obtained is then applied to the electrode E ₁ by methods familiar to the person skilled in the art.

1.3.2 Polymerizing a mixture M _pel

By polymerizing the mixture M _pel comprising at least one compound selected from compounds of the formula (I), and compounds of the formula (II):

where R ^A , R ^M are independently selected from the group consisting of hydrogen, alkyl group,

(poly)ether group, aryl group, aralkyl group, alkaryl group, haloalkyl group,

and optionally at least one ionic liquid IL ₃ , the polymer electrolyte P _el is obtained.

R ^A , R ^M are independently selected from the group consisting of hydrogen, alkyl group, (poly)ether group, aryl group, aralkyl group, alkaryl group, fluoroalkyl group.

Preferably, R ^A , R ^M are independently selected from hydrogen, alkyl group, polyether group, alkaryl group, even more preferably from hydrogen, benzyl, -(CH ₂ CH ₂ 0) _V R ^V , even more preferably independently from benzyl, -(CH ₂ CH ₂ 0) _V R ^V , where v is an integer ³ 3 and v is especially an integer in the range of 3 to 50, more preferably in the range of 5 to 15, even more preferably in the range of 8 to 9; and R ^v is selected from the group consisting of hydrogen, alkyl group, which is preferably methyl.

This involves polymerizing the compounds of the formula (I) and/or (II) with one another, while any IL ₃ included in the mixture M _pel does not take part in the polymerization reaction but, when it is used in the mixture M _pel , is incorporated in the polymer electrolyte P _el obtained.

The compound of the formula (I) is an acrylate-based compound (“acrylate compound”). The compound of the formula (II) is a methacrylate-based compound (“methacrylate compound”).

Processes for polymerizing these and corresponding monomers are known to those skilled in the art and are described, for example, in K.-H. Choi, J. Yoo, C. K. Lee, S.-Y. Lee, Energy Environ. Sci. 2016, 9, 2812-2821. For example, the production of the polymer electrolyte P _el takes place in a one-stage process via a polymerization, optionally in the presence of the ionic liquid IL ₃ .

It is preferable that the mixture M _pel comprises a mixture of compounds of formula (I) and compounds of the formula (II). In that case, in particular, the molar ratio of all compounds of formula (I) included in the mixture M _pel to all compounds of the formula (II) included in the mixture M _pel is in the range of 99:1 to 1 :99, preferably in the range of 49:1 to 1 :19, more preferably in the range of 97:3 to 1 :9, even more preferably in the range of 24:1 to 1 :4, still more preferably in the range of 49:1 to 1 :3, yet more preferably still in the range of 49:1 to 1 :1 , and most preferably in the range of 9:1 to 4:1 , where the ratio of 9:1 is the very most preferred.

This is because it has been found that, surprisingly, organic batteries comprising a polymer electrolyte P _el that has been prepared from a mixture M _pel comprising compounds of formula (I) and compounds of the formula (II) have high capacities.

For production of the polymer electrolyte P _el , for example as electrolyte film, the mixture M _pel is first mixed as a paste from all components present and especially applied to the electrode E ₁ . After initiation of the polymerization, the mechanically stable and elastic electrolyte film is then formed.

The properties of the paste, in particular the viscosity, can be further optimized here in order to make it employable for printing processes, for example stencil printing or screen printing. The method described enables performance of the polymerization even in the presence of all components of the electrolyte film, and so no subsequent swelling with electrolyte liquid or other downstream processes such as evaporating of a solvent are required. After performance of step (c) of the process according to the invention, a polymer electrolyte P _el is accordingly obtained on the electrode E ₁ .

1.4 Step (d) of the process according to the invention

In step d) of the process according to the invention, a mixture M ₂ comprising at least one organic redox-active polymer P _redox2 , at least one conductivity additive L ₂ , at least one solvent Solv ₂ , optionally at least one binder additive B and optionally at least one ionic liquid IL is applied to the polymer electrolyte Pei.

1.4.1 Mixture M _?

The mixture M ₂ used in step (d) of the process according to the invention comprises at least one organic redox-active polymer P _redox2 , at least one conductivity additive L ₂ , at least one solvent Solv ₂ , optionally at least one binder additive B2 and optionally at least one ionic liquid IL ₂ .

The mixture M is especially an electrode slurry, especially a solution or suspension, with which the constituents of the electrode E ₂ obtained at a later stage are applied to the polymer electrolyte P _el .

1.4.2 Organic redox-active polymer

The polymers usable as organic redox-active polymer P _redox that are included in the mixture M are known to those skilled in the art and are described, for example, in US 2016/0233509 A1 , US 2017/01 14162 A1 , US 2017/0179525 A1 , US 2018/0108911 A1 , US 2018/0102541 A1 , WO

2017/207325 A1 , WO 2015/032951 A1. An overview of further usable organic redox-active polymers is given by the article S. Muench, A. Wild, C. Friebe, B. Haupler, T. Janoschka, U.S. Schubert, Chem. Rev. 2016, 116, 9438-9484. The polymers P _redox can be prepared by the methods described under point 1.1.2.1.

The organic redox-active polymer P _redox is preferably selected from the group consisting of polyimides and polymers comprising m units of the general formula (III): where m is an integer ³ 4, preferably an integer ³ 10, more preferably an integer ³ 100, even more preferably an integer in the range of 1000 to 10 ⁹ , yet more preferably an integer in the range of 2000 to 10 000, W is a repeat unit, Sp is an organic spacer and R ^x is an organic redox-active group, where the bond identified by (i) in a unit of the formula (III) binds to the bond identified by (ii) in the adjacent unit of the formula (III).

R ^x in the structure (III) is preferably selected from the group consisting of compounds of the general formulae (lll-A), (lll-B), (lll-C), (lll-D), (lll-E), (lll-F) where

and where, in the structures (lll-A), (lll-B) and (lll-C), at least one aromatic carbon atom may be substituted by a group selected from alkyl group, halogen group, alkoxy group, hydroxyl group. Even more preferably, R ^x in the structure (III) is selected from the group consisting of compounds of the general formulae (lll-A), (lll-B), (lll-C), (lll-D), with (lll-B), (lll-C) being more preferred and (lll-B) being the very most preferred. W in the structure (III) is a repeat unit, and the person skilled in the art is able to select this using his knowledge in the art. The spacer units Sp are connecting units between the redox-active units and the repeat units W that may especially likewise be selected by the person skilled in the art in a routine manner drawing on knowledge in the art.

Preferably, the W radical in the structure (III) is selected from the group consisting of the structures

(W1), (W2), (W3):

where the bond identified by (i) in a unit of the formula (W1), (W2), (W3) binds in each case to the bond identified by (ii) in the adjacent unit of the formula (W1), (W2) or (W3), where the bond identified by (iii) in each case identifies the bond to Sp, and where R ^W1 , R ^W2 , R ^W3 , R ^W4 , R ^W5 , R ^W6 , R ^W7 are independently selected from the group consisting of hydrogen, alkyl group, haloalkyl group, -COOR ^W8 with R ^W8 = H or alkyl, R ^W1 , R ^W2 , R ^W3 , R ^W4 , R ^W5 , R ^W6 , R ^W7 are preferably independently selected from the group consisting of hydrogen, methyl, -COOH, -COOCH ₃ , and where, even more preferably, the W radical in the structure (III) has the structure (W1) in which one of R ^W1 , R ^W2 , R ^W3 is methyl and the other two are hydrogen or all of R ^W1 , R ^W2 , R ^W3 are hydrogen; and the Sp radical in the structure (III) is selected from the group consisting of direct bond, (Sp1), (Sp2):

where pA1 , pA2, pA3 are each 0 or 1 , excluding the case that“pA2 = 0, pA1 = pA3 = 1”, where qA1 , qA2, qA3 are each 0 or 1 , excluding the case that“qA2 = 0, qA1 = qA3 = 1”, where qA4, qA5, qA6 are each 0 or 1 , where at least one of qA4, qA5, qA6 = 1 and where the case that“qA5 = 0, qA4 = qA6 = 1” is excluded, where B ^Sp is selected from the group consisting of

divalent (hetero)aromatic radical, preferably phenyl,

divalent aliphatic radical, which is preferably alkylene, optionally substituted by at least one group selected from nitro group, -NH ₂ , -CN, -SH, -OH, halogen and optionally having at least one group selected from ether, thioether, amino ether, carbonyl group, carboxylic ester, carboxamide group, sulfonic ester, phosphoric ester, and where in the cases in which Sp binds to a non-carbon atom in the R ^x radical, the structure (Sp1) is subject to the additional condition“qA3 = 0, qA2 = 1 , qA1 = 1 or qA3 = qA2 = qA1 = 0 or qA3 = 0, qA2 = 1 , qA1 = 0”, preferably the condition“qA3 = qA2 = qA1 = 0”, and the structure (Sp2) to the additional condition“qA6 = 0, qA5 = 1 , qA4 = 1 or qA6 = 0, qA5 = 1 , qA4 = 0”, and where denotes the bond pointing toward R ^x ,

and where denotes the bond pointing toward W.

It is pointed out that the condition“where at least one of qA4, qA5, qA6 = 1”, in respect of Sp2, relates solely to the definition of the respective variables qA4, qA5, qA6 and does not mean that the Sp radical in the structure (III) cannot also be a direct bond. More preferably, the Sp radical is selected from the group consisting of direct bond, (Sp2) with more preferably from the group consisting of direct bond, denotes the bond pointing toward R ^x , and where denotes the bond pointing toward W. If the polymer P _redox2 is a polyimide, it is preferably selected from the group consisting of the structures (IV-1), (IV-2), (IV-3), (IV-4), (IV-5), (IV-6), (IV-7), (IV-8), (IV-9):

where n is an integer ³ 4, preferably an integer ³ 10, more preferably an integer ³ 100, even more preferably an integer in the range of 1000 to 10 ⁹ , yet more preferably an integer in the range of 2000 to 10 000,

and the bond identified by (iv) in the structures (IV-1), (IV-2), (IV-3), (IV-4), (IV-5), (IV-6), (IV-7), (IV- 8), (IV-9) binds in each case to the bond identified by (v), and where Ar ^I , Ar ^II are each independently a hydrocarbyl group having at least one aryl radical and especially having 6 to 30, preferably 6 to 15, more preferably 6 to 13, carbon atoms. and where in the structures (IV-1), (IV-2), (IV-3), (IV-4), (IV-5), (IV-6), (IV-7), (IV-8), (IV-9), at least one aromatic carbon atom may be substituted by a group selected from alkyl, halogen, alkoxy, OH, preferably halogen, OH,

If the polymer P _redox2 is a polyimide, this is more preferably selected from the group consisting of the structures (IV-1), (IV-2), (IV-3), (IV-4), (IV-5), (IV-6), (IV-7), (IV-8), (IV-9), where n is an integer ³ 4, preferably an integer ³ 10, more preferably an integer ³ 100, even more preferably an integer in the range of 1000 to 10 ⁹ , yet more preferably an integer in the range of 2000 to 10 000, and the bond identified by (iv) in the structures (IV-1), (IV-2), (IV-3), (IV-4), (IV-5), (IV-6), (IV-7), (IV-8), (IV-

9) binds in each case to the bond identified by (v), and where Ar ^I , Ar ^II are each independently a hydrocarbyl group having at least one aryl radical and especially having 6 to 30, preferably 6 to 15, more preferably 6 to 13, carbon atoms.

More preferably, the polymer P _redox2 comprises t repeat units joined to one another, selected from the group consisting of the structures P1 , P2, P3, P4, P5, P6:

P4 P5 P6 where t is an integer ³ 4, preferably an integer ³ 10, more preferably an integer ³ 100, even more preferably an integer in the range of 1000 to 10 ⁹ , yet more preferably an integer in the range of 2000 to 10 000, where R ^P5 , R ^P6 are each independently selected from the group consisting of hydrogen, methyl, and are especially each hydrogen, and the bond identified by (vi) in a unit of the formula P1 binds to the bond identified by (vii) in the adjacent unit of the formula P1 ,

and the bond identified by (viii) in a unit of the formula P2 binds to the bond identified by (ix) in the adjacent unit of the formula P2, and the bond identified by (x) in a unit of the formula P3 binds to the bond identified by (xi) in the adjacent unit of the formula P3,

and the bond identified by (xii) in a unit of the formula P4 binds to the bond identified by (xiii) in the adjacent unit of the formula P4,

and the bond identified by (xiv) in a unit of the formula P5 binds to the bond identified by (xv) in the adjacent unit of the formula P5,

and the bond identified by (xvi) in a unit of the formula P6 binds to the bond identified by (xvii) in the adjacent unit of the formula P6.

The end groups of the first repeat unit of the polymer P _redox2 which is present for these on the bonds defined by "(i)" in the chemical structure (III), and is present for these on the bonds defined by "(vi)" in the chemical structure P1 , and is present for these on the bonds defined by "(viii)" in the chemical structure P2, and is present for these on the bonds defined by "(x)" in the chemical structure P3, and is present for these on the bonds defined by "(xii)" in the chemical structure P4, and is present for these on the bonds defined by "(xiv)" in the chemical structure P5, and is present for these on the bonds defined by "(xvi)" in the chemical structure P6, and is present for these on the bonds defined in each case by "(iv)" in the chemical structures (IV-1), (IV-2), (IV-3), (IV-4), (IV- 5), (IV-6), (IV-7), (IV-8), (IV-9), and the end groups of the last repeat unit of the polymer P _redox2 according to the invention which is present for these on the bonds defined by "(ii)” in the chemical structure (III), and is present for these on the bonds defined by "(vii)" in the chemical structure P1 , and is present for these on the bonds defined by "(ix)" in the chemical structure P2, and is present for these on the bonds defined by "(xi)" in the chemical structure P3, and is present for these on the bonds defined by "(xiii)" in the chemical structure P4, and is present for these on the bonds defined by "(xv)" in the chemical structure P5, and is present for these on the bonds defined by "(xvii)" in the chemical structure P6, and is present for these on the bonds defined in each case by "(v)" in the chemical structures (IV- 1), (IV-2), (IV-3), (IV-4), (IV-5), (IV-6), (IV-7), (IV-8), (IV-9), are not particularly restricted and are apparent from the polymerization method used in the preparation method for the polymer P _redox2 · Thus, they may be termination fragments of an initiator or of a repeat unit. Preferably, these end groups are selected from hydrogen, halogen, hydroxyl, unsubstituted aliphatic radical or aliphatic radical substituted by -CN, -OH, halogen (which may especially be an unsubstituted or correspondingly substituted alkyl group), (hetero)aromatic radical, which is preferably a phenyl radical, benzyl radical or a-hydroxybenzyl. 1.4.3 Conductivity additive L ₂

1.4.3.1 Preferred conductivity additive L ₂

The at least one conductivity additive L ₂ which is included in the mixture M ₂ which is used in step (d) of the process according to the first aspect of the invention is at least one electrically conductive material, especially selected from the group consisting of carbon materials, electrically conductive polymers, metals, semimetals, (semi)metal compounds, preferably selected from carbon materials, electrically conductive polymers.

According to the invention,“(semi)metals” are selected from the group consisting of metals, semimetals, and are preferably metals.

Metals are especially selected from the group consisting of zinc, iron, copper, silver, gold, chromium, nickel, tin, indium.

Semimetals are especially selected from silicon, germanium, gallium, arsenic, antimony, selenium, tellurium, polonium.

The conductivity additive L ₂ is more preferably a carbon material. Carbon materials are especially selected from the group consisting of carbon fibres, carbon nanotubes, graphite, graphene, carbon black, fullerene.

Electrically conductive polymers are especially selected from the group consisting of polypyrroles, polyanilines, polyphenylenes, polypyrenes, polyazulenes, polynaphthylenes, polycarbazoles, polyindoles, polyazepines, polyphenylene sulfides, polythiophenes, polyacetylenes, poly(3,4- ethylenedioxythiophene) polystyrenesulfonate (= PEDOT:PSS), polyarcenes, poly-(p- phenylenevinylenes). 1.4.3.2 Preferred amount of the conductivity additive L ₂

The amount of the conductivity additive L ₂ included in the mixture M ₂ in step (d) of the process according to the first aspect of the invention is not subject to any further restriction. However, it is preferable that the total weight of all conductivity additives L ₂ included in the mixture M ₂ , based on the total weight of the redox polymers P _redox2 included in the mixture M ₂ , is in the range of 0.1 % to 1000% by weight, preferably in the range of 10% to 500% by weight, more preferably in the range of 30% to 100% by weight, yet more preferably in the range of 40% to 80% by weight, even more preferably in the range of 50% by weight to 60% by weight, most preferably 58.3% by weight. 1.4.4 Solvent Solv ₂

The at least one solvent Solv ₂ included in the mixture M ₂ is especially a solvent having a high boiling point, preferably selected from the group consisting of N-methyl-2-pyrrolidone, water, dimethyl sulfoxide, ethylene carbonate, propylene carbonate, dimethyl carbonate, methyl ethyl carbonate, y-butyrolactone, tetrahydrofuran, dioxolane, sulfolane, N./V-dimethylformamide, N,N'- dimethylacetamide, more preferably dimethyl sulfoxide or water, even more preferably water.

More particularly, the mixture M ₂ comprises a sufficient amount of solvent Solv ₂ that the concentration of the organic redox-active polymer P _redox2 in the mixture M ₂ is between 1 and 100 mg/ml, preferably between 5 and 50 mg/ml.

1.4.5 Binder additive B ₂

More particularly, the mixture M ₂ also comprises at least one binder additive B ₂ .

Binder additives B2 are familiar to the person skilled in the art as materials having binding properties. Preference is given to polymers selected from the group consisting of PVdF-HFP, polytetrafluoroethylene, polyvinylidene fluoride, polyhexafluoropropylene, polyvinyl chloride, polycarbonate, polystyrene, polyacrylate, polymethacrylate, polysulfone, cellulose derivatives, polyurethane, and the binder additive more preferably comprises cellulose derivatives, e.g. sodium carboxymethylcellulose or PVdF-HFP or polyvinylidene fluoride.

In the cases in which the mixture M ₂ comprises at least one binder additive B2, the amount of all binder additives B2 included in the mixture M ₂ in step (d) of the process according to the invention in the first aspect of the invention is not subject to any further restriction.

The amount of all binder additives B2 used, in the cases in which the mixture M ₂ comprises one, is not particularly restricted. However, it is preferable in these cases that the total weight of all binder additives B2 included in the mixture M ₂ , based on the total weight of the redox polymer P _redox2 included in the mixture M ₂ , is in the range of 0.001 % to 100% by weight, more preferably in the range of 0.1 % to 90% by weight, yet more preferably in the range of 3% to 70% by weight, still more preferably in the range of 5% to 50% by weight, even more preferably in the range of 7.5% by weight to 20% by weight, and is most preferably 16.6% by weight. 1.4.6 Ionic liquid IL ₂

More particularly, the mixture M ₂ also comprises at least one ionic liquid IL ₂ . The at least one ionic liquid IL2 included in the mixture M ₂ is not particularly restricted and is described, for example, in WO 2004/016631 A1 , WO 2006/134015 A1 , US 201 1/0247494 A1 or US 2008/0251759 A1 .

More particularly, the at least one ionic liquid IL2 included in the mixture M ₂ in step (d) of the process according to the invention has the structure Q ⁺ A-.

1.4.6.1 Preferred cation Q ⁺ of IL ₂

Q ⁺ therein is a cation selected from the group consisting of the following structures (Q1), (Q2), (Q3), (Q4), (Q5):

where R ^Q1 , R ^Q2 , R ^Q3 , R ^Q4 , R ^Q5 , R ^Q6 , R ^Q7 , R ^Q8 are each independently selected from the group consisting of alkyl group, haloalkyl group, cycloalkyl group, where R ^Q9 RQ ¹⁰ R ^Q11 R ^Q12 R ^Q13 R ^Q14 R ^Q15 R ^Q16 R ^Q17 R ^Q18 R ^Q19 R ^Q20 R ^Q21 R ^Q22 R ^Q23 R ^Q24

R ^Q25 , R ^Q26 , R ^Q27 , R ^Q28 , R ^Q29 , R ^Q30 , R ^Q31 , R ^Q32 , R ^Q33 , R ^{Q3 4 35} are each independently selected from the group consisting of hydrogen, alkyl group, (poly)ether group, haloalkyl group, cycloalkyl group.

Preferably, Q ⁺ is a cation selected from the group consisting of the structures (Q1), (Q2), (Q3), (Q4), (Q5) where R ^Q1 , R ^Q2 , R ^Q3 , R ^Q4 , R ^Q5 , R ^Q6 , R ^Q7 , R ^Q8 are each independently selected from the group consisting of alkyl group having 6 to 40, more preferably 10 to 30, carbon atoms, cycloalkyl group having 6 to 40, more preferably 10 to 30, carbon atoms, where R ^Q9 R ^Q10 R ^Q11 R ^Q12 R ^Q13 R ^Q14 R ^Q15 R ^Q16 R ^Q17 R ^Q18 R ^Q19 R ^Q20 R ^Q21 R ^Q22 R ^Q23 R ^Q24

R ^Q25 , R ^Q26 , R ^Q27 , R ^Q28 , R ^Q29 , R ^Q30 , R ^Q31 , R ^Q32 , R ^Q33 , R ^{Q3 4 35} are each independently selected from the group consisting of hydrogen, alkyl group having 1 to 25, preferably 1 to 10, carbon atoms, (poly)ether group having 1 to 25, preferably 1 to 10, carbon atoms.

More preferably, Q ⁺ is a cation selected from the group consisting of the structures (Q1), (Q3) where R ^Q1 , R ^Q2 , R ^Q3 , R ^Q4 are each independently selected from the group consisting of alkyl group having 6 to 30, preferably 10 to 25, carbon atoms, where R ^Q9 , R ^Q10 , R ^Q11 , R ^Q12 , R ^Q13 are each independently selected from the group consisting of hydrogen, alkyl group having 1 to 25, preferably 1 to 10, carbon atoms and R ^Q10 , R ^Q11 , R ^Q13 are more preferably each hydrogen and R ^Q9 , R ^Q12 are each independently an alkyl radical having 1 to 6 carbon atoms.

Even more preferably, Q ⁺ is a cation of the structure (Q3) where R ^Q10 , R ^Q11 , R ^Q13 are each hydrogen and R ^Q9 is selected from the group consisting of methyl, ethyl, n-propyl, iso-propyl, n- butyl, sec-butyl, tert- butyl, and R ^Q12 is selected from the group consisting of methyl, ethyl, n-propyl, iso-propyl, n-butyl, sec-butyl, tert- butyl.

Even more preferably, Q ⁺ is a cation of the structure (Q3) where R ^Q10 , R ^Q11 , R ^Q13 are each hydrogen and R ^Q9 is selected from the group consisting of methyl, ethyl, n-butyl, preferably selected from the group consisting of ethyl, n-butyl, where R ^Q9 is most preferably ethyl, and R ^Q12 is selected from the group consisting of methyl, ethyl, where R ^Q12 is most preferably methyl.

Particularly preferred as Q ⁺ is the 1-ethyl-3-methylimidazolium cation.

1.4.6.2 Preferred anion A- of IL ₂

In the aforementioned formula Q ⁺ A-, A- is an anion, especially selected from the group consisting of phosphate, phosphonate, alkylphosphonate, monoalkylphosphate, dialkylphosphate,

bis[trifluoromethanesulfonyl]imide, alkylsulfonate, haloalkylsulfonate, alkylsulfate, haloalkylsulfate, bis[fluorosulfonyl]imide, halide, dicyanamide, hexafluorophosphate, sulfate, tetrafluoroborate, trifluoromethanesulfonate, perchlorate, hydrogensulfate, haloalkylcarboxylate, alkylcarboxylate, formate, bisoxalatoborate, tetrachloroaluminate, dihydrogenphosphate,

monoalkylhydrogenphosphate, nitrate. In the aforementioned formula Q ⁺ A-, A- is preferably selected from the group consisting of phosphate, phosphonate, alkylphosphonate, monoalkylphosphate, dialkylphosphate,

bis[trifluoromethanesulfonyl]imide, alkylsulfonate, alkylsulfate, bis[fluorosulfonyl]imide, halide, dicyanamide, hexafluorophosphate, sulfate, tetrafluoroborate, trifluoromethanesulfonate, perchlorate, hydrogensulfate, alkylcarboxylate, formate, bisoxalatoborate, tetrachloroaluminate, dihydrogenphosphate, monoalkylhydrogenphosphate, nitrate, where the alkyl groups in alkylphosphonate, monoalkylphosphate, dialkylphosphate, alkylsulfonate, alkylsulfate, alkylcarboxylate, monoalkylhydrogenphosphate each have 1 to 10, preferably 1 to 6, more preferably 1 to 4, carbon atoms.

In the aforementioned formula Q ⁺ A-, A- is more preferably selected from the group consisting of dialkylphosphate, bis[trifluoromethanesulfonyl]imide, alkylsulfonate, bis[fluorosulfonyl]imide, chloride, dicyanamide, hexafluorophosphate, tetrafluoroborate, trifluoromethanesulfonate, perchlorate, acetate, propionate, formate, tetrachloroaluminate, monoalkylhydrogenphosphate, nitrate, where the alkyl groups in dialkylphosphate, alkylsulfonate, monoalkylhydrogenphosphate each have 1 to 10, preferably 1 to 6, more preferably 1 to 4, carbon atoms.

In the aforementioned formula Q ⁺ A-, A- is even more preferably selected from the group consisting of diethylphosphate, bis[trifluoromethanesulfonyl]imide, methanesulfonate, bis[fluorosulfonyl]imide, chloride, dicyanamide, hexafluorophosphate, tetrafluoroborate, trifluoromethanesulfonate, perchlorate, acetate, propionate, formate, tetrachloroaluminate, monoethylhydrogenphosphate, nitrate.

In the aforementioned formula Q ⁺ A-, A- is even more preferably selected from the group consisting of trifluoromethanesulfonate, bis[trifluoromethanesulfonyl]imide, diethylphosphate, dicyanamide, most preferably from the group consisting of trifluoromethanesulfonate,

bis[trifluoromethanesulfonyl]imide, and is at the very most preferably

bis[trifluoromethanesulfonyl]imide.

1.4.6.3 Amount of IL ₂ used

In the cases in which the mixture M ₂ comprises at least one ionic liquid IL ₂ , the amount of the ionic liquid IL included in the mixture M ₂ in step (d) of the process according to the invention in the first aspect of the invention is not subject to any further restriction.

In the cases in which the mixture M ₂ comprises at least one ionic liquid IL ₂ , however, it is preferable that the total molar amount of all ionic liquids IL included in the mixture M in step (d) of the process according to the invention, based on the total molar amount of all organic redox-active polymers P _redox included in the mixture M , is in the range from 0.1 % to 1000% by weight, more preferably in the range of 1 % to 500% by weight, yet more preferably in the range of 5% to 200% by weight, still more preferably in the range of 40 to 160% by weight, even more preferably in the range of 80% to 120% by weight, and is most preferably 100% by weight. 1.4.6.4 Applying the mixture M ₂ to the polymer electrolyte P _el

The mixture M ₂ can be applied to the polymer electrolyte P _el by methods familiar to the person skilled in the art.

Bar coating, slot die coating, screen printing or stencil printing are familiar to the person skilled in the art and are preferably used for the purpose.

1.5 Step (el of the process according to the invention

After step (d) of the process according to the invention, the solvent Solv ₂ is at least partly removed in step (e). The removal from the mixture M ₂ that has been applied to the polymer electrolyte P _el is effected by methods known to the person skilled in the art, for example by drying under air, in the presence of inert gas (preferably nitrogen or argon) or under reduced pressure, in each case especially at elevated temperature.

On conclusion of step (e), an electrode E ₂ applied to the polymer electrolyte P _el is obtained.

1.6 Step (f) of the process according to the invention

In step (f) of the process according to the invention, a second substrate S2 is then applied to the electrode E ₂ . This can be accomplished by methods familiar to the person skilled in the art. The substrate S2 is especially selected from conductive materials, preferably from the group consisting of metals, carbon materials, oxide substances. These conductive materials may form the substrate S2 on their own or, as is preferred in the present invention, may have been applied to nonconductive materials such as, in particular, a material selected from the group consisting of plastics, which are especially PET or polyurethane, textiles, cellulose, especially paper, wood. Useful substrates S2 include cellulose fibres coated with carbon nanotubes (CNTs) (production described in WO 2015/100414, paragraphs [0104], [0105]).

Further preferred substrates S2 are metal foils.

Metals that are preferentially suitable as substrate S2 and may also be used in the form of nanoparticles or foils are selected from silver, platinum, gold, iron, copper, aluminium, zinc or a combination of these metals. Preferred carbon materials suitable as substrate are selected from carbon black, glassy carbon, graphite foil, graphene, carbon skins, carbon nanotubes (CNTs). Preferred oxide substances suitable as substrate for the electrode element are, for example, selected from the group consisting of indium tin oxide (ITO), indium zinc oxide (IZO), antimony zinc oxide (AZO), fluorine tin oxide (FTO) or antimony tin oxide (ATO), zinc oxide (ZO). Substrates S2 used may also be mixtures of the groups mentioned, for example of metals and carbon materials, for example silver with carbon.

The form of the substrate S2 in step (f) is not subject to further restriction. However, it is preferable when the substrate S ₁ in step (a) of the process is planar; the substrate S2 is also planar at least in the region in which the mixture M ₁ has been applied in step (b). This means that the surface of the substrate S2 which is applied to the electrode E ₂ in step (f) of the process according to the invention in the first aspect of the invention is in a plane.

The substrate S2 may overlap the electrode E ₂ or cover the same area as E ₂ .

On conclusion of step (f), a distinction is possible between two sides of the substrate S ₁ : One side is that on which layers E1/P _el /E ₂ /S2 are present. This is abbreviated hereinafter as side“S _L ”. The other side is that on which layers E1/P _el /E ₂ /S2 are not present. This is abbreviated hereinafter as side“SN”.

1.7 Characterizing step (g) of the process according to the invention

In the characterizing step (g) of the process according to the invention, the substrate S ₁ is shaped in the region of the substrate S ₁ covered by E ₁ . As a result, the charge storage unit L _org produced in steps (a) to (f) is then likewise shaped in the region of the substrate S ₁ covered by the electrode E ₁ and hence a shaped organic charge storage unit L _org is obtained.

For this purpose, it is possible to use all processes known to those skilled in the art. These depend particularly on the type of use of the shaped charge storage unit L _org obtained after performance of the process according to the invention.

Especially in the preferred embodiment of the process according to the invention in which the substrate S ₁ in step (a) is planar, the shaping is conducted in such a way that at least one edge K, a concave surface O _A , or a convex surface O _x , preferably at least one edge K forms in the region of the substrate S ₁ covered by the electrode E ₁ . It will be apparent that, in the case of formation of an edge K, a concave surface O _A or a convex surface O _x in the region of the substrate S ₁ covered by the electrode E ₁ , the charge storage unit L _org is also shaped.

According to the invention, an“edge K in the region of the substrate S ₁ covered by the electrode E ₁ ” is understood to mean the line of intersection of two planar, mutually adjoining and non-parallel surfaces O ₁ and O ₂ of the substrate S ₁ . Surfaces O ₁ and O ₂ are surfaces of the side S _L of the substrate S ₁ . The angle a at which the two at least partly planar surfaces O ₁ and O ₂ of the side S _L of the substrate S ₁ intersect is not subject to any further restriction. The angle a may be selected from acute angles, right angles, oblique angles, reflex angles, particular preference being given to acute angles, right angles and oblique angles, and very particular preference to acute angles and right angles.

Acute angles are ³ 0° but < 90°, preferably > 0° but < 90°, more preferably in the range of 45° to 60°. One embodiment of the charge storage unit L _org according to the invention in which there is an edge having an angle of 0° is shown, for example, in Figure 1 D.

A right angle is an angle of 90°.

An oblique angle is > 90° but < 180°, preferably in the range of 135° to 150°.

Edges having right and acute angles are shown, for example, in Figure 2.

A reflex angle is > 180° but < 360°, preferably 270°.

An edge in the context of the invention may be a sharp edge or else a rounded edge, as shown, for example, in Figure 3. In the latter cases, the angle a can then be determined by extending the respective surfaces Oi and O ₂ of the substrate S ₁ (shown in Figure 3 by dotted lines).

What is meant in accordance with the invention by a "concave surface O _A " and a "convex surface O _x " is that no region of the substrate S ₁ covered by the electrode E ₁ is planar; instead, the part of the substrate S ₁ covered by the electrode E ₁ is completely curved. The curvature here in the case of a concave surface O _A is such that the side S _N of the substrate S ₁ is curved outward.

The curvature here in the case of a convex surface O _x is such that the side S _L of the substrate S ₁ is curved outward.

A combination of concave and convex curvatures ("wavy shape") is also possible.

2. Second aspect: Charge storage unit according to the invention

The present invention relates, in a second aspect, to a shaped organic charge storage unit L _org comprising: a) a substrate S ₁ ; b) an electrode E ₁ applied to the substrate S ₁ and comprising at least one organic redox-active polymer P _redox1 , at least one conductivity additive L ₁ , optionally at least one solvent Solv ₁ , optionally at least one binder additive B ₁ and optionally at least one ionic liquid IL1; c) a polymer electrolyte P _el applied to the electrode E ₁ ; d) an electrode E ₂ applied to the polymer electrolyte P _el and comprising at least one organic redox- active polymer P _redox2 , at least one conductivity additive L ₂ , optionally at least one solvent Solv ₂ , optionally at least one binder additive B and optionally at least one ionic liquid IL ; e) a substrate S ₂ applied to the electrode E ₂ ; characterized in that the substrate S ₁ is at least partly nonplanar in the region of the substrate S ₁ covered by the electrode E ₁ .

The charge storage unit L _org as per the second aspect of the invention can be produced by the process according to the invention as per the first aspect of the invention.

2.1 Substrates S ₁ , S ₂

The two substrates S ₁ and S ₂ of the charge storage unit L _org according to the invention in the second aspect of the invention are each independently selected from conductive materials, preferably from the group consisting of metals, carbon materials, oxide substances. These conductive materials may form the substrate S ₁ or S ₂ on their own or, as is preferred in the present invention, may have been applied to nonconductive materials such as, in particular, a material selected from the group consisting of plastics (PET, polyurethane), textiles, cellulose, especially paper, wood. Useful substrates S ₁ and/or S ₂ include cellulose fibres coated with carbon nanotubes (CNTs) (production described in WO 2015/100414, paragraphs [0104], [0105]).

Further preferred substrates S ₁ and/or S ₂ are metal foils.

Metals suitable with preference as substrate S ₁ and/or S ₂ are selected from silver, platinum, gold, iron, copper, aluminium, zinc or a combination of these metals. Preferred carbon materials suitable as substrate S ₁ and/or S ₂ are selected from carbon black, glassy carbon, graphite foil, graphene, carbon skins, carbon nanotubes (CNTs). Preferred oxide substances suitable as substrate for the electrode element are, for example, selected from the group consisting of indium tin oxide (ITO), indium zinc oxide (IZO), antimony zinc oxide (AZO), fluorine tin oxide (FTO) or antimony tin oxide (ATO), zinc oxide (ZO). Substrates S ₁ and/or S ₂ used may also be mixtures of the groups mentioned, for example mixtures of metals and carbon materials, for example silver with carbon.

2.2 Electrodes E ₁ , E ₂

The electrode E ₁ of the charge storage unit L _org according to the invention in the second aspect of the invention comprises at least one organic redox-active polymer P _redox1 , at least one conductivity additive L ₁ , optionally at least one solvent Solv ₁ , optionally at least one binder additive B ₁ and optionally at least one ionic liquid IL ₁ .

The organic redox-active polymer P _redox1 in the charge storage unit L _org according to the invention in the second aspect of the invention is as defined under point 1.1.2.1.

The conductivity additive L ₁ in the charge storage unit L _org according to the invention in the second aspect of the invention is as defined under point 1.1.2.2.1. The amount of the conductivity additive L ₁ included in the electrode E ₁ in the charge storage unit L _org according to the invention in the second aspect of the invention is not subject to any further restriction. However, it is preferable that the total weight of all conductivity additives L ₁ included in the electrode E ₁ , based on the total weight of the redox polymers P _redox1 included in the electrode E ₁ , is in the range of 0.1 % to 1000% by weight, preferably in the range of 10% to 500% by weight, more preferably in the range of 30% to 100% by weight, yet more preferably in the range of 40% to 80% by weight, even more preferably in the range of 50% by weight to 60% by weight, most preferably 58.3% by weight.

The electrode E ₁ in the charge storage unit L _org according to the invention in the second aspect of the invention optionally also comprises at least one solvent Solv ₁ . This is especially as defined in point 1.1.2.3. However, it is preferable that the electrode E ₁ in the charge storage unit L _org according to the invention in the second aspect of the invention comprises less than 1 % by weight, especially less than 0.1 % by weight, of a solvent Solv ₁ .

The electrode E ₁ in the charge storage unit L _org according to the invention in the second aspect of the invention optionally also comprises at least one ionic liquid IL ₁ . This is especially as defined in points 1.1.2.5.1 , 1.1.2.5.2.

In the cases in which the electrode E ₁ in the charge storage unit L _org according to the invention in the second aspect of the invention comprises at least one ionic liquid IL ₁ , the amount of the ionic liquid IL ₁ included in the electrode E ₁ in the charge storage unit L _org according to the invention in the second aspect of the invention is not subject to any further restriction.

In the cases in which the electrode E ₁ in the charge storage unit L _org according to the invention in the second aspect of the invention comprises at least one ionic liquid IL ₁ , however, it is preferable that the total molar amount of all ionic liquids IL ₁ included in the electrode E ₁ in the charge storage unit L _org according to the invention in the second aspect of the invention, based on the total molar amount of all organic redox-active polymers P _redox1 included in the electrode E ₁ in the charge storage unit L _org according to the invention in the second aspect of the invention is in the range of 0.1 % to 1000% by weight, more preferably in the range of 1 % to 500% by weight, even more preferably in the range of 5% to 200% by weight, yet more preferably in the range of 40% to 160% by weight, yet more preferably still in the range of 80% to 120% by weight, most preferably 100% by weight.

In the cases in which the electrode E ₁ in the charge storage unit L _org according to the invention in the second aspect of the invention comprises at least one binder additive B ₁ , the binder additive B ₁ is especially as described in point 1.1.2.4.

In the cases in which the electrode E ₁ in the charge storage unit L _org according to the invention in the second aspect of the invention comprises at least one binder additive B ₁ , however, it is preferable that the total molar amount of all binder additives B ₁ included in the electrode E ₁ in the charge storage unit L _org according to the invention in the second aspect of the invention, based on the total molar amount of all organic redox-active polymers P _redox1 included in the electrode E ₁ in the charge storage unit L _org according to the invention in the second aspect of the invention is in the range of 0.001 % to 100% by weight, more preferably in the range of 0.1 % to 90% by weight, even more preferably in the range of 3% to 70% by weight, yet more preferably in the range of 5% to 50% by weight, yet more preferably still in the range of 7.5% to 20% by weight, most preferably 16.6% by weight.

The electrode E ₂ of the charge storage unit L _org according to the invention in the second aspect of the invention comprises at least one organic redox-active polymer P _redox2 , at least one conductivity additive L ₂ , optionally at least one solvent Solv ₂ , optionally at least one binder additive B2 and optionally at least one ionic liquid IL2.

The organic redox-active polymer P _redox2 in the charge storage unit L _org according to the invention in the second aspect of the invention is as defined under point 1.4.2.

The conductivity additive L ₂ in the charge storage unit L _org according to the invention in the second aspect of the invention is as defined under point 1.4.3.1. The amount of the conductivity additive L ₂ included in the electrode E ₂ in the charge storage unit L _org according to the invention in the second aspect of the invention is not subject to any further restriction. However, it is preferable that the total weight of all conductivity additives L ₂ included in the electrode E ₂ , based on the total weight of the redox polymers P _redox2 included in the electrode E ₂ , is in the range of 0.1 % to 1000% by weight, preferably in the range of 10% to 500% by weight, more preferably in the range of 30% to 100% by weight, yet more preferably in the range of 40% to 80% by weight, even more preferably in the range of 50% by weight to 60% by weight, most preferably 58.3% by weight.

The electrode E ₂ in the charge storage unit L _org according to the invention in the second aspect of the invention optionally also comprises at least one solvent Solv ₂ . This is especially as defined in point 1.4.4. However, it is preferable that the electrode E ₂ in the charge storage unit L _org according to the invention in the second aspect of the invention comprises less than 1 % by weight, especially less than 0.1 % by weight, of a solvent Solv ₂ .

The electrode E ₂ in the charge storage unit L _org according to the invention in the second aspect of the invention optionally also comprises at least one ionic liquid IL2. This is especially as defined in points 1.4.6.1 , 1.4.6.2.

In the cases in which the electrode E ₂ in the charge storage unit L _org according to the invention in the second aspect of the invention comprises at least one ionic liquid IL2, the amount of the ionic liquid IL2 included in the electrode E ₂ in the charge storage unit L _org according to the invention in the second aspect of the invention is not subject to any further restriction.

In the cases in which the electrode E ₂ in the charge storage unit L _org according to the invention in the second aspect of the invention comprises at least one ionic liquid IL2, however, it is preferable that the total molar amount of all ionic liquids IL2 included in the electrode E ₂ in the charge storage unit Lor _g according to the invention in the second aspect of the invention, based on the total molar amount of all organic redox-active polymers P _redox2 included in the electrode E ₂ in the charge storage unit L _org according to the invention in the second aspect of the invention is in the range of 0.1 % to 1000% by weight, more preferably in the range of 1 % to 500% by weight, even more preferably in the range of 5% to 200% by weight, yet more preferably in the range of 40% to 160% by weight, yet more preferably still in the range of 80% to 120% by weight, most preferably 100% by weight.

In the cases in which the electrode E ₂ in the charge storage unit L _org according to the invention in the second aspect of the invention comprises at least one binder additive B2, the binder additive B2 is especially as described in point 1.4.5.

In the cases in which the electrode E ₂ in the charge storage unit L _org according to the invention in the second aspect of the invention comprises at least one binder additive B2, however, it is preferable that the total molar amount of all binder additives B2 included in the electrode E ₂ in the charge storage unit L _org according to the invention in the second aspect of the invention, based on the total molar amount of all organic redox-active polymers P _redox2 included in the electrode E ₂ in the charge storage unit L _org according to the invention in the second aspect of the invention is in the range of 0.001 % to 100% by weight, more preferably in the range of 0.1 % to 90% by weight, even more preferably in the range of 3% to 70% by weight, yet more preferably in the range of 5% to 50% by weight, yet more preferably still in the range of 7.5% to 20% by weight, most preferably 16.6% by weight. 2.3 Polymer electrolytes P _el

The polymer electrolyte P _el included in the charge storage unit L _org according to the invention in the second aspect of the invention is as described in point 1.3.1 and obtainable by the methods described in point 1.3.2.

2.4 Shaping

The charge storage unit in the second aspect of the present invention has additionally also

been shaped. According to the invention, shaping is when the substrate S ₁ is at least partly nonplanar in the region of the substrate S ₁ covered by the electrode E ₁ , the inevitable result of which is that the layers E ₁ /P _el /E ₂ /S ₂ are also nonplanar.

This is the case especially when the substrate S ₁ has a concave surface O _A , a convex surface O _x , a combination of the two or at least one edge K, one edge K being the most preferred.

3. Figures

Figure 1 A shows a preferred embodiment of the production process in the first aspect of the present invention. Figures 1 B, 1 C, 1 D show preferred embodiments of the charge storage unit L _org in the second aspect of the present invention.

Figure 1 A shows how, in step (a), a mixture M ₁ is applied to a substrate S ₁ via a method known to the person skilled in the art, for example screen printing. The solvent Solv ₁ included in the mixture M ₁ is then removed at least partly, but preferably completely, in step (b), which gives an electrode E ₁ applied to the substrate S ₁ . Then, in a further step (c), a polymer electrolyte P _el is applied to the electrode E ₁ . In the subsequent step (d), a mixture M ₂ is applied to the polymer electrolyte P _el , from which the solvent Solv ₂ is removed at least partly, preferably completely, in the subsequent step (e). This gives an electrode E ₂ . A further substrate S ₂ is then applied thereto in step (f). This gives an organic charge storage unit L _org . Two sides of the substrate S ₁ can now be distinguished: One side is that on which layers E ₁ /P _el /E ₂ /S ₂ are present (“S _L ” side). The other side is that on which layers E ₁ /P _el /E ₂ /S ₂ are not present (“S _N ” side).

Figures 1 B, 1 C and 1 D show various embodiments in which the shaping of the substrate S ₁ can be configured in the region of the substrate S ₁ covered by the electrode E ₁ . This shaping is performed in step (g) of the process according to the invention in the first aspect of the invention. For instance, the substrate S ₁ may be shaped in a convex (Figure 1 B; O _x ) or concave (Figure 1 C; O _A ) manner. These two shaping operations do not leave any planar surfaces in the substrate S ₁ . Alternatively, as shown in figure 1 D, where the substrate S ₁ then has at least partly planar surfaces O ₁ and O ₂ , the substrate S ₁ can also be shaped to form an edge K. Figures 2 A, 2 B and 2 C show preferred embodiments of the charge storage unit L _org in the second aspect of the present invention. In these embodiments, a sharp edge K is formed, in which the surfaces Oi and O ₂ of the planar faces of the S _L side (symbol S _L as shown in Figure 1 A) of the substrate S ₁ form a line of intersection and intersect at a right angle a (Figure 2 A), an acute angle a (Figure 2 B) or an oblique angle a (Figure 2 C).

Figures 3 A, 3 B and 3 C show embodiments of the charge storage unit L _org in the second aspect of the present invention. These correspond to those shown in Figures 2 A, 2 B and 2 C, except that no sharp edge K is formed, and the edge K is instead rounded.