CN108666500B - Preparation method of glass fiber partition plate for dual-functional lead-carbon battery - Google Patents
Preparation method of glass fiber partition plate for dual-functional lead-carbon battery Download PDFInfo
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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
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
- H01M50/403—Manufacturing processes of separators, membranes or diaphragms
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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
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/06—Lead-acid accumulators
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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
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
- H01M10/4235—Safety or regulating additives or arrangements in electrodes, separators or electrolyte
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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
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
- H01M50/409—Separators, membranes or diaphragms characterised by the material
- H01M50/431—Inorganic material
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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
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
- H01M50/409—Separators, membranes or diaphragms characterised by the material
- H01M50/44—Fibrous material
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
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Abstract
The invention discloses a preparation method of a glass fiber separator for a lead-carbon battery with dual functions of in-situ pore increasing and negative hydrogen evolution inhibition, which comprises the steps of firstly preparing glass fiber separator slurry, and then adding an in-situ pore increasing and negative hydrogen evolution inhibition dual-function additive; diluting with dilute sulfuric acid, adjusting the pH value, filtering and forming the slurry to obtain a semi-finished product of the glass fiber separator, and drying, cutting edges, slicing and the like to prepare the glass fiber separator for the lead-carbon battery with the dual functions of in-situ pore increasing and negative electrode hydrogen evolution inhibition. The invention adds and evenly distributes the additive particles with acid-soluble in-situ pore increasing and negative hydrogen evolution inhibiting functions between the glass fiber partition boards and is used between the positive and negative electrodes of the lead-carbon battery, when acid is added in the lead-carbon battery manufacturing process, micron-sized bifunctional additive particles in the partition boards are dissolved, released ions are directionally adsorbed and electroreduced and deposited on the surface of a carbon material in the charging process, the hydrogen evolution overpotential of the negative electrode is improved, the hydrogen evolution side reaction is inhibited, and the self-discharge of the battery during the storage period is reduced.
Description
Technical Field
The invention relates to the technical field of lead-carbon batteries, in particular to a preparation method of a glass fiber separator for a lead-carbon battery with dual functions of in-situ pore increasing and negative hydrogen evolution inhibition.
Background
The lead-carbon battery is a negative-electrode capacitance type lead-acid battery, has the characteristics of both a lead storage battery and a super capacitor, not only exerts the advantage of instantaneous high-current charging of the super capacitor, but also exerts the advantage of specific energy of the lead-acid battery. However, the lead-carbon battery has the characteristics that the negative electrode introduces carbon materials and is subjected to heavy-current charging and discharging work, so that the problems that the negative electrode is easy to generate hydrogen during battery storage or charging and the oxygen recombination efficiency is reduced under heavy-current charging exist.
The oxygen recombination of the lead storage battery means that the valve-controlled lead storage battery adopts a safety valve seal and an ultrafine glass fiber clapboard to absorb electrolyte, and simultaneously, a proper proportion of positive and negative active substances is designed, so that in the final charging stage of the battery, oxygen is firstly separated out from a positive electrode, passes through pores of a glass fiber diaphragm and is transmitted to a negative electrode, reacts with active lead of the negative electrode to generate lead oxide, the lead oxide reacts with sulfuric acid to generate lead sulfate and water, and the lead sulfate is charged to generate lead, so that oxygen byproducts generated by electrolyzing water in the positive electrode charging process are reduced into water in the negative electrode, and through reasonable design, the oxygen recombination efficiency of the common lead storage battery can reach more than 97. Due to the characteristics of heavy-current charging and discharging work of the lead-carbon battery, when the lead-carbon battery is charged by heavy current, the amount of oxygen separated out from the positive electrode is large, the oxygen recombination efficiency is reduced to 90% or even lower, and in addition, the hydrogen separation of the negative electrode of the lead-carbon battery is obvious compared with the negative electrode of a common lead-acid battery, so that the water loss of the lead-carbon battery in the charging and discharging process is aggravated integrally, and the phenomenon of damaging the battery such.
Aiming at the problem of hydrogen evolution self-discharge caused by a carbon material, researchers effectively improve the problem by taking measures of hydrogen evolution inhibition modification on the carbon material of the negative electrode active material of the lead-carbon battery, addition of an additive in lead paste and the like. The problem of oxygen recombination efficiency reduction under the condition of large-current charging of the battery can be improved and solved by increasing the oxygen channel of the partition plate or arranging a catalytic plug in theory. The catalyst suppository is made of rare metal and is expensive; by applying the method of increasing the oxygen channel of the separator (the plane aperture is 10-25 μm, and the average aperture is 10-15 μm after three-dimensional superposition), the battery pole group assembly pressure is large, and a large number of pores are easy to cause deformation and even collapse of the separator, so that the current distribution during charging and discharging is influenced, and further lead dendrite and other adverse effects are caused. Therefore, the existing improvement of the glass fiber separator is mostly based on the nanometer pore increasing technology.
Disclosure of Invention
The invention aims to solve the defects that the lead-carbon battery in the prior art has hydrogen evolution self-discharge, is easy to dehydrate due to quick charge and floating charge overcharge, further causes thermal runaway and the like, and provides a preparation method of a glass fiber separator for the lead-carbon battery with dual functions of in-situ pore increasing and negative hydrogen evolution inhibition.
The preparation method of the glass fiber separator for the lead-carbon battery with the dual functions of in-situ pore increasing and negative electrode hydrogen evolution inhibition is characterized by comprising the following steps:
1) preparing glass fiber separator slurry: adding water, superfine glass fiber, common glass fiber, sodium silicate, organic polymer fiber and fibrous Al into a stirrer in sequence2O3Spherical Al2O3Stirring and pulping to obtain glass fiber partition plate slurry;
2) adding an in-situ pore-increasing and negative hydrogen evolution inhibition dual-function additive into the glass fiber separator slurry obtained in the step 1);
3) diluting the slurry obtained in the step 2) by using dilute sulfuric acid, adjusting the pH value, and continuously stirring;
4) filtering and molding the slurry obtained in the step 3) to obtain a semi-finished product of the glass fiber partition plate with the water content of 30-50 wt%;
5) and (3) drying, cutting edges, slicing and the like of the semi-finished product of the glass fiber separator in the step 4) to prepare the glass fiber separator for the lead-carbon battery with the dual functions of in-situ hole increasing and negative electrode hydrogen evolution inhibition.
The preparation method of the glass fiber separator for the lead-carbon battery with the dual functions of in-situ pore increasing and hydrogen evolution inhibition at the negative electrode is characterized in that the fibrous Al in the step 1)2O3Spherical Al2O3All have alpha-type crystal structures.
The preparation method of the glass fiber separator for the lead-carbon battery with the dual functions of in-situ pore increasing and hydrogen evolution inhibition at the negative electrode is characterized in that the diameter of the superfine glass fiber in the step 1) is 0.5-1.5 mu m; ordinary glass fiber, organic polymer fiber, and fibrous Al2O3Are all 1.5 to 3 mu m in diameter and are spherical Al2O3The particle size is 5 to 20 μm.
The preparation method of the glass fiber separator for the lead-carbon battery with the double functions of in-situ pore increasing and hydrogen evolution inhibition at the negative electrode is characterized in that the feeding mass of the sodium silicate in the step 1) is 1-3% of the total mass of the superfine glass fiber, the common glass fiber and the organic polymer fiber, and SiO is used2And (6) counting.
The preparation method of the glass fiber separator for the lead-carbon battery with the double functions of in-situ pore increasing and hydrogen evolution inhibition at the negative electrode is characterized in that the auxiliary agent in the step 1) is one or more of sodium dodecyl sulfate, polyacrylamide, sodium tripolyphosphate and sodium hexametaphosphate.
The preparation method of the glass fiber separator for the lead-carbon battery with the dual functions of in-situ pore increasing and negative electrode hydrogen evolution inhibition is characterized in that the fibrous Al2O3Spherical Al2O3The feeding mass ratio of the in-situ pore-increasing and negative electrode hydrogen evolution inhibition dual-functional additive to the raw material is 1: 5-10: 3-6; fibrous Al2O3Spherical Al2O3The total feeding amount of the double-function additive for in-situ pore increasing and negative electrode hydrogen evolution inhibition is 3-5% of the total mass of the superfine glass fiber, the common glass fiber and the organic polymer fiber.
The preparation method of the glass fiber partition board for the lead-carbon battery with the dual functions of in-situ pore increasing and negative electrode hydrogen evolution inhibition is characterized in that the in-situ pore increasing and negative electrode hydrogen evolution inhibition dual-function additive in the step 2) selects a material which can be dissolved in the lead storage battery electrolyte and can inhibit hydrogen evolution, the material comprises one or more of stannous oxide, indium oxide and bismuth oxide, and the particle size of the in-situ pore increasing and negative electrode hydrogen evolution inhibition dual-function additive is 5-20 mu m.
The preparation method of the glass fiber separator for the lead-carbon battery with the dual functions of in-situ pore increasing and negative electrode hydrogen evolution inhibition is characterized in that the grain diameter of the additive with the dual functions of in-situ pore increasing and negative electrode hydrogen evolution inhibition in the step 2) is 5-20 mu m.
The preparation method of the glass fiber separator for the lead-carbon battery with the dual functions of in-situ pore increasing and negative electrode hydrogen evolution inhibition is characterized in that the concentration of dilute sulfuric acid in the step 3) is 5-10%; and adjusting the pH value of the slurry to 5-6.
The high-efficiency oxygen composite water loss prevention lead-carbon battery is characterized in that the glass fiber partition plate for the lead-carbon battery with the dual functions of in-situ pore increasing and negative hydrogen evolution inhibition, which is prepared by the method, is arranged between the positive electrode and the negative electrode of the lead-carbon battery.
By adopting the technology, compared with the prior art, the invention has the following beneficial effects:
1) in the preparation process of the glass fiber separator pulp, acid-soluble in-situ pore increasing and negative hydrogen evolution inhibiting bifunctional additive are added, so that the additive particles are uniformly distributed among formed separator fibers, after acid is added to lead carbon of the glass fiber separator for the lead carbon battery prepared by the invention between a positive electrode and a negative electrode, micron-sized bifunctional additive particles in the separator can be dissolved to form secondary micron-sized pores which are regularly distributed, the oxygen recombination efficiency can be effectively improved, and meanwhile, ions dissolved by the bifunctional additive can be adsorbed on the surface of a negative active material or subjected to electro-reduction deposition in the battery formation charging process, the hydrogen evolution overpotential is improved, and the self-discharge of the battery is reduced;
2) in order to prevent the deformation and even collapse of the separator after the dissolution of the bifunctional additive particles under the assembly pressure of a large battery pole group due to a large number of pores, further influence the current distribution during the charge and discharge of the battery and cause the adverse consequences of lead dendrites and the like, the invention arranges the micron-sized fibrous and spherical Al2O3Mixing, adding, uniformly dispersing in the separator to play a role in supporting and filling, enhancing the strength of the separator, simultaneously adding a proper amount of sodium silicate in the preparation and pulping process of the separator, and adjusting the pH value of the slurry by using dilute sulfuric acid to form a gel state, thereby preventing micron-sized Al from appearing in the process of slurry storage and forming of the separator2O3The sedimentation distribution of the particles of the bifunctional additive is not uniform;
3) the invention adds and evenly distributes the additive particles with acid-soluble in-situ pore increasing and negative hydrogen evolution inhibiting functions between the glass fiber partition boards and is used between the positive and negative electrodes of the lead-carbon battery, when acid is added in the lead-carbon battery manufacturing process, micron-sized bifunctional additive particles in the partition boards are dissolved, released ions are directionally adsorbed and electroreduced and deposited on the surface of a carbon material in the charging process, the hydrogen evolution overpotential of the negative electrode is improved, the hydrogen evolution side reaction is inhibited, and the self-discharge of the battery during the storage period is reduced.
Detailed Description
The following description is merely exemplary in nature and is not intended to limit the present disclosure, application, or uses. The following is a further description of a specific embodiment of the method for preparing a glass fiber separator for a lead-carbon battery with dual functions of in-situ pore formation and hydrogen evolution inhibition at the negative electrode.
In the invention, the acid-soluble in-situ pore-increasing and negative hydrogen evolution inhibiting bifunctional additive is added in the pulping process of preparing the glass fiber separator, so that the particles of the additive are uniformly distributed among the fibers of the formed separator. After acid is added in the manufacturing process of the lead-carbon battery, micron-sized bifunctional additive particles in the partition plate can be dissolved to form secondary micron-sized pores which are regularly distributed, and ions dissolved by the bifunctional additive can be adsorbed, electroreduced or deposited on a negative electrode in the formation and charging process of the battery, so that the hydrogen evolution overpotential of the negative electrode is improved, and the self-discharge of the battery is reduced.
In the actual use process, because the assembly pressure of the battery pole group is large, along with the continuous dissolution of the bifunctional additive particles, the pores in the separator are easy to deform or even collapse, the current distribution during charging and discharging is influenced, and the adverse consequences such as lead dendrite and the like are further caused. The invention uses micron-sized fibrous and spherical Al2O3Is compatible with the bifunctional additive particles to be used as a composite additive, and when the bifunctional additive particles are dissolved, the micron-sized Al2O3Can play a role of supporting the framework.
Example 1:
adding 200mL of water, 50g of superfine glass fiber with the diameter of 0.5-1.5 mu m, 40g of common glass fiber with the diameter of 1.5-3 mu m and 5g of Na into a stirrer in sequence2SiO3·9 H2O, 5g of organic Polymer fiber, 0.3g of fibrous Al2O33g of spherical Al2O3Stirring and pulping 1.5g of SnO and 0.5g of sodium dodecyl sulfate for 10min, diluting the pulp with 5% dilute sulfuric acid, adjusting the pH value to 6, and continuing stirring for 30 min; and then, carrying out vacuum filtration on the slurry until no liquid drops drop and form in a filter opening within 10s (the water content of the partition plate is measured to be 33%).
The formed separator is finally dried, cut into edges, sliced and the like to prepare an AGM separator product, and the modified glass fiber separator has the maximum aperture of 13 mu m, the porosity of 82 percent and the capillary acid absorption height of 81mm/5min through detection.
Fixing the two sides of the glass fiber separator with plastic wire mesh, and dripping 1.28g/cm3Is washed with a 5% FeCl solution3And (5) checking the solution, rinsing the solution for 2 times by using distilled water after the solution does not change into green, and measuring the porosity of the partition again after drying to reach 89%.
The glass fiber separator is applied to a 12V 50Ah lead-carbon battery plate wrapping sheet, after the battery is assembled through subsequent assembly procedures and manufactured, the oxygen recombination efficiency is tested to reach 95%, and after the battery is placed for 90 days (5-35 ℃), the capacity of the battery is directly tested to be 43.2Ah (2 hour rate) without electricity supplement.
Example 2:
adding 200mL of water, 50g of superfine glass fiber with the diameter of 0.5-1.5 mu m, 40g of common glass fiber with the diameter of 1.5-3 mu m and 10 g of Na into a stirrer in sequence2SiO3·9 H2O, 5g of organic Polymer fiber, 0.3g of fibrous Al2O32g of spherical Al2O3Stirring and pulping 1g of SnO and 0.5g of sodium dodecyl sulfate for 10min, diluting the pulp with 5% dilute sulfuric acid, adjusting the pH value to 6, and continuing stirring for 30 min; and then, carrying out vacuum filtration on the slurry until no liquid drops drop and forming within 10s of a filter opening (the water content of the partition plate is measured to be 36%).
The formed separator is finally dried, cut into edges, sliced and the like to prepare an AGM separator product, and the modified glass fiber separator has the maximum aperture of 13 mu m, the porosity of 80 percent and the capillary acid absorption height of 79mm/5min through detection.
Fixing the two sides of the glass fiber separator with plastic wire mesh, and dripping 1.28g/cm3Is washed with a 5% FeCl solution3And (5) checking the solution, rinsing the solution for 2 times by using distilled water after the solution does not change into green, and measuring the porosity of the partition again after drying to reach 86%.
The glass fiber separator is applied to a 12V 50Ah lead-carbon battery plate wrapping sheet, after the battery is assembled through subsequent assembly procedures and manufactured, the oxygen recombination efficiency is tested to reach 93%, and after the battery is placed for 90 days (5-35 ℃), the capacity of the battery is directly tested to be 42.9Ah (2 hour rate) without electricity supplement.
Example 3:
adding 200mL of water, 50g of superfine glass fiber with the diameter of 0.5-1.5 mu m, 40g of common glass fiber with the diameter of 1.5-3 mu m and 5g of Na into a stirrer in sequence2SiO3·9 H2O, 5g of organic Polymer fiber, 0.3g of fibrous Al2O33g of spherical Al2O3Stirring and pulping 1.5g of bismuth oxide and 0.5g of sodium hexametaphosphate for 10min, diluting the pulp with 5% dilute sulfuric acid, adjusting the pH value to 6, and continuing stirring for 30 min; then the slurry is filtered in vacuum until the filter opening is not available within 10sThe droplets were formed (separator water content was measured to be 33%).
The formed separator is finally dried, cut into edges, sliced and the like to prepare an AGM separator product, and the modified glass fiber separator has the maximum aperture of 12 mu m, the porosity of 80 percent and the capillary acid absorption height of 80mm/5min through detection.
Fixing the two sides of the glass fiber separator with plastic wire mesh, and dripping 1.28g/cm3The washing solution is detected by 10 percent KI solution, when no yellow complex is generated, the washing solution is rinsed for 2 times by distilled water, and the porosity of the clapboard is detected again after drying, and reaches 88 percent.
The glass fiber separator is applied to a 12V 50Ah lead-carbon battery plate wrapping sheet, after the battery is assembled through subsequent assembly procedures and manufactured, the oxygen recombination efficiency is tested to reach 95%, and after the battery is placed for 90 days (5-35 ℃), the capacity of the battery is directly tested to be 43.0Ah (2 hour rate) without electricity supplement.
The preparation method of the glass fiber separator for the lead-carbon battery with the functions of in-situ pore increasing and negative hydrogen evolution inhibition comprises any combination of the parts in the specification. These combinations are not described in detail herein for the sake of brevity and clarity, but the scope of the invention, which is defined by any combination of the parts constructed in this specification, will become apparent after review of this specification.
Claims (10)
1. A preparation method of a glass fiber separator for a lead-carbon battery with dual functions of in-situ pore increasing and negative electrode hydrogen evolution inhibition is characterized by comprising the following steps:
1) preparing glass fiber separator slurry: adding water, superfine glass fiber, common glass fiber, sodium silicate, organic polymer fiber and fibrous Al into a stirrer in sequence2O3Spherical Al2O3Stirring and pulping to obtain glass fiber partition plate slurry;
2) adding an in-situ pore-increasing and negative hydrogen evolution inhibition dual-function additive into the glass fiber separator slurry obtained in the step 1);
3) diluting the slurry obtained in the step 2) by using dilute sulfuric acid, adjusting the pH value, and continuously stirring;
4) filtering and molding the slurry obtained in the step 3) to obtain a semi-finished product of the glass fiber partition plate with the water content of 30-50 wt%;
5) and (3) drying, cutting edges and slicing the semi-finished product of the glass fiber separator in the step 4) to prepare the glass fiber separator for the lead-carbon battery with dual functions of in-situ hole increasing and negative electrode hydrogen evolution inhibition.
2. The method for preparing the glass fiber separator for the lead-carbon battery with the functions of in-situ pore increasing and hydrogen evolution inhibition at the negative electrode according to claim 1, wherein the fibrous Al in the step 1)2O3Spherical Al2O3All have alpha-type crystal structures.
3. The method for preparing the glass fiber separator for the lead-carbon battery with the functions of in-situ pore increasing and hydrogen evolution inhibition at the negative electrode according to claim 1, wherein the diameter of the superfine glass fiber in the step 1) is 0.5-1.5 μm; ordinary glass fiber, organic polymer fiber, and fibrous Al2O3Are all 1.5 to 3 mu m in diameter and are spherical Al2O3The particle size is 5 to 20 μm.
4. The method for preparing the glass fiber separator for the lead-carbon battery with the dual functions of in-situ pore increasing and hydrogen evolution inhibition at the negative electrode as claimed in claim 1, wherein the mass of the sodium silicate fed in the step 1) is 1-3% of the total mass of the superfine glass fiber, the common glass fiber and the organic polymer fiber, and SiO is used2And (6) counting.
5. The method for preparing the glass fiber separator for the lead-carbon battery with the functions of in-situ pore increasing and hydrogen evolution inhibition and negative electrode as claimed in claim 1, wherein the auxiliary agent in the step 1) is one or more of sodium dodecyl sulfate, polyacrylamide, sodium tripolyphosphate and sodium hexametaphosphate.
6. The in situ pore-increasing as in claim 1And a preparation method of the glass fiber separator for the lead-carbon battery with the double functions of inhibiting hydrogen evolution of the negative electrode, which is characterized in that the fibrous Al2O3Spherical Al2O3The feeding mass ratio of the in-situ pore-increasing and negative electrode hydrogen evolution inhibition dual-functional additive to the raw material is 1: 5-10: 3-6; fibrous Al2O3Spherical Al2O3The total feeding amount of the double-function additive for in-situ pore increasing and negative electrode hydrogen evolution inhibition is 3-5% of the total mass of the superfine glass fiber, the common glass fiber and the organic polymer fiber.
7. The method for preparing the glass fiber separator for the lead-carbon battery with the dual functions of in-situ pore increasing and negative hydrogen evolution inhibition according to claim 1, wherein the dual-function additive for in-situ pore increasing and negative hydrogen evolution inhibition in the step 2) is a material which is soluble in the lead storage battery electrolyte and can inhibit hydrogen evolution, and comprises one or more of stannous oxide, indium oxide and bismuth oxide, and the particle size of the dual-function additive for in-situ pore increasing and negative hydrogen evolution inhibition is 5-20 μm.
8. The method for preparing the glass fiber separator for the lead-carbon battery with the dual functions of in-situ pore increasing and negative hydrogen evolution inhibition according to claim 1, wherein the grain size of the additive with the dual functions of in-situ pore increasing and negative hydrogen evolution inhibition in the step 2) is 5-20 μm.
9. The method for preparing the glass fiber separator for the lead-carbon battery with the functions of in-situ pore increasing and hydrogen evolution inhibition at the negative electrode according to claim 1, wherein the concentration of dilute sulfuric acid in the step 3) is 5-10%; and adjusting the pH value of the slurry to 5-6.
10. The high-efficiency oxygen composite water loss prevention lead-carbon battery is characterized in that the glass fiber separator for the lead-carbon battery with dual functions of in-situ pore increasing and negative hydrogen evolution inhibition, which is prepared according to any one of claims 1 to 9, is arranged between the positive electrode and the negative electrode of the lead-carbon battery.
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