CN113178574A - Positive pole lead plaster of lead-acid storage battery and bipolar horizontal storage battery containing positive pole lead plaster - Google Patents
Positive pole lead plaster of lead-acid storage battery and bipolar horizontal storage battery containing positive pole lead plaster Download PDFInfo
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- CN113178574A CN113178574A CN202110466585.6A CN202110466585A CN113178574A CN 113178574 A CN113178574 A CN 113178574A CN 202110466585 A CN202110466585 A CN 202110466585A CN 113178574 A CN113178574 A CN 113178574A
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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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- 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
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/14—Electrodes for 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
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- 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
- 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
- H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
- H01M2004/028—Positive electrodes
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- 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 belongs to the technical field of lead-acid storage batteries, and particularly relates to a lead paste for a positive electrode of a lead-acid storage battery and a bipolar horizontal storage battery containing the same. The lead-acid storage battery positive electrode lead plaster comprises the following components: 1000 + -10 kg of lead powder with a density of 1.40g/cm at 25 DEG C3100 plus or minus 2kg of sulfuric acid, 120 plus or minus 5kg of pure water, 0.2 to 0.25 percent of aluminum sulfate and 1 plus or minus 0.02kg of short fiber, and 1 to 2 percent of lithium carbonate. The lead-acid storage battery positive lead plaster provided by the invention is added with aluminum sulfate and lithium carbonate for mixed use, so that the aging speed of positive active substances is greatly slowed down, the cycle life of the battery can be prolonged by more than 30%, and the generation of vulcanization of the battery can be reducedAnd the early capacity loss of the storage battery is avoided.
Description
Technical Field
The invention belongs to the technical field of lead-acid storage batteries, and particularly relates to a lead paste for a positive electrode of a lead-acid storage battery and a bipolar horizontal storage battery containing the same.
Background
Common VRLA valve-regulated batteries include EFB flooded batteries and AGM flooded batteries, and currently have the following defects: short cycle life, early capacity loss (PCL), etc. The appearance of PCL phenomenon, called PCL-1, PCL-2 and PCL-3, shortens the life of VRLA batteries, deteriorates the reliability of VRLA batteries, and causes PCL to be suddenly lost in capacity, slowly lost in capacity and incapable of being recharged on the negative electrode.
One of the reasons for the premature failure of VRLA batteries with PCL-2 is the failure of the positive active material. In the new positive plate, the active material is mainly alpha-PbO2Is present in the form of alpha-PbO with repetition of charge-discharge cycles2Gradually become beta-PbO2Due to beta-PbO2Has a crystal size smaller than alpha-PbO2And beta-PbO2The bonding force between the crystal grains is poor, so that the active substance is softened and falls off at the later stage of use.
In view of the above problems, the control methods can be roughly classified into the following methods: changing the composition and structure of the positive active material; carrying out special surface treatment on the electrode; adding a suitable additive to the electrolyte; the combination of the structure of the grid corrosion layer and the positive active material is improved; and the high-quality AGM separator is adopted, so that the assembly pressure is increased.
In the prior art, patents CN109216805A and CN109755671A provide a method for solving the problems of expansion, softening and falling of the positive active material of the storage battery, and the problem is solved by changing the charging and discharging system; CN103337667A discloses a negative active material, a positive active material and an electrolyte of a valve-controlled sealed lead-acid storage battery, wherein aviation oil and anisaldehyde are added into the negative active material, carboxymethyl cellulose is added into the positive active material, and an ethyl-naphthol and p-phenolsulfonic acid solution are added into the electrolyte, so that the self-discharge of the active material is limited, and the capacity loss of the battery is reduced.
The method for solving the PCL problem is complex and high in cost.
Disclosure of Invention
The invention aims to provide a lead-acid storage battery positive electrode lead paste and a bipolar horizontal storage battery containing the lead-acid storage battery positive electrode lead paste, so as to solve at least one problem in the prior art.
According to one aspect of the invention, the lead-acid storage battery positive electrode lead paste comprises the following components: 1000 + -10 kg of lead powder with a density of 1.40g/cm at 25 DEG C3100 plus or minus 2kg of sulfuric acid, 120 plus or minus 5kg of pure water, 0.2 to 0.25 percent of aluminum sulfate and 1 plus or minus 0.02kg of short fiber, and 1 to 2 percent of lithium carbonate.
The lead-acid storage battery positive lead plaster provided by the invention is added with aluminum sulfate and lithium carbonate for mixed use, wherein,
after the aluminum sulfate is added into the positive lead plaster, PbO in the charging and discharging process of the storage battery can be effectively relieved2-PbSO4The stress caused by the volume change during the mutual conversion causes the problem that the active substances are softened and fall off. This is because PbO2Is only PbSO41/2 volume, PbO is generated when the battery is charged2Volume reduction and generation of PbSO during discharge4The volume is increased, the change of the volume in the charging and discharging process causes the stress change among the substances, and the long-term repeated stress change reduces the bonding strength among the active substances, thereby promoting the softening and falling of the active substances. After aluminum sulfate is added, the aluminum sulfate is 'embedded' between active substances to be used as a cross-linking agent, is relaxed during charging (volume reduction) and is compressed during discharging (volume increase), and the action similar to that of a spring greatly slows down the aging speed of the active substances of the positive electrode, and can prolong the cycle life of the battery by more than 30 percent;
lithium carbonate is added into the positive active substance, the lithium carbonate plays the role of a nucleating agent, the lithium carbonate is different from lead sulfate in crystal, and the addition of the lithium carbonate has positive influence on the crystal structure of the positive active substance.
After deep discharge of lead-acid accumulator with pure lead positive grid, the grid is corroded to compact PbSO with poor permeability4The film, which forms a barrier layer, deteriorates or even fails the charge acceptance of the battery. The phenomenon is more obvious in low-rate complete discharge of the lead-acid storage battery, the parking battery is mainly used for vehicle-mounted air conditioners and vehicle-mounted household appliances, the low-rate complete discharge is normal, and the antimony-free effect is more serious. So that the conventional storage battery has early capacity loss in use and is poor in parkingLiquid batteries are more susceptible to early capacity loss.
The process of charging and discharging of the lead-acid storage battery is the process of electrochemical reaction, lead sulfate forms lead oxide during charging, and the lead oxide is reduced into lead sulfate during discharging. Lead sulfate is a substance which is easy to crystallize, when the concentration of lead sulfate in an electrolytic solution in a battery is too high or static idle time is too long, the lead sulfate is "embraced" into a cluster and is agglomerated into small crystals, the small crystals attract surrounding lead sulfate to form large inert crystals like snowballing, and the crystallized lead sulfate can not be reduced into lead oxide during charging and can be deposited and attached on an electrode plate, so that the working area of the electrode plate is reduced, and the phenomenon of vulcanization is caused.
The lithium carbonate has the function of solving the problem of sulfuration of the battery, because lithium is more active than lead, a small amount of lithium carbonate is added, most of final products generated during discharging are lithium sulfate, the generated lead sulfate is less, the lithium sulfate is not crystallized, and no large block of lead sulfate is crystallized during charging, so that the sulfuration of the battery can be reduced, and the early capacity loss of the storage battery is avoided.
In some embodiments, the lead-acid battery positive lead paste comprises the following components: 1000 + -10 kg of lead powder with a density of 1.40g/cm at 25 DEG C3100 plus or minus 2kg of sulfuric acid, 120 plus or minus 5kg of pure water, 2.25 plus or minus 0.02kg of aluminum sulfate, 1 plus or minus 0.02kg of short fiber and 15 plus or minus 0.2kg of lithium carbonate.
In some embodiments, the lead powder has a degree of oxidation of 75-80%; the apparent density is 1.3-1.5g/cm3。
In some embodiments, the staple fibers comprise at least one of polyester, acrylic, polypropylene fibers; the length of the fiber is 3-5 mm.
The invention also provides a preparation method of the lead paste for the positive electrode of the lead-acid storage battery, which comprises the following steps:
firstly, preparing dilute sulfuric acid mixed solution containing aluminum sulfate and lithium carbonate;
adding fiber into pure water, wet stirring for 2 + -1 min, adding lead powder, stirring for 2 + -1 min, adding the above dilute sulfuric acid mixture, stirring for 20 + -2 min while adding, and stirring for 7 + -2 min after adding acid.
In some embodiments, the step of preparing the dilute sulfuric acid mixture containing aluminum sulfate and lithium carbonate comprises: adding 98% concentrated sulfuric acid into pure water, and making into a product with a density of 1.40g/cm at 25 deg.C3When the acid temperature is controlled to be 80-90 ℃, adding aluminum sulfate and lithium carbonate, and mixing to obtain the sulfuric acid. Therefore, the uniform mixing degree of the aluminum sulfate and the lithium carbonate in the lead plaster is improved.
The invention also provides application of the lead paste for the positive electrode of the lead-acid storage battery in preparation of the positive plate.
The invention also provides application of the lead paste for the positive electrode of the lead-acid storage battery in preparation of a bipolar horizontal storage battery.
The invention also provides a bipolar horizontal lead-acid storage battery, and the positive lead paste of the bipolar horizontal lead-acid storage battery is the positive lead paste of the lead-acid storage battery.
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 paste for the positive electrode of the lead-acid storage battery is prepared by the following steps:
(1) preparing each component by weight;
(2) in order to uniformly mix aluminum sulfate and lithium carbonate, concentrated sulfuric acid is firstly utilized to prepare dilute sulfuric acid to release heat, and the aluminum sulfate and the lithium carbonate are fully mixed and dissolved at the temperature of 80-90 ℃ to obtain a dilute sulfuric acid mixed solution of the aluminum sulfate and the lithium carbonate, wherein the dilute sulfuric acid is 1.40 +/-0.005 g/cm3(25 ℃ C.); specifically, 98% concentrated sulfuric acid is added into pure water, diluted by the concentrated sulfuric acid to release heat, and prepared to have a density of 1.40g/cm at 25 DEG C3Starting an acid circulating pump and a cooling pump, cooling by a plate heat exchanger, adding aluminum sulfate and lithium carbonate when the acid temperature is controlled to be 80-90 ℃, closing the cooling pump, continuing to start the acid circulating pump for 30-40 minutes, and uniformly mixing the aluminum sulfate, the lithium carbonate and the acid liquor to obtain the sulfuric acid;
the amount of the aluminum sulfate and the lithium carbonate added into the dilute sulfuric acid is calculated according to the formula: i.e. 100 +/-2 kg1.4g/cm3Sulfuric acid in dilute sulfuric acid at 25 deg.C2.25 plus or minus 0.02kg of aluminum and 15 plus or minus 0.2kg of lithium carbonate; (ii) a
(3) Adding fiber into pure water, wet stirring for about 2min, adding lead powder, stirring for about 2min, adding the above dilute sulfuric acid mixture, stirring for about 20min while adding, and stirring for about 7min after the acid is added.
Meanwhile, the performance of the battery made of the positive electrode lead paste of example 1 was compared with that of the battery made of the conventional positive electrode lead paste, and a 6-QW-100Ah cell test was assembled with the same plate size, plate weight, paste application amount and manufacturing process.
The conventional positive electrode lead paste has the following formula: lead powder 1000 + -10 kg, 1.4g/cm3100 plus or minus 2kg of dilute sulphuric acid (25 ℃), 120 plus or minus 5kg of pure water, 50 plus or minus 1kg of red lead, 0.8 plus or minus 0.02kg of short fiber with the diameter of 3-5mm and 1 plus or minus 0.2kg of antimony trioxide; the oxidation degree of the lead powder is 75-80%, and the apparent density is 1.3-1.5g/cm3。
Firstly, a comparison experiment of the storage battery capacity is carried out.
Testing according to GB/T5008.1-2013 standard 5.4.1, firstly, using I20The current is charged to the terminal voltage of the storage battery of 14.4V, and the charging is continued for 5 h. With I20Discharging current to the terminal voltage of the storage battery by 10.5V, wherein the first discharge capacity is larger than C20Then with I20Charging current to discharge capacity value of I20Discharging the current to the terminal voltage of the storage battery by 10.5V, and recording the ratio of the discharge capacity for the second time to the reduction value of the ratio. Repeating the second time for the third time, and comparing the capacity reduction values. The results are shown in Table 1.
TABLE 1 comparison of Battery capacities (Unit: Ah)
| First discharge | 2 nd discharge | 3 rd time discharge | |
| Storage battery of the prior art | 100 | 92.5 | 90.1 |
| Storage battery comprising the battery of example 1 | 100.7 | 100.6 | 100.2 |
As can be seen from the data in Table 1, the capacity of the conventional storage battery was reduced by 7.5Ah and 2.4Ah, respectively; the capacity of the storage battery containing the positive electrode lead paste in the example 1 is respectively reduced by 0.1Ah and 0.4Ah, which are far smaller than the capacity reduction value of the storage battery in the prior art, and the lithium carbonate is added, so that the charge acceptance of the storage battery is improved, and the charge acceptance is high when the power is supplemented according to the discharge capacity.
Second, capacity loss comparative experiment
Testing according to GB/T5008.1-2013 standard 5.4.1, firstly, using I20The current is charged to the terminal voltage of the storage battery of 14.4V, and the charging is continued for 5 h. With I20The current was discharged to a battery terminal voltage of 10.5V, and the above charge and discharge was repeated to the times shown in the following table, and the discharge capacity was calculated, and the results are shown in table 2.
TABLE 2 comparison of capacity loss (unit: Ah)
| 60 times of charge and discharge | 100 times of charge and discharge | 120 times of charge and discharge | |
| Storage battery of the prior art | 90.6 | 85.6 | 76.2 |
| Storage battery comprising the battery of example 1 | 100 | 99.2 | 97.5 |
As can be seen from table 2, the capacity loss of the battery containing the positive electrode lead paste of example 1 was reduced by only 2.5Ah after 120 charge-discharge cycles, while the capacity loss of the battery of the prior art was reduced by 23.8Ah, indicating that after the charge-discharge cycles of the battery, vulcanization occurred, and a part of the lead sulfate was no longer active due to the vulcanization, that is, did not participate in the charge-discharge reaction, and the discharge capacity of the battery was reduced. And the lithium carbonate is added into the storage battery containing the positive electrode lead paste in the embodiment 1, and the lithium carbonate plays a role of nucleation, so that the reduction of active substances is effectively restrained, and the reduction amplitude of the capacity is smaller.
Third, battery life experiment
According to the test of the general standard of VW75073-2017, the cycle life of 50 percent DOD of the storage battery is more than 120 times (5I in a constant-temperature water bath at 40 +/-2℃)20Discharging for 2h, the battery terminal voltage is not lower than 10V after discharging, and then charging for 5h at a constant voltage of 16V, which constitutes a cycle). The test was terminated at a discharge below 10V, the number of cycles was recorded and a cold start test was subsequently carried out, with the standard V10s≥7.2V，V40sThe results are shown in Table 3, for. gtoreq.6.0V.
TABLE 3 comparison of cycle life (unit: times)
As can be seen from the results of comparing the cycle life of table 3, the cycle life of the battery containing the positive electrode lead paste of example 1 reached 227 times, which was improved by 80% compared to the battery of the prior art, indicating that the addition of aluminum sulfate acts as a "crosslinking agent" to effectively alleviate the softening and dropping of the active material of the positive electrode plate, thereby improving the cycle life of the battery.
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 positive electrode lead paste is characterized by comprising the following components: 1000 + -10 kg of lead powder with a density of 1.40g/cm at 25 DEG C3100 plus or minus 2kg of sulfuric acid, 120 plus or minus 5kg of pure water, 0.2 to 0.25 percent of aluminum sulfate and 1 plus or minus 0.02kg of short fiber, and 1 to 2 percent of lithium carbonate.
2. The lead-acid battery positive electrode lead paste according to claim 1, wherein the lead powder is 1000 ± 10kg, and the density is 1.40g/cm at 25 ℃3100 plus or minus 2kg of sulfuric acid, 120 plus or minus 5kg of pure water, 2.25 plus or minus 0.02kg of aluminum sulfate, 1 plus or minus 0.02kg of short fiber and 15 plus or minus 0.2kg of lithium carbonate.
3. The lead-acid battery positive electrode lead paste according to claim 1 or 2, characterized in that the degree of oxidation of the lead powder is 75-80%; the apparent density is 1.3-1.5g/cm3。
4. The lead-acid battery positive lead paste according to claim 3, wherein the short fibers comprise at least one of polyester fibers, acrylic fibers and polypropylene fibers; the length of the fiber is 3-5 mm.
5. The method for preparing the lead-acid battery positive electrode lead paste according to any one of claims 1 to 4, characterized by comprising the following steps: firstly, preparing dilute sulfuric acid mixed solution containing aluminum sulfate and lithium carbonate; adding fiber into pure water, wet stirring for 2 + -1 min, adding lead powder, stirring for 2 + -1 min, adding the above dilute sulfuric acid mixture, stirring for 20 + -2 min while adding, and stirring for 7 + -2 min after adding acid.
6. Use of a lead-acid battery positive lead paste according to any of claims 1 to 4 for the preparation of a positive plate.
7. Use of the lead-acid battery positive lead paste according to any of claims 1 to 4 for the preparation of a bipolar horizontal battery.
8. A bipolar horizontal lead-acid battery, characterized in that the positive lead paste of the lead-acid battery is the positive lead paste of any one of claims 1-4.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN113745501A (en) * | 2021-08-09 | 2021-12-03 | 安徽理士电源技术有限公司 | Silicon-based lead-acid storage battery positive lead paste and preparation method thereof |
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