CN113782842A - Aqueous zinc ion battery electrolyte and battery - Google Patents
Aqueous zinc ion battery electrolyte and battery Download PDFInfo
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- CN113782842A CN113782842A CN202110981039.6A CN202110981039A CN113782842A CN 113782842 A CN113782842 A CN 113782842A CN 202110981039 A CN202110981039 A CN 202110981039A CN 113782842 A CN113782842 A CN 113782842A
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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
- H01M10/36—Accumulators not provided for in groups H01M10/05-H01M10/34
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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
- H01M10/42—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
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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
- H01M2300/00—Electrolytes
- H01M2300/0002—Aqueous electrolytes
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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
- H01M2300/00—Electrolytes
- H01M2300/0088—Composites
- H01M2300/0091—Composites in the form of mixtures
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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 discloses a water-based zinc ion battery electrolyte and a battery. The electrolyte includes: the battery positive electrode material comprises a zinc salt solution, sodium polyalkylsulfonate and salt containing cations in the battery positive electrode material, wherein the number of alkyl groups of the sodium polyalkylsulfonate is 10-30. According to the invention, a surfactant sodium polyalkylsulfonate is added into the electrolyte as an additive component, so that the hydrogen evolution reaction accompanying the zinc in the electrochemical deposition process can be effectively inhibited, the corrosion to a zinc cathode caused by the increase of the pH value of the electrolyte due to hydrogen ion evolution is reduced, and meanwhile, the sodium polyalkylsulfonate can play a dispersing role in the conduction of zinc ions when being adsorbed on the surface of a non-polar zinc sheet, so that the formation of concentrated nucleation and dendritic crystals is avoided. Thereby improving the electrochemical performance of the zinc ion battery and improving the safety of the battery.
Description
Technical Field
The invention belongs to the technical field of zinc ion batteries, and particularly relates to a water-based zinc ion battery electrolyte and a battery.
Background
With the continuous consumption of fossil energy and the increasingly urgent need for environmental pollution abatement, clean energy will gradually become the main energy source for people's life in the near future, but the current mainstream clean energy, whether wind energy or solar energy, has temporal heterogeneity in the power generation process, so there is an urgent need for a large-scale energy storage device to store wind energy and solar energy that are not uniformly generated in time, so that the effect of uniform and effective supply in time is achieved. Battery devices have been generally considered as the best choice for large-scale energy storage systems, and water-based zinc-ion batteries are considered as the second choice for large-scale energy storage systems due to their advantages of low cost, high safety, environmental friendliness, and higher energy density. However, the practical application of the current water-based zinc ion battery faces serious safety problems, not only the growth of zinc dendrite may cause the piercing of a diaphragm to cause short circuit, but also the gas production caused by side reactions such as hydrogen evolution and the like may cause the short circuit and even explosion of the battery, thereby causing serious battery safety problems.
At present, the inhibition method for hydrogen evolution on the surface of a zinc cathode mainly comprises the steps of reducing dendritic crystal growth on the surface of the cathode from the aspect of the cathode so as to avoid sharp hydrogen evolution caused by point discharge, adding a modification additive to inhibit dendritic crystal and corrosion from the aspect of electrolyte so as to inhibit hydrogen evolution reaction, or reducing the content of water molecules by using solid or quasi-solid electrolyte, wherein the cost of adding the modification additive into the electrolyte is low, and the inhibition on the hydrogen evolution reaction is direct, so that the inhibition method brings extensive and attention to researchers. The south kayak university army research team (nat. commun.2018, 9, 1656.) discloses a sodium sulfate additive that suppresses dendrite growth by electrostatic shielding effect to achieve a reduction in hydrogen evolution reaction to some extent; the Beijing condensation state physical national laboratory Chen spring research team (ChemElectrochem 2018, 5, 2409.) of the physical research institute of Chinese academy of sciences discloses a lithium bis (trifluoromethanesulfonyl) imide and a zinc bis (trifluoromethanesulfonyl) imide additive, the reaction activity of water molecules is weakened through eutectic structures, and the hydrogen evolution reaction is also inhibited to a certain extent, but inorganic additives are difficult to directly act on the hydrogen evolution reaction, and organic high-salt additives greatly improve the cost of the battery, so that the double problems of safety and cost cannot be solved substantially.
Disclosure of Invention
Aiming at the defects or improvement requirements of the prior art, the invention provides a water-system zinc ion battery electrolyte and a battery, and aims to avoid hydrogen evolution reaction of water in an electrochemical deposition process and effectively avoid the concentrated nucleation of zinc ions and the formation of zinc dendrites by adding a surfactant, namely sodium polyalkylsulfonate, into the electrolyte, so that the electrochemical performance of the zinc ion battery is improved by effectively avoiding side reactions such as dendrites and corrosion, the hydrogen evolution reaction is also inhibited, and the safety of the battery is improved.
In order to achieve the above object, according to one aspect of the present invention, there is provided an aqueous zinc-ion battery electrolyte comprising: the battery positive electrode material comprises a zinc salt solution, sodium polyalkylsulfonate and salt containing cations in the battery positive electrode material, wherein the number of alkyl groups of the sodium polyalkylsulfonate is 10-30.
Preferably, the zinc salt solution is a zinc sulphate solution.
Preferably, the concentration of the zinc salt in the zinc salt solution is 1-3 mol/L.
Preferably, the sodium polyalkylsulfonate is sodium dodecyl sulfonate or sodium hexadecyl sulfonate.
Preferably, the sodium polyalkylsulfonate is in a saturated concentration in the electrolyte.
Preferably, the salt containing the cations in the positive electrode material of the battery is specifically manganese sulfate when the positive electrode material of the battery is manganese dioxide, and lithium sulfate when the positive electrode material of the battery is a positive electrode of a mixed lithium ion battery (where the mixed ion battery refers to that the metal cations extracted from the negative electrode and the metal cations inserted into the positive electrode are two different ions).
In accordance with another aspect of the invention, an aqueous zinc-ion battery is provided that includes an aqueous zinc-ion battery electrolyte.
Preferably, the positive electrode of the battery is manganese dioxide or a positive electrode material of a mixed lithium ion battery, and the negative electrode of the battery is zinc. The mixed ion battery refers to that metal cations extracted from a negative electrode and metal cations embedded in a positive electrode are two different ions.
In general, at least the following advantages can be obtained by the above technical solution contemplated by the present invention compared to the prior art.
(1) According to the invention, the surfactant sodium polyalkylsulfonate is used as an additive component and added into the aqueous zinc ion electrolyte, so that the water and zinc ions can be effectively inhibited from simultaneously contacting the surface of a negative electrode in the electrochemical deposition process of zinc through the adsorption effect of the sodium polyalkylsulfonate on a zinc sheet and the hydrophobicity of a hydrophobic group, thereby avoiding the hydrogen evolution reaction of the water in the electrochemical deposition process, and effectively reducing the side reactions of the electrolyte, such as corrosion and the like caused by the increase of pH value due to the precipitation of the hydrogen ions. In addition, when the sodium polyalkyl sulfonate is adsorbed on the surface of the zinc sheet, the conduction of zinc ions is also dispersed by the uniformly distributed sodium polyalkyl sulfonate, so that the concentrated nucleation of the zinc ions and the formation of zinc dendrites are avoided. Therefore, the electrochemical performance of the zinc ion battery is improved by effectively avoiding side reactions such as dendrite and corrosion, the hydrogen evolution reaction is inhibited, and the safety of the battery is improved.
(2) According to the invention, the sodium polyalkylsulfonate surfactant is used as an electrolyte additive, and the adsorption effect of hydrophilic groups on zinc sheets and the repulsion effect of hydrophobic groups on water molecules can be utilized to effectively prevent the water molecules from approaching the surface of the negative electrode to participate in hydrogen evolution reaction.
(3) The sodium polyalkylsulfonate surfactant selected by the invention is matched with zinc ion batteries such as MnO2、LiMn2O4The positive electrode has a certain adsorption effect, so that the contact of positive active substances and water molecules can be effectively avoided, and the dissolution of positive materials is reduced.
(4) The electrolyte provided by the invention has the advantages of low cost of raw materials, simple preparation and great application prospect and research value in the safety field of zinc ion batteries.
Drawings
FIG. 1(a) is a 2mol/L zinc sulfate +1mmol/L sodium dodecylsulfate aqueous zinc ion battery electrolyte pack constructed according to a preferred embodiment of the present inventionThe current density of the zinc cathode of the battery is 4mA cm-2And 1mAh cm-2SEM image after 20 cycles of circulation under the condition, and (b) in figure 1 is the current density of 4mA cm of the negative electrode of the symmetrical battery system without the sodium dodecyl sulfate additive-2And 1mAh cm-2SEM images after cycling 20 cycles under conditions;
FIG. 2 is a diagram of a zinc symmetrical cell assembled with 2mol/L zinc sulfate +0.9mmol/L sodium dodecyl sulfate aqueous zinc ion cell electrolyte constructed according to a preferred embodiment of the present invention at a current density of 8mA cm-2And 1mAh cm-2Long cycle performance under conditions; wherein, bare Zn refers to a comparison group without additives, SLS-Zn refers to an experimental group added with sodium dodecyl sulfate;
FIG. 3 is a zinc vs. α -MnO assembly of 2mol/L zinc sulfate +1.1mmol/L sodium dodecylsulfate +0.2mol/L manganese sulfate aqueous zinc ion battery electrolyte constructed in accordance with a preferred embodiment of the present invention2Full cell is 0.3A g-1The capacity exertion of the cycle and the coulombic efficiency; wherein, bare Zn refers to a comparison group without additives, SLS-Zn refers to an experimental group added with sodium dodecyl sulfate;
FIG. 4 is a zinc pair LiMn assembled from 1.5mol/L zinc sulfate +1mmol/L sodium hexadecylsulfonate +1mol/L lithium sulfate aqueous zinc ion battery electrolyte constructed in accordance with a preferred embodiment of the present invention2O4The total battery is 0.1A g-1The charge-discharge curve of the first turn under the condition (1).
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is described in further detail below with reference to the accompanying drawings and embodiments. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention. In addition, the technical features involved in the embodiments of the present invention described below may be combined with each other as long as they do not conflict with each other.
Example 1
The embodiment provides a preparation method of an aqueous zinc-ion battery electrolyte, the aqueous zinc-ion battery electrolyte prepared by the method and a corresponding battery, wherein the method comprises the following steps:
preparing 2mol/L zinc sulfate solution, then adding sodium dodecyl sulfate to enable the concentration of the sodium dodecyl sulfate to be 1mmol/L, and magnetically stirring for 12 hours to enable the sodium dodecyl sulfate to be uniformly dispersed to obtain electrolyte.
Results and analysis:
the method comprises the following steps of (1) assembling a 2032 button type symmetrical battery by taking zinc sheets as a positive electrode and a negative electrode, taking glass fiber as a diaphragm, adding 80 mu L of sodium dodecyl sulfate as electrolyte of an additive, assembling the 2032 button type symmetrical battery by taking 2mol/L of zinc sulfate electrolyte without the sodium dodecyl sulfate as a comparison group under the same condition, and carrying out electrochemical circulation on the obtained button battery by using a blue electricity electrochemical test system, wherein the circulation condition is as follows: the current density was 4mA cm-2The circulation surface capacity is 1mA cm-2The cycle frequency is 20 times, and a charging process is added after the cycle is completed to observe the deposition morphology of the zinc anode after the sodium dodecyl sulfate additive is added.
The button cell after circulation is disassembled, and SEM test is carried out on the positive pole piece, the result is shown in figures 1(a) - (b), it can be seen that after the sodium dodecyl sulfate additive is added, the deposition morphology of the zinc piece is more uniform, and the reaction active area is increased after the hydrogen evolution reaction is inhibited, so that more nucleation sites are provided, and the zinc deposition is uniform, so that the formation of dendritic crystals is avoided.
Example 2
The embodiment provides a preparation method of an aqueous zinc-ion battery electrolyte, the aqueous zinc-ion battery electrolyte prepared by the method and a corresponding battery, wherein the method comprises the following steps:
preparing 2mol/L zinc sulfate solution, then adding sodium dodecyl sulfate to enable the concentration of the sodium dodecyl sulfate to be 0.9mmol/L, and magnetically stirring for 12 hours to enable the sodium dodecyl sulfate to be uniformly dispersed to obtain electrolyte.
Results and analysis:
using zinc sheets as a positive electrode and a negative electrode, using glass fiber as a diaphragm, adding 80 mu L of sodium dodecyl sulfate as an electrolyte of an additive, assembling a 2032 button-type symmetrical battery, and adding no sodium dodecyl sulfate2mol/L zinc sulfate electrolyte of sodium is as the contrast group to same condition equipment 2032 button symmetry battery, carries out the electrochemical performance test with the button cell who obtains with blue electricity electrochemistry test system, and the circulation condition is: the current density was 8mA cm-2The circulation surface capacity is 1mA cm-2。
The results of observing the cycling stability of the zinc symmetrical battery under long cycle after the electrolyte with sodium dodecyl sulfate as the additive is added are shown in figure 2, and the results show that the cycling stability of the zinc symmetrical battery after the electrolyte with sodium dodecyl sulfate as the additive is added is greatly improved compared with the ordinary zinc symmetrical battery even at 8mA cm-2The current density of the cell was still stable for over 500 hours, while the control rapidly produced an open circuit, indicating that gas accumulation ultimately led to cell failure.
Example 3
The embodiment provides a preparation method of an aqueous zinc-ion battery electrolyte, the aqueous zinc-ion battery electrolyte prepared by the method and a corresponding battery, wherein the method comprises the following steps:
preparing 2mol/L zinc sulfate and 0.2mol/L manganese sulfate solution, then adding sodium dodecyl sulfate to enable the concentration of the sodium dodecyl sulfate to be 1.1mmol/L, and magnetically stirring for 12 hours to enable the sodium dodecyl sulfate to be uniformly dispersed to obtain electrolyte.
Results and analysis:
using zinc sheet as negative electrode, alpha-MnO2As the positive electrode, glass fiber is used as the diaphragm, 80 μ L of sodium dodecyl sulfate is added as the electrolyte of the additive, 2032 button full cells are assembled, 2mol/L zinc sulfate without sodium dodecyl sulfate and 0.2mol/L manganese sulfate electrolyte are used as the comparison group, 2032 button full cells are assembled under the same conditions, the obtained button cells are tested for electrochemical performance by a blue electrochemical testing system, and the cycle conditions are as follows: the current density was 0.3A/g.
Observation of Zinc vs. alpha-MnO after adding sodium dodecyl sulfate as additive to electrolyte2The electrical performance of the full cell under long circulation to test the practical application prospect of the sodium dodecyl sulfate is shown in figure 3, and the figure shows that the dodecyl sulfonic acid is addedZinc-to-alpha-MnO after electrolyte with sodium as additive2The cycle stability of the whole battery is still compared with that of common zinc to alpha-MnO2The full battery is obviously improved, higher specific capacity and coulombic efficiency can be kept under the condition of 0.3A/g, and a comparison sample is obviously reduced along with the time extension, which shows that the specific discharge capacity is continuously reduced due to the rapid reduction of the reaction active area on the surface of the negative electrode caused by the accumulation of gas along with the circulation.
Example 4
The embodiment provides a preparation method of an aqueous mixed ion battery electrolyte, the aqueous mixed ion battery electrolyte prepared by the method and a corresponding battery, wherein the method comprises the following steps:
preparing 1.5mol/L zinc sulfate and 1mol/L lithium sulfate solution, then adding sodium hexadecylsulfonate to enable the concentration of the sodium hexadecyl sulfonate to be 1mmol/L, and magnetically stirring for 12 hours to enable the sodium hexadecyl sulfonate to be uniformly dispersed to obtain electrolyte.
Results and analysis:
zinc sheet as negative electrode, LiMn2O4And (2) as a mixed ion anode, glass fiber as a diaphragm, adding 80 mu L of sodium hexadecyl sulfonate as electrolyte of an additive, assembling 2032 button full cells, and carrying out charge-discharge test on the button cells by using a blue electrochemical test system under the following cycle conditions: the current density was 0.1A/g.
Observation of zinc vs LiMn after addition of electrolyte with sodium hexadecylsulfonate as additive2O4The results of the charging and discharging of the whole cell are shown in FIG. 4, which shows the zinc vs. LiMn after the electrolyte solution containing sodium hexadecyl sulfonate as an additive is added2O4The full battery can complete normal charging and discharging and give play to LiMn2O4The electrolyte can be charged to 2V, and has no obvious overcharge phenomenon caused by hydrogen evolution, which shows that the sodium hexadecyl sulfonate as an additive successfully widens the electrochemical window of the electrolyte and inhibits water decomposition, so that zinc can react with LiMn2O4Long-term cycling of the full cell is a practical possibility.
It will be understood by those skilled in the art that the foregoing is only a preferred embodiment of the present invention, and is not intended to limit the invention, and that any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the scope of the present invention.
Claims (8)
1. An aqueous zinc ion battery electrolyte, comprising: the battery positive electrode material comprises a zinc salt solution, sodium polyalkylsulfonate and salt containing cations in the battery positive electrode material, wherein the number of alkyl groups of the sodium polyalkylsulfonate is 10-30.
2. The aqueous zinc ion battery electrolyte of claim 1 wherein the zinc salt solution is a zinc sulfate solution.
3. The aqueous zinc ion battery electrolyte according to claim 2, wherein the concentration of the zinc salt in the zinc salt solution is 1 to 3 mol/L.
4. The aqueous zinc ion battery electrolyte of claim 1 wherein the sodium polyalkylsulfonate is sodium dodecyl sulfonate or sodium hexadecyl sulfonate.
5. The aqueous zinc ion battery electrolyte of claim 1 wherein the sodium polyalkylsulfonate is at a saturated concentration in the electrolyte.
6. The aqueous zinc-ion battery electrolyte according to claim 1, wherein the salt containing the cation in the battery positive electrode material is specifically manganese sulfate when the battery positive electrode material is manganese dioxide, and lithium sulfate when the battery positive electrode material is a mixed lithium-ion battery positive electrode.
7. An aqueous zinc-ion battery comprising the aqueous zinc-ion battery electrolyte according to any one of claims 1 to 6.
8. The battery of claim 7, wherein the positive electrode of the battery is manganese dioxide or a mixed lithium ion battery positive electrode material, and the negative electrode of the battery is zinc.
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Cited By (2)
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| CN114249860A (en) * | 2021-12-14 | 2022-03-29 | 青岛科技大学 | Preparation and application of water-system zinc ion battery gel electrolyte |
| CN114447444A (en) * | 2021-12-21 | 2022-05-06 | 广东工贸职业技术学院 | Compound additive electrolyte and application thereof in water-based zinc ion battery |
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