CN116315146A - Lead-manganese battery electrolyte and preparation method thereof - Google Patents
Lead-manganese battery electrolyte and preparation method thereof Download PDFInfo
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- CN116315146A CN116315146A CN202310119440.8A CN202310119440A CN116315146A CN 116315146 A CN116315146 A CN 116315146A CN 202310119440 A CN202310119440 A CN 202310119440A CN 116315146 A CN116315146 A CN 116315146A
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- electrolyte
- lead
- manganese
- sulfate
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- 239000003792 electrolyte Substances 0.000 title claims abstract description 36
- 239000011572 manganese Substances 0.000 title claims abstract description 31
- 229910052748 manganese Inorganic materials 0.000 title claims abstract description 28
- 238000002360 preparation method Methods 0.000 title abstract description 7
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 claims abstract description 22
- 239000003115 supporting electrolyte Substances 0.000 claims abstract description 14
- 239000004094 surface-active agent Substances 0.000 claims abstract description 14
- 229940099596 manganese sulfate Drugs 0.000 claims abstract description 12
- 239000011702 manganese sulphate Substances 0.000 claims abstract description 12
- 235000007079 manganese sulphate Nutrition 0.000 claims abstract description 12
- SQQMAOCOWKFBNP-UHFFFAOYSA-L manganese(II) sulfate Chemical compound [Mn+2].[O-]S([O-])(=O)=O SQQMAOCOWKFBNP-UHFFFAOYSA-L 0.000 claims abstract description 12
- PMZURENOXWZQFD-UHFFFAOYSA-L Sodium Sulfate Chemical compound [Na+].[Na+].[O-]S([O-])(=O)=O PMZURENOXWZQFD-UHFFFAOYSA-L 0.000 claims abstract description 6
- 229910052938 sodium sulfate Inorganic materials 0.000 claims abstract description 6
- 235000011152 sodium sulphate Nutrition 0.000 claims abstract description 6
- LZZYPRNAOMGNLH-UHFFFAOYSA-M Cetrimonium bromide Chemical compound [Br-].CCCCCCCCCCCCCCCC[N+](C)(C)C LZZYPRNAOMGNLH-UHFFFAOYSA-M 0.000 claims abstract description 5
- DPKBAXPHAYBPRL-UHFFFAOYSA-M tetrabutylazanium;iodide Chemical compound [I-].CCCC[N+](CCCC)(CCCC)CCCC DPKBAXPHAYBPRL-UHFFFAOYSA-M 0.000 claims abstract description 5
- 239000013504 Triton X-100 Substances 0.000 claims abstract description 4
- 229920004890 Triton X-100 Polymers 0.000 claims abstract description 4
- DPXJVFZANSGRMM-UHFFFAOYSA-N acetic acid;2,3,4,5,6-pentahydroxyhexanal;sodium Chemical compound [Na].CC(O)=O.OCC(O)C(O)C(O)C(O)C=O DPXJVFZANSGRMM-UHFFFAOYSA-N 0.000 claims abstract description 4
- BFNBIHQBYMNNAN-UHFFFAOYSA-N ammonium sulfate Chemical compound N.N.OS(O)(=O)=O BFNBIHQBYMNNAN-UHFFFAOYSA-N 0.000 claims abstract description 4
- 229910052921 ammonium sulfate Inorganic materials 0.000 claims abstract description 4
- 235000011130 ammonium sulphate Nutrition 0.000 claims abstract description 4
- 239000001768 carboxy methyl cellulose Substances 0.000 claims abstract description 4
- GVGUFUZHNYFZLC-UHFFFAOYSA-N dodecyl benzenesulfonate;sodium Chemical compound [Na].CCCCCCCCCCCCOS(=O)(=O)C1=CC=CC=C1 GVGUFUZHNYFZLC-UHFFFAOYSA-N 0.000 claims abstract description 4
- 239000001267 polyvinylpyrrolidone Substances 0.000 claims abstract description 4
- 229920000036 polyvinylpyrrolidone Polymers 0.000 claims abstract description 4
- 235000013855 polyvinylpyrrolidone Nutrition 0.000 claims abstract description 4
- OTYBMLCTZGSZBG-UHFFFAOYSA-L potassium sulfate Chemical compound [K+].[K+].[O-]S([O-])(=O)=O OTYBMLCTZGSZBG-UHFFFAOYSA-L 0.000 claims abstract description 4
- 229910052939 potassium sulfate Inorganic materials 0.000 claims abstract description 4
- 235000011151 potassium sulphates Nutrition 0.000 claims abstract description 4
- 235000019812 sodium carboxymethyl cellulose Nutrition 0.000 claims abstract description 4
- 229920001027 sodium carboxymethylcellulose Polymers 0.000 claims abstract description 4
- 229940080264 sodium dodecylbenzenesulfonate Drugs 0.000 claims abstract description 4
- JRMUNVKIHCOMHV-UHFFFAOYSA-M tetrabutylammonium bromide Chemical compound [Br-].CCCC[N+](CCCC)(CCCC)CCCC JRMUNVKIHCOMHV-UHFFFAOYSA-M 0.000 claims abstract description 4
- 238000000034 method Methods 0.000 claims description 10
- 239000000203 mixture Substances 0.000 claims 1
- 238000003756 stirring Methods 0.000 claims 1
- NUJOXMJBOLGQSY-UHFFFAOYSA-N manganese dioxide Chemical compound O=[Mn]=O NUJOXMJBOLGQSY-UHFFFAOYSA-N 0.000 abstract description 22
- 230000000694 effects Effects 0.000 abstract description 8
- 230000000052 comparative effect Effects 0.000 description 15
- 239000000243 solution Substances 0.000 description 5
- 238000002484 cyclic voltammetry Methods 0.000 description 3
- 238000004146 energy storage Methods 0.000 description 3
- 239000000693 micelle Substances 0.000 description 3
- 239000007774 positive electrode material Substances 0.000 description 3
- 238000009210 therapy by ultrasound Methods 0.000 description 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 2
- 239000002000 Electrolyte additive Substances 0.000 description 2
- DBMJMQXJHONAFJ-UHFFFAOYSA-M Sodium laurylsulphate Chemical compound [Na+].CCCCCCCCCCCCOS([O-])(=O)=O DBMJMQXJHONAFJ-UHFFFAOYSA-M 0.000 description 2
- 239000002253 acid Substances 0.000 description 2
- 239000000654 additive Substances 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- 229910052799 carbon Inorganic materials 0.000 description 2
- 238000000151 deposition Methods 0.000 description 2
- 230000008021 deposition Effects 0.000 description 2
- 238000009826 distribution Methods 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 239000011259 mixed solution Substances 0.000 description 2
- 239000002245 particle Substances 0.000 description 2
- 229940083575 sodium dodecyl sulfate Drugs 0.000 description 2
- 235000019333 sodium laurylsulphate Nutrition 0.000 description 2
- 229910003174 MnOOH Inorganic materials 0.000 description 1
- 229910010967 Ti—Sn Inorganic materials 0.000 description 1
- 230000032683 aging Effects 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 150000001768 cations Chemical class 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 238000005137 deposition process Methods 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 238000004070 electrodeposition Methods 0.000 description 1
- 239000008151 electrolyte solution Substances 0.000 description 1
- 229940021013 electrolyte solution Drugs 0.000 description 1
- 238000004299 exfoliation Methods 0.000 description 1
- 230000002687 intercalation Effects 0.000 description 1
- 238000009830 intercalation Methods 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 229910001437 manganese ion Inorganic materials 0.000 description 1
- 239000011159 matrix material Substances 0.000 description 1
- 230000033116 oxidation-reduction process Effects 0.000 description 1
- 238000011056 performance test Methods 0.000 description 1
- 230000010287 polarization Effects 0.000 description 1
- 239000011148 porous material Substances 0.000 description 1
- 230000001105 regulatory effect Effects 0.000 description 1
- 238000001179 sorption measurement Methods 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 238000010408 sweeping Methods 0.000 description 1
- 230000007704 transition Effects 0.000 description 1
Images
Classifications
-
- 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
- H01M10/08—Selection of materials as electrolytes
-
- 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
- H01M10/12—Construction or manufacture
-
- 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
-
- 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
- H01M2300/0005—Acid electrolytes
- H01M2300/0011—Sulfuric acid-based
-
- 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
Abstract
The invention discloses a lead-manganese battery electrolyte and a preparation method thereof, wherein each liter of the lead-manganese battery electrolyte contains 1-3mol/L of manganese sulfate, 0.1-1.5mol/L of supporting electrolyte, 1.6-5.2g/L of surfactant and 0.1-1mol/L of sulfuric acid. The supporting electrolyte is one or a combination of sodium sulfate, ammonium sulfate and potassium sulfate. The surfactant is one or a combination of more of tetrabutylammonium bromide, tetrabutylammonium iodide, sodium dodecyl benzene sulfonate, cetyltrimethylammonium bromide, polyvinylpyrrolidone, sodium carboxymethyl cellulose and Triton X-100. By using the electrolyte, the conductivity and electrochemical activity of the electrolyte can be effectively enhanced, and the electrochemical activity and reversibility of manganese dioxide can be improved, so that the rate performance and discharge capacity of the lead-manganese battery can be improved.
Description
Technical Field
The invention relates to a lead-manganese battery electrolyte, in particular to an electrolyte additive for improving the discharge capacity and rate capability of a lead-manganese battery and a preparation method thereof.
Background
Lead acid batteries 1859 were invented by the french physicist plurally, which has been a hundred years old since now, due to their low cost, mature technology, and safetyThe full-automatic energy storage system is high in full performance and is widely applied to large-scale energy storage power grids. However, due to the positive electrode active material PbO of lead acid battery 2 Low utilization rate of PbO 2 /PbSO 4 The reaction kinetics is poor, the reaction potential is high in the charge and discharge process, and the volume change is large, so that some unavoidable problems such as grid corrosion, positive electrode aging, falling and the like are caused. For this purpose, mnO-based methods have been proposed 2 /Mn 2+ And PbSO 4 Lead-manganese cell as new chemical cell for Pb redox process and its positive electrode material MnSO 4 Is dissolved in electrolyte, does not need to synthesize positive electrode material, mn 2+ /MnO 2 The reaction can generate oxidation-reduction potential of 1.23Vvs SHE, and the theoretical capacity is up to 616mAh g -1 ，1370F g -1 . The lead-manganese battery has the characteristics of low cost, high safety, long cycle life and high energy density, and is hopeful to become a novel battery technology for large-scale energy storage application.
However, lead-manganese batteries have disadvantages in that the charging process of the lead-manganese battery corresponds to the electrodeposition process of manganese dioxide, and the deposited manganese dioxide has problems such as MnO 2 Exfoliation and deposited MnO 2 Kinetic retardation due to poor electron conductivity of (a) including intercalation of positive ions (formation of Mn 3+ And MnOOH) and phase transition (formation of Mn (OH) 2 ) The electrolyte is required to be added with additives to give a battery with better performance, because it exhibits an uneven voltage distribution during gradual occupying of the crystal lattice, or a large overpotential due to electrochemical polarization, resulting in an influence on the rate capability and discharge capacity. For example, adding sodium sulfate to the electrolyte can provide the deposited manganese dioxide with a larger specific surface area and smaller particle size, improving the reversibility thereof; sodium dodecyl sulfate is added into the electrolyte, so that the porosity of manganese dioxide can be increased, and the capacity fade can be reduced.
Disclosure of Invention
The invention aims to improve the conductivity of electrolyte, enhance the electrochemical activity of the electrolyte and improve the electrochemical activity and reversibility of manganese dioxide by using an electrolyte additive, thereby improving the rate capability and discharge capacity of a lead-manganese battery.
The invention aims at realizing the following technical method:
a lead-manganese battery electrolyte comprising the following components: manganese sulfate, supporting electrolyte, surfactant and sulfuric acid; wherein the electrolyte comprises the following components: 1-3mol/L of manganese sulfate, 0.1-1.5mol/L of supporting electrolyte, 1.6-5.2g/L of surfactant and 0.1-1mol/L of sulfuric acid; the supporting electrolyte is one or a combination of sodium sulfate, ammonium sulfate and potassium sulfate.
Preferably, the surfactant is one or a combination of a plurality of tetrabutylammonium bromide, tetrabutylammonium iodide, sodium dodecyl benzene sulfonate, cetyltrimethylammonium bromide, polyvinylpyrrolidone, sodium carboxymethyl cellulose, triton X-100 and the like.
The preparation method of the lead-manganese battery electrolyte comprises the following steps:
a. and adding supporting electrolyte and surfactant into the sulfuric acid solution with the concentration of 0.1-1mol/L in sequence to prepare the lead-manganese battery electrolyte containing 1-3mol of manganese sulfate, 0.1-1.5mol of supporting electrolyte and 1.6-5.2g of surfactant per liter.
b. The mixed solution is fully stirred at the temperature of 30-50 ℃ until the mixed solution is completely dissolved.
The invention has the beneficial effects that:
(1) The addition of the supporting electrolyte can increase the conductivity of the electrolyte, reduce the charge transfer impedance of the electrolyte and improve the electrochemical activity of the electrolyte, and cations in the supporting electrolyte can be adsorbed on active sites to influence the adsorption of divalent manganese ions and the deposition of manganese dioxide, so that the deposited manganese dioxide in the charging process has larger porosity and higher electrochemical activity.
(2) The surfactant can form micelle between solid-liquid interfaces, the formed micelle can be used as a template in the manganese dioxide deposition process, and the size and morphology of the micelle can be effectively regulated and controlled, so that the deposited manganese dioxide has smaller particle size and better reversibility, and the rate performance and discharge capacity of the battery are improved; surfactants tend to maintain interfacial tension at the surface of the growing electrode, resulting in ordered growth of atoms at the appropriate locations on the electrode surface. The surface of the electrode is formed into a compact deposition layer, the surface area is large, the pore size distribution is narrow, the adhesion force between the electrode and a matrix is enhanced, and the shedding of manganese dioxide is reduced.
Drawings
FIG. 1 is a cyclic voltammogram of example 1 versus comparative example 1.
Fig. 2 is a graph of the ratio performance of example 2 versus comparative example 1.
Fig. 3 is a graph showing the discharge capacity of example 3 compared with that of comparative example 1.
Detailed Description
For a further understanding of the invention, preferred embodiments of the invention are further described below in conjunction with examples. The following examples are only a part of the invention and not all of them.
Example 1
A preparation method of lead-manganese battery electrolyte comprises the steps of preparing 1L of 0.5mol/L sulfuric acid solution, sequentially adding 169g of manganese sulfate and 142g of sodium sulfate, and carrying out ultrasonic treatment at 30 ℃ for 10 minutes.
Example 2
A method for preparing lead-manganese battery electrolyte prepares 1L of 0.8mol/L sulfuric acid solution, 338g of manganese sulfate and 3.38g of hexadecyl trimethyl ammonium bromide are sequentially added into the solution, and ultrasonic treatment is carried out for 10 minutes at 35 ℃.
Example 3
A preparation method of lead-manganese battery electrolyte comprises preparing 1L of 1mol/L sulfuric acid solution, sequentially adding 253.5g of manganese sulfate and 1.69g of tetrabutylammonium iodide, and performing ultrasonic treatment at 45 ℃ for 10 minutes.
Comparative example 1
The electrolyte without additives contained 1M manganese sulfate and 0.5M sulfuric acid.
The electrolytes of comparative example 1, example 2, and example 3 were added to lead-manganese batteries, respectively, and the tests were performed.
1. Cyclic voltammetry test
The carbon felt was subjected to cyclic voltammetry in the electrolyte solutions of example 1 and comparative example 1, and testedThe system is a three-electrode system, the counter electrode is a Ru-Ti-Sn electrode, the working electrode is a carbon felt, and the reference electrode is Hg/Hg 2 SO 4 Electrode with a sweeping speed of 10mV s -1 The potential window is 0.1V-0.75V. The CV chart of example 1 was denoted as true 1, and the CV chart of comparative example 1 was denoted as pair 1. CV diagrams of example 1 and comparative example 1 are shown in fig. 1.
2. And (3) multiplying power performance test:
the lead-manganese cell to which the electrolyte of example 2, comparative example 1 was added was charged to 1mAh cm at 1.8V -2 Then at 10mA cm -2 、30mAcm -2 、50mAcm -2 、100mA cm -2 The current density of (2) was discharged to a voltage of 1V, and the rate performance was measured. The magnification curve of example 2 is denoted as true 2, and the magnification curve of comparative example 1 is denoted as pair 1. The ratio performance curve pairs of example 2 and comparative example 1 are shown in fig. 2.
3. Discharge capacity test:
the lead-manganese cell charged with the electrolyte of example 3, comparative example 1 was charged to 268mAh at 1.8V and then at 0.5mA cm -2 The discharge was performed at a current density of 1V, and a discharge curve was recorded. The discharge curve of example 3 is denoted as true 3, and the discharge curve of comparative example 1 is denoted as pair 1. The discharge curve pairs of example 3 and comparative example 1 are shown in fig. 3.
From the experimental results of example 1, example 2, example 3 and comparative example 1, the electrochemical activity of the lead-manganese battery electrolyte and the rate capability and discharge capacity of the lead-manganese battery can be effectively improved.
The test results show that the electrochemical activity of the electrolyte and the discharge capacity and the multiplying power performance of the battery are not greatly different from those of the examples by replacing sodium sulfate in example 1, cetyltrimethylammonium bromide in example 2 and tetrabutylammonium iodide in example 3 with any one of ammonium sulfate, potassium sulfate, tetrabutylammonium bromide, sodium dodecylbenzenesulfonate, sodium dodecylsulfate, polyvinylpyrrolidone, sodium carboxymethyl cellulose and Triton X-100.
The above examples are only some of the preferred embodiments of the present invention in all examples, and should not be construed as limiting the invention, and the skilled person can make various changes thereto, and any equivalent or similar changes to the present invention shall be covered by the scope of the claims of the present invention.
Claims (4)
1. A lead-manganese battery electrolyte, characterized in that the electrolyte comprises the following components: manganese sulfate, supporting electrolyte, surfactant and sulfuric acid; wherein the electrolyte comprises the following components: 1-3mol/L of manganese sulfate, 0.1-1.5mol/L of supporting electrolyte, 1.6-5.2g/L of surfactant and 0.1-1mol/L of sulfuric acid; the supporting electrolyte is one or a combination of sodium sulfate, ammonium sulfate and potassium sulfate.
2. The lead-manganese battery electrolyte according to claim 1, wherein the surfactant is one or a combination of several of tetrabutylammonium bromide, tetrabutylammonium iodide, sodium dodecylbenzene sulfonate, cetyltrimethylammonium bromide, polyvinylpyrrolidone, sodium carboxymethyl cellulose and Triton X-100.
3. The method for preparing the lead-manganese battery electrolyte according to claim 1, which is characterized by comprising the following steps:
sequentially adding manganese sulfate, supporting electrolyte and surfactant into sulfuric acid solution with the concentration of 0.1-1mol/L, and uniformly mixing, so that each liter of lead-manganese battery electrolyte contains 1-3mol of manganese sulfate, 0.1-1.5mol of supporting electrolyte and 1.6-5.2g of surfactant.
4. The method for preparing the lead-manganese battery electrolyte according to claim 3, wherein the temperature of the mixture is 30-50 ℃ by stirring.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202310119440.8A CN116315146A (en) | 2023-02-16 | 2023-02-16 | Lead-manganese battery electrolyte and preparation method thereof |
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202310119440.8A CN116315146A (en) | 2023-02-16 | 2023-02-16 | Lead-manganese battery electrolyte and preparation method thereof |
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| Publication Number | Publication Date |
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| CN116315146A true CN116315146A (en) | 2023-06-23 |
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| CN202310119440.8A Pending CN116315146A (en) | 2023-02-16 | 2023-02-16 | Lead-manganese battery electrolyte and preparation method thereof |
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| Country | Link |
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| CN (1) | CN116315146A (en) |
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2023
- 2023-02-16 CN CN202310119440.8A patent/CN116315146A/en active Pending
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