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WO2021234597A1 - Procédés destinés à produire de l'énergie électrique à partir d'oxyde de graphène réduit au moyen de l'énergie ambiante, piles et systèmes associés - Google Patents

Procédés destinés à produire de l'énergie électrique à partir d'oxyde de graphène réduit au moyen de l'énergie ambiante, piles et systèmes associés Download PDF

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Publication number
WO2021234597A1
WO2021234597A1 PCT/IB2021/054322 IB2021054322W WO2021234597A1 WO 2021234597 A1 WO2021234597 A1 WO 2021234597A1 IB 2021054322 W IB2021054322 W IB 2021054322W WO 2021234597 A1 WO2021234597 A1 WO 2021234597A1
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Prior art keywords
rgo
cell
coal
solution
alkali
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Inventor
Sabyasachi Sarkar
Ankit SAMANTA
Debashish Bhattacharjee
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Tata Steel Ltd
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Tata Steel Ltd
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
    • H01M4/583—Carbonaceous material, e.g. graphite-intercalation compounds or CFx
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M12/00—Hybrid cells; Manufacture thereof
    • H01M12/04—Hybrid cells; Manufacture thereof composed of a half-cell of the fuel-cell type and of a half-cell of the primary-cell type
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0002—Aqueous electrolytes
    • H01M2300/0014—Alkaline electrolytes
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries

Definitions

  • the present disclosure relates to the field of electricity generation. It relates to a method for producing electrical energy, a cell for producing electrical energy, and a system comprising a plurality of said cells. Particularly, the present disclosure relates to all the aspects to produce electrical energy from carbonaceous material using ambient energy.
  • Plant photosynthesis involves two connected complimentary events where, in the first phase, visible sun light initiates the release of electrons that reduce CO2 to sugar and in its complimentary phase, splitting of water by a manganese cluster supplies electrons to the holes to balance the electrons consumed in the reduction process.
  • the release of oxygen in such water splitting process is a bonus for the nature and led to the evolution of respiration-based animal kingdom.
  • the present disclosure relates to a method for producing electrical energy comprising reacting reduced graphene oxide (rGO) with oxygen in presence of ambient energy, wherein the rGO is impregnated with alkali.
  • rGO reduced graphene oxide
  • the present disclosure also relates to a cell comprising: a) an anode comprising reduced graphene oxide (rGO), wherein the rGO is impregnated with an alkali solution; b) means for introducing oxygen into the cell; and c) a cathode.
  • rGO reduced graphene oxide
  • the present disclosure further provides a system comprising a plurality of the cells as described above, wherein the plurality of cells is connected in series or in parallel or a combination thereof.
  • Figure 1 shows the detection of potential of about 460 mV in presence of air whereas negligible potential was detected in presence of argon.
  • Figure 2A shows a hysteresis plot of Temperature vs Potential (voltage) and Figure 2B shows a hysteresis plot of Temperature vs Current in two consecutive cyclic scans from 5°C to 65°C showing the temperature effect on the output of the associated chemical reactions.
  • Figures 3A and 3B show exemplary embodiments of a system comprising a plurality of cells with series and parallel connections to glow a LED lamp and to drive a DC motor.
  • Figure 4A shows a graph of current vs layers of coal containing rGO and Figure 4B shows a graph of current vs surface area of coal containing rGO.
  • Figure 5 shows cells covered with different coloured filters.
  • the top row shows cells covered with red, yellow, and blue colored transparent sheets from left to right; middle row shows cells covered with green colored transparent sheet and white transparent sheets from left to right; and the last row shows cells covered with a black sheet.
  • Figure 6A shows the spectrophotometric analysis of formic acid
  • Figure 6B shows a standard calibration curve of sodium formate
  • Figure 6C shows a yellow brown coloration developed on the Whatman filter paper (using iodide oxidation) indicating the generation of peroxide during the redox reaction.
  • Figures 7(a)-7(d) show analysis of purified low-grade coal: a) FT-IR spectrum, b) Raman spectrum, c) XRD patter and d) TEM image.
  • Figures 8(a)-8(d) show analysis of isolated GO from low-grade coal: a) FT-IR spectrum, b) Raman spectrum, c) XRD pattern and d) TEM image.
  • Figures 9(a)-9(d) show analysis of rGO from low-grade coal: a) FT-IR spectrum, b) Raman spectrum, c) XRD pattern and d) TEM image.
  • Figures 10(a)-10(d) show analysis of recovered GO after few hours of cell reaction: a) FT-IR spectrum, b) Raman spectrum, c) XRD patter and d) TEM image.
  • Figure 11A depicts the picture of a cell
  • Figure 11B depicts an exemplary embodiment of a system comprising a plurality of cells wherein the individual cells are connected in series to produce higher voltage
  • Figure 11C depicts an exemplary embodiment of a system comprising a plurality of cells wherein the individual cells are connected in parallel to produce higher current
  • Figure 12 depicts an exemplary embodiment of a system comprising a plurality of cells wherein the individual cells are connected in parallel and series to produce higher voltage and current (individual cell voltage - 450mV; individual cell current - 10mA).
  • Figure 13 depicts an exemplary embodiment of a system comprising a plurality of cells wherein the individual cells are arranged in stacks to generate 12 volt and 3A, (36W).
  • ambient energy refers to different forms of natural energies possessed by the surface of the earth or present in the earth’s atmosphere, without active addition of thermal or other energy forms.
  • the term encompasses any and all forms of energies, including, but not limited to, electromagnetic energy, solar energy, radiant energy, thermal energy, or a combination thereof.
  • ambient temperature refers to a temperature of the earth’s atmosphere. In some embodiments, ambient temperature ranges from about 5°C to about 65°C.
  • impregnation or “impregnated” refers to soaking, saturation, coating, or infusion of rGO or source comprising rGO with an alkali.
  • the inventors have found that carbonaceous materials could be oxidized by aerial oxygen in presence of an electrolyte under atmospheric conditions to generate electricity.
  • reduced graphene oxide (rGO) present in carbonaceous materials like coal can react with oxygen in the presence of ambient energy in the earth’s atmosphere to generate electricity at the ambient temperatures.
  • the present disclosure provides a method for producing electricity that mimics the redox cycle of aerobic respiration in mammals.
  • the present inventors have found that the specific carbon containing compound viz. reduced graphene oxide (rGO) present in carbonaceous materials like coal can be oxidized by reacting with oxygen in presence of ambient energy and an electrolyte such as an alkali to produce electricity.
  • rGO reduced graphene oxide
  • an electrolyte such as an alkali
  • the first step in this composite cycle is the interaction of rGO with triplet oxygen (aerial or pure) under ambient energy to produce ⁇ rG0*
  • This step activates oxygen to its singlet state to produce a second adduct, ⁇ rG0 +
  • the second adduct participates in electron transfer to generate the charge transfer exciton, ⁇ rG0 ⁇
  • the second adduct in presence of a hydroxide (OH " ) radical produces a HO2 " radical and a ⁇ rGO + OIT ⁇ adduct
  • the ⁇ rGO OIT ⁇ adduct reacts with the HO2 " radical to produce graphene oxide (GO), a formate ion (HCO2 " ), and a carbonate ion (CO3 2" ).
  • the GO in the presence of the ambient energy and a OH " radical regenerates the rGO to complete the cycle.
  • the redox steps of aerial oxygen on reacting with rGO under ambient energy forming singlet oxygen, superoxide and finally hydroperoxide ion have been experimentally verified as described in the examples below.
  • the present disclosure provides a method for producing electrical energy comprising reacting reduced graphene oxide (rGO) with oxygen in presence of ambient energy, wherein the rGO is impregnated with an alkali.
  • the rGO is in pure form, or a source comprising rGO, or a combination thereof.
  • rGO is naturally present in carbonaceous materials like coal.
  • a source comprising rGO is a carbonaceous material.
  • a carbonaceous material comprising rGO includes charred grass, charred dry leaves, charred wood charcoal, and coal.
  • a source comprising rGO is soot obtained by burning a vegetable or mineral oil.
  • a source comprising rGO is an exhaust or soot generated by combustion of fuel such as exhaust from automobiles or soot collected from chimneys.
  • a source comprising rGO is coal.
  • coal comprising rGO can be a low-grade coal to a high-grade coal including lignite, sub-bituminous coal, bituminous coal and anthracite coal.
  • coal employed in the methods and cells of the invention is selected from the group consisting of sub-bituminous coal, bituminous coal, anthracite coal, coking coal, non- coking coal, and any combination thereof.
  • any grade of coking coal can be employed.
  • Grades I-IV of coking coal are employed.
  • non-coking coal of Grades A to G is used.
  • the coal is first oxidized to increase the content of rGO and then employed in the methods and products of the disclosure.
  • oxygen that reacts with rGO can be pure oxygen, aerial oxygen, or a combination thereof.
  • the reaction of rGO with oxygen takes place in presence of ambient energy.
  • ambient energy refers to these forms of energies which include, but are not limited to, electromagnetic energy, solar energy, radiant energy, thermal energy, or a combination thereof. It is noted that no source of energy (thermal or otherwise) is actively provided for the reaction of rGO with oxygen to take place.
  • the reaction of rGO with oxygen takes place in presence of electromagnetic energy. In some embodiments, the reaction of rGO with oxygen takes place in presence of solar energy. In some embodiments, the reaction of rGO with oxygen takes place in presence of radiant energy. In some embodiments, radiant energy comprises radiations having a wavelength ranging from about 100 nm to about 2500 nm. In some embodiments, radiant energy comprises cosmic radiations on the surface of the earth. In some embodiments, the reaction of rGO with oxygen takes place in presence of thermal energy. In some embodiments, the reaction of rGO with oxygen takes place in presence of global warming of the earth’s atmosphere. In this embodiment, global warming of the earth’s atmosphere is a form of ambient energy.
  • the reaction of rGO with oxygen takes place in presence of a combination of any of these energies.
  • rGO in the reaction of rGO with oxygen, rGO is impregnated with an alkali.
  • the alkali maintains a pH of at least 12.
  • the alkali maintains a pH of about 12 or more.
  • the alkali maintains a pH of about 12 to about 14.
  • the alkali maintains a pH of about 11.8, 11.9, 12, 12.1, 12.2, 12.3, 12.4, 12.5, 12.6, 12.7, 12.8, 12.9, 13, 13.1, 13.2, 13.3, 13.4, 13.5, 13.6, 13.7, 13.8, 13.9, or 14.
  • the pH of 12 or more helps in: i) increasing the stability of a superoxide anion and thus, increases the life of the exciton with spatial separation between the electron and hole, and ii) generating the potent oxidant HO2 " radical.
  • the hydroperoxide oxidation of rGO + involves a moulting process where rGO’s peripheral carbonyl groups are removed in the form of carbonate and formate to complete the cycle.
  • the inventors have quantified the extrusion of peripheral carbons, present as carbonyl groups in rGO, in the form of carbonate and formate.
  • a mass loss of carbon to the tune of about 5% has been measured when a cell in accordance with the invention was run for 30 days, day and night.
  • the overall redox potential of such a system has been measured around 0.430 mV at 25°C, which slightly varies with temperature.
  • the alkali is an alkali solution having a concentration of at least 1M. In some embodiments, the alkali solution has a concentration of about 1M or more. In some embodiments, the alkali solution has a concentration of about 1M, about 1.25M, about 1.5M, about 1.75M, about 2M, about 2.25M, about 2.5M, about 2.75M, about 3M, about 3.25M, about 3.5M, about 3.75M, or about 4M, including values and ranges thereof. In some embodiments, the alkali solution has a concentration of about 1M to about 4M.
  • the amount of alkali is about 10% to about 25%, including all values and ranges therebetween, by weight of the total weight of the rGO or the source containing rGO and the alkali. In some embodiments, the amount of alkali is about 10%, about 15%, about 20%, or about 25% by weight of the total weight of the rGO or the source containing rGO and the alkali.
  • the alkali is an alkali or alkaline earth metal oxide; alkali or alkaline earth metal hydroxide; alkali or alkaline earth metal carbonates; quaternary ammonium hydroxides or carbonates such as tetraalkyl ammonium hydroxide, tetraaryl ammonium hydroxide, tetraalkyl ammonium carbonate; asymmetric tetraalkyl ammonium salt; or asymmetric tetraalkyl phosphonium salt, alone or a combination thereof, or in combination with a neutral electrolyte.
  • alkali metal oxides include lithium oxide, sodium oxide, potassium oxide, rubidium oxide, and caesium oxide.
  • alkaline earth metal oxides include beryllium oxide, magnesium oxide, calcium oxide, strontium oxide, barium oxide, and radium oxide.
  • alkali metal hydroxides include lithium hydroxide, sodium hydroxide, potassium hydroxide, rubidium hydroxide, and caesium hydroxide.
  • alkaline earth metal hydroxides include beryllium hydroxide, magnesium hydroxide, calcium hydroxide, strontium hydroxide, barium hydroxide, and radium hydroxide.
  • tetraalkyl ammonium hydroxides include tetramethyl ammonium hydroxide, tetrabutyl ammonium hydroxide, and the like.
  • tetraaryl ammonium hydroxides include tetraphenyl ammonium hydroxide and the like.
  • alkali metal carbonates include lithium carbonate, sodium carbonate, potassium carbonate, rubidium carbonate, and caesium carbonate.
  • alkaline earth metal carbonates include beryllium carbonate, magnesium carbonate, calcium carbonate, strontium carbonate, barium carbonate.
  • tetraalkyl ammonium carbonates include tetramethyl ammonium carbonate, tetrabutyl ammonium hydroxide, and the like.
  • the alkali is an asymmetric tetraalkyl ammonium salt such as a cetyltrialkyl ammonium salt. In some embodiments, the alkali is an asymmetric tetraalkyl phosphonium salt. In some embodiments, a combination of these alkalis is used. In some embodiments, any of these alkalis are used in combination with a neutral electrolyte.
  • the alkali is selected from the group consisting of sodium hydroxide, potassium hydroxide, sodium carbonate, potassium carbonate, and combinations thereof. In some embodiments, any of these alkalis are used in combination with a neutral electrolyte.
  • the method of the present disclosure is carried out at an ambient temperature.
  • ambient temperature refers to a temperature of the earth's atmosphere.
  • the ambient temperature is the temperature of surroundings.
  • the ambient temperature is room temperature.
  • ambient temperature ranges from about 5°C to about 65°C, about 5°C to about 60°C, about 5°C to about 55°C, about 5°C to about 50°C, about 5°C to about 45°C, about 5°C to about 40°C, about 10°C to about 65°C, about 10°C to about 60°C, about 10°C to about 55°C, about 10°C to about 50°C, about 10°C to about 45°C, about 10°C to about 40°C, about 15°C to about 65°C, about 15°C to about 60°C, about 15°C to about 55°C, about 15°C to about 50°C, about 15°C to about 45°C, about 15°C to about 40°C, about 20°C to about 65°C, about 20°C to about 60°C, about 20°C to about 55°C, about 20°C to about 50°C, about 20°C to about 45°C, about 20°C to about 40°C, about 20°C to about 65°C
  • the ambient temperature is about 5°C, about 10°C, about 15°C, about 20°C, about 25°C, about 30°C, about 35°C, about 40°C, about 45°C, about 50°C, about 55°C, or about 65°C.
  • the current invention does not require any external source of heat as it works well at ambient temperature however this cannot be construed as limitation since the current process can work well beyond 65°C as well.
  • the ambient temperature is more than 65°C, for example, up to about 200°C.
  • the ambient temperature is about 70°C, 75°C, 80°C, 85°C, 90°C, 95°C, 100°C, 105°C, 110°C, 115°C, 120°C, 125°C, 130°C, 135°C, 140°C, 145°C, 150°C, 155°C, 160°C, 165°C, 170°C, 175°C, 180°C, 185°C, 190°C, 195°C, or 200°C.
  • the methods described above provide a voltage of about 450 mV and a current of about 2 mA from one unit of 500 mg coal (GO/rGO) cell.
  • a pure 50 mg of GO/rGO sample isolated from coal generates about 6 mA current and a voltage of about 460 mV.
  • the present disclosure also provides an electrochemical cell that employs the method described above to produce electrical energy or electricity.
  • the cell comprises: (a) an anode comprising reduced graphene oxide (rGO), wherein the rGO is impregnated with an alkali solution; (b) means for introducing oxygen into the cell; and (a) a cathode.
  • rGO impregnated with an alkali solution acts as an anode.
  • the rGO is in pure form, or a source comprising rGO, or a combination thereof.
  • rGO is naturally present in carbonaceous materials like coal. Accordingly, in some embodiments, a source comprising rGO is a carbonaceous material. In some embedments, a source comprising rGO is coal.
  • coal comprising rGO can be a low-grade coal to a high-grade coal including lignite, sub-bituminous coal, bituminous coal and anthracite coal.
  • coal employed in the cells of the invention is selected from the group consisting of sub-bituminous coal, bituminous coal, anthracite coal, coking coal, non-coking coal, and any combination thereof.
  • any grade of coking coal can be employed.
  • Grades I-IV of coking coal are employed.
  • non-coking coal of Grades A to G is used.
  • the coal is first oxidized to increase the content of rGO and then employed in the cells of the disclosure.
  • the alkali solution is a solution of an alkali or alkaline earth metal oxide; a solution of alkali or alkaline earth metal hydroxide; a solution of alkali or alkaline earth metal carbonates; a solution of a quaternary ammonium hydroxide or carbonate such as a solution of tetraalkyl ammonium hydroxide, a solution of tetraaryl ammonium hydroxide, a solution of tetraalkyl ammonium carbonate; a solution of asymmetric tetraalkyl ammonium salt or a solution of asymmetric tetraalkyl phosphonium salt, alone or a combination thereof or in combination with other neutral electrolyte.
  • alkali metal oxides include lithium oxide, sodium oxide, potassium oxide, rubidium oxide, and caesium oxide.
  • alkaline earth metal oxides include beryllium oxide, magnesium oxide, calcium oxide, strontium oxide, barium oxide, and radium oxide.
  • alkali metal hydroxides include lithium hydroxide, sodium hydroxide, potassium hydroxide, rubidium hydroxide, and caesium hydroxide.
  • alkaline earth metal hydroxides include beryllium hydroxide, magnesium hydroxide, calcium hydroxide, strontium hydroxide, barium hydroxide, and radium hydroxide.
  • tetraalkyl ammonium hydroxides include tetramethyl ammonium hydroxide, tetrabutyl ammonium hydroxide, and the like.
  • tetraaryl ammonium hydroxides include tetraphenyl ammonium hydroxide and the like.
  • alkali metal carbonates include lithium carbonate, sodium carbonate, potassium carbonate, rubidium carbonate, and caesium carbonate.
  • alkaline earth metal carbonates include beryllium carbonate, magnesium carbonate, calcium carbonate, strontium carbonate, and barium carbonate.
  • tetraalkyl ammonium carbonates include tetramethyl ammonium carbonate, tetrabutyl ammonium hydroxide, and the like.
  • the alkali solution is a solution of an asymmetric tetraalkyl ammonium salt such as a solution of cetyltrialkyl ammonium salt.
  • the alkali solution is a solution of an asymmetric tetraalkyl phosphonium salt.
  • a combination of these alkalis is used.
  • any of these alkali solutions are used in combination with a neutral electrolyte.
  • the alkali solution is selected from the group consisting of sodium hydroxide solution, potassium hydroxide solution, sodium carbonate solution, potassium carbonate solution, and combinations thereof. In some embodiments, any of these alkali solutions are used in combination with a neutral electrolyte. In some embodiments, the alkali solution maintains a pH of at least 12. In some embodiments, the alkali solution maintains a pH of about 12 or more. In some embodiments, the alkali solution maintains a pH of about 12 to about 14.
  • the alkali solution maintains apH of about 11.8, 11.9, 12, 12.1, 12.2, 12.3, 12.4, 12.5, 12.6, 12.7, 12.8, 12.9, 13, 13.1, 13.2, 13.3, 13.4, 13.5, 13.6, 13.7, 13.8, 13.9, or 14.
  • the alkali solution has a concentration of at least 1M. In some embodiments, the alkali solution has a concentration of about 1M or more. In some embodiments, the alkali solution has a concentration of about 1M, about 1.25M, about 1.5M, about 1.75M, about 2M, about 2.25M, about 2.5M, about 2.75M, about 3M, about 3.25M, about 3.5M, about 3.75M, or about 4M, including values and ranges thereof. In some embodiments, the alkali solution has a concentration of about 1M to about 4M.
  • the amount of alkali solution is about 10% to about 25%, including all values and ranges therebetween, by weight of the total weight of the rGO or the source containing rGO and the alkali solution. In some embodiments, the amount of alkali solution is about 10%, about 15%, about 20%, or about 25% by weight of the total weight of the rGO or the source containing rGO and the alkali solution.
  • the alkali solution employed in the cell is a solution comprising any of the above-mentioned alkalis at any of the concentration and pH values mentioned above and present at any of the weight percentages mentioned above.
  • the cell comprises means for introducing oxygen or air into the cell allowing oxygen to react with rGO and the oxygen is introduced into the cell by any means.
  • the means for introducing oxygen into the cell comprise one or more pores made into the cell.
  • the terms “pores”, “perforations”, “holes” could be used interchangeably to refer to the openings made into the cell to allow passage of oxygen, pure or aerial.
  • oxygen is introduced into the cell passively, i.e., entry of oxygen is not under pressure.
  • the cathode comprises graphite. In some embodiments, cathode comprises a noble metal. In some embodiments, the noble metal is platinum, gold, or a combination thereof.
  • the anode and the cathode of the cell are connected by a conductive material.
  • the anode and the cathode are connected by metallic connectors or wires comprising a conductive material.
  • said conductive material is selected from the group consisting of copper, aluminum, tin, iron, nickel, cobalt, silver, platinum, gold, any noble metal, and combinations thereof.
  • the direction of the flow of electrons is from anode/rGO (negative) to cathode (positive).
  • one end of one of the conductive materials is connected to the anode (rGO) and one end of the other conductive material is connected to the cathode.
  • the other ends of the conductive materials can be connected to a load to be powered from the cell.
  • the electrons flow through the electrical path powering the load.
  • the cell of the present disclosure works like a conventional cell configured to power a load.
  • the load may have positive and negative terminals and the terminals of the load can be connected to the anode/rGO and the cathode, respectively.
  • an Light Emitting Diode LED
  • the LED can have a positive terminal and a negative terminal.
  • the positive terminal of the LED can be connected to the cathode and the negative terminal of the LED can be connected to the anode/rGO.
  • a motor powering a fan can be connected to the cell.
  • a plurality of cells can be connected in parallel to enable maximum current to flow through the load.
  • a plurality of cells can be connected in series to maintain a constant current and resultant voltage supplied to the load is a sum of voltage of each cell.
  • sodium ions or potassium ions or the corresponding metal ions of the alkali used in the cell
  • the corresponding formate salt which gets deposited in the cell reducing the efficiency of the cell.
  • Deposits of formate salts need to be removed as well as fresh supply of alkali needs to be provided to the cell.
  • deposits of formate salts can be removed by simply washing the cell with water and the cell can be recharged with a fresh alkali solution. The washed solution containing dissolved formate salt on evaporation can yield solid residue of the formate salt, which is a valuable by-product.
  • the cell attachment is modular in a cartridge form whereby the old (used) cell is readily exchanged with a new one and the old cell is regenerated by proper washing and refilling with alkali.
  • the amount of electric current generated by the cell increases as the surface area of rGO or the thickness or layers of rGO increases until the diffusion of oxygen through rGO is no longer possible.
  • FIG. 3A shows that the electric current increases as the number of layers of coal comprising rGO increases. However, the current does not increase after a certain number of layers of coal, as the diffusion of oxygen through the increasing number of layers is no longer possible.
  • FIG. 3B further shows that the current increases as the surface area of rGO increases.
  • rGO is present in the form of layers and each layer has a thickness ranging from about 0.1 mm to 0.3 mm (100 ⁇ to 300 ⁇ ), including all values and ranges therebetween. In some embodiments, each layer of rGO has a thickness of about 100 ⁇ , about 125 ⁇ , about 150 ⁇ , about 175 ⁇ , about 200 ⁇ , about 225 ⁇ , about 250 ⁇ , about 275 ⁇ , or about 300 ⁇ .
  • the cell can be constructed in any shape.
  • the cell can be of a rectangular shape, square shape, circular shape, oval shape, cylindrical shape, cube shape, cuboid shape, sheet type, a collective sheet type forming a book of different sizes, and the likes.
  • the cell is constructed from any suitable material.
  • the cell is constructed of a plastic material.
  • the plastic material is selected from the group consisting of polypropylene, polyethylene, polystyrene, polyvinyl chloride, polyamide, polyester, polyurethane, and a combination thereof.
  • the present disclosure also provides systems comprising a plurality of cells.
  • Each of said cells comprises features as described above.
  • the plurality of cells can be connected in various configurations.
  • the plurality of cells are connected in series.
  • the plurality of cells are connected in parallel.
  • a first plurality of cells are connected in series, a second plurality of cells are connected in parallel, and the first and the second plurality of cells are connected in series or in parallel.
  • Figures 1 IB, llC, 12, and 13 show exemplary embodiments of systems comprising a plurality of cells in various configurations encompassed by the present disclosure.
  • the methods, cells, and systems disclosed herein provide many advantages. Firstly, the present methods, cells, and systems are environmental-friendly and contribute to the field of green technology. In particular, the disclosure provides for very low-cost, energy efficient and green energy employed methods, cells, and systems for generating electricity. For example, electrical energy is generated by harnessing ambient energy present in the surroundings of the cell and no separate/actively added energy source is required for the functioning of the methods, cells, and systems of the present disclosure. This saves costs and resources required for providing a separate energy source.
  • the present methods, cells and systems are also advantageous over conventional methods for generating electricity such as methods involving combustion of coal (which requires fiiel and high temperature burning for combustion and contributes to air pollution), solar-powered cells (high cost of silicon-based raw material, availability of sunlight), etc.
  • the present simple ambient energy induced rGO-oxygen reaction allows to produce electrical energy that is operative day and night as well as indoors and outdoors.
  • the methods, cells, and systems of the present disclosure are operated at an ambient temperature, i.e., the temperature of the atmosphere surrounding the cell. While the amount of current produced varies with the temperature surrounding the cell, such variations can be mitigated by connecting a plurality of cells in series, in parallel, or a combination thereof.
  • Example 1 Oxveen for generation of electricity
  • a cell was constructed by placing sub-bituminous coal containing 8% by weight of reduced graphene oxide (rGO) (anode) in a perforated (allowing air to pass) polypropylene container with graphite (cathode) at the bottom.
  • the coal was impregnated with saturated NaOII solution.
  • a copper wire was placed in the coal impregnated with NaOH and a second copper wire was connected to the graphite.
  • the copper wires act as terminals and the ends of the copper wires were connected to a LED bulb.
  • Two such cells were constructed and placed inside small Erlenmeyer flasks. The mouth of the two flasks were properly sealed with septum and glue.
  • Example 2 Temperature dependency of voltage and current To understand the effect of temperature on voltage and current, the cell was constructed as described in Example 1. The temperature was varied from 5°C to 65°C and the hysteresis plots shown in Figures 2A and 2B were generated. A hysteresis plot is generated based on a heating cycle and a cooling cycle in the given temperature range (5-65°C). Two such consecutive cycles result in four readings at a given temperature. The purpose of plotting hysteresis plots is to see if there is a lag between input and output in a system upon a change in direction. Voltage showed a smaller variation as the temperature of the surrounding changes ( Figure 2A), whereas current showed a larger variation with the temperature ( Figure 2B).
  • the spread of the coal layers comprising rGO was calculated based on the amount of coal spread over a given surface area. Based on this, an approximate number of layers of the coal and the thickness of the layers were calculated. It was determined that the thickness of approximately three to four layers was about 0.5 mm.
  • the current increased with the number of layers of coal comprising rGO. However, after 15 layers (5 mg mass spread over 1 cm 2 area), the current value did not change. The current did not increase after 15 layers of coal, as air could not diffuse further through the layers.
  • Figure 4B shows that the current increases as the surface area of coal containing rGO increases.
  • a polypropylene container having 4.5 cm diameter and 1 cm height with lots of pores on its surface to pass air was prepared.
  • a circular graphite sheet (0.25 mm thick) (cathode) connected with a copper wire (metallic connector) was placed at its bottom.
  • Powdered low-grade coal (anode) washed by acetone and hydrochloric acid (2.5g) was placed on the graphite sheet inside the container and a copper wire (metallic connector) was placed on the top to function as an electrode.
  • This coal powder was impregnated with saturated NaOH solution to constitute a cell.
  • Such cells were also constructed in an Eppendorf vial where the amount of coal taken was 0.5 g-
  • Example 5 Radiant energy for eeneration of electricity
  • Example 6 Generation of intermediates and by-products
  • reaction for producing electrical energy by reacting rGO with oxygen in presence of ambient energy wherein the rGO is impregnated with an alkali
  • several intermediates and by-products are formed as follows:
  • Detection of formate The concentration of formic acid produced from the cell reaction was measured by measuring the amount of formate. For this, a pre-determined amount of rGO was taken in a test tube containing 50% aqueous NaOH solution (10 mL). Fresh air, freed from atmospheric carbon dioxide and other environmental gases by bubbling through 3 M hydrochloric acid followed by 10% sodium hydroxide, was allowed to bubble through the NaOH solution containing rGO for 10 days using an aquarium pump.
  • Coal contains naturally formed GO and rGO.
  • coal was purified to remove impurities; naturally occurring rGO was converted to GO using a nitric acid treatment; GO was extracted using an alkali and converted to rGO.
  • Low grade coal in powdered form was first freed from aromatic hydrocarbons and other soluble organic compounds by repeatedly washing with acetone, using
  • Figures 9A-9C show the FT-IR spectrum, Raman spectrum, and the X-ray diffraction patter and Figure 9D shows the transmission electron micrograph (TEM) of the rGO.
  • the FT-1R spectra, Raman spectra, and the X-ray diffraction patterns from Figures 7, 8, and 9 show the characteristic signature of rGO indicating that rGO is naturally present in coal.
  • the TEM for each sample visually shows the morphology of these samples and indicates that the samples comprise nano carbon domain retaining graphitic structures.
  • Figures 10A- lOC show the FT-TR spectrum, Raman spectrum, and the X-ray diffraction patter and Figure 10D shows the transmission electron micrograph (TEM) of the recovered GO after few hours of cell reaction.
  • Figure 10 shows that the rGO is still present and the cell can be further operated.
  • FTIR and Raman spectra were recorded using JASCO FT/IR-4000 Series machine using KBr disk and LabRam HR 800 Raman Spectrometer respectively.
  • TEM mages were taken on FEI, TECHNAJ-T-20 machine attached with EDAX operated on the voltage at 200 kV. Electrochemical measurements were carried out with BioLogic SP-150 Potentiostats/Galvanostats. INCORPORATION BY REFERENCE

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Abstract

La présente invention concerne des procédés, une pile, et des systèmes destinés à générer de l'électricité en faisant réagir l'oxyde de graphène réduit (rGO) avec de l'oxygène en présence de l'énergie ambiante et d'un électrolyte. Le présent procédé est écologique, économe en énergie, et économique lorsqu'on le compare à des procédés conventionnels destinés à générer de l'électricité comme la combustion de charbon, des piles à puissance solaire, etc.
PCT/IB2021/054322 2020-05-20 2021-05-19 Procédés destinés à produire de l'énergie électrique à partir d'oxyde de graphène réduit au moyen de l'énergie ambiante, piles et systèmes associés Ceased WO2021234597A1 (fr)

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Citations (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2016036607A1 (fr) * 2014-09-02 2016-03-10 Graphene 3D Lab Inc. Dispositifs électrochimiques comprenant des matériaux en carbone nanoscopiques conçus par fabrication additive

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2016036607A1 (fr) * 2014-09-02 2016-03-10 Graphene 3D Lab Inc. Dispositifs électrochimiques comprenant des matériaux en carbone nanoscopiques conçus par fabrication additive

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
CHENG HUHU, HUANG YAXIN, ZHAO FEI, YANG CE, ZHANG PANPAN, JIANG LAN, SHI GAOQUAN, QU LIANGTI: "Spontaneous power source in ambient air of a well-directionally reduced graphene oxide bulk", ENERGY & ENVIRONMENTAL SCIENCE, vol. 11, no. 10, 10 October 2018 (2018-10-10), pages 2839 - 2845, XP055874852, ISSN: 1754-5692, DOI: 10.1039/C8EE01502C *

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