CN111834705B - Air battery - Google Patents
Air battery Download PDFInfo
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- CN111834705B CN111834705B CN201910324522.XA CN201910324522A CN111834705B CN 111834705 B CN111834705 B CN 111834705B CN 201910324522 A CN201910324522 A CN 201910324522A CN 111834705 B CN111834705 B CN 111834705B
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- 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
- H01M12/04—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
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
- H01M4/383—Hydrogen absorbing alloys
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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 an air battery with a novel structure, which comprises a hydrogen storage alloy electrode (5), an aluminum electrode (21), an air electrode (31), a diaphragm (4) and electrolyte, wherein the hydrogen storage alloy electrode (5) and the diaphragm (4) divide the electrolyte into a replacement part (2) and an oxidation part (3); therefore, the electrolyte of the oxidation part does not need to be changed in the oxidation process of the whole air battery, and the electrolyte of the replacement part is replaced in the whole process. The air battery has a novel internal structure, and has high electron utilization rate under the condition of equivalent alkali concentration; a higher volume density can be maintained under the condition of less alkali concentration; in addition, the air battery has a simple structure and can be used for industrial production and application.
Description
Technical Field
The invention relates to the field of air batteries, in particular to an air battery.
Background
The aluminum air battery is a primary battery with huge theoretical specific capacity (8100Wh/kg), has wide application in offshore power supplies and submarine AIP systems, and has the advantages of light weight, no toxicity, harm and the like.
And the aluminum-air battery can complete the recycling process by mechanically replacing aluminum and recycling the consumed alkaline electrolyte during the utilization process. Fig. 1 shows two typical prior battery structures, wherein the positive electrode and the negative electrode of the battery are not isolated by a diaphragm, or the replacement part and the oxidation part are only separated from electrolyte by an ion exchange membrane. In the electrode structure, when the alkali in the electrolyte is not excessive relative to the alkali consumed by the aluminum, and when the aluminum electrode is nearly completely consumed, a large amount of aluminum hydroxide precipitates appear in the electrolyte to block the ion diffusion in the solution, so that the internal resistance of the battery is high. Further oxidation of the hydride of the hydrogen storage alloy is hindered, resulting in loss of electrode energy.
In order to make the aluminum react completely and ensure that the internal resistance of the battery is still small, the alkali content in the electrolyte needing to be replaced is higher than the alkali content consumed by corresponding aluminum. This means that an excess of electrolyte needs to be provided each time the alkaline electrolyte is replaced, thereby reducing the overall mass capacity density of the battery.
Disclosure of Invention
In order to solve the above problems, the present inventors have conducted intensive studies to adopt a novel battery structure in which an electrolyte part of the battery structure is divided into a replacement part and an oxidation part by a separator and a hydrogen storage alloy electrode. The electrolyte of the oxidation part does not need to be changed in the oxidation process of the whole air battery, and the electrolyte of the replacement part is replaced in the whole process. And the aluminum electrode and the hydrogen storage alloy electrode are in composite contact. In the electrode structure, when the alkali in the electrolyte is not excessive relative to the alkali consumed by the aluminum, and when the aluminum electrode is nearly completely consumed, a large amount of aluminum hydroxide precipitates appear in the replacement part of the electrolyte to block the ion diffusion in the solution, and the aluminum electrode and the hydrogen storage alloy electrode can still discharge by oxidizing part of the electrolyte. At this time, the energy density of the electrode can be maintained, an excessive amount of electrolyte is not required, and the overall mass capacity density of the battery can be increased, thereby completing the present invention.
The invention aims to provide an air battery with a novel structure, which is embodied in the following aspects:
(1) an air battery having a novel structure, wherein the air battery comprises a hydrogen storage alloy electrode, an aluminum electrode, an air electrode, a separator, and an electrolyte, wherein the hydrogen storage alloy electrode and the separator divide the electrolyte into a replacement part and an oxidation part.
(2) The air battery according to the above (1), wherein,
the aluminum electrode is arranged on the replacement part; and/or
The air electrode is disposed at the oxidation part.
(3) The air battery according to the above (1), wherein,
the hydrogen storage alloy electrode is simultaneously contacted with the electrolyte of the replacement part and the electrolyte of the oxidation part; and/or
The separator is in contact with the electrolyte of the replacement part and simultaneously in contact with the electrolyte of the oxidation part; and/or
The hydrogen storage alloy electrode is compounded with the aluminum electrode to form a compound electrode; are constrained to be compounded together by mechanical forces.
(4) The air battery according to one of the above (1) to (3), wherein,
the aluminum electrode is made of an aluminum material selected from aluminum and/or aluminum alloy; and/or
The hydrogen storage alloy electrode is made of a hydrogen storage alloy; and/or
The diaphragm is an ion exchange membrane, preferably selected from an anion exchange membrane, a cation exchange membrane or a proton exchange membrane.
(5) The air battery according to the above (1), wherein,
the air battery comprises a battery shell 1 filled with electrolyte, wherein a baffle plate 11 is arranged in the battery shell 1 to divide the battery shell 1 into a replacing part 2 and an oxidizing part 3.
(6) The air battery according to the above (5), wherein,
an aluminum electrode 21 is provided in the replacement part 2; and/or
An air electrode 31 is provided in the oxidation part 3.
(7) The air battery according to the above (5), wherein,
a first hole is formed in the baffle plate 11, and a diaphragm 4 is arranged at the first hole; and/or
The baffle 11 is also provided with a second hole, and a hydrogen storage alloy electrode 5 is arranged at the second hole.
(8) The air battery according to one of (5) to (7), wherein a fastening screw hole 7 is formed in the battery case 1 at a position corresponding to the aluminum electrode, and the fastening screw 6 passes through the fastening screw hole 7 and abuts against the aluminum electrode 21 to combine the aluminum electrode 21 and the hydrogen storage alloy electrode 5.
(9) The air battery according to the above (8), wherein an electrode replacement port 9 is provided in the battery case 1 adjacent to the aluminum electrode 21 for replacing the aluminum electrode.
(10) The air battery according to the above (9), wherein,
the battery shell and the replacement part are provided with at least one liquid injection port 8 for injecting electrolyte;
at least one liquid injection port 8 is formed in the oxidation part of the battery shell and used for injecting electrolyte.
Drawings
FIGS. 1-2 show two schematic structural views of an air cell disclosed in the prior art;
fig. 3 is a schematic view showing the structure of an air battery according to the present invention;
FIGS. 4, 5-1 and 6-1 show cross-sectional views of the invention for an air cell;
FIG. 5-2 shows a cross-sectional view at A-A in FIG. 5-1;
FIG. 6-2 shows a cross-sectional view at B-B in FIG. 6-1;
FIG. 7 shows the constant current discharge curves at 300mA/g current density for the example and comparative air cells;
fig. 8 shows the multi-cycle performance of the composite electrode prepared in the example.
Reference numerals
1. A battery case; 11. a baffle plate; 1-1, a first shell; 1-2 and a second shell; 1-3, connecting screw holes; 2. a replacement part; 21. an aluminum electrode; 3. an oxidizing moiety; 31. an air electrode; 4. a diaphragm; 5. a hydrogen storage alloy electrode; 4-5, rubber ring; 6. fastening screws; 7. fastening screw holes; 8. a liquid injection port; 9. the electrode replaces the port.
Detailed Description
The features and advantages of the present invention will become more apparent and appreciated from the following detailed description of the invention.
The present invention provides an air battery having a novel structure, as shown in fig. 3, which includes a hydrogen storage alloy electrode, an aluminum electrode, an air electrode, a separator, and an electrolyte, wherein the hydrogen storage alloy electrode and the separator divide the electrolyte into a replacement part and an oxidation part, and the aluminum electrode is disposed at the replacement part and the air electrode is disposed at the oxidation part.
In a further preferred embodiment, the hydrogen storage alloy electrode is in simultaneous contact with the replacement part of the electrolyte and the oxidation part of the electrolyte.
In a still further preferred embodiment, the separator is in simultaneous contact with the replacement part of the electrolyte and the oxidation part of the electrolyte.
In the present invention, the electrolyte is divided into two parts by the hydrogen storage alloy electrode and the diaphragm, so that the aluminum electrode is located at the replacement part and the air electrode is located at the oxidation part, and thus, precipitation of aluminum hydroxide occurs in only the replacement part of the electrolyte. Due to the barrier effect of the hydrogen storage alloy electrode and the diaphragm, the aluminum hydroxide precipitate does not migrate to the oxidized part, i.e., does not affect the oxidized part, and exists only in the replacement part. Therefore, the electrolyte does not need to be excessively existed, and only the electrolyte of the replacement part is replaced when the aluminum electrode is nearly completely consumed. And the hydrogen storage alloy electrode is also contacted with the electrolyte of the oxidation part at the same time, the alkali concentration of the electrolyte of the oxidation part (oxidation part) is still high, and sufficient ion diffusion can be realized, so that the electrode can normally operate, and the energy of the electrode can be stored.
According to a preferred embodiment of the present invention, the hydrogen storage alloy electrode is combined with an aluminum electrode to form a combined electrode.
Therefore, a large amount of hydrogen generated by the self-corrosion of the aluminum-air battery is absorbed by the hydrogen storage alloy electrode, and the hydrogen absorbed hydrogen storage alloy electrode can lose hydrogen through the electrochemical process, thereby becoming a battery for providing energy. Therefore, in the present invention, the hydrogen storage alloy electrode absorbs the unused hydrogen gas, and the unused energy of the aluminum-air battery due to self-corrosion can be utilized, thereby improving the overall energy utilization rate.
In a further preferred embodiment, the hydrogen storage alloy electrode and the aluminum electrode are composited together by mechanical force.
According to a preferred embodiment of the present invention, the aluminum electrode is made of an aluminum material selected from aluminum and/or aluminum alloys.
In a further preferred embodiment, the aluminum material is in the form of flakes, powder, rods and/or foils.
In a further preferred embodiment, the aluminum material is in the form of a sheet, a rod and/or a foil, for example a sheet.
According to a preferred embodiment of the present invention, the hydrogen storage alloy electrode is made of a hydrogen storage alloy.
In a further preferred embodiment, the hydrogen storage alloy is selected from the group consisting of AB5Type A2B type, AB2Any one or more of type, V-based hydrogen storage alloy, and Mg-based hydrogen storage alloy.
In a further preferred embodiment, the AB is5The type hydrogen storage alloy is selected from LaNi5、Mm(NiCoMnAl)5And Mm (NiCoMnTi)5One or more of; a is described2The B-type hydrogen storage alloy is selected from Mg2One or more of Ni, Mg-Fe alloy, Mg-Ti alloy and Mg-Co alloy; the AB type hydrogen storage alloy is selected from TiFe and/or TiFe partially substituted with TiFe-based element, such as Ti1.1Fe0.9Ni0.1、TiFe0.9Mn0.1Etc.; the AB is2The type hydrogen storage alloy is selected from Ti-Zr-V-Cr-Mn alloy and/or Ti-Zr-V-Ni-Cr alloy; the Mg-based hydrogen storage alloy is an alloy consisting of Mg, La and Y, such as La2Mg17、MgY2、Mg24Y5And the like.
According to a preferred embodiment of the present invention, said air electrode 31 comprises a waterproof and breathable layer, a supporting layer and a catalytic layer.
Wherein, the air electrode can be an electrode of a common oxygen reduction reaction.
According to a preferred embodiment of the present invention, the electrolyte is an alkaline electrolyte.
In a further preferred embodiment, the electrolyte is a sodium hydroxide solution and/or a potassium hydroxide solution with a concentration of 1-7M.
According to a preferred embodiment of the present invention, as shown in fig. 4 to 6, the air battery includes a battery case 1 filled with an electrolyte, and a baffle plate 11 is provided in the battery case 1 to divide the battery case 1 into a replacement part 2 and an oxidation part 3.
In a further preferred embodiment, an aluminum electrode 21 is provided within the replacement part 2.
In a further preferred embodiment, an air electrode 31 is provided in the oxidation part 3, and preferably, the air electrode 31 is provided on a wall of the battery case 1, and one side of the air electrode 31 is in contact with air and the other side is in contact with the electrolyte.
The whole electrolyte tank is divided into two parts, during the working process of the battery, the electrolyte of the oxidation part keeps the initial alkali concentration unchanged, and the alkali concentration of the electrolyte of the replacement part is reduced. The initial electrolyte concentration of the battery and the oxidation part only need to have certain alkali concentration, the alkali concentration of the replacement part corresponds to the alkali consumption of the aluminum, and excessive electrolyte is not needed.
In a preferred embodiment, the battery case may be integrally formed or may be assembled together. As shown in fig. 6-2, the battery case is formed by butt-jointing and combining a case body 1-1 and a case body two 1-2, preferably, corresponding connecting screw holes 1-3 are formed on the case body 1-1 and the case body two 1-2, and more preferably, connecting screws sequentially penetrate through the connecting screw holes on the case body 1-1 and the case body 1-2 to connect and fix the case body 1-1 and the case body 1-2.
According to a preferred embodiment of the present invention, the baffle 11 is provided with a first hole.
In a further preferred embodiment, a membrane 4 is arranged at said first aperture.
In a still further preferred embodiment, the membrane is an ion exchange membrane, preferably selected from an anion exchange membrane, a cation exchange membrane or a proton exchange membrane, such as CMI-7000, AMI-7001, Nafion or the like.
Wherein the membrane only allows electrons to pass through, and aluminum hydroxide precipitates generated in the replacement part are blocked in the replacement part and cannot migrate into the oxidation part, so that the reaction of the oxidation part is not influenced.
According to a preferred embodiment of the present invention, the baffle 11 is further provided with a second hole.
In a further preferred embodiment, a hydrogen storage alloy electrode 5 is provided at the second hole.
Thus, the hydrogen storage alloy material is located intermediate the replacement section and the oxidation section and is in simultaneous contact with the electrolyte of the replacement section and the electrolyte of the oxidation section. And when the reaction of the aluminum electrode of the replacement part is complete and the part contains a large amount of aluminum hydroxide precipitates, only the electrolyte in the replacement part needs to be replaced, and the electrolyte in the oxidation part does not need to be replaced.
And, when the aluminum electrode of the replacement part is completely consumed, the main electrode structure which further becomes the electrode source is a hydrogen storage alloy electrode. The hydrogen storage alloy electrode is also contacted with the electrolyte of the oxidation part at the same time, the alkali concentration of the electrolyte of the oxidation part is still high, and sufficient ion diffusion can be realized, so that the electrode can normally operate, and the energy of the electrode can be stored.
In the present invention, it is preferable that the diaphragm 4 and the hydrogen storage alloy electrode 5 are fixedly connected to the baffle plate 11 through rubber rings 4 to 5.
Wherein, the rubber ring 4-5 is used for fixing the diaphragm and the hydrogen storage alloy at the hole of the baffle plate 11 respectively.
According to a preferred embodiment of the present invention, the hydrogen storage alloy electrode is directly combined with an aluminum electrode to form a combined electrode.
In a further preferred embodiment, the hydrogen storage alloy electrode and the aluminum electrode are mechanically composited together, for example, by fastening screws 6.
In a further preferred embodiment, a fastening screw hole 7 is formed on the battery case 1 at a position corresponding to the aluminum electrode, and the fastening screw 6 passes through the fastening screw hole 7 and abuts against the aluminum electrode 21 to combine the aluminum electrode 21 and the hydrogen storage alloy electrode 5.
The aluminum electrode and the hydrogen storage alloy electrode are compounded to form the composite electrode, so that a large amount of hydrogen generated by the self-corrosion of the aluminum-air battery is absorbed by the hydrogen storage alloy electrode, and the hydrogen storage alloy electrode after hydrogen absorption can lose hydrogen through the electrochemical process, thereby becoming a battery for providing energy. Wherein, the fastening screw hole and the fastening screw are both common screw holes and screws, and are defined as the fastening screw hole and the fastening screw for distinguishing from the connecting screw holes 1-3.
According to a preferred embodiment of the present invention, an electrode replacement port 9 is formed in the battery case 1 adjacent to the aluminum electrode 21.
Wherein the electrode replacement port is used for replacing the aluminum electrode.
According to a preferred embodiment of the present invention, at least one liquid inlet 8 for injecting the electrolyte is provided in the battery case at the replaceable portion.
In a further preferred embodiment, at least one liquid pouring port 8 is provided in the battery case at the oxidized portion.
The liquid inlet 8 is used for injecting the electrolyte.
The invention has the following beneficial effects:
(1) the air battery has a novel internal structure, and has high electron utilization rate under the condition of equivalent alkali concentration;
(2) the air battery can keep a higher capacity density under the condition of less alkali concentration;
(3) the air battery has a simple structure and can be used for industrial production and application.
Examples
The present invention is further described below by way of specific examples. However, these examples are only illustrative and do not set any limit to the scope of the present invention.
In implementation, the air electrode of the aluminum-air battery is purchased from yunan yun aluminum comet-invasive green battery limited.
Example 1
600mg LaNi5 powder with the particle size of about 1 micron is pressed into a sheet with the area of 1.33cm2 under the pressure of 40Mpa, and then the sheet and foamed nickel are pressed into the hydrogen storage alloy electrode;
preparing an aluminum sheet with the mass of 45mg and the area of 1.33cm2 by using a slicer, and pressing the aluminum sheet and foamed nickel into an aluminum electrode;
fixing the prepared hydrogen storage alloy electrode and the purchased air electrode in the air battery designed according to the figures 4-6, enabling an aluminum electrode to enter from an electrode replacing port in the figure 3, and fixing the aluminum electrode and the hydrogen storage alloy electrode together by depending on the mechanical force in the battery to finish the assembly of the aluminum hydrogen storage alloy composite electrode;
fixing the anion permeable membrane of CMJ-7001 in the cell designed as shown in FIG. 3, and sealing the whole cell structure by a rubber gasket;
the electrolyte was oxidized by adding 20mL of 1MKOH in the oxidation portion and 10mL of 1MKOH in the replacement portion.
Comparative example
The procedure of example 1 was repeated except that: the cell structure is a cell designed as in the right side of fig. 1.
The air batteries described in the examples and comparative examples were subjected to a constant current discharge test of 300 mA/g; as a result, as shown in FIG. 7, it can be seen that the discharge performance of the example is significantly superior to that of the comparative example at a constant current of 300 mA/g;
after the reaction of the air battery of the embodiment is completed, the aluminum electrode is taken out from the electrode replacement port and the replacement part of the electrolyte is taken out from the electrolyte injection port, a new aluminum electrode and 10mL of 1MKOH are added, and the constant current discharge test of 300mA/g is repeatedly carried out, and the structure is shown in FIG. 8, and it can be seen that the mass specific capacity of the air battery of the embodiment is still high after the air battery is repeatedly used for many times. Moreover, the inventor finds that the recycling can go through dozens of cycles through a large amount of experiments.
The invention has been described in detail with reference to specific embodiments and illustrative examples, but the description is not intended to be construed in a limiting sense. Those skilled in the art will appreciate that various equivalent substitutions, modifications or improvements may be made to the technical solution of the present invention and its embodiments without departing from the spirit and scope of the present invention, which fall within the scope of the present invention. The scope of the invention is defined by the appended claims.
Claims (9)
1. An air battery, comprising a hydrogen storage alloy electrode, an aluminum electrode, an air electrode, a separator, and an electrolyte, wherein the hydrogen storage alloy electrode and the separator divide the electrolyte into a replacement part and an oxidation part,
the electrolyte of the oxidation part does not need to be changed in the oxidation process of the whole air battery, and the electrolyte of the replacement part is replaced in the whole process;
the aluminum electrode is arranged on the replacement part;
the air electrode is arranged on the oxidation part;
the hydrogen storage alloy electrode is simultaneously contacted with the electrolyte of the replacement part and the electrolyte of the oxidation part;
the separator is in contact with the electrolyte of the replacement part and simultaneously in contact with the electrolyte of the oxidation part;
the initial electrolyte concentration of the cell, the amount of alkali concentration of the replacement part and the amount of alkali consumed by the aluminum electrode correspond.
2. The air battery of claim 1, wherein the hydrogen storage alloy electrode is composited with an aluminum electrode to form a composite electrode; are constrained to be compounded together by mechanical forces.
3. The air battery according to claim 1 or 2,
the aluminum electrode is made of an aluminum material selected from aluminum and/or aluminum alloy; and/or
The hydrogen storage alloy electrode is made of a hydrogen storage alloy; and/or
The diaphragm is an ion exchange membrane.
4. The air cell of claim 3, wherein the membrane is selected from an anion exchange membrane, a cation exchange membrane, or a proton exchange membrane.
5. The air battery of claim 1,
the air battery comprises a battery shell (1) filled with electrolyte, wherein a baffle (11) is arranged in the battery shell (1) and divides the battery shell (1) into a replacement part (2) and an oxidation part (3).
6. The air battery of claim 5,
a first hole is formed in the baffle (11), and a diaphragm (4) is arranged at the first hole; and/or
The baffle (11) is also provided with a second hole, and a hydrogen storage alloy electrode (5) is arranged at the second hole.
7. The air battery of claim 5 or 6, wherein the battery case (1) is provided with fastening screw holes (7) at positions corresponding to the aluminum electrodes, and the fastening screws (6) pass through the fastening screw holes (7) and abut against the aluminum electrodes (21) to combine the aluminum electrodes (21) and the hydrogen storage alloy electrodes (5).
8. The air battery according to claim 7, wherein an electrode replacement port (9) is provided on the battery case (1) adjacent to the aluminum electrode (21) for replacing the aluminum electrode.
9. The air battery of claim 8,
the battery shell and the replacement part are provided with at least one liquid injection port (8) for injecting electrolyte; and/or
At least one liquid injection port (8) is formed in the oxidation part of the battery shell and used for injecting electrolyte.
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| CN201910324522.XA CN111834705B (en) | 2019-04-22 | 2019-04-22 | Air battery |
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| CN201910324522.XA CN111834705B (en) | 2019-04-22 | 2019-04-22 | Air battery |
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| CN111834705B true CN111834705B (en) | 2022-01-14 |
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| CN108615850A (en) * | 2018-04-20 | 2018-10-02 | 北京大学 | A kind of Combined electrode and its preparation for air cell |
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2019
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| CN1871728A (en) * | 2003-10-21 | 2006-11-29 | 瑞沃特科技有限公司 | Electrode, method of its production, metal-air fuel cell and metal hydride cell |
| WO2012056301A1 (en) * | 2010-10-29 | 2012-05-03 | Toyota Jidosha Kabushiki Kaisha | Air electrode for metal-air battery, membrane/air electrode assembly for a metal-air battery having such air electrode, and metal-air battery |
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