CN113178575A - Lead-acid storage battery negative electrode lead paste and bipolar horizontal lead-acid storage battery containing same - Google Patents
Lead-acid storage battery negative electrode lead paste and bipolar horizontal lead-acid storage battery containing same 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
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
- H01M4/56—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of lead
- H01M4/57—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of lead of "grey lead", i.e. powders containing lead and lead oxide
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- B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
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- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/06—Lead-acid accumulators
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- H—ELECTRICITY
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- H01M4/14—Electrodes for lead-acid accumulators
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- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
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- H—ELECTRICITY
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- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M4/628—Inhibitors, e.g. gassing inhibitors, corrosion inhibitors
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- H—ELECTRICITY
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- 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
- H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
- H01M2004/027—Negative electrodes
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Abstract
The invention belongs to the technical field of lead-acid storage batteries, and particularly relates to a lead paste for a negative electrode of a lead-acid storage battery and a bipolar horizontal lead-acid storage battery containing the same. The lead-acid storage battery negative electrode lead plaster comprises the following components: lead powder (1000 + -10) kg with density of (1.40 + -0.005) g/cm at 20 deg.C3The components comprise 84 plus or minus 2 kg of sulfuric acid, 110 plus or minus 5 kg of pure water, 4.5 plus or minus 0.03 kg of valonea extract, 2 plus or minus 0.02 kg of plant tanning agent, 2.2 plus or minus 0.02 kg of acetylene black, 2.5 plus or minus 0.02 kg of sodium lignosulfonate, 1 plus or minus 0.02 kg of short fiber and barium carbonate, wherein the addition amount of the components is 5-10% of the mass of lead powder. The negative electrode lead paste of the inventionBarium carbonate reacts with dilute sulfuric acid to generate barium sulfate instead of directly adding barium sulfate, the barium sulfate reacts with the dilute sulfuric acid in the paste to generate barium sulfate with the average particle size of about 0.02um, the barium sulfate with small particle size can be highly dispersed in active substances, the specific surface area of the active substances is increased, the utilization rate of the active substances is increased, and the initial capacity of the storage battery is improved.
Description
Technical Field
The invention belongs to the technical field of lead-acid storage batteries, and particularly relates to a lead paste for a negative electrode of a lead-acid storage battery and a bipolar horizontal lead-acid storage battery containing the same.
Background
For years, the research direction of lead-acid storage batteries is always to increase the utilization rate of active substances and improve the initial capacity of the storage batteries, and the utilization rate of the active substances is difficult to improve under the original production process and conditions.
Disclosure of Invention
The invention aims to provide a lead-acid storage battery negative electrode lead plaster and a preparation method thereof, so as to improve the utilization rate of active substances.
According to one aspect of the invention, the negative electrode lead paste of the lead-acid storage battery comprises the following components: lead powder (1000 + -10) kg with density of (1.40 + -0.005) g/cm at 20 deg.C3The components comprise 84 plus or minus 2 kg of sulfuric acid, 110 plus or minus 5 kg of pure water, 4.5 plus or minus 0.03 kg of valonea extract, 2 plus or minus 0.02 kg of plant tanning agent, 2.2 plus or minus 0.02 kg of acetylene black, 2.5 plus or minus 0.02 kg of sodium lignosulfonate, 1 plus or minus 0.02 kg of short fiber and barium carbonate, wherein the addition amount of the components is 5-10% of the mass of lead powder.
Therefore, the negative electrode lead paste uses barium carbonate to react with dilute sulfuric acid to generate barium sulfate instead of directly adding barium sulfate, the effect is that barium carbonate reacts with dilute sulfuric acid in the paste to generate barium sulfate with the average particle size of about 0.02um, barium sulfate with small particle size can be highly dispersed in the active substance, the specific surface area of the active substance is increased, the utilization rate of the active substance is increased, and the initial capacity of the storage battery is improved.
Meanwhile, the cathode uses barium carbonate, when barium carbonate reacts with sulfuric acid, part of produced carbon dioxide forms carbonate, and the carbonate reacts with saturated lead ions on the surface of the electrode during low-temperature large-current discharge to generate lead carbonate with high activity, so that passivation of the cathode is avoided, electrochemical behavior is enhanced, and low-temperature large-current discharge capacity is improved.
In some embodiments, a lead-acid battery negative lead paste comprises the following components: lead powder (1000 + -10) kg with a density of 1.40g/cm at 20 deg.C3The tanning agent comprises 84 plus or minus 2 kg of sulfuric acid, 110 plus or minus 5 kg of pure water, 7 plus or minus 0.09 kg of barium carbonate, 4.5 plus or minus 0.03 kg of valonea extract, 2 plus or minus 0.02 kg of plant tanning agent, 2.2 plus or minus 0.02 kg of acetylene black, 2.5 plus or minus 0.02 kg of sodium lignosulphonate and 1 plus or minus 0.02 kg of short fibers.
In some embodiments, the lead powder has an oxidation level of 80-82% and an apparent density of 1.3-1.4g/cm3。
In some embodiments, the plant tanning agent is commercially available, mainly extracted from chestnut shells, eucalyptus bark, gordon euryale seeds, echinacea leaves, pomegranate rind and other plants, and is rich in resources, easily available in raw materials and convenient for large-scale production. Thus, the valonea extract is used as a bulking agent together with a vegetable tanning agent.
In some embodiments, the staple fibers comprise at least one of polyester, acrylic, polypropylene fibers; the length of the short fiber is 3-5 mm.
According to another aspect of the invention, a preparation method of a lead-acid storage battery negative electrode lead paste is provided, which comprises the following steps: adding barium carbonate, lignin, carbon black, oak baking gum, plant tanning agent and short fiber, adding pure water for 4-5min, stirring for 2-3min, adding lead powder for 3-4min, mixing and stirring for 2-3min, adding dilute sulfuric acid, stirring for 15-17min while adding, and stirring for 7-8min after the acid is added; performing paste mixing by using a paste mixer under the following conditions: the rotating speed is 115-125 r/m, and the temperature of the paste is controlled within the range of 65-70 ℃. Therefore, the 4BS generation amount in the lead plaster is excessive when the temperature of the lead plaster is too high, the charging of the storage battery is difficult, and the cycle life of the storage battery is reduced; the rotating speed is more than 125 rpm, the uniformity of the lead paste in the paste mixer is influenced, and the consistency of the performance of the accumulator plate is influenced.
In the actual production process, barium carbonate is added into the lead paste formula to react to generate barium sulfate, so that in order to promote the smooth reaction, barium carbonate powder is required to be used and fully stirred, the paste mixing temperature is required to be 65-70 ℃, and the rotating speed is 115-125 revolutions per minute, so as to avoid generating barium sulfate insoluble substances to cover the surface of barium carbonate and prevent the further reaction; wherein, the mesh number of the barium carbonate powder is 325-400 meshes.
The cathode lead paste uses barium carbonate to replace leadAdding barium sulfate, the solubility of barium carbonate is greater than that of barium sulfate, during the preparation of lead plaster with barium carbonate, the dilute sulfuric acid first reacts with lead oxide plaster to release heat, the temperature can gradually reach above 60 ℃, at the moment, the reaction of dilute sulfuric acid and barium carbonate is accelerated, barium sulfate and water are generated by the reaction, and CO is released2The lead paste is formed with pores, the specific area of the lead paste is increased, and the active substances participating in the reaction are increased, so that the capacity of the storage battery is improved.
Meanwhile, the barium sulfate produced by the reaction is nano barium sulfate particles with small particle size and narrow distribution, the average particle size is about 20nm, the smaller the barium sulfate particle size is, the smaller the average particle size of lead sulfate after discharge is, and the higher the initial capacity is.
In addition, highly dispersed barium sulfate generated by the reaction exists in the negative electrode active material, and can serve as a crystal center of lead sulfate during discharge. Because the lead sulfate can be crystallized and separated on the isomorphous barium sulfate, lead sulfate crystal nucleus does not need to be formed, and the supersaturation degree required for forming the crystal nucleus is not generated. PbSO produced under conditions of low supersaturation4Is relatively loose and porous and is beneficial to H2SO4The concentration polarization is mitigated.
The presence of barium sulfate leads to a product of PbSO4Not on lead but on barium sulphate, so that the active substance lead is not PbSO4The barium sulfate is covered by the passivation layer, so that the passivation effect is delayed, lead sulfate which cannot perform charge-discharge reversible reaction is generated in the passivation of the storage battery, the active substance quantity is reduced in the passivation of the storage battery, the capacity of the storage battery is reduced, and the starting capability is reduced.
Wherein, the cathode is easy to be passivated when the storage battery discharges under low temperature and large current density. The reason for the passivation of the negative plate is that the negative active material is converted into the nucleation rate of lead sulfate, and the nucleation rate of lead ions entering the electrolyte at a great rate cannot be kept up with the nucleation rate of lead ions entering the electrolyte at a great rate, so that the lead ions staying on the surface of the electrode have great saturation, and compared with the condition of adopting normal discharge current at normal temperature, a great number of lead sulfate crystal nuclei with small size are formed, and the lead sulfate forms a compact layer with small gaps on the surface of the electrode.
Barium sulfate also has the effect of preventing the specific surface area of lead from shrinking during the charging of the battery. Since barium sulfate is inert and does not participate in the redox process of the electrode, it is highly dispersed in the active material, mechanically separating lead from lead or lead sulfate, making it less likely to coalesce between particles, thereby maintaining a developed specific surface area of the electrode material.
The invention also provides a bipolar horizontal lead-acid storage battery, and the negative lead plaster of the bipolar horizontal lead-acid storage battery is the lead-acid storage battery negative lead plaster.
Detailed Description
The present invention will be described in further detail with reference to specific examples. Unless otherwise specified, the starting materials used in the present invention are commercially available.
Example 1
The lead-acid storage battery negative electrode lead paste is prepared by the following steps:
(1) the following components are prepared by weight: lead powder (1000 +/-10) kg, density of 1.40g/cm3The tanning agent comprises 84 plus or minus 2 kg of sulfuric acid, 110 plus or minus 5 kg of pure water, 7 plus or minus 0.09 kg of barium carbonate, 4.5 plus or minus 0.03 kg of valonea extract, 2 plus or minus 0.02 kg of plant tanning agent, 2.2 plus or minus 0.02 kg of acetylene black, 2.5 plus or minus 0.02 kg of sodium lignosulphonate and 1 plus or minus 0.02 kg of short fibers;
(2) firstly adding barium carbonate, sodium lignosulphonate, acetylene black, valonea baking gum, a plant tanning agent and short fibers, then adding pure water for 4min, carrying out wet stirring for 2min, then adding lead powder for 3min, mixing and stirring for 2min, then adding dilute sulfuric acid, stirring for 15min while adding, and stirring for 7min after adding acid;
(3) performing paste mixing by using a paste mixer under the following conditions: the rotating speed is 120 r/min, and the temperature of the paste is controlled within the range of 65-70 ℃.
Comparative example 1
The negative electrode lead paste of comparative example 1 was prepared by changing the barium carbonate component in example 1 to a barium sulfate component (commercially available, having a particle size of about 20 um), changing the paste rotation speed to 60 rpm, and controlling the paste temperature to 55 to 60 ℃.
Comparative example 2
The rotating speed of the neutralization paste in the example 1 is changed to 60 revolutions per minute, the temperature of the neutralization paste is controlled within the range of 55-60 ℃, and the negative lead paste of the comparative example 2 is prepared under the same other conditions and formula.
Comparative example 3
The temperature of the neutralization paste in the embodiment 1 is controlled within the range of 55-60 ℃, and the negative lead paste of the comparative example 3 is prepared under the same conditions and formula.
| Barium sulfate content (%) | Barium carbonate content (%) | Speed of mixing paste (rotation/minute) | Lead paste temperature (. degree. C.) | |
| 1 | 0.7 | 0 | 60 | 55-60 |
| 2 | 0 | 0.7 | 60 | 55-60 |
| 3 | 0 | 0.7 | 120 | 55-60 |
| 4 | 0 | 0.7 | 120 | 65-70 |
The capacity was measured as shown in table 1.
TABLE 1 comparison of capacities of different examples
| Example 1 | Comparative example 1 | Comparative example 2 | Comparative example 3 | |
| Initial capacity (Ah) | 116.8 | 100 | 106.5 | 110.2 |
| Utilization (%) | 63.5 | 50.1 | 58.2 | 59.7 |
The comparison shows that the mixing paste condition of the invention is favorable for converting barium carbonate into barium sulfate, the mixing paste temperature is increased to be favorable for 4BS production, the initial performance of the battery can be improved, and the service life of the battery can be prolonged. If no barium sulfate crystal nucleus with the grain diameter of 0.02um is formed, the size of the 4BS crystal is larger and is between 5um and 100um, the formation of the battery is influenced, and the utilization rate of the active substance is reduced. The barium sulfate crystal nucleus provides a crystallization center for the 4BS, so that the 4BS crystal size is reduced, and the utilization rate of the lead paste active material is improved.
Meanwhile, the applicant also tests the influence of the particle size of barium sulfate on the capacity of the storage battery, wherein commercially available barium sulfate is adopted, the currently commercially available barium sulfate is generally 96% or 98% barium sulfate, and the average particle size of the barium sulfate is 30um or 20 um; table 2 shows the effect of different barium sulfate particle sizes on the initial capacity of the battery, wherein the content of barium sulfate is 1% by weight of the lead powder, and the initial capacity of barium sulfate particles with different particle sizes increases with the decrease of the particle size of barium sulfate, indicating that the smaller the particle size of barium sulfate added to the battery is, the more advantageous the barium sulfate particles are. The smaller the barium sulfate particle size, the smaller the average particle size of lead sulfate after discharge, and the higher the initial capacity.
TABLE 2 influence of different barium sulfate particle sizes on battery capacity
The negative electrode lead paste of example 1 and the commonly used positive electrode lead paste were used to prepare a new battery, and the performance of the new battery was compared with that of the existing battery prepared from the commonly used positive and negative electrode lead pastes, wherein the compositions of the commonly used positive electrode lead paste and the commonly used negative electrode lead paste are shown in tables 3 to 4, and the specifications of the prepared electrode plate are shown in table 5:
TABLE 3 common Positive lead plaster Components (unit: kg)
TABLE 4 common negative lead plaster Components (unit: kg)
TABLE 5 Pole plate Specification
| Polar plate | Polar plate size (height X width X thickness mm) | Single pole plate weight (g) | Weight of dried paste (g) |
| Positive plate | 110×142×2.2/1.7 | 178.6 | 117.6 |
| Negative plate | 110×142×1.9/1.2 | 145.9 | 103.9 |
The performance of the new storage battery is compared with that of the existing storage battery, and the comparison result is shown in table 6.
TABLE 6 Battery Performance test comparison
The active material utilization ratio of the new storage battery and the existing storage battery was compared, and the comparison results are shown in table 7.
Assembling the battery: the type of the sealed valve-controlled lead-acid storage battery is 6-QW-220Ah, and 6 grids are formed by 17 positive plates, 16 negative plates and 12V batteries.
The positive plate active material utilization rate (detection capacity × 4.463)/(effective positive plate number × dry paste weight) — (235 × 4.463)/(16.4 × 117.6) — 54.4%;
the active material utilization rate was calculated based on the positive electrode plate, and the negative electrode plate active material utilization rate was positive plate × 1.057.
TABLE 7 comparison of active material utilization of batteries
| C20 capacity | Active material utilization ratio (positive electrode) | Active material utilization ratio (cathode) | |
| Novel accumulator | 235Ah | 54.4％ | 57.5％ |
| Existing storage battery | 223Ah | 51.6％ | 54.5％ |
The performance of the new battery was compared with that of the existing battery in a low temperature environment (-29 ℃), and the comparison results are shown in Table 8.
TABLE 8 comparison of Low-temperature Environment Performance of storage batteries
Thus, the storage battery prepared by using the negative electrode lead paste of the invention can be normally used at low temperature.
What has been described above are merely some embodiments of the present invention. It will be apparent to those skilled in the art that various changes and modifications can be made without departing from the inventive concept thereof, and these changes and modifications can be made without departing from the spirit and scope of the invention.
Claims (8)
1. The lead-acid storage battery negative electrode lead paste is characterized by comprising the following components: lead powder (1000 + -10) kg with density of (1.40 + -0.005) g/cm at 20 deg.C3The components comprise 84 plus or minus 2 kg of sulfuric acid, 110 plus or minus 5 kg of pure water, 4.5 plus or minus 0.03 kg of valonea extract, 2 plus or minus 0.02 kg of plant tanning agent, 2.2 plus or minus 0.02 kg of acetylene black, 2.5 plus or minus 0.02 kg of sodium lignosulfonate, 1 plus or minus 0.02 kg of short fiber and barium carbonate, wherein the addition amount of the components is 5-10% of the mass of lead powder.
2. The negative lead paste for the lead-acid storage battery of claim 1, which is characterized by comprising the following components: lead powder (1000 + -10) kg with a density of 1.40g/cm at 20 deg.C3The tanning agent comprises 84 plus or minus 2 kg of sulfuric acid, 110 plus or minus 5 kg of pure water, 7 plus or minus 0.09 kg of barium carbonate, 4.5 plus or minus 0.03 kg of valonea extract, 2 plus or minus 0.02 kg of plant tanning agent, 2.2 plus or minus 0.02 kg of acetylene black, 2.5 plus or minus 0.02 kg of sodium lignosulphonate and 1 plus or minus 0.02 kg of short fibers.
3. The negative electrode lead paste for lead-acid storage batteries according to claim 1 or 2, characterized in that the degree of oxidation of the lead powder is 80-82% and the apparent density is 1.3-1.4g/cm3。
4. The lead-acid battery negative electrode lead paste as claimed in claim 1 or 2, wherein the mesh number of the barium carbonate is 325-400 meshes.
5. The lead-acid battery negative electrode lead paste according to claim 1 or 2, wherein the short fiber comprises at least one of polyester fiber, acrylic fiber and polypropylene fiber; the length of the short fiber is 3-5 mm.
6. The method for preparing the lead-acid battery negative electrode lead paste of any one of claims 1 to 5, which is characterized by comprising the following steps: adding barium carbonate, lignin, carbon black, valonea baking gum, plant tanning agent and short fiber, adding pure water for 4-5min, stirring for 2-3min, adding lead powder for 3-4min, mixing and stirring for 2-3min, adding dilute sulfuric acid, stirring for 15-17min while adding, and stirring for 7-8min after adding acid; performing paste mixing by using a paste mixer under the following conditions: the rotating speed is 115-125 r/m, and the paste temperature is controlled within the range of 65-70 ℃.
7. Use of the negative lead paste of a lead-acid battery as claimed in any one of claims 1 to 5 for the preparation of a negative plate.
8. A bipolar horizontal lead-acid battery, characterized in that the negative lead paste of the lead-acid battery is the negative lead paste of any one of claims 1-5.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN114203977A (en) * | 2021-11-17 | 2022-03-18 | 淄博火炬能源有限责任公司 | Negative lead paste for low-temperature lead-carbon battery and preparation method and application thereof |
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| US4382883A (en) * | 1981-07-27 | 1983-05-10 | Allied Corporation | Method for producing a storage battery plate |
| JPS58111262A (en) * | 1981-12-24 | 1983-07-02 | Shin Kobe Electric Mach Co Ltd | Manufacture of cathode plate for lead-acid battery |
| CN101847718A (en) * | 2010-05-31 | 2010-09-29 | 张天任 | Negative pole lead plaster for enhancing charging receptivity of lead-acid battery and preparation method thereof |
| CN102299337A (en) * | 2011-07-26 | 2011-12-28 | 山东金科力电源科技有限公司 | Composite additive to negative electrodes for lead acid batteries, preparation method and application method thereof |
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2021
- 2021-04-28 CN CN202110468193.3A patent/CN113178575B/en active Active
Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US4382883A (en) * | 1981-07-27 | 1983-05-10 | Allied Corporation | Method for producing a storage battery plate |
| JPS58111262A (en) * | 1981-12-24 | 1983-07-02 | Shin Kobe Electric Mach Co Ltd | Manufacture of cathode plate for lead-acid battery |
| CN101847718A (en) * | 2010-05-31 | 2010-09-29 | 张天任 | Negative pole lead plaster for enhancing charging receptivity of lead-acid battery and preparation method thereof |
| CN102299337A (en) * | 2011-07-26 | 2011-12-28 | 山东金科力电源科技有限公司 | Composite additive to negative electrodes for lead acid batteries, preparation method and application method thereof |
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN114203977A (en) * | 2021-11-17 | 2022-03-18 | 淄博火炬能源有限责任公司 | Negative lead paste for low-temperature lead-carbon battery and preparation method and application thereof |
| CN114203977B (en) * | 2021-11-17 | 2024-01-02 | 淄博火炬能源有限责任公司 | Negative electrode lead plaster for low-temperature lead-carbon battery and preparation method and application thereof |
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| CN113178575B (en) | 2023-03-21 |
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