CN113363627A - Corrosion inhibitor for aluminum-air battery and application thereof - Google Patents
Corrosion inhibitor for aluminum-air battery and application thereof Download PDFInfo
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- CN113363627A CN113363627A CN202110619779.5A CN202110619779A CN113363627A CN 113363627 A CN113363627 A CN 113363627A CN 202110619779 A CN202110619779 A CN 202110619779A CN 113363627 A CN113363627 A CN 113363627A
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- aluminum
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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
- H01M12/00—Hybrid cells; Manufacture thereof
- H01M12/04—Hybrid cells; Manufacture thereof composed of a half-cell of the fuel-cell type and of a half-cell of the primary-cell type
- H01M12/06—Hybrid cells; Manufacture thereof composed of a half-cell of the fuel-cell type and of a half-cell of the primary-cell type with one metallic and one gaseous electrode
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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
- H01M12/00—Hybrid cells; Manufacture thereof
- H01M12/02—Details
Abstract
The invention relates to a corrosion inhibitor for an aluminum-air battery and application thereof, wherein the corrosion inhibitor comprises a combination of sodium stannate and glycerol in a molar ratio of 1 (1-300). The electrolyte corrosion inhibitor is composed of glycerol and sodium stannate, so that a layer of uniform and porous layered structure can be formed on the surface of the aluminum electrode. Thereby effectively making the electrode erosion rate small. The composite action of the glycerol and the sodium stannate can effectively inhibit the self-corrosion reaction of the aluminum electrode, effectively improve the discharge capacity of the aluminum electrode, and obviously improve the utilization rate of the aluminum electrode, thereby prolonging the service life of the electrode and enabling the battery to be more durable. The electrolyte corrosion inhibitor has the advantages of simple structure, easy preparation, low cost and the like, and is easy to apply in a large area.
Description
Technical Field
The invention relates to the technical field of batteries, in particular to a corrosion inhibitor for an aluminum-air battery and application thereof.
Background
In recent years, with the decrease of fossil energy reserves, people pay more and more attention to the field of new energy. As a new type of energy battery, the metal-air battery has the advantages of both primary battery and fuel cell, and has the advantages of convenient replacement, high specific energy, low cost,The advantages of energy conservation, environmental protection and the like are widely concerned. Among the numerous metal-air batteries, aluminum-air batteries offer high theoretical energy density (8100 Wh. kg)-1) And a high theoretical volumetric energy density (21.9Wh cm)-3)。
In addition, aluminum electrode replacement is relatively easy to operate, low cost and environmentally friendly, making it an attractive anode material for metal-air battery systems. However, the self-corrosion of aluminum anodes in alkaline electrolytes severely limits the normal use and storage of aluminum air cells. To solve this problem, two methods are generally employed. The first method is to add Mg, Mn, Pb, Bi, Cd, Zn, Sn, In, Ga or other metals to the aluminum electrode. However, many researchers have studied this method, and the results show that this method is costly and less effective. Another method is to add a corrosion inhibitor to the alkaline electrolyte. These inhibitors may be inorganic, organic, or complex. Organic additives have been widely studied because of their low toxicity and susceptibility to decomposition. However, the single corrosion inhibitor does not achieve satisfactory results.
CN102088115A discloses a composite corrosion inhibitor of alkaline aluminum battery alkaline electrolyte, the electrolyte and a preparation method, wherein the disclosed alkaline battery aluminum anode corrosion inhibitor is compounded by an inorganic corrosion inhibitor and an organic corrosion inhibitor, the inorganic corrosion inhibitor comprises sodium stannate, indium hydroxide, sodium citrate, calcium oxide and zinc oxide; the organic corrosion inhibitor comprises a chitosan derivative and an organic surfactant; the concentration of each component in the alkaline electrolyte is as follows: 0.015-0.1 mol/L of sodium stannate; 0.005-0.05 mol/L of indium hydroxide; 0.03-0.1 mol/L of sodium citrate; 0.003-0.05 mol/L of calcium oxide; 0.02-0.1 mol/L of zinc oxide; 0.01-0.1 wt% of chitosan derivative; 0.05-0.5 wt% of organic surfactant. The corrosion inhibitor disclosed by the invention can effectively inhibit the corrosion of the aluminum electrode in an alkaline solution, does not affect the electrochemical activity of the aluminum anode, but has complex components and higher cost.
CN112103562A discloses an electrolyte additive, an electrolyte containing the additive and a lithium metal battery, wherein the disclosed additive is an organic phosphonic acid scale and corrosion inhibitor, and the organic phosphonic acid is one or more of amino trimethylene phosphonic acid, ethylene diamine tetra methylene phosphonic acid, hydroxy ethylidene diphosphonic acid, hexamethylene diamine tetra methylene phosphonic acid, diethylene triamine methylene phosphonate, diethylene triamine penta methylene phosphonic acid, dihexyl triamine penta methylene phosphonic acid, hydroxyl phosphonoacetic acid and polyamino polyether methylene phosphonic acid. The electrolyte additive disclosed by the invention can form a stable complex with iron, copper, zinc and other metal ions, can dissolve oxides on the metal surface, is stable under the condition of high pH value, can effectively improve the cycling stability of the battery in the charging and discharging process and inhibit the generation of lithium dendrites in the cycling process of the lithium metal battery, thereby improving the safety of the lithium metal battery. The electrolyte additive disclosed by the patent requires the addition of other metals, and is high in cost and low in benefit.
Therefore, it is necessary to find an inorganic-organic composite corrosion inhibitor with good effect and low cost.
Disclosure of Invention
In view of the defects of the prior art, the invention aims to provide a corrosion inhibitor for an aluminum-air battery and application thereof, wherein the corrosion inhibitor is applied to an electrolyte, and the further formed aluminum-air battery has higher battery energy density and electrode utilization rate.
In order to achieve the purpose, the invention adopts the following technical scheme:
in a first aspect, the invention provides a corrosion inhibitor for an aluminum-air battery, which comprises a combination of sodium stannate and glycerol in a molar ratio of 1 (1-300), wherein 1-300 can be 2, 4, 6, 8, 10, 20, 50, 80, 100, 120, 150, 180, 200, 220, 250, 280 and the like.
Glycerol of the formula C3H8O3It is colorless, odorless, sweet at normal temperature, and has clear, viscous and liquid appearance, and is an organic substance. Can be mixed and dissolved with water in any proportion, can stably exist in alkaline solution, and has no corrosiveness to metal. The glycerol contains three hydroxyl polar functional groups, has strong adsorption capacity and high viscosity, has the advantages of low toxicity, easy degradation and the like, and is an additive with research value.
Sodium stannate as aThe inorganic corrosion inhibitor can play a role in inhibiting hydrogen evolution, can reduce the polarization of the electrode and can make the electrode potential shift negatively, because the sodium stannate can generate a metal Sn layer on the surface of the electrode after being dissolved, and the corresponding reaction equation is SnO3 2-+3H2O+4e-→Sn+6OH-Tin as a high hydrogen evolution overpotential metal can effectively weaken the hydrogen evolution reaction, thereby playing a role in inhibiting the self-corrosion reaction of the electrode.
However, when sodium stannate is used alone as an additive, the tin layer deposited on the surface of the electrode of the aluminum-air battery is not uniform, and the formed tin layer has high porosity, so that the tin layer cannot play a good role in inhibiting corrosion. When adding glycerine, because the adsorption of propanol, can adsorb on the electrode surface with the compound absorption of electrode surface's tin layer for the distribution of tin layer is more even, and is also more stable at the absorption on electrode surface.
Therefore, the electrolyte corrosion inhibitor composed of glycerol and sodium stannate can form a layer of uniform and porous layered structure on the surface of the electrode of the aluminum-air battery, so that the corrosion rate of the electrode is effectively reduced.
Preferably, the sodium stannate comprises anhydrous sodium stannate and/or sodium stannate trihydrate.
Preferably, the corrosion inhibitor comprises a combination of sodium stannate and glycerol in a molar ratio of 1 (5-200), wherein 5-200 may be 6, 7, 9, 11, 15, 17, 21, 31, 41, 52, 62, 72, 82, 92, 102, 112, 122, 132, 142, 152, 162, 172, 182, 192, and the like.
In a second aspect, the present invention provides an electrolyte for an aluminum-air battery, the electrolyte comprising a strong base, a solvent and the corrosion inhibitor of the first aspect.
Preferably, the strong base comprises sodium hydroxide and/or potassium hydroxide.
Preferably, the solvent comprises deionized water.
Preferably, the molar concentration of the strong base in the electrolyte is 0.5-7mol/L, such as 1mol/L, 1.5mol/L, 2mol/L, 2.5mol/L, 3mol/L, 3.5mol/L, 4mol/L, 4.5mol/L, 5mol/L, 5.5mol/L, 6mol/L, 6.5mol/L, etc., preferably 2-6 mol/L.
Preferably, the molar concentration of the sodium stannate in the electrolyte is 0.01-0.10mol/L, such as 0.02mol/L, 0.03mol/L, 0.04mol/L, 0.05mol/L, 0.06mol/L, 0.07mol/L, 0.08mol/L, 0.09mol/L, and the like, preferably 0.05-0.06 mol/L.
Preferably, the molar concentration of the glycerol in the electrolyte is 0.1-3mol/L, such as 0.2mol/L, 0.4mol/L, 0.6mol/L, 0.8mol/L, 1mol/L, 1.2mol/L, 1.4mol/L, 1.6mol/L, 1.8mol/L, 2mol/L, 2.2mol/L, 2.4mol/L, 2.6mol/L, 2.8mol/L, etc., preferably 0.5-2mol/L, and more preferably 1 mol/L.
In a third aspect, the present invention provides a method for preparing the electrolyte for an aluminum-air battery according to the second aspect, the method comprising the steps of:
mixing strong base, solvent and the corrosion inhibitor according to the formula ratio to obtain the electrolyte.
In a fourth aspect, the present invention provides an aluminum-air battery comprising the electrolyte of the second aspect.
Compared with the prior art, the invention has the following beneficial effects:
the electrolyte corrosion inhibitor is composed of glycerol and sodium stannate, so that a layer of uniform and porous layered structure can be formed on the surface of the aluminum electrode. Thereby effectively making the electrode erosion rate small. The composite action of the glycerol and the sodium stannate can effectively inhibit the self-corrosion reaction of the aluminum electrode, effectively improve the discharge capacity of the aluminum electrode, and obviously improve the utilization rate of the aluminum electrode, thereby prolonging the service life of the electrode and enabling the battery to be more durable. The electrolyte corrosion inhibitor has the advantages of simple structure, easy preparation, low cost and the like, and is easy to apply in a large area. The energy density of the aluminum-air battery formed by applying the corrosion inhibitor in the electrolyte is 249.6 Wh-kg-1In the above, the electrode utilization rate was 7.51% or more.
Drawings
FIG. 1 is a scanning electron micrograph of an aluminum anode after static self-etching in the electrolyte described in example 1;
FIG. 2 is a scanning electron micrograph of an aluminum anode after static self-etching in the electrolyte described in example 2;
FIG. 3 is a scanning electron micrograph of an aluminum anode after static self-etching in the electrolyte described in example 3;
FIG. 4 is a scanning electron micrograph of an aluminum anode after static self-etching in the electrolyte described in comparative example 2.
Detailed Description
For the purpose of facilitating an understanding of the present invention, the present invention will now be described by way of examples. It should be understood by those skilled in the art that the examples are only for the understanding of the present invention and should not be construed as the specific limitations of the present invention.
Example 1
This example provides a corrosion inhibitor consisting of anhydrous sodium stannate and glycerol in a molar ratio of 1: 1.
The embodiment also provides an electrolyte, which comprises strong base (sodium hydroxide), solvent (deionized water) and the corrosion inhibitor;
in the electrolyte, the concentration of the anhydrous sodium stannate is 0.1mol/L, the concentration of the glycerol is 0.1mol/L, and the concentration of the sodium hydroxide is 4 mol/L.
The preparation method of the electrolyte comprises the following steps:
and mixing strong base with a formula amount with a solvent, and then mixing with a corrosion inhibitor to obtain the electrolyte.
Example 2
This example provides a corrosion inhibitor consisting of anhydrous sodium stannate and glycerol in a molar ratio of 1: 300.
The embodiment also provides an electrolyte, which comprises strong base (potassium hydroxide), solvent (deionized water) and the corrosion inhibitor;
in the electrolyte, the concentration of the anhydrous sodium stannate is 0.01mol/L, the concentration of the glycerol is 3mol/L, and the concentration of the potassium hydroxide is 2 mol/L.
The preparation method of the electrolyte comprises the following steps:
and mixing strong base with a formula amount with a solvent, and then mixing with a corrosion inhibitor to obtain the electrolyte.
Example 3
This example provides a corrosion inhibitor consisting of sodium stannate trihydrate and glycerol in a molar ratio of 1: 10.
The embodiment also provides an electrolyte, which comprises strong base (potassium hydroxide), solvent (deionized water) and the corrosion inhibitor;
in the electrolyte, the concentration of the sodium stannate trihydrate is 0.04mol/L, the concentration of the glycerol is 0.4mol/L, and the concentration of the potassium hydroxide is 6 mol/L.
The preparation method of the electrolyte comprises the following steps:
and mixing strong base with a formula amount with a solvent, and then mixing with a corrosion inhibitor to obtain the electrolyte.
Examples 4 to 6
Examples 4-6 differ from example 1 in that the concentrations of sodium stannate trihydrate were 0.05mol/L, 0.06mol/L and 0.02mol/L, respectively, and accordingly the molar ratios of anhydrous sodium stannate to glycerol were 1:2, 3:5 and 1:5, the remainder being the same as in example 1.
Examples 7 to 9
Examples 7-9 differ from example 1 in that the glycerol concentrations were 0.5mol/L, 2mol/L and 2.5mol/L, respectively, and accordingly, the molar ratios of anhydrous sodium stannate to glycerol were 1:5, 1:20 and 1:25, and the remainder was the same as example 1.
Comparative example 1
This comparative example provides a corrosion inhibitor that is anhydrous sodium stannate.
The present comparative example provides an electrolyte comprising a strong base (sodium hydroxide), a solvent (deionized water), and the corrosion inhibitor described above;
in the electrolyte, the concentration of the anhydrous sodium stannate is 0.1mol/L, and the concentration of the sodium hydroxide is 4 mol/L.
The preparation method of the electrolyte comprises the following steps:
and mixing strong base with a formula amount with a solvent, and then mixing with a corrosion inhibitor to obtain the electrolyte.
Comparative example 2
This comparative example provides a corrosion inhibitor that is glycerol.
The present comparative example provides an electrolyte comprising a strong base (sodium hydroxide), a solvent (deionized water), and the corrosion inhibitor described above;
in the electrolyte, the concentration of the glycerol is 0.1mol/L, and the concentration of the sodium hydroxide is 4 mol/L.
The preparation method of the electrolyte comprises the following steps:
and mixing strong base with a formula amount with a solvent, and then mixing with a corrosion inhibitor to obtain the electrolyte.
Comparative example 3
This comparative example differs from example 1 in that glycerin was replaced with ethylene glycol, and the rest was the same as example 1.
Performance testing
Examples 1-9 and comparative examples 1-3 were tested as follows:
(1) assembling the electrolyte with an aluminum cathode, an air anode and an electrolytic tank to form an aluminum-air battery, testing the aluminum-air battery by using a discharge test, wherein the test time is 60min, the discharge current is set to be 5mA, and after the test is finished, calculating the average voltage, the electrode utilization rate and the battery energy density, wherein a 4mol/L sodium hydroxide aqueous solution is used as a blank comparative example for comparison;
(2) performing static self-corrosion on an aluminum anode in the aluminum-air battery in the electrolyte to obtain a scanning electron microscope image;
the test results are summarized in table 1.
TABLE 1
| Average voltage/V | Energy density/Wh.kg-1 | Electrode utilization rate% | |
| Example 1 | 1.22 | 268.5 | 8.65 |
| Example 2 | 1.18 | 275.6 | 8.91 |
| Example 3 | 1.25 | 288.4 | 10.01 |
| Example 4 | 1.23 | 287.3 | 9.89 |
| Example 5 | 1.24 | 296.7 | 11.32 |
| Example 6 | 1.21 | 249.6 | 7.51 |
| Example 7 | 1.28 | 310.5 | 13.11 |
| Example 8 | 1.29 | 316.2 | 13.18 |
| Example 9 | 1.25 | 270.3 | 8.86 |
| Blank comparative example | 1.14 | 166.5 | 5.07 |
| Comparative example 1 | 1.24 | 187.6 | 6.32 |
| Comparative example 2 | 1.17 | 191.3 | 6.97 |
| Comparative example 3 | 1.19 | 225.3 | 7.21 |
Analysis of the data in Table 1 shows that the corrosion inhibitor of the invention is applied to an aluminum air battery formed in an electrolyte, and the energy density is 249.6 Wh-kg-1Above, electrode utilization ratioMore than 7.51 percent of the corrosion inhibitor is applied to the aluminum air battery formed by the electrolyte, and the aluminum air battery has higher battery energy density and electrode utilization rate.
Analysis of comparative example 1 and example 1 shows that comparative example 1 is inferior to example 1 in performance, which is mainly due to the fact that glycerol and ethylene glycol have different molecular structures, glycerol contains three hydroxyl groups, and the hydroxyl group is one more hydroxyl group than ethylene glycol, and the hydroxyl group is a polar functional group, so that the glycerol has higher adsorption performance on an aluminum electrode, tin simple substance can be adsorbed on the surface of the aluminum electrode more firmly, the discharge performance of the aluminum electrode is improved, and the synergistic effect of glycerol and sodium stannate is proved to be beneficial to improvement of the performance of an aluminum air battery.
As can be seen from the analysis of the blank comparative example, comparative examples 2 to 3 and example 1, the voltage of the battery was stably increased and the energy density of the battery was partially increased when sodium stannate was added alone (comparative example 2) relative to the blank comparative example, but the degree of the increase was not significant; when glycerol is added alone (comparative example 3), the average voltage of the battery is reduced to a certain extent, because the glycerol is an organic substance and has higher viscosity, the conductivity of the solution is reduced, but the glycerol can be adsorbed on the surface of an aluminum electrode as a polar molecule, so that the corrosion rate of the glycerol is reduced, and the energy density of the battery is correspondingly improved. When both sodium stannate and glycerol were added (example 1), there was a steady increase in the energy density, the most important indicators for the cell.
As can be seen from the analysis of examples 4 to 6 and example 1, the performance of examples 1 and 6 is inferior to that of examples 4 to 5, and it is confirmed that the overall performance of the aluminum-air battery is better when the concentration of sodium stannate in the electrolyte is 0.05 to 0.06 mol/L.
As can be seen from the analysis of examples 7 to 9 and example 1, examples 1 and 9 are inferior to examples 7 to 8 in performance, and it is confirmed that the overall performance of the aluminum-air battery obtained is better when the concentration of glycerol in the electrolyte is 0.5 to 2 mol/L.
As can be seen from the analysis of fig. 1-4, in fig. 4, compared with fig. 1-3, after the aluminum anode in the aluminum-air battery in fig. 4 undergoes static self-corrosion in the electrolyte, the surface is better porous and the corrosion strength is greater, which proves that the corrosion inhibitor of the present invention is more favorable for reducing the corrosion rate of the aluminum electrode in the aluminum-air battery.
The applicant states that the present invention is illustrated in detail by the above examples, but the present invention is not limited to the above detailed methods, i.e. it is not meant that the present invention must rely on the above detailed methods for its implementation. It should be understood by those skilled in the art that any modification of the present invention, equivalent substitutions of the raw materials of the product of the present invention, addition of auxiliary components, selection of specific modes, etc., are within the scope and disclosure of the present invention.
Claims (10)
1. The corrosion inhibitor for the aluminum-air battery is characterized by comprising a combination of sodium stannate and glycerol in a molar ratio of 1 (1-300).
2. The corrosion inhibitor for an aluminum air cell as recited in claim 1, wherein the sodium stannate comprises anhydrous sodium stannate and/or sodium stannate trihydrate.
3. The corrosion inhibitor for an aluminum-air battery according to claim 1, wherein the corrosion inhibitor comprises a combination of sodium stannate and glycerol in a molar ratio of 1 (5-200).
4. An electrolyte for an aluminum air battery, characterized in that the electrolyte comprises a strong base, a solvent and the corrosion inhibitor of any one of claims 1-3.
5. The electrolyte for an aluminum-air cell of claim 4, wherein the strong base comprises sodium hydroxide and/or potassium hydroxide.
6. The electrolyte for an aluminum-air battery according to claim 5, wherein the molar concentration of the strong base in the electrolyte is 0.5-7 mol/L.
7. The electrolyte for an aluminum-air battery according to claim 4, wherein the molar concentration of the sodium stannate in the electrolyte is 0.01-0.10 mol/L.
8. The electrolyte for an aluminum-air battery according to claim 4, wherein the molar concentration of the glycerol in the electrolyte is 0.1 to 3 mol/L.
9. A method for preparing the electrolyte for an aluminum-air battery according to any one of claims 4 to 8, comprising the steps of:
mixing a strong base, a solvent and the corrosion inhibitor of any one of claims 1-3 according to a formula ratio to obtain the electrolyte.
10. An aluminum-air battery, characterized in that it comprises an electrolyte according to any one of claims 4 to 8.
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| CN106887650A (en) * | 2015-12-16 | 2017-06-23 | 中国科学院大连化学物理研究所 | A kind of aluminium-air cell electrolyte and its preparation |
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| CN111416139A (en) * | 2020-03-06 | 2020-07-14 | 中科院过程工程研究所南京绿色制造产业创新研究院 | Electrolyte corrosion inhibitor, aluminum-air battery, alkaline electrolyte and preparation method thereof |
| CN111430741A (en) * | 2020-04-13 | 2020-07-17 | 中国地质大学（武汉） | Alkaline electrolyte composite corrosion inhibitor and aluminum-air battery |
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2021
- 2021-06-03 CN CN202110619779.5A patent/CN113363627A/en active Pending
Patent Citations (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2002086984A2 (en) * | 2001-04-19 | 2002-10-31 | Eontech Group, Inc. | Alkaline aluminum-air battery |
| CN103633396A (en) * | 2013-07-31 | 2014-03-12 | 河南科技大学 | Electrolyte corrosion inhibitor for aluminum-air cell, electrolyte and preparation method |
| CN106887650A (en) * | 2015-12-16 | 2017-06-23 | 中国科学院大连化学物理研究所 | A kind of aluminium-air cell electrolyte and its preparation |
| CN109216782A (en) * | 2018-09-20 | 2019-01-15 | 曹大平 | Alkaline chlorine aluminium mixed solvent constant pressure sealed colloidal accumulator |
| CN110165340A (en) * | 2019-05-21 | 2019-08-23 | 常州优特科新能源科技有限公司 | A kind of aluminium-air cell alkaline electrolyte and aluminium-air cell |
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| CN111430741A (en) * | 2020-04-13 | 2020-07-17 | 中国地质大学（武汉） | Alkaline electrolyte composite corrosion inhibitor and aluminum-air battery |
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Application publication date: 20210907 |