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1. (WO2019025785) POLYMER-BASED ENERGY STORAGE DEVICE
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CLAIMS:

1. An energy storage device comprising:

two electrodes; and

an electrolyte,

wherein each of said two electrodes comprises an interpenetrating network of an electrically conducting polymer and an ionically conducting polymer, and

wherein in said interpenetrating network each of said electrically conducting polymer and said ionically conducting polymer forms a continuous phase, and

said two electrodes are each in the form of a freestanding film.

2. An energy storage device as claimed in claim 1 , wherein said interpenetrating network is a fully interpenetrating network or a semi-interpenetrating network, preferably a semi-interpenetrating network.

3. An energy storage device as claimed in claim 1 or claim 2, wherein said interpenetrating network comprises 10 to 90 wt%, preferably 50 to 65 wt%, of said electrically conducting polymer, based on the total weight of the interpenetrating network.

4. An energy storage device as claimed in any one of claims 1 to 3, wherein said interpenetrating network comprises 10 to 90 wt%, preferably 35 to 50 wt%, of said ionically conducting polymer, based on the total weight of the interpenetrating network.

5. An energy storage device as claimed in any one of claims 1 to 4, wherein said interpenetrating network extends throughout the whole thickness of each electrode.

6. An energy storage device as claimed in any one of claims 1 to 5, wherein said interpenetrating network further comprises one or more further polymers, preferably one or more functional polymers selected from rubber, shape-memory polymers, epoxy resins, self-healing polymers and mixtures thereof.

7. An energy storage device as claimed in any one of claims 1 to 6, wherein said electrically conducting polymer comprises repeat units comprising substituted or unsubstituted thiophene or derivatives thereof, substituted or unsubstituted aniline or derivatives thereof, substituted or unsubstituted pyrrole or derivatives thereof, substituted or unsubstituted vinylene or derivatives thereof, substituted or unsubstituted phenylene or derivatives thereof, substituted or unsubstituted polycyclic aromatic hydrocarbons (e.g. fluoranthene) or derivatives thereof, or mixtures thereof.

8. An energy storage device as claimed in any one of claims 1 to 7, wherein said electrically conducting polymer is selected from poly(3,4-ethylenedioxythiophene) (PEDOT), polypyrrole (PPy), polyaniline (PANI), polythiophene (PT), poly(p-phenylene), poly(p-phenylene vinylene), poly(3-vinylperylene), polyaniline-polypyrrole (PANI-PPy), polyacetylene and mixtures thereof, preferably from poly(3,4-ethylenedioxythiophene) (PEDOT), polypyrrole (PPy) and polyaniline (PANI).

9. An energy storage device as claimed in any one of claims 1 to 8, wherein said electrically conducting polymer has a theoretical specific capacitance of 100 to 2000 F/g, preferably 200 to 800 F/g.

10. An energy storage device as claimed in any one of claims 1 to 9, wherein said ionically conducting polymer is a gel, preferably a solvent swellable gel.

1 1. An energy storage device as claimed in any one of claims 1 to 10, wherein said ionically conducting polymer is a cross-linked polymer.

12. An energy storage device as claimed in any one of claims 1 to 1 1 , wherein said ionically conducting polymer comprises polyethylene oxide (PEO), polyvinyl alcohol (PVA), polyacrylonitrile (PAN), polyacrylic acid (PAA), poly(methyl methacrylate) (PMMA), polyvinyl carbonate (PVC), polyvinylidene fluoride (PVDF), sulfonated tetrafluoroethylene based fluoropolymer-copolymer (e.g. Nafion) and chemically modified derivatives thereof, polyacrylamide (PAM), or mixtures thereof, preferably polyethylene oxide (PEO).

13. An energy storage device as claimed in any one of claims 1 to 12, wherein said electrolyte comprises an ionically conducting polymer, and preferably comprises polyethylene oxide (PEO), polyvinyl alcohol (PVA), polyacrylonitrile (PAN), polyacrylic acid (PAA), poly(methyl methacrylate) (PMMA), polyvinyl carbonate (PVC)), polyvinylidene fluoride (PVDF), sulfonated tetrafluoroethylene based

fluoropolymer-copolymer (e.g. Nafion) and chemically modified derivatives thereof, polyacrylamide (PAM), or mixtures thereof.

14. An energy storage device as claimed in any one of claims 1 to 13, wherein said electrolyte further comprises a salt, preferably selected from lithium chloride (LiCI), lithium perchlorate (LiCI04), lithium sulfate (Li2S04), lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), lithium hexafluorophosphate (LiPF6), sodium chloride (NaCI), sodium perchlorate (NaCI04), sodium sulfate (Na2S04), sodium nitrate (NaN03), sodium hexafluorophosphate (NaPF6), potassium chloride (KCI), potassium iodide (Kl), potassium perchlorate (KCI04), potassium sulfate (K2S04), magnesium chloride (MgCI2), magnesium perchlorate (Mg(CI04)2), magnesium sulfate (MgS04), tetraethylammonium tetrafluoroborate (TEABF4) and 1-ethyl-3-methylimidazolium tetrafluoroborate (EMIMBF4).

15. An energy storage device as claimed in any one of claims 1 to 14, wherein said electrolyte further comprises an acid (e.g. H2S04).

16. An energy storage device as claimed in any one of claims 1 to 15, wherein said energy storage device is selected from a battery, a capacitor and a supercapacitor, preferably a supercapacitor.

17. An energy storage device as claimed in any one of claims 1 to 16, wherein said energy storage device has a capacitance of 10 to 2500 F/g, preferably 100 to 2500 F/g at a scan rate of 5 mV/s.

18. An energy storage device as claimed in any one of claims 1 to 17, wherein said electrodes each have a thickness of 10 μηι to 3 mm, preferably of 40 μηι to 500 μηι.

19. An energy storage device as claimed in any one of claims 1 to 18, wherein said electrodes can be bent to a 150 μηι to 500 μηι radius of curvature without breaking and especially preferably to a 150 μηι to 200 μηι (e.g. about 180 μηι) radius of curvature without breaking.

20. An energy storage device as claimed in any one of claims 1 to 19, wherein said electrodes retain 99% of their initial capacitance after 1000 cycles of bending/unbending to a 1.5 mm radius of curvature.

21. An energy storage device as claimed in any one of claims 1 to 20, wherein said two electrodes and said electrolyte are each separate bodies.

22. An energy storage device as claimed in any one of claims 1 to 21 , wherein said two electrodes and said electrolyte are formed as a single body.

23. A process for preparing an energy storage device according to any one of claims 1 to 22 comprising:

(i) preparing two electrodes each comprising an interpenetrating network of an electrically conducting polymer and an ionically conducting polymer; and

(ii) providing an electrolyte between said two electrodes.

24. A process as claimed in claim 23, wherein said electrodes are prepared by a process comprising:

(i) mixing one or more ionically conducting polymer precursors with one or more electrically conducting polymer precursors (and optionally one or more further polymers, one or more further polymer precursors and/or one or more additional active materials); and

(ii) polymerising and/or cross-linking (preferably polymerising) said polymer precursors to produce an interpenetrating network of an electrically conducting polymer and an ionically conducting polymer.

25. A process as claimed in claim 24, wherein said polymer precursors are selected from monomers, oligomers and polymers, preferably from monomers and oligomers.

26. An energy storage device obtainable by a process as claimed in any one of claims 23 to 25.

27. An energy storage device obtained by a process as claimed in any one of claims 23 to 25.

28. Use of an interpenetrating network of an electrically conducting polymer and an ionically conducting polymer to form an energy storage device according to any one of claims 1 to 22, 26 and 27.

29. A regenerative braking system comprising an energy storage device as claimed in any one of claims 1 to 22, 26 and 27.

30. A memory backup system, preferably for portable electronics, comprising an energy storage device as claimed in any one of claims 1 to 22, 26 and 27.

31. A power buffer comprising an energy storage device as claimed in any one of claims 1 to 22, 26 and 27.

32. A load-leveling device, preferably for an industrial scale system, comprising an energy storage device as claimed in any one of claims 1 to 22, 26 and 27.

33. A wearable electronic device comprising an energy storage device as claimed in any one of claims 1 to 22, 26 and 27.

34. A roll-up display comprising an energy storage device as claimed in any one of claims 1 to 22, 26 and 27.

35. A bio-implantable device comprising an energy storage device as claimed in any one of claims 1 to 22, 26 and 27.

36. A process for preparing an electrode comprising an interpenetrating network of an electrically conducting polymer and an ionically conducting polymer, wherein in said interpenetrating network each of said electrically conducting polymer and said ionically conducting polymer forms a continuous phase, said process comprising:

(i) mixing one or more ionically conducting polymer precursors with one or more electrically conducting polymer precursors and a solvent (and optionally one or more further polymers, one or more further polymer precursors and/or one or more additional active materials);

(ii) printing the mixture onto a substrate; and

(iii) polymerising and/or cross-linking (preferably polymerising) said polymer precursors to produce an interpenetrating network of an electrically conducting polymer and an ionically conducting polymer.

37. A process as claimed in claim 36, wherein said polymer precursors are selected from monomers, oligomers and polymers, preferably from monomers and oligomers.

38. A process as claimed in claim 36 or claim 37, wherein the solvent is selected from ethanol, methanol, isopropanol, toluene, hexane chloroform and acetone, and preferably ethanol.

39. A process as claimed in any one of claims 36 to 38, wherein the mixture produced in step (i) has a viscosity of 1 cP to 20 cP, more preferably a viscosity of 1 cP to 10 cP.

40. A process as claimed in any one of claims 36 to 39, wherein the mixture produced in step (i) comprises 1 to 40% solvent by volume.

41. A process as claimed in any one of claims 36 to 40, wherein the substrate is selected from glass (e.g. a glass slide), textiles, clothing, leather, paper, cellulose films, ionically conducting films or membranes (e.g. polyethylene oxide (PEO), polyvinyl alcohol (PVA), polyacrylonitrile (PAN), polyacrylic acid (PAA), poly(methyl methacrylate) (PMMA), polyvinyl carbonate (PVC), polyvinylidene fluoride (PVDF), sulfonated tetrafluoroethylene based fluoropolymer-copolymer (e.g. Nafion) and chemically modified derivatives thereof, polyacrylamide (PAM), or mixtures thereof) and flexible plastic films (e.g. polyethylene terephthalate (PET) films, nylon films).

42. A process as claimed in any one of claims 36 to 41 , wherein the mixture is printed in step (ii) using an inkjet printing technique, an aerogel printing technique or a roll-to-roll printing technique.

43. A process as claimed in any one of claims 36 to 42, wherein the mixture is printed in step (ii) in the form of a pattern (e.g. a grid).

44. A process as claimed in any one of claims 36 to 43, wherein the mixture formed in step (i) is exposed to polymerisation conditions as soon as it has been printed in step (ii).

45. A process as claimed in any one of claims 36 to 44, wherein polymerisation of the ionically conducting polymer precursors is carried out using free radical polymerisation (e.g. using UV light).

46. A process as claimed in any one of claims 36 to 45, wherein polymerisation of the electrically conducting polymer precursors is carried out using oxidative chemical polymerisation (e.g. using FeCI3).

47. A process as claimed in any one of claims 36 to 46, wherein the one or more ionically conducting polymer precursors are polymerised and/or cross-linked to form the ionically conducting polymer before the one or more electrically conducting poymers are polymerised and/or cross-linked to form the electrically conducting polymer.

48. A process for preparing an energy storage device, said process comprising:

(i) preparing an electrode according to the process of any one of claims 36 to 47;

(ii) printing one or more ionically conducting polymer precursors onto said electrode;

(iii) polymerising and/or cross-linking (preferably polymerising) said polymer precursors to produce an ionically conducting polymer layer;

(iv) mixing one or more ionically conducting polymer precursors with one or more electrically conducting polymer precursors and a solvent (and optionally one or more further polymers, one or more further polymer precursors and/or one or more additional active materials);

(v) printing the mixture onto said ionically conducting polymer layer; and

(vi) polymerising and/or cross-linking (preferably polymerising) said polymer precursors to produce an interpenetrating network of an electrically conducting polymer and an ionically conducting polymer.