CN111463499B - Electrolyte for secondary zinc-nickel battery - Google Patents

Electrolyte for secondary zinc-nickel battery Download PDF

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Publication number
CN111463499B
CN111463499B CN202010188924.4A CN202010188924A CN111463499B CN 111463499 B CN111463499 B CN 111463499B CN 202010188924 A CN202010188924 A CN 202010188924A CN 111463499 B CN111463499 B CN 111463499B
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electrolyte
zinc
battery
nickel battery
nickel
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CN111463499A (en
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王江林
赵磊
马永泉
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Shandong Hetai New Energy Co ltd
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Shandong Hetai New Energy Co ltd
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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
    • H01M10/24—Alkaline accumulators
    • H01M10/26—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
    • H01M10/42—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
    • H01M2300/0088—Composites
    • 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 an electrolyte for a secondary zinc-nickel battery, which comprises the following components in percentage by weight: 25-50 w% of alkali solution, 0.01-5 w% of LiOH, 0.1-5 w% of boric acid and/or borate, 0.01-1 w% of aluminum-containing substance, 5-15 w% of ZnO, 0.005-0.03 w% of SiO2And the balance being pure water. The invention adds aluminum-containing substance into electrolyte for rechargeable zinc-nickel battery, which can effectively inhibit zinc grain growth, LiOH and Li in the electrolyte+Into Ni (OH)2The crystal lattice improves the migration capability of protons and effectively inhibits K+The doping of (2) stabilizes the electrolyte in the crystal lattice and improves Ni in the charging and discharging process2+And Ni3+The conversion efficiency is improved, the cycle performance of the nickel anode is improved, and SiO is added into the electrolyte2Then, the viscosity of the electrolyte can be increased, so that the solubility of the active substance in the electrolyte is reduced, the deformation of the zinc electrode is slowed down, and boric acid or borate and alkali liquor are added into the electrolyte to form B4O7 2‑，B4O7 2‑The presence of the zinc oxide can inhibit the adsorption of ZnO on the surface of the electrode and inhibit the passivation of the zinc electrode.

Description

Electrolyte for secondary zinc-nickel battery
Technical Field
The invention relates to a battery electrolyte, in particular to an electrolyte for a zinc-nickel battery.
Background
The research of the zinc-nickel battery starts in 1887, has already been carried out for over a hundred years now, and relatively intensive research is carried out by relevant experts all over the world, and the zinc-nickel battery also has related use in the market. The zinc-nickel battery is a novel secondary alkaline battery, has high safety and can not generate combustion and explosion. The mass specific energy density is higher, can reach 80-120Wh/kg, is far higher than that of lead-acid batteries and cadmium-nickel batteries, and is close to that of the current lithium iron phosphate commercial batteries. Secondly, the zinc-nickel battery is nontoxic and pollution-free, and the zinc is used as the main material of the cathode of the battery, so that the global content is high and the price is low. And thirdly, the zinc-nickel battery has high rate performance and can carry out charging and discharging of large current. The zinc-nickel battery also has good low-temperature performance, so that the zinc-nickel battery becomes one of the most potential batteries in the field of power batteries.
However, the zinc-nickel battery has not been truly industrialized, and has become the fifth battery in the market. The main reason is that the zinc-nickel battery has poor cycle performance, and zinc dendrites grow on the surface of a zinc cathode to pierce a diaphragm in the cyclic process of the zinc-nickel battery, so that the battery is short-circuited, and then the zinc electrode can be dissolved and deformed. The main reason for these situations can be attributed to the defect of the zinc electrode itself, that is, the zinc electrode generates zinc oxide and zinc hydroxide during discharge, while the electrolyte of the zinc-nickel battery is a strongly alkaline electrolyte, which causes the zinc oxide and zinc hydroxide to dissolve in the electrolyte. Along with the circulation of the battery, the dendritic crystal growth is more serious, short circuit occurs, the charge and discharge capacity of the battery is sharply reduced, and the cycle life is terminated early.
In order to solve the above problems of the zinc-nickel battery, researchers have conducted related studies in three aspects: firstly, modifying zinc electrode materials, including coating doping of zinc oxide, secondly designing electrolyte formula, thirdly, adopting a novel anti-dendrite diaphragm. In current research, corresponding improvements and improvements in battery performance have been achieved in all three directions. The improvement of the electrolyte has the most obvious effect of inhibiting the dissolution of the zinc electrode.
US patent No. US4224391 discloses a zinc-nickel electrolyte formulation in which one or more of boric acid, phosphoric acid or arsenic acid is added to an alkaline solution to provide a zinc-nickel battery having an improved cycle life of about 200 cycles, which is still not fully satisfactory.
Patent No. CN201510604420 discloses a zinc-nickel battery electrolyte formula, wherein a certain amount of bismuth compound is added into electrolyte, bismuth ions are dissolved in an electrolyte system, and can be deposited on the surface of a zinc electrode and form a layer of bismuth-containing compact protective film after being contacted with the zinc electrode, and the layer of protective film can fix zinc on the zinc electrode on the surface of the electrode, so that the zinc electrode is fundamentally prevented from being dissolved in the electrolyte, and the dissolution of the zinc electrode is minimized. Secondly, a certain amount of fluoride ions are added into the electrolyte, so that the dissolution of the zinc electrode can be further reduced, and the solubility of zinc in the electrolyte can be reduced. However, the existence of fluorine ions is liable to corrode the cathode using an aluminum plate as an electrode, which limits the application range of the electrolyte.
Disclosure of Invention
In order to solve the technical problems, the invention provides an electrolyte for a secondary zinc-nickel battery, which can reduce the dissolution of a zinc electrode and inhibit the growth of zinc dendrites.
The invention provides an electrolyte for a secondary zinc-nickel battery, which comprises the following components in percentage by weight:
25-50 w% of alkali, 0.01-5 w% of LiOH and/or lithium salt, 0.1-5 w% of boric acid and/or borate, 0.01-1 w% of aluminum-containing substance, 5-15 w% of ZnO, 0.005-0.03 w% of SiO2And the balance being pure water.
Further, the aluminum-containing substance is Al simple substance, Al (OH)3、Al2O3、AlF3One or more of.
Further, the alkali is one or two of industrial-grade potassium hydroxide and industrial-grade sodium hydroxide.
Further, the lithium salt is lithium carbonate.
Further, the purity of the alkali is more than or equal to 99.9 percent.
Further, SiO2Is fumed silica.
Further, the pure water is industrial pure water, and has a resistivity (25 ℃) of 0.1 to 1.0X 10cm and a salt content of 1 to 5 mg/L.
The invention has the advantages and beneficial effects that: according to the invention, an aluminum-containing substance is added into the electrolyte for the rechargeable zinc-nickel battery, aluminum in the electrolyte has influence on the appearance of zinc deposition, and can effectively inhibit the growth of zinc grains, Al is added into the electrolyte and is firstly reduced into an Al simple substance during electrochemical circulation, so that the zinc cathode has higher conductivity, and aluminum has influence on the appearance of zinc deposition, and can inhibit the growth of zinc grains to improve the performance of the zinc electrode. FromThereby improving the performance of the zinc electrode. The electrolyte is high-alkali high-concentration electrolyte, can bring excellent rate performance to the battery, increases the concentration of the electrolyte, improves the energy density of the battery, and improves the capacity retention rate. In addition, LiOH and Li are added into the electrolyte+Into Ni (OH)2And improve the mobility of protons, Li+Is much less than K+Can effectively inhibit K+The doping of (2) stabilizes the electrolyte in the crystal lattice and improves Ni in the charging and discharging process2+And Ni3+The conversion efficiency of the nickel anode is improved, and the cycle performance of the nickel anode is improved. Li+And the poisoning effect of impurity Fe in the electrolyte or the electrode can be reduced, and the efficiency of the battery is influenced. Adding SiO into electrolyte2Then, SiO is formed with the electrolyte3 2+The viscosity of the electrolyte is increased, and the fluidity of the electrolyte is reduced, so that the solubility of active substances in the electrolyte is reduced, the deformation of a zinc electrode is slowed down, and the distribution uniformity of electrode current is facilitated. Adding H into electrolyte3BO3And/or borates, H3BO3And/or borate formation in lye B4O7 2-，B4O7 2-The presence of the zinc oxide can inhibit the adsorption of ZnO on the surface of the electrode and inhibit the passivation of the zinc electrode, thereby improving the charge and discharge performance of the zinc electrode.
Drawings
Fig. 1 shows the results of the charge and discharge efficiency test in example 1 of the present invention.
Fig. 2 shows the results of the charge and discharge efficiency test in example 2 of the present invention.
Fig. 3 shows the results of the charge and discharge efficiency test in example 3 of the present invention.
Fig. 4 shows the results of the charge and discharge efficiency test in example 4 of the present invention.
Detailed Description
The present invention will be further described with reference to the following embodiments.
In order to solve the problem of dendritic crystal growth of the zinc-nickel battery, the invention provides an electrolyte for a secondary zinc-nickel battery, which comprises 25-50 w% of alkali solution and 0.01-5 w%0.1-5 w% of boric acid and/or borate, 0.01-1 w% of aluminum-containing substance, 5-15 w% of ZnO, 0.005-0.03 w% of SiO2And the balance being pure water. The reason for adopting the electrolyte with the formula is that a certain amount of aluminum-containing substance is added into the electrolyte for the rechargeable zinc-nickel battery, and aluminum has influence on the appearance of zinc deposition in the electrolyte, so that the growth of zinc grains can be effectively inhibited, and the performance of a zinc electrode is improved.
Secondly, the electrolyte is high-concentration electrolyte, the increase of alkalinity can bring excellent rate performance to the battery, and the battery shell carries out charging and discharging of heavy current. The increase of the concentration of the electrolyte improves the energy density of the battery and improves the capacity retention rate.
And thirdly, the battery performance can be improved by adding LiOH into the electrolyte. Li+Into Ni (OH)2And improve the mobility of protons, Li+Is much less than K+Can effectively inhibit K+The doping of (2) stabilizes the electrolyte in the crystal lattice and improves Ni in the charging and discharging process2+And Ni3+The conversion efficiency of the nickel anode is improved, and the cycle performance of the nickel anode is improved. Li+The poisoning effect of impurity Fe in electrolyte or electrode can be reduced, the formation of micro battery by Fe and zinc codeposition is avoided, the hydrogen precipitation potential is reduced, the zinc is reversely dissolved, and the current efficiency is reduced. However, too high a concentration of LiOH can also compromise the performance of the cell. The ionic conductivity of LiOH is low, and an excessively high Li ion concentration lowers the operating voltage of the battery.
Adding SiO into electrolyte2Then, SiO is formed with the electrolyte3 2+The viscosity of the electrolyte is increased, and the fluidity of the electrolyte is reduced, so that the solubility of active substances in the electrolyte is reduced, the deformation of a zinc electrode is slowed down, and the distribution uniformity of electrode current is facilitated.
Adding H into electrolyte3BO3And/or borates, H3BO3And/or borate with lye to form B4O7 2-，B4O7 2-Can adsorb ZnO on the surface of the electrodeHas the effect of inhibiting the passivation of the zinc electrode, thereby improving the charge and discharge performance of the zinc electrode.
Example 1
35 w% base (technical Potassium hydroxide), 2 w% LiOH, 2 w% boric acid, 0.1 w% Al (OH)310 w% of ZnO, 0.01 w% of SiO2And the balance being water.
Adding the substances into pure water in a certain sequence, stirring and cooling until no precipitate is generated, fixing the volume, adding the mixture into a 10AH battery according to the technical requirements of battery manufacture to form the battery, and carrying out a battery cycle test by using a current of 1C. The results are shown in FIG. 1. It is found that the charge/discharge efficiency of the battery was still maintained at 95% or more after 1250 cycles, and the cycle performance of the battery was good.
Example 2
45 w% base (technical potassium hydroxide), 1 w% LiOH, 1 w% boric acid and/or borate, 0.2 w% Al2O312 w% of ZnO, 0.005 w% of SiO2And the balance being water.
Adding the substances into pure water in a certain sequence, stirring and cooling until no precipitate is generated, fixing the volume, adding the mixture into a 10AH battery according to the technical requirements of battery manufacture to form the battery, and carrying out a battery cycle test by using a current of 1C. The results are shown in FIG. 2. It is known that the charge/discharge efficiency of the battery was still maintained at 90% or more after 1250 cycles, and the cycle performance of the battery was good.
Example 3
40% by weight of base (technical-grade potassium hydroxide), 1.5% by weight of LiOH, 1.5% by weight of boric acid and/or borate, 0.1% by weight of AlF315 w% of ZnO, 0.01 w% of SiO2And the balance being water.
Adding the substances into pure water in a certain sequence, stirring and cooling until no precipitate is generated, fixing the volume, adding the mixture into a 10AH battery according to the technical requirement for formation, and carrying out a battery circulation test by using a 1C current. The results are shown in FIG. 3. It is found that the charge/discharge efficiency of the battery was maintained at 85% or more even after 1250 cycles, and the cycle performance of the battery was good.
Example 4
The electrolyte formulation of example 1 was added to a zinc-nickel battery (2v10Ah) and subjected to a high current charge-discharge cycle test, i.e., a current rush at 1C (10A), the results of which are shown in fig. 4. As can be seen from fig. 4, the cell was cycled approximately 1200 times, the efficiency of the cell was still above 95%, and no efficiency decay occurred. It can be confirmed that the electrolyte uses large current, the high rate performance of the battery is excellent, and the cycle life of the battery is remarkably prolonged along with the cycle. The best level can reach about 2000 times at present.
Materials, reagents and experimental equipment related to the embodiment of the invention are all commercial products in accordance with the field of battery electrolyte if no special description is provided.
The foregoing is only a preferred embodiment of the present invention, and it should be noted that, for those skilled in the art, modifications and decorations can be made without departing from the core technology of the present invention, and these modifications and decorations shall also fall within the protection scope of the present invention. Any changes which come within the meaning and range of equivalency of the claims are to be embraced within their scope.

Claims (6)

1. The electrolyte for the secondary zinc-nickel battery is characterized by comprising the following components in percentage by weight: 25-50 w% of alkali, 0.01-5 w% of LiOH and/or lithium salt, 0.1-5 w% of boric acid and/or borate, 0.01-1 w% of aluminum-containing substance, 5-15 w% of ZnO, 0.005-0.03 w% of SiO2The balance being pure water; the aluminum-containing substance is Al simple substance, Al (OH)3、Al2O3、AlF3One or more of.
2. The electrolyte for a secondary zinc-nickel battery according to claim 1, wherein the alkali is one or both of industrial-grade potassium hydroxide and industrial-grade sodium hydroxide.
3. The electrolyte for a secondary zinc-nickel battery according to claim 1, characterized in that the lithium salt is lithium carbonate.
4. The electrolyte for a secondary zinc-nickel battery according to claim 1, wherein the alkali has a purity of not less than 99.9%.
5. The electrolyte for secondary zinc-nickel battery as claimed in claim 1, wherein SiO is SiO2Is fumed silica.
6. The electrolyte for secondary zinc-nickel battery as claimed in claim 1, wherein the pure water is industrial pure water, and has a resistivity of 0.1 to 1.0 x 10cm at 25 ℃ and a salt content of 1 to 5 mg/L.
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Publication number Priority date Publication date Assignee Title
CN1139824A (en) * 1995-10-10 1997-01-08 刘建政 High energy and capacity zinc negative pole basic accumulator and dry battery
JPH10223228A (en) * 1997-02-06 1998-08-21 Sanyo Electric Co Ltd Alkaline battery
WO2002039521A1 (en) * 2000-11-10 2002-05-16 Powergenix Systems, Inc. Negative electrode formulation for a low toxicity zinc electrode having additives with redox potentials positive to zinc potential
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CN101677136A (en) * 2008-09-18 2010-03-24 中国人民解放军63971部队 Electrolyte solution for alkaline zinc flow battery
CN104752777A (en) * 2013-12-31 2015-07-01 王家祥 High-proportion zinc borate battery electrolyte and preparation method
CN205159452U (en) * 2015-11-19 2016-04-13 广州道动新能源有限公司 Two electrolyte zinc secondary cell of a new generation
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CN1139824A (en) * 1995-10-10 1997-01-08 刘建政 High energy and capacity zinc negative pole basic accumulator and dry battery
JPH10223228A (en) * 1997-02-06 1998-08-21 Sanyo Electric Co Ltd Alkaline battery
WO2002039521A1 (en) * 2000-11-10 2002-05-16 Powergenix Systems, Inc. Negative electrode formulation for a low toxicity zinc electrode having additives with redox potentials positive to zinc potential
CN101252204A (en) * 2008-02-21 2008-08-27 中国科学院化学研究所 Liquid state electrolyte for zinc-nickel secondary batteries and preparing method thereof
CN101677136A (en) * 2008-09-18 2010-03-24 中国人民解放军63971部队 Electrolyte solution for alkaline zinc flow battery
CN104752777A (en) * 2013-12-31 2015-07-01 王家祥 High-proportion zinc borate battery electrolyte and preparation method
CN205159452U (en) * 2015-11-19 2016-04-13 广州道动新能源有限公司 Two electrolyte zinc secondary cell of a new generation
CN108232333A (en) * 2017-12-29 2018-06-29 东莞市朗泰通实业有限公司 A kind of low-temperature electrolyte of Ni-MH battery

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