CN100568589C - Zinc cathode of zinc-nickel secondary battery and preparation method thereof - Google Patents
Zinc cathode of zinc-nickel secondary battery and preparation method thereof Download PDFInfo
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- CN100568589C CN100568589C CNB2008101409138A CN200810140913A CN100568589C CN 100568589 C CN100568589 C CN 100568589C CN B2008101409138 A CNB2008101409138 A CN B2008101409138A CN 200810140913 A CN200810140913 A CN 200810140913A CN 100568589 C CN100568589 C CN 100568589C
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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
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- 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 zinc cathode of a zinc-nickel secondary battery and a preparation method thereof, relates to a cathode of a secondary battery, and aims to provide the zinc cathode of the zinc-nickel secondary battery and the preparation method thereof, wherein the zinc cathode of the zinc-nickel secondary battery can reduce the internal pressure of the battery and prolong the cycle service life of the zinc-nickel battery. The key point of the technical scheme is that the zinc cathode of the zinc-nickel secondary battery comprises a zinc cathode active substance, wherein the zinc cathode active substance also contains sodium sulfite, and the weight of the sodium sulfite is 0.01-1% of the total weight of the zinc cathode active substance. The invention is used for the zinc-nickel secondary battery.
Description
The technical field is as follows:
the invention relates to a negative electrode of a secondary battery, in particular to a zinc negative electrode of a zinc-nickel secondary battery and a preparation method thereof.
Background art:
in recent years, among alkaline secondary batteries using zinc as a negative electrode, zn — Ni batteries have attracted much attention in recent years because of their advantages such as high operating voltage and large current charge and discharge. A zinc-nickel battery having a high open circuit voltage of 1.65V is more suitable as a power source for various small electric tools, electric vacuum cleaners, electric bicycles, etc. than a metal hydride-nickel battery, a nickel battery, and an alkaline zinc-manganese battery having a nominal voltage of 1.2V. However, a disadvantage of the rechargeable zinc-nickel battery using zinc as the negative electrode is that the capacity of the zinc negative electrode for oxygen recombination is poor, and as the charge-discharge cycle of the battery progresses, especially under the condition of a large charging current, oxygen generated by the over-charge of the nickel electrode cannot be smoothly recombined on the zinc negative electrode, and when the rate of oxygen generated by the positive electrode is greater than the rate of oxygen absorption of the negative electrode, the pressure inside the battery gradually increases due to the accumulation of oxygen, causing the leakage of the battery and premature failure of the battery. In order to improve the oxygen recombination on the zinc cathode, U.S. Pat. No. 5,460,899 mentions that in the design of the isolated negative electrode stack, a hydrophobic gas diffusion membrane is used to separate two zinc half-electrode plates, and a complete zinc cathode is formed by the two zinc half-electrode plates and the gas diffusion membrane in the middle; patent 200610109961.1 mentions a multilayer zinc negative electrode unit comprising zinc negative electrode material layers on both sides of a current collector and a current collector, wherein the method further comprises providing a groove on at least one material layer surface of each layer of zinc negative electrode unit before stacking the multilayer zinc negative electrode unit, wherein at least one end of the groove extends to one edge of the material layer surface, and the material layer on the side of the groove of the zinc negative electrode unit of the adjacent layer is opposite. Patent 200510002899.1 mentions that hydrophobic air permeable particles are prepared from porous particles with good conductivity and hydrophobic substances (the conductive porous hydrophobic particles are carbon black with hydrophobic substances adsorbed thereon), and the particles are uniformly distributed on the surface and inside of a zinc cathode, which not only functions as a conductive agent to provide a gas channel for oxygen transmission and compounding, so that the purpose of enabling oxygen to smoothly reach the surface and inside of the zinc cathode to be compounded can be achieved. Although the above patents improve the oxygen recombination on the zinc cathode to a certain extent, the processes are relatively complicated, and the common idea is to start with the improvement of the oxygen transmission channel, but not to consider the improvement of the oxygen recombination capability of the zinc cathode itself. Therefore, the problem of reducing the internal pressure of the secondary zinc-nickel battery is still a subject of research.
The invention content is as follows:
the invention aims to provide a zinc cathode of a zinc-nickel secondary battery and a preparation method thereof, wherein the zinc cathode can reduce the internal pressure of the battery and prolong the cycle service life of the zinc-nickel battery. The invention has the technical scheme that the zinc cathode of the zinc-nickel secondary battery comprises a zinc cathode active substance, and is characterized in that: the zinc negative active material also contains sodium sulfite, and the weight of the sodium sulfite is 0.01-1% of the total weight of the zinc negative active material. A preparation method of a zinc cathode of a zinc-nickel secondary battery comprises the following working procedures of preparing zinc cathode slurry: the method is characterized in that: the preparation method of the zinc cathode slurry comprises the following steps: mixing 100 parts by weight of zinc oxide doped with calcium zincate and zinc powder, 2.03 parts by weight of conductive agent, 0.01-1 part by weight of sodium sulfite and 0.5-1 part by weight of hydrophilic binder powder to obtain a semi-finished mixture of a zinc cathode active material and a hydrophilic binder, (2) dissolving 0.05 part by weight of dispersing agent in 15-30 parts by weight of distilled water, (3) adding the mixture obtained in the step (1) into the solution obtained in the step (2), and adding 0.5-3 parts by weight of hydrophobic binder emulsion under stirring to obtain uniform zinc cathode slurry fluid; (4) And (4) coating the two surfaces of the zinc electrode current collector with the zinc cathode slurry fluid prepared in the step (3), drying, and punching a zinc cathode finished product sheet according to the required specification and size. Compared with the prior art, the invention has the obvious advantages of strong composite oxidation capability, low internal pressure of the zinc-nickel battery and long cycle service life.
The specific implementation mode is as follows:
in order to reduce the internal pressure of the battery, improve the electrochemical performance of the secondary zinc-nickel battery and prolong the service life of the battery, the invention adopts a method of adding sodium sulfite into a zinc cathode, the sodium sulfite with good oxygen absorbability effectively compounds oxygen generated by overcharge, the internal pressure of the battery is reduced, and the leakage problem in the later cycle period of the battery is solved.
The zinc cathode material contains a cathode active substance and a binder, wherein the cathode active substance mainly contains zinc oxide powder, calcium zincate, zinc powder, a conductive agent, an oxygen scavenger and a dispersant. The content of the calcium zincate and the zinc powder is 13 to 35 percent of the total weight of the zinc cathode active material. The conductive agent of the negative active material is a mixture of conductive graphite and carbon black. The dispersing agent of the negative active substance is one or more of water glass, sodium tripolyphosphate, sodium pyrophosphate, sodium hexametaphosphate, triethylhexylphosphonic acid, sodium dodecyl sulfate, methylpentanol, polyacrylamide, fatty acid polyglycol ester and polyacrylic acid. The binder is a mixture of a hydrophobic binder and a hydrophilic binder. The hydrophobic binder is styrene butadiene rubber, and the hydrophilic binder is at least one of hydroxypropyl methylcellulose and sodium carboxymethylcellulose.
A preparation method of a zinc cathode of a secondary zinc-nickel battery comprises the following steps:
(1) Mechanically mixing 70.5-80.5 parts by weight of zinc oxide, 3-5 parts by weight of conductive agent, 0.01-1 part by weight of sodium sulfite and 13-35 parts by weight of calcium zincate and zinc powder and metal compound additive if necessary with 0.5-1 part by weight of hydrophilic binder powder to obtain a semi-finished mixture of negative electrode active substance and hydrophilic binder;
(2) Dissolving 0.01-2 parts by weight of dispersant in 15-30 parts by weight of distilled water;
(3) Adding the semi-finished mixture of the negative active material and the hydrophilic binder obtained in the step (1) into the solution obtained in the step (2), and then adding the hydrophobic binder emulsion with the dry-basis dosage of 0.5-3 parts by weight while stirring to obtain uniform zinc negative electrode slurry fluid;
(4) And (4) coating the zinc cathode slurry fluid obtained in the step (3) on two surfaces of a zinc electrode current collector, drying, and punching into a zinc cathode finished product sheet with a certain specification according to a required size.
Detailed description of the preferred embodiments
0.05g of sodium tripolyphosphate is placed in a beaker, 28g of deionized water is added, the beaker is placed on an electric heating stirrer to be slowly stirred, after the sodium tripolyphosphate is completely dissolved, 100g of zinc oxide doped with calcium zincate and zinc powder, 2g of conductive graphite, 0.03g of carbon black, 0.01g of sodium sulfite and 1.0g of sodium carboxymethyl cellulose powder are uniformly mixed, the mixture is added into the beaker to be fully stirred, 1.5g of styrene-butadiene rubber emulsion with the concentration of 50 percent is added, uniform cathode active substance slurry is obtained by stirring, the slurry is coated on two sides of a brass net by a slurry pulling machine and dried, and a plurality of zinc cathode finished product sheets with the specification size of 100mm multiplied by 36mm are prepared by punching. The positive electrode was a commercial nickel positive electrode sheet having a gauge size of 75mm × 32 mm. The composite diaphragm formed by hot pressing or bonding the modified polypropylene felt and the wettable polyethylene microporous graft membrane is sandwiched between the zinc cathode and the nickel cathode, the battery pole core is formed by winding a plurality of turns by a winding machine and is arranged in an AA type battery steel shell, an electrolyte solution containing 20 percent of KOH and 1.8 percent of LiOH is injected through notching, spot welding and sealing, and the AA type sealed cylindrical rechargeable zinc-nickel battery is assembled.
Embodiment two
0.05g of sodium tripolyphosphate is placed in a beaker, 28g of deionized water is added, the beaker is placed on an electric heating stirrer to be heated and slowly stirred, after the sodium tripolyphosphate is completely dissolved, 100g of zinc oxide doped with calcium zincate and zinc powder, 2g of conductive graphite, 0.03g of carbon black, 1g of sodium sulfite and 1.0g of sodium carboxymethyl cellulose powder are uniformly mixed, added into the beaker and fully stirred, then 1.5g of styrene butadiene rubber emulsion with the concentration of 50% is added, uniform cathode active substance slurry is obtained by stirring, the slurry is coated on two sides of a brass net and dried by a pulp puller, and a plurality of zinc cathode finished product sheets with the specification size of 100mm multiplied by 36mm are prepared by punching. The zinc negative electrode is assembled into an AA type sealed cylindrical rechargeable zinc-nickel battery according to the same method as the first embodiment.
EXAMPLE III
0.05g of sodium tripolyphosphate is placed in a beaker, 28g of deionized water is added, the beaker is placed on an electric heating stirrer to be heated and slowly stirred, after the sodium tripolyphosphate is completely dissolved, 100g of zinc oxide doped with calcium zincate and zinc powder, 2g of conductive graphite, 0.03g of carbon black, 0.05g of sodium sulfite and 1.0g of sodium carboxymethyl cellulose powder are uniformly mixed and added into the beaker to be fully stirred, 1.5g of styrene-butadiene rubber emulsion with the concentration of 50 percent are added, uniform cathode active substance slurry is obtained by stirring, the slurry is coated on two sides of a brass net by a slurry pulling machine and dried, and a plurality of zinc cathode finished product sheets with the specification size of 100mm multiplied by 36mm are prepared by punching. The zinc negative electrode is assembled into an AA type sealed cylindrical rechargeable zinc-nickel battery according to the same method as the first embodiment.
Embodiment four
Putting 0.05g of sodium dodecyl sulfate into a beaker, adding 28g of deionized water, putting the beaker on an electric heating stirrer, heating and slowly stirring, after the sodium dodecyl sulfate is completely dissolved, uniformly mixing 100g of zinc oxide doped with calcium zincate and zinc powder, 2g of conductive graphite, 0.03g of carbon black, 0.05g of sodium sulfite and 1.0g of sodium carboxymethyl cellulose powder, adding the mixture into the beaker, fully stirring, then adding 1.5g of styrene butadiene rubber emulsion with the concentration of 50%, stirring to obtain uniform cathode active substance slurry, coating the slurry on two sides of a brass net by using a slurry drawing machine, drying, and punching to prepare a plurality of zinc cathode finished sheets with the specification size of 100mm multiplied by 36 mm. The zinc negative electrode is assembled into an AA type sealed cylindrical rechargeable zinc-nickel battery according to the same method as the first embodiment.
EXAMPLE five
Putting 0.05g of water glass into a beaker, adding 28g of deionized water, putting the beaker on an electric heating stirrer to be heated and slowly stirred, after the water glass is completely dispersed, uniformly mixing 100g of zinc oxide doped with calcium zincate and zinc powder, 2g of conductive graphite, 0.03g of carbon black, 0.05g of sodium sulfite and 1.0g of sodium carboxymethylcellulose powder, adding the mixture into the beaker, fully stirring the mixture, then adding 1.5g of styrene-butadiene rubber emulsion with the concentration of 50 percent, stirring the mixture to obtain uniform cathode active substance slurry, coating the slurry on two sides of a brass net by using a slurry drawing machine, drying the slurry, and punching to prepare a plurality of zinc cathode finished product sheets with the specification size of 100mm multiplied by 36 mm. The zinc negative electrode is assembled into an AA type sealed cylindrical rechargeable zinc-nickel battery according to the same method as the first embodiment.
In the above embodiment, sodium sulfite, sodium dodecyl sulfate and water glass are all analytical pure grades.
Comparison scheme one
100g of zinc oxide doped with calcium zincate and zinc powder, 2g of conductive graphite, 0.03g of carbon black and 1.0g of sodium carboxymethylcellulose powder are uniformly mixed, added into the beaker, fully and uniformly stirred, then 1.5g of styrene-butadiene rubber emulsion with the concentration of 50% is added, uniform cathode active substance slurry is obtained by stirring, the slurry is coated on two sides of a brass net by a slurry drawing machine and dried, and a plurality of zinc cathode finished product sheets with the specification size of 100mm multiplied by 36mm are prepared by punching. The zinc negative electrode is assembled into an AA type sealed cylindrical rechargeable zinc-nickel battery according to the same method as the first embodiment.
Comparison scheme two
0.05g of sodium tripolyphosphate is placed in a beaker, 28g of deionized water is added, the beaker is placed on an electric heating stirrer to be heated and slowly stirred, after the sodium tripolyphosphate is completely dissolved, 100g of zinc oxide doped with calcium zincate and zinc powder, 2g of conductive graphite and 0.03g of carbon black are uniformly mixed with 1.0g of sodium carboxymethyl cellulose powder, the mixture is added into the beaker to be fully stirred, 1.5g of styrene-butadiene rubber emulsion with the concentration of 50 percent is added, uniform slurry of negative active substances is obtained by stirring, the slurry is coated on two sides of a brass net and dried by a slurry drawing machine, and a plurality of zinc negative finished product pieces with the specification size of 100mm multiplied by 36mm are prepared by punching. The above zinc negative electrode was assembled into an AA-type sealed cylindrical rechargeable zinc-nickel battery in the same manner as in the first embodiment.
Comparison scheme three
100g of zinc oxide doped with calcium zincate and zinc powder, 2g of conductive graphite, 0.03g of carbon black, 0.05g of sodium sulfite and 1.0g of sodium carboxymethylcellulose powder are uniformly mixed, added into the beaker and fully stirred, then 1.5g of styrene-butadiene rubber emulsion with the concentration of 50% is added, the uniform cathode active substance slurry is obtained by stirring, the slurry is coated on two sides of a brass net by a slurry drawing machine and dried, and a plurality of zinc cathode finished product sheets with the specification size of 100mm multiplied by 36mm are prepared by punching. The zinc cathode is assembled into an AA type sealed cylindrical rechargeable zinc-nickel battery according to the same method as the first embodiment.
And (3) testing the battery performance:
the batteries assembled by the above embodiment and comparative scheme (20 batteries assembled by each scheme) were charged for the first time at 40mA for 15 hours and then discharged to 1.4V at 80mA, and the activation of the batteries was completed. And then charging for 1.25 hours at 400mA, standing for 5 minutes, discharging to 1.4V at 400mA, recording discharge capacity, carrying out a cycle life test by using the discharge capacity as reference for each battery in a 1C charge-discharge cycle life test method, stopping the test when the capacity is attenuated to 80% of the designed capacity, and simultaneously checking whether a leakage battery exists or not after the cycle is finished. The results are shown in Table 1. The results in table 1 show that the addition of sodium sulfite in the negative electrode can effectively compound and seal the zinc-nickel battery with oxygen generated by overcharge, reduce the internal pressure of the battery, and solve the leakage phenomenon of the battery in the later period of circulation, thereby greatly prolonging the cycle service life of the sealed and chargeable zinc-nickel battery, and simultaneously, the addition of the dispersant in the negative electrode can obviously improve the uniformity of the battery performance.
The AA type sealed cylindrical rechargeable zinc-nickel battery has the following performances:
| testing of Battery with a battery cell | Zinc acid Calcium and zinc Powder, oxygen Dissolving zinc (g) | Sulphurous acid Sodium salt (g) | Trimerization of benzene and toluene Phosphoric acid Sodium (g) | Twelve aspects Alkyl radical Sulfuric acid Sodium (g) | Water glass Glass (g) | 400m A is put Capacitor with a capacitor element Quantity of (mAh ) | Capacity of Holding Rate of change (％) | Circulation of Life span (times) | Leakage of liquid Phenomenon(s) | Qualified Battery with a battery cell (only) |
| Scheme one | 100 | 0.01 | 0.05 | 398 | 80％ | 252 | Is free of | 20 | ||
| Scheme two | 100 | 1 | 0.05 | 392 | 80％ | 216 | Is free of | 19 | ||
| Scheme(s) III | 100 | 0.05 | 0.05 | 395 | 80％ | 243 | Is free of | 19 | ||
| Scheme(s) Fourthly | 100 | 0.05 | 0.05 | 395 | 80％ | 240 | Is free of | 19 | ||
| Scheme(s) Five of them | 100 | 0.05 | 0.05 | 394 | 80％ | 241 | Is free of | 19 | ||
| Comparison of Scheme one | 100 | 396 | 80％ | 167 | Is provided with | 14 | ||||
| Comparison of Scheme two | 100 | 0.05 | 396 | 80％ | 211 | Is provided with | 19 | |||
| Comparison of Scheme three | 100 | 0.05 | 393 | 80％ | 236 | Is composed of | 16 |
Claims (2)
1. A zinc-nickel secondary battery zinc cathode comprises a zinc cathode active material, and is characterized in that: the zinc negative active material also contains sodium sulfite, and the weight of the sodium sulfite is 0.01-1% of the total weight of the zinc negative active material.
2. A preparation method of a zinc cathode of a zinc-nickel secondary battery comprises a process of preparing zinc cathode slurry, and is characterized in that the preparation method of the zinc cathode slurry comprises the following steps: mixing 100 parts by weight of zinc oxide doped with calcium zincate and zinc powder, 2.03 parts by weight of a conductive agent, 0.01-1 part by weight of sodium sulfite and 0.5-1 part by weight of hydrophilic binder powder to obtain a semi-finished mixture of a zinc negative active material and a hydrophilic binder, (2) dissolving 0.05 part by weight of a dispersing agent in 15-30 parts by weight of distilled water, and (3) adding the mixture obtained in the step (1) into the solution obtained in the step (2), and adding 0.5-3 parts by weight of a hydrophobic binder emulsion under stirring to obtain a uniform zinc negative slurry fluid; (4) And (4) coating the two sides of the zinc electrode current collector with the zinc cathode slurry fluid prepared in the step (3), drying, and punching a zinc cathode finished product sheet according to the required specification and size.
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| CNB2008101409138A CN100568589C (en) | 2008-07-25 | 2008-07-25 | Zinc cathode of zinc-nickel secondary battery and preparation method thereof |
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| CNB2008101409138A CN100568589C (en) | 2008-07-25 | 2008-07-25 | Zinc cathode of zinc-nickel secondary battery and preparation method thereof |
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| CN108832128A (en) * | 2018-05-30 | 2018-11-16 | 沈阳理工大学 | A kind of iron nickel secondary batteries iron negative electrode binder |
| US11450847B2 (en) * | 2019-01-23 | 2022-09-20 | Energizer Brands, Llc | Alkaline electrochemical cells comprising increased zinc oxide levels |
| CN110755200B (en) * | 2019-10-08 | 2022-07-22 | 东华大学 | Preparation method of Ag/Zn micro-current medical dressing |
| CN111463408A (en) * | 2020-03-18 | 2020-07-28 | 山东合泰新能源有限公司 | Preparation method of coating type zinc electrode |
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