Electrodes for energy storage devices and methods for their preparation

1. An energy storage structure comprising:

a first graphitized carbon structure layer;

a second graphitized carbon structure layer;

wherein one or both of the first graphitized carbon structure layer and the second graphitized carbon structure layer comprise graphitized poly-acrylonitrile fibers, vapor-grown carbon fibers, graphitized activated carbon fibers, or any combination thereof;

a first active material stack disposed between the first graphitized carbon structure layer and the second graphitized carbon structure layer; wherein the first active material stack comprises:

a first positive active material layer;

a first negative active material layer, wherein each of the first positive active material layer and the first negative material layer includes at least one active metal ion complex comprising of at least one counter ion and at least one ligand, and wherein the at least one ligand comprises methanolamine, ethanolamine, di-ethanesulfonate, x-methanesulfonate, x-trifluoromethanesulfonate, thiocyanate, or any combination thereof;

a first electrolyte layer disposed between the first positive active material layer and the first negative active material layer; and

a first layer of carbon nanotubes disposed between the first active material stack and the first graphitized carbon structure layer; a second layer of carbon nanotubes disposed between the first active material stack and the second graphitized carbon structure layer, or both.

2. The energy storage structure of claim 1 , wherein one or both of the first graphitized carbon structure layer and the second graphitized carbon structure layer have a thickness of about 5 μm to about 200 μm.

3. The energy storage structure of claim 1 , wherein one or both of the first graphitized carbon structure layer and the second graphitized carbon structure layer have a porosity of about 5% to about 99%.

4. The energy storage structure of claim 1 , wherein one or both of the first graphitized carbon structure layer and the second graphitized carbon structure layer are substantially non-porous.

5. The energy storage structure of claim 1 , wherein one or both of the first positive active material layer and the first negative active material layer have a thickness of about 50 μm to about 5000 μm.

6. The energy storage structure of claim 1 , wherein the first positive active material layer and the first negative active material layer have a combined volume of about 60% to about 85% of the total volume of the energy storage structure.

7. The energy storage structure of claim 1 , wherein the first electrolyte layer has a thickness of about 1 μm to about 50 μm.

8. The energy storage structure of claim 1 , further comprising at least a second active material stack disposed between the second graphitized carbon structure layer and a third graphitized carbon structure layer, wherein the second active material stack comprises:

a second positive active material layer;

a second negative active material layer, wherein each of the second positive active material layer and the second negative material layer includes at least one active metal ion complex comprising of at least one counter ion and at least one ligand, wherein the at least one ligand comprises methanolamine, ethanolamine, di-ethanesulfonate, x-methanesulfonate, x-trifluoromethanesulfonate, thiocyanate, or any combination thereof; and

a second electrolyte layer disposed between the second positive active material layer and the second negative active material layer.

9. The energy storage structure of claim 8 , wherein the third graphitized carbon structure layer comprises graphitized poly-acrylonitrile fibers, vapor-grown carbon fibers, pyrolytic carbon nanotubes, carbon aerogels, graphitized activated carbon fibers, exfoliated graphite, or any combination thereof.

10. The energy storage structure of claim 8 , wherein the third graphitized carbon structure layer has a thickness of about 5 μm to about 200 μm.

11. The energy storage structure of claim 8 , wherein the third graphitized carbon structure layer has a porosity of about 5% to about 99%.

12. The energy storage structure of claim 8 , wherein the third graphitized carbon structure layer is substantially non-porous.

13. The energy storage structure of claim 8 , wherein one or both of the second positive active material layer and the second negative active material layer have a thickness of about 50 μm to about 5000 μm.

14. The energy storage structure of claim 8 , wherein the second positive active material layer and the second negative active material layer have a combined volume of about 60% to about 85% of the total volume of the energy storage structure.

15. The energy storage structure of claim 8 , wherein the second electrolyte layer has a thickness of about 5 μm to about 40 μm.

16. The energy storage structure of claim 8 , further comprising two current collectors adjacent to two outer graphitized carbon structure layers.

17. A method of making an energy storage structure, the method comprising:

forming a first graphitized carbon structure layer;

disposing a first active material stack over the first graphitized carbon structure layer, wherein the first active material stack comprises:

a first positive active material layer;

a first negative active material layer, wherein each of the first positive active material layer and the first negative material layer includes at least one active metal ion complex comprising of at least one counter ion and at least one ligand, and wherein the at least one ligand comprises methanolamine, ethanolamine, di-ethanesulfonate, x-methanesulfonate, x-trifluoromethanesulfonate, thiocyanate, or any combination thereof; and

a first electrolyte layer disposed between the first positive active material layer and the first negative active material layer;

disposing a second graphitized carbon structure layer over the first active material stack; wherein one or both of the first graphitized carbon structure layer and the second graphitized carbon structure layer comprise graphitized poly-acrylonitrile fibers, vapor-grown carbon fibers, graphitized activated carbon fibers, or any combination thereof;

disposing a first layer of carbon nanotubes over the first active material stack and the first graphitized carbon structure layer; and

disposing a second layer of carbon nanotubes over the first active material stack and the second graphitized carbon structure layer, or both.

18. The method of claim 17 , wherein the first graphitized carbon structure layer is formed on a first conductive substrate.

19. The method of claim 18 , wherein forming the first graphitized carbon structure layer comprises:

depositing a solution comprising polymer fibers onto the first conductive substrate to form a layer of polymer fibers;

coating the polymer fibers with a resin binder; and

sintering the polymer fibers to form the first graphitized carbon structure layer.

20. The method of claim 17 , further comprising disposing a second conductive substrate on the second graphitized carbon structure layer.

21. The method of claim 17 , further comprising:

disposing a second active material stack over the second graphitized carbon structure layer, wherein the second active material stack comprises:

a second positive active material layer;

a second negative active material layer, wherein each of the second positive active material layer and the second negative material layer includes at least one active metal ion complex comprising of at least one counter ion and at least one ligand, and wherein the at least one ligand comprises methanolamine, ethanolamine, di-ethanesulfonate, x-methanesulfonate, x-trifluoromethanesulfonate, thiocyanate, or any combination thereof; and

a second electrolyte layer disposed between the second positive active material layer and the second negative active material layer; and

disposing a third graphitized carbon structure layer over the second active material stack.

22. The method of claim 21 , further comprising:

disposing a third layer of carbon nanotubes on the second graphitized carbon structure layer before disposing the second active material stack; and

disposing a fourth layer of carbon nanotubes on the second active material stack before disposing the third graphitized carbon structure layer.

23. The method of claim 21 , further comprising disposing a second conductive substrate on the third graphitized carbon structure layer.