TECHNICAL FIELD

[0001] The present invention relates in general to nanocarbon products. Particularly present invention relates to nanocarbon product blended into the electrolyte compositions and use thereof in manufacturing of the energy storage devices.

BACKGROUND

[0002] Nanocarbon materials have recently been widely utilised in energy storage devices, because they are suitable for increasing the electric conductivity of commercial electrode materials at already very low mass percentage. Various geometries of carbon and graphitic carbon have been tested, such as a rod, plates, paper, felt, cloth, mesh, brush, and granules. Because the irregular physical structure of some of these materials, the electrical resistance is greater than desirable, others present a low specific surface area for biofilm formation, or high charge transfer resistance. To enhance the performance of nanocarbon materials several modifications have been proposed. Ideal characteristics of anode electrodes include high electrical conductivity, chemically inert, resistance to corrosion, mechanical resistance, high electrochemically active area, high specific surface area, biocompatible, and low-cost.

[0003] Modifications of the surface of materials can be grouped as chemical and physical. Chemical modifications include coverage with conducting polymers, such as polyaniline, an increase of surface chemical groups, such as ammonium or quinones, and incorporation of electroactive compounds, such as FeiCh, RuCh, or AQDS, in the form of composites. Physical modifications are an increase of porosity by heating at high temperatures and an increase of roughness by incorporation of nanotubes.

[0004] Although nanocarbon materials have provided numerous application- specific efficient electrodes for energy storage and conversion, yet there are many more promises contained in the properties of nanocarbon materials which either have not been invented or need further refining or modification for commercial level applications. Among such applications, flexible and wearable energy devices are very attractive for portable electronic systems. Carbon-based lightweight structural energy storing systems are crucial for future communication vehicles on ground, through water, and in the air. Furthermore, load-bearing carbon structures for energy systems are desirable for advanced applications. Metal-air battery and solid-state electrolyte batteries are very promising to achieve higher energy and power density beyond their present state. No doubt, further innovation in nanocarbon materials fabrication, processing and applicability is essential for commercial level success in this field.

SUMMARY

[0005] The present invention relates to a method for preparing an electrolyte composition, said method comprises blending a nanocarbon material in an electrolyte, thereby creating a flowing liquid dispersion, wherein said nanocarbon material has a carbon particle size from about 0.5 microns to about 1000.0 microns and comprises a plurality of carbon layers, wherein each said carbon layer has a surface wetted with said electrolyte, wherein the thickness of each said carbon layer is from about 20 nm to about 120 nm, wherein the gap between the carbon layers is from about 0.5 gm (microns) to about 30 gm (microns), and wherein said nanocarbon material and the wetted surface of said carbon layers are suitable for increasing a battery electrode capacity and ions mobility.

[0006] In some embodiments, a contact angle of drops of the electrolyte to the wetted surface of the carbon layers is less than 90°, or from about 10° to about 40°, or from about 15° to about 30°.

[0007] In one embodiment, said nanocarbon material has a high metal-ion storage capacity of approximately 6.24 x 10 ¹⁷ Li-ions per 1 mm ² . In some other embodiments, the surface area of the carbon layers is in the range of about 100.0 m ² /gr to about 400.0 m ² /gr.

[0008] In a certain embodiment, the nanocarbon material is mixed with a graphite powder or with a cathode powder comprising a cathode active material. Non-limiting examples of the cathode active materials are Lithium Nickel Cobalt Manganese Oxide (LiNiCoMnO2), Lithium Iron Phosphate (LiFePO4), Lithium Nickel Manganese Spinel (LiNio.5Mn1.5O4), Lithium Nickel Cobalt Aluminium Oxide (LiNiCoAlO2), Lithium Manganese Oxide (LiMn2O4) and Lithium Cobalt Oxide (LiCoO2).

[0009] In another embodiment, said nanocarbon material is blended inside said electrolyte composition, thereby creating a flowing liquid dispersion. The electrolyte can be either liquid or solid. [0010] In a particular embodiment, the electrolyte composition comprises ionic liquid, polymer gel, solid, liquid or semi liquid to be solidified further on in the process. In another particular embodiment, said electrolyte further comprising an electrolyte liquid or solvent. Non-limiting examples of the electrolyte liquid or solvent are ethylene carbonate, ethyl methyl carbonate, dimethyl carbonate, diethyl carbonate, vinylene carbonate and aqueous solution of inorganic salts. In a specific embodiment, the electrolyte composition further comprises a lithium hexafluorophosphate (LiPFe). [0011] In still another embodiment, the nanocarbon material is blended inside said electrolyte composition in the concentration ratio of about 0.01-1.0% of the electrolyte by weight. Non-limiting examples of the electrolyte composition of the present invention are: a) 1.0- 1.4 M of lithium hexafluorophosphate in a solvent mixture of ethylene carbonate with ethyl methyl carbonate having the weight ratio 2.0-4.0:5.0-8.0 (wt/wt); b) 0.8-1.2 M of lithium hexafluorophosphate in a solvent mixture of ethylene carbonate with diethyl carbonate having the weight ratio 2.0-4.0:5.0-8.0 (wt/wt); c) 1.1 -1.5 M of lithium hexafluorophosphate in a solvent mixture of ethylene carbonate with dimethyl carbonate and ethyl methyl carbonate having the weight ratio 25-35:30-40:25-35 (wt/wt); d) 0.8-1.2 M of lithium hexafluorophosphate in a solvent mixture of ethylene carbonate with ethyl methyl carbonate having the weight ratio 40-60:40-60 (wt/wt); and e) 1.0- 1.4 M of lithium hexafluorophosphate in a solvent mixture of ethylene carbonate (EC) with ethyl methyl carbonate (EMC) having the weight ratio 2.0-4.0:5.0-8.0 (wt/wt) and vinylene carbonate (VC) 2% w/w.

[0012] In a further embodiment, the electrolyte composition is suitable for use in preparing a cathode electrolyte substrate for increasing a cathode capacity. In yet further embodiment, the electrolyte composition is suitable for use preparing an anode electrolyte substrate for increasing an anode capacity.

[0013] In another aspect of the present invention, an electrolyte composition comprises the nanocarbon material of the present invention, wherein said nanocarbon material is blended inside said electrolyte composition, thereby creating an aqueous flowing dispersion or liquid suspension. In some embodiments, the electrolyte composition of the present invention comprises lithium hexafluorophosphate and a solvent or mixture of solvents selected from ethylene carbonate, ethyl methyl carbonate, diethyl carbonate, dimethyl carbonate, and ethyl methyl carbonate. In a particular embodiment, the electrolyte composition of the present invention comprises approximately 0.01-1.0% of said nanocarbon material by weight of the above electrolyte.

[0014] In a further aspect, an energy storage device comprises the electrolyte composition of the present invention and further comprises: a) A cathode prepared from a composition containing an active material and a binder and coated on a current collector; b) An anode prepared from a composition containing an active material and a binder and coated on a current collector; and c) Separator between the cathode and anode, said separator constitutes an electric insulator allowing ions movement via pores, but blocking an electron flow.

[0015] In a specific embodiment, the energy storage device of the present invention is selected from a supercapacitor of either an aqueous or organic solvent electrolyte type, nickel/metal hydride battery, lead-acid battery, Li-ion batteries and Li-ion polymer battery.

[0016] In yet further aspect, the present invention relates to use of the electrolyte composition of the present invention in an anode electrolyte substrate for increased capacity of the anode of energy storage devices. In still another aspect, the present invention relates to use of the electrolyte composition of the present invention in a cathode electrolyte substrate for increased capacity of the cathode of energy storage devices.

BRIEF DESCRIPTION OF THE DRAWINGS

[0017] Disclosed embodiments will be understood and appreciated more fully from the following detailed description taken in conjunction with the appended figures. The drawings included and described herein are schematic and are not limiting the scope of the disclosure. It is also noted that in the drawings, the size of some elements may be exaggerated and, therefore, not drawn to scale for illustrative purposes. The dimensions and the relative dimensions do not necessarily correspond to actual reductions to practice of the disclosure.

[0018] Fig. la shows the scanning -electron microscope (SEM, Zeiss) image of the nanocarbon layered product of the present invention. Magnification is 25.00k X, scan speed is 1, system vacuum is 3.87 x 10’ ⁶ mbar, EHT is 3.0 kV, ESB grid is 0 V, aperture size is 30.00 pm, and focus is 5.2 mm.

[0019] Fig. lb shows the scanning-electron microscope (SEM, Zeiss) image of the nanocarbon layered product of the present invention. The structure of the nanocarbon layered product and the distance between layers are clearly visible.

[0020] Fig. 1c schematically shows the multi-layered nanocarbon structure of the product of the present invention. Fig. Id shows the bar chart for the distance distribution between the nanocarbon layers.

[0021] Fig. 2 shows the BET multi-point results of the BET measurements of the nanocarbon layered product of the present invention. Weight of the sample is 0.1085 g, adsorbate is nitrogen, duration is 154.93 min. The linear plot of the isotherm branch adsorption has the following parameters: slope = 11.6392, intercept = 0.095484, correlation coefficient R = 0.999686, constant C = 122.561. The obtained surface area is 296.764 m ² /g.

[0022] Fig. 3a shows the scanning electron microscope (SEM, Zeiss) image of Li ions moving into nanocarbon multi-layered material penetrating between carbon layers. Magnification is 25.00k X, scan speed is 1, system vacuum is 3.87 x 10’ ⁶ mbar, EHT is 3.0 kV, ESB grid is 0 V, focus is 5.2 mm, and aperture size is 30.00 pm.

[0023] Fig. 3b schematically shows the Li ions movement between two adjacent nanocarbon layers of the product of the present invention.

[0024] Fig. 4a schematically shows the wettability degree between a nanocarbon layer and an electrolyte drop.

[0025] Figs. 4b and 4c show the snapshots from OCA15EC optical contact angle measurements by DataPhysics Instruments GmbH (Germany).

DETAILED DESCRIPTION

[0026] In the following description, various aspects of the present invention will be described. For purposes of explanation, specific details are set forth in order to provide a thorough understanding of the present invention. However, it will also be apparent to one skilled in the art that the present invention may be practiced without the specific details presented herein. Furthermore, well-known features may be omitted or simplified in order not to obscure the present invention.

[0027] The term "comprising", used in the claims, is "open ended" and means the elements recited, or their equivalent in structure or function, plus any other element or elements which are not recited. It should not be interpreted as being restricted to the means listed thereafter; it does not exclude other elements or steps. It needs to be interpreted as specifying the presence of the stated features, integers, steps or components as referred to, but does not preclude the presence or addition of one or more other features, integers, steps or components, or groups thereof. Thus, the scope of the expression "a composition comprising x and z" should not be limited to compositions consisting only of components x and z. Also, the scope of the expression "a method comprising the steps x and z" should not be limited to methods consisting only of these steps.

[0028] Unless specifically stated, as used herein, the terms "about" and “approximately” are understood as within a range of normal tolerance in the art, for example within two standard deviations of the mean. In one embodiment, the term "about" means within 10% of the reported numerical value of the number with which it is being used, preferably within 5% of the reported numerical value. For example, the term "about" can be immediately understood as within 10%, 9%, 8%, 7%, 6%, 5%, 4%, 3%, 2%, 1%, 0.5%, 0.1%, 0.05%, or 0.01% of the stated value. In other embodiments, the term "about" can mean a higher tolerance of variation depending on for instance the experimental technique used. Said variations of a specified value are understood by the skilled person and are within the context of the present invention. As an illustration, a numerical range of "about 1 to about 5" should be interpreted to include not only the explicitly recited values of about 1 to about 5, but also include individual values and sub-ranges within the indicated range. Thus, included in this numerical range are individual values such as 2, 3, and 4 and sub-ranges, for example from 1-3, from 2-4, and from 3- 5, as well as 1, 2, 3, 4, 5, or 6, individually. This same principle applies to ranges reciting only one numerical value as a minimum or a maximum. Unless otherwise clear from context, all numerical values provided herein are modified by the term "about". Other similar terms, such as "substantially", "generally", "up to" and the like are to be construed as modifying a term or value such that it is not an absolute. Such terms will be defined by the circumstances and the terms that they modify as those terms are understood by those of skilled in the art. This includes, at very least, the degree of expected experimental error, technical error and instrumental error for a given experiment, technique or an instrument used to measure a value.

[0029] As used herein, the term "and/or" includes any and all combinations of one or more of the associated listed items. Unless otherwise defined, all terms (including technical and scientific terms) used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs. It will be further understood that terms, such as those defined in commonly used dictionaries, should be interpreted as having a meaning that is consistent with their meaning in the context of the specification and relevant art and should not be interpreted in an idealized or overly formal sense unless expressly so defined herein. Well-known functions or constructions may not be described in detail for brevity and/or clarity.

[0030] By definition, an “electrolyte” is a medium, which contains ions, that is electrically conducting through the movement of those ions, but not conducting electrons. This includes most soluble salts, acids, and bases dissolved in a polar solvent, such as water. Upon dissolving, the substance separates into cations and anions, which disperse uniformly throughout the solvent. Electrically, such a solution is neutral. If an electric potential is applied to such a solution, the cations of the solution are drawn to the electrode that has an abundance of electrons, while the anions are drawn to the electrode that has a deficit of electrons. The movement of anions and cations in opposite directions within the solution creates a current. [0031] In the present invention, the term “nanocarbon materials” define nanomaterials composed of carbon atoms arranged in various geometries. Non-limiting examples of the nanocarbon materials are Ceo and other fullerenes arranged in the form of cages, carbon nanotubes (CNTs, single-walled or multiwalled) arranged in the form of tubes, and graphene arranged in the form of sheets. In the present invention, an electrolyte composition comprises the nanocarbon material. The nanocarbon material of the present invention is blended inside this composition and creates a flowing liquid dispersion. In a particular embodiment, the electrolyte composition comprises approximately 0.01-1.0% of said nanocarbon material by weight of the aforementioned electrolyte.

[0032] The present invention relates to a method for preparing an electrolyte composition, said method comprises blending a nanocarbon material in an electrolyte, thereby creating a flowing liquid dispersion, wherein said nanocarbon material having carbon particle size from about 0.5 microns (gm) to about 1000.0 microns (gm) and comprising a plurality of carbon layers, wherein each said carbon layer has a surface wetted with said electrolyte, wherein the thickness of said carbon layers is from about 20 nm to about 120 nm, wherein the gap between the carbon layers is from about 0.5 microns (pm) to about 30 microns (gm), wherein said nanocarbon material and the wetted surface of said carbon layers are designed to increase a battery electrode capacity and ions mobility. In the present invention, the term “wetted surface” means that the surface of the nanocarbon material or of each individual carbon layer is wetted with the electrolyte. The aspect of “wettability” will be discussed further in the description.

[0033] The reason for the certain range of the particle size of the nanocarbon material from 0.5 micron to 1000.0 microns, is that when the particles are larger than 1000 micron, the particles are not able to form a stable liquid dispersion in the electrolyte. When the particle size is smaller than 0.5 micron, the particles tend to increase the liquid dispersion viscosity, thereby negatively affecting the liquid electrolyte dispersion flow ability.

[0034] In one embodiment, said nanocarbon material has a high metal-ion storage capacity of approximately 6.24 x 10 ¹⁷ Li-ions per 1 mm ² . In some other embodiments, the surface area of the carbon layers is in the range of about 100.0 m ² /gr to about 400.0 m ² /gr.

[0035] In a certain embodiment, the nanocarbon material is mixed with a graphite powder or with a cathode powder comprising a cathode active material. Non-limiting examples of the cathode active materials are Lithium Nickel Cobalt Manganese Oxide (LiNiCoMnO2), Lithium Iron Phosphate (LiFePO4), Lithium Nickel Manganese Spinel (LiNio.5Mn1.5O4), Lithium Nickel Cobalt Aluminium Oxide (LiNiCoAlO2), Lithium Manganese Oxide (LiMn2O4) and Lithium Cobalt Oxide (LiCoO2). [0036] In another embodiment, said nanocarbon material is blended inside said electrolyte composition, thereby creating a flowing liquid dispersion. The electrolyte can be either liquid or solid. [0037] In a particular embodiment, the electrolyte composition comprises ionic liquid, polymer gel, solid, liquid or semi liquid to be solidified further on in the process. In another particular embodiment, said electrolyte further comprising an electrolyte liquid or solvent. Non-limiting examples of the electrolyte liquid or solvent are ethylene carbonate, ethyl methyl carbonate, dimethyl carbonate, diethyl carbonate, vinylene carbonate and aqueous solution of inorganic salts. In a specific embodiment, the electrolyte composition further comprises a lithium hexafluorophosphate (LiPFe).

[0038] In still another embodiment, the nanocarbon material is blended inside said electrolyte composition in the concentration ratio of about 0.01-1.0% of the electrolyte by weight. Non-limiting examples of the electrolyte composition of the present invention are: a) 1.0- 1.4 M of lithium hexafluorophosphate in a solvent mixture of ethylene carbonate with ethyl methyl carbonate having the weight ratio 2.0-4.0:5.0-8.0 (wt/wt); b) 0.8-1.2 M of lithium hexafluorophosphate in a solvent mixture of ethylene carbonate with diethyl carbonate having the weight ratio 2.0-4.0:5.0-8.0 (wt/wt); c) 1.1 -1.5 M of lithium hexafluorophosphate in a solvent mixture of ethylene carbonate with dimethyl carbonate and ethyl methyl carbonate having the weight ratio 25-35:30-40:25-35 (wt/wt); d) 0.8-1.2 M of lithium hexafluorophosphate in a solvent mixture of ethylene carbonate with ethyl methyl carbonate having the weight ratio 40-60:40-60 (wt/wt); and e) 1.0- 1.4 M of lithium hexafluorophosphate in a solvent mixture of ethylene carbonate (EC) with ethyl methyl carbonate (EMC) having the weight ratio 2.0-4.0:5.0-8.0 (wt/wt) and vinylene carbonate (VC) 2% w/w.

[0039] In a further embodiment, the electrolyte composition is suitable for use in preparing a cathode electrolyte substrate for increasing a cathode capacity. In yet further embodiment, the electrolyte composition is suitable for use preparing an anode electrolyte substrate for increasing an anode capacity.

[0040] In another aspect of the present invention, an electrolyte composition comprises the nanocarbon material of the present invention, wherein said nanocarbon material is blended inside said electrolyte composition, thereby creating a liquid flowing dispersion or liquid suspension. In some embodiments, the electrolyte composition of the present invention comprises lithium hexafluorophosphate and a solvent or mixture of solvents selected from ethylene carbonate, ethyl methyl carbonate, diethyl carbonate, dimethyl carbonate, and ethyl methyl carbonate. In a particular embodiment, the electrolyte composition of the present invention comprises approximately 0.01-1.0% of said nanocarbon material by weight of the above electrolyte.

[0041] In a further aspect, an energy storage device comprises the electrolyte composition of the present invention and further comprises: a) A cathode prepared from a composition containing an active material and a binder and coated on a current collector; b) An anode prepared from a composition containing an active material and a binder and coated on a current collector; and c) Separator between the cathode and anode, said separator constitutes an electric insulator allowing ions movement via pores, but blocking an electron flow.

[0042] In a specific embodiment, the energy storage device of the present invention is selected from a supercapacitor of either an aqueous or organic solvent electrolyte type, nickel/metal hydride battery, lead-acid battery, Li-ion batteries and Li-ion polymer battery.

[0043] In yet further aspect, the present invention relates to use of the electrolyte composition of the present invention in an anode electrolyte substrate for increased capacity of the anode of energy storage devices. In still another aspect, the present invention relates to use of the electrolyte composition of the present invention in a cathode electrolyte substrate for increased capacity of the cathode of energy storage devices. Reference is now made to Figs, la and lb showing the scanningelectron microscope (SEM) images of the carbon-based layered product of the present invention.

[0044] Fig. la shows the scanning -electron microscope (SEM, Zeiss) image of the nanocarbon layered product of the present invention. Magnification is 25.00k X, scan speed is 1, system vacuum is 3.87 x 10’ ⁶ mbar, EHT is 3.0 kV, ESB grid is 0 V, aperture size is 30.00 pm, and focus is 5.2 mm.

[0045] Fig. lb shows the scanning-electron microscope (SEM, Zeiss) image of the nanocarbon layered product of the present invention. The structure of the nanocarbon layered product and the distance between layers are clearly visible. Fig. 1c schematically shows the multi-layered nanocarbon structure of the product of the present invention. Fig. Id is the bar chart showing the distance distribution between the nanocarbon layers. Table 1 below summarises the distance distribution values from the bar chart for 50 measurements:

Table 1. Distance distribution values from the bar chart for 50 measurements.

[0046] In the present invention, the electrolyte penetrates into carbon nanomaterial wherein penetration being capillary mechanism of electrolyte moving between carbon layers. The reason for this mechanism is a very high wettability of the nanocarbon material as will be explained further in the description.

[0047] In some embodiments, the surface area of the layers of the nanocarbon material of the present invention is in the range of approximately 100.0 m ² /gr to about 400.0 m ² /gr. Reference is now made to Fig. 2 showing the BET multi-point results of the BET measurements of the nanocarbon layered product of the present invention. Weight of the sample is 0.1085 g, adsorbate is nitrogen, duration is 154.93 min. The linear plot of the isotherm branch adsorption has the following parameters: slope = 11.6392, intercept = 0.095484, correlation coefficient R = 0.999686, constant C = 122.561. The obtained BET of this product was found to be 296.764 m ² /gr.

[0048] In a further embodiment, graphite particles are added to the nanocarbon material comprising carbon layers. In yet further embodiment, cathode active material particles are added to the nanocarbon material comprising carbon layers.

[0049] In one embodiment, the electrolyte composition of the present invention is used in preparing a cathode electrolyte substrate for increasing a cathode capacity. In another embodiment, the electrolyte composition of the present invention is used in preparing an anode electrolyte substrate for increasing an anode capacity.

[0050] A non-limiting example of the electrolyte composition, in which the carbon-based layered material of the present invention is blended, is 1.2 M of the LFP6 in a solvent mixture of ethylene carbonate (EC) - ethyl methyl carbonate (EMC) having the weight ratio 3:7 (wt/wt), where LPF6 (lithium hexafluorophosphate, LiPFe) is an active component salt.

[0051] In yet further embodiment, the nanocarbon material of the present invention is blended in the electrolyte composition. As mentioned above, the small gap between the layers of the nanocarbon material enhances ions absorption ability of the internal surface inside the layers, thereby generating the energy storage capacity. Thus, ions conductivity is created following the electrolyte penetrating between the carbon layers by a capillary mechanism.

[0052] In another embodiment, an energy storage device, or power cell, or battery comprises:

1) A cathode prepared from a composition containing an active material and a binder and coated on aluminium, nickel or copper foil current collector. The coating thickness is normally in the range of 10 pm to 50 pm (micron). Non-limiting examples of a suitable binder in the present invention are styrene butadiene copolymer (SBR), polyvinylidene fluoride (PVDF) and polyvinylidene difluoride (PVDDF) used in the cathode and anode electrode slurry making process for Li-ion batteries. Binders such as SBR, PVDF and PVDDF hold the active material particles together and in contact with the current collectors, i.e., the aluminium, nickel or copper foil. PVDF and PVDDF are highly non-reactive thermoplastic polymers produced by polymerisation of vinylidene difluoride and used in applications requiring the highest purity, as well as resistance to solvents, acids and hydrocarbons. Thanks to their high crystallinity levels, PVDF and PVDDF offer high resistance in typical electrolytes used in lithium batteries. The aforementioned binders may be mixed with Carbon Black to form a binder in the electrolyte composition of the present invention. In general, the binder is very important for mechanical stabilisation. Non-limiting examples of the cathode active materials are:

■ NMC (NCM) - Lithium Nickel Cobalt Manganese Oxide (LiNiCoMnO2)

■ LFP - Lithium Iron Phosphate (LiFePO4)

■ LNMO - Lithium Nickel Manganese Spinel (LiNio.5Mn1.5O4)

■ NCA - Lithium Nickel Cobalt Aluminium Oxide (LiNiCoAlO2)

■ LMO - Lithium Manganese Oxide (LiMn2O4)

■ LCO - Lithium Cobalt Oxide (LiCoO2).

2) An anode prepared from a composition containing an active material and a binder coated, for example, on copper foil. A non-limiting example of the active material for the anode is a natural, synthetic or composite graphite. Graphite is a crystalline solid with a black/grey colour and a metallic sheen. Due to its electronic structure, it is highly conductive and can reach 25,000 S/cm ² in the plane of a single crystal. Graphite is commonly used as the active material in negative electrodes mainly because it can reversibly place Li-ions between its many layers. This reversible electrochemical capability is maintained over several of thousands of cycles in batteries with optimised electrodes. However, one requirement for this application is that the graphite surface must be compatible with the electrolyte solution and binders. Non-limiting examples of the suitable binders in this case are Carbon Black, SBR and carboxymethyl cellulose (CMC). These binders could increase the content of Li ions in the whole energy storage device (battery). The discharge platform of the battery is high and the degree of polarisation small, exhibiting excellent electrochemical performance.

3) A polymer separator, for example, polyethylene (PE) or polypropylene (PP), glass fibre (GF) having coating thickness of 10 pm to 50 pm (micron).

[0053] In the present invention, the terms “energy storage device”, “power cell” and “battery” are considered equivalent and used therefore interchangeably. These terms herein refer to batteries or super-capacitors comprised of at least one cell or a plurality of cells, such as Li-ion cells, connected in series, parallel or combinations thereof. Li-ions move from cathode to anode of the cell during the charge step, moving through the electrolyte. Ions move through separator pores of a nanometric size. Li-ions move from the anode to cathode during the discharge step. The polymer separator is an electric insulator, allowing ions movement via pores but blocking the electrons flow.

[0054] In a particular embodiment, the energy storage device is selected from a nickel/metal hydride batteries, lead-acid batteries, Li-ion batteries and Li-ion polymer batteries. In a specific embodiment, the energy storage device is a Li-ion cell.

[0055] Reference is now made to Fig. 3a showing the scanning electron microscope (SEM, Zeiss) image of Li ions moving into nanocarbon multi-layered material penetrating between carbon layers. Magnification is 25.00k X, scan speed is 1, EHT is 3.0 kV, ESB grid is 0 V, focus is 5.2 mm, aperture size is 30.00 pm, and system vacuum is 3.87 x 10’ ⁶ mbar. Fig. 3b schematically shows the Li ions movement between two adjacent nanocarbon layers of the product of the present invention.

[0056] Reference is now made to Fig. 4a schematically showing the wettability degree between a nanocarbon layer and electrolyte drop. Figs. 4b and 4c show the snapshots from OCA15EC optical contact angle measurements by DataPhysics Instruments GmbH (Germany). By definition, “wetting” or “wettability” is the ability of a liquid to maintain contact with a solid surface, and it is controlled by the balance between the intermolecular interactions of adhesive type (liquid to surface) and cohesive type (liquid to liquid). Wettability is characterised by a “contact angle”, which is the angle at which the liquid-vapor interface meets the solid-liquid interface. The contact angle is determined by the balance between the adhesive and cohesive forces. As the tendency of a drop to spread out over a flat, solid surface increases, the contact angle decreases. Thus, the contact angle provides an inverse measure of wettability. Table 2 below summarises the contact angle measurements of the electrolyte drops to the nanolayered carbon material surface of the present invention.

Table 2. Contact angle measurements of the electrolyte drops to the nanolayered carbon material surface.

Abbreviations and units used in the table: CA - contact angle [°] ; (M) - mean value; (R) - right side; (L) - left side; IFT - interfacial tension [mN/m]; Err - fitting error [pm]; Vol - drop volume [pl].

[0057] Contact angles less than 90° (low contact angle) generally mean that wettability of the surface is favourable, so the fluid will maximise contact with the wetted surface and spread over the entire surface. For water, a wettable surface may also be termed hydrophilic and a non-wettable surface hydrophobic. Superhydrophobic surfaces have contact angles greater than 150°, showing almost no contact between the liquid drop and the surface. Hydrophilic surfaces as in the present invention, have contact angles less than 90°, showing a very tight contact between the liquid drops and the surface. As seen in Figs. 4a-4c, the nanocarbon layer is hydrophilic having the experimentally measured contact angle with the electrolyte drop approximately 30°. In other words, the electrolyte liquid in the present invention forms good contact with the nanocarbon layer and therefore, it spreads over the nanocarbon layers with strong adhesive interactions to these layers. Such high wettability of the electrolyte to the nanolayered carbon material is one of the aspects of the present invention. In some embodiments, a contact angle of drops of the electrolyte to the wetted surface of the carbon layers is less than 90°, or from about 10° to about 40°, or from about 15° to about 30°.

[0058] The electrolyte is added into the cell filling the space between the anode and separator, and between the cathode and separator. The electrolyte is then absorbed into both the cathode and anode coatings. Thus, the electrolyte penetrates into the carbon-based layered material of the present invention within the substrate of the power cell electrodes, thereby significantly enhancing mobility of the Li ions through the substrate and increasing conductivity of the power cell. The present inventors showed that the Li ions are efficiently adsorbed on the surface of the carbon-based layered material of the present invention inside the substrate.

[0059] In yet another embodiment, the present invention is used in non-energy storage devices using electrolyte.

[0060] In a certain embodiment, the carbon-based layered material of the present invention and the electrolyte composition comprising thereof are used in the anode electrolyte substrate for the increased capacity of the anode of the energy storage devices. Non-limiting examples of these devices are supercapacitors of either the aqueous or organic solvent electrolyte types, nickel/metal hydride batteries, lead-acid batteries, Li-ion cells and Li-ion polymer batteries. As mentioned above, the nonlimiting examples of the anode powder comprises graphite, SiCL, Si or compositions of above for increased capacity of the cathode of the energy storage device.

[0061] In a certain embodiment, the carbon-based layered material of the present invention and the electrolyte composition comprising thereof are used in the cathode electrolyte substrate for the increased capacity of the cathode of the energy storage devices. In a particular embodiment, the cathode-based materials comprise the mixture of the carbon-based layered material of the present invention and cathode powder. As mentioned above, the non-limiting examples of the cathode powder comprises NCA, NMC811, NMC622, NMC532, LCO, LFP, LMO for increased capacity of the cathode of the energy storage device.

[0062] In a specific embodiment, the energy storage device comprises the cathode comprising graphite, the anode comprising lithium metal and the electrolyte composition comprising thereof of the present invention filling the power storage device.