CN110048129B - Metal electrode material of metal-air battery and preparation method and application thereof - Google Patents
Metal electrode material of metal-air battery and preparation method and application thereof Download PDFInfo
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Abstract
The invention discloses a metal electrode material of a metal-air battery, and a preparation method and application thereof. The metal air battery metal electrode material is a magnesium alloy with a loose structure, wherein alloy elements in the magnesium alloy comprise at least one of aluminum, zinc, lithium, indium, gallium and manganese. The preparation method comprises the steps of carrying out smelting alloying treatment on magnesium metal and alloy metal and carrying out casting rolling treatment and rolling treatment on the magnesium alloy. The metal electrode material of the metal-air battery has the advantages of refining magnesium alloy grains, increasing hydrogen evolution reaction overpotential, destroying the structure of a passivation film, and reducing the problem of magnesium alloy passivation, so that the active dissolution of the electrode is promoted, and the electrochemical performance of the magnesium alloy is improved. And the preparation method has easily controlled conditions, and the prepared metal air battery metal electrode material has stable performance and high efficiency. The metal-air battery metal electrode material can be used for preparing metal-air battery metal electrodes and metal-air batteries.
Description
Technical Field
The invention belongs to the field of electrochemical energy, and particularly relates to a metal electrode material of a metal-air battery, and a preparation method and application thereof.
Background
The metal-air battery is a semi-fuel battery, which uses oxygen in the air as positive active material, uses metal (zinc, magnesium or aluminum, etc.) as negative active material, and the oxygen reaches the gas-solid-liquid three-phase interface through gas diffusion electrode to react with the metal to release electric energy. The metal-air battery has higher energy density, large capacity, high specific energy, stable working voltage, long service life, safety and reliability in use, rich raw materials, renewable utilization, high cost performance, no pollution, green energy, and good market application prospect in civil and military fields, such as emergency lighting and communication in disaster relief, emergency rescue, field and the like, and can be used as a power battery of an electric bicycle and an electric automobile.
In the metal electrode material of the metal-air battery, the metal magnesium is a very active anode material, the theoretical specific energy of the metal magnesium is up to 3910Wh/kg, which is 9 times of that of the lithium ion battery, the source is wide, the reserve is rich, the price is low, the reaction product does not cause environmental pollution, and the metal-air battery is an ideal electrode material of the metal-air battery. Since magnesium is a very active metal, the electrode potential is low and the chemical activity is very high, in most electrolyte solutions, the dissolution rate of magnesium is quite fast, a large amount of hydrogen is generated, and the faradaic efficiency of the anode is reduced. The common magnesium (with the purity of 99.0-99.9%) is easy to generate microscopic galvanic cell corrosion reaction due to the existence of harmful impurities, and the self-corrosion speed is high; at the same time, denser Mg (OH) is produced during the reaction2Passive film, which affects the active dissolution of the magnesium anode. Therefore, the search for the preparation of high-performance magnesium anodes is one of the key difficulties for practical application of magnesium air batteries.
Although reports of magnesium alloy anode materials appear at present, in the technical application process, the problems of contradiction between corrosion, activation and passivation of hydrogen evolution and the like are difficult to solve well by using the current commercial magnesium alloy anode materials, and the industrialization and the practical application of the magnesium air battery are limited.
Disclosure of Invention
The invention aims to overcome the defects in the prior art and provides a metal electrode material of a metal-air battery and a preparation method thereof, so as to solve the technical problems of hydrogen evolution, self-corrosion and passivation of the existing magnesium anode.
The invention also aims to provide a metal air battery metal electrode and a metal air battery, so as to solve the technical problem that the electrochemical performance of the metal air battery is not ideal due to the bad phenomena of hydrogen evolution, self-corrosion, passivation and the like of a magnesium anode contained in the metal electrode of the existing metal air battery.
In order to achieve the above object, according to one aspect of the present invention, a metal-air battery metal electrode material is provided. The metal air battery metal electrode material is a magnesium alloy with a loose structure, wherein alloy elements in the magnesium alloy comprise at least one of aluminum, lithium, zinc, indium, gallium and manganese.
In another aspect of the invention, a preparation method of the metal electrode material of the metal-air battery is provided. The preparation method of the metal electrode material of the metal-air battery comprises the following steps:
carrying out smelting alloying treatment on magnesium metal and alloy metal to form magnesium alloy; the alloy metal comprises at least one metal of aluminum, lithium, zinc, indium, gallium and manganese;
and (3) carrying out casting and rolling treatment on the magnesium alloy by adopting auxiliary heating to the temperature of 300-500 ℃, and then continuously carrying out rolling and rolling treatment for a plurality of times.
In still another aspect of the present invention, a metal-air battery metal electrode and a metal-air battery containing the metal-air battery metal electrode are provided. The metal air battery metal electrode is prepared from the metal air battery metal electrode material or the metal air battery metal electrode material prepared by the preparation method.
The metal-air battery comprises an air electrode, a metal electrode and electrolyte, wherein the metal electrode is the metal electrode of the metal-air battery.
Compared with the prior art, the invention has the following technical effects:
the metal electrode material of the metal-air battery adopts the magnesium alloy which is in a loose structure and is formed by at least one alloy element of aluminum, lithium, zinc, indium, gallium and manganese and magnesium, so that under the existence and the action of the alloy element, not only can the crystal grains of the magnesium alloy be refined, but also the overpotential of hydrogen evolution reaction is increased, and the self-corrosion speed is reduced; meanwhile, the structure of the passive film can be damaged, so that the complete and compact passive film is changed into a loose, porous and easily-falling corrosion product, the problem of magnesium alloy passivation is solved, the active dissolution of an electrode is promoted, and the electrochemical performance of the magnesium alloy is improved.
The preparation method of the metal-air battery metal electrode material provided by the invention has the advantages that the alloy metal and the magnesium metal are subjected to smelting alloying treatment, and the formed magnesium alloy is subjected to subsequent casting rolling treatment and rolling treatment, so that the formed metal-air battery metal electrode material has refined magnesium alloy grains, large overpotential of hydrogen evolution reaction, low self-corrosion speed and porosity. In addition, the preparation method has easily controlled conditions, and the prepared metal air battery metal electrode material has stable performance and high efficiency.
The metal electrode of the metal-air battery is prepared by adopting the metal electrode material of the metal-air battery, so that the overpotential of the hydrogen evolution reaction can be increased, and the self-corrosion speed is reduced; meanwhile, the structure of the passivation film can be damaged, so that the problem of magnesium alloy passivation is reduced, the active dissolution of an electrode is promoted, and the electrochemical performance of the magnesium alloy is improved. Therefore, the metal-air battery of the invention has excellent electrochemical performance.
Drawings
The invention will be further described with reference to the accompanying drawings and examples, in which:
FIG. 1 is a schematic process flow diagram of a method for preparing a metal electrode material of a metal-air battery according to an embodiment of the invention;
FIG. 2 is an X-ray diffraction pattern of a metal-air battery metal electrode material provided in example 1 of the present invention;
FIG. 3 is a scanning electron microscope image of a metal-air battery metal electrode material provided in embodiment 1 of the present invention;
fig. 4 is a spectrum analysis diagram of a metal-air battery metal electrode material provided in example 1 of the present invention.
Detailed Description
In order to make the technical problems, technical solutions and advantageous effects to be solved by the present invention more clearly apparent, the present invention is further described in detail below with reference to the following 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.
The mass of each component mentioned in the description of the embodiment of the present invention may not only refer to the specific content of each component, but also represent the proportional relationship of the mass between each component, and therefore, it is within the scope of the disclosure of the description of the embodiment of the present invention to scale up or down the content of each component according to the description of the embodiment of the present invention. Specifically, the mass described in the description of the embodiments of the present invention may be a mass unit known in the chemical industry field, such as μ g, mg, g, and kg.
In one aspect, embodiments of the present invention provide a metal-air battery metal electrode material. The metal air battery metal electrode material is a magnesium alloy with a porous loose structure, and a Scanning Electron Microscope (SEM) picture of the magnesium alloy is shown in figure 4, and the magnesium alloy has a rich microporous structure. Wherein, the alloy element in the magnesium alloy comprises at least one of aluminum, lithium, zinc, indium, gallium and manganese. Therefore, in the presence of the alloy elements and under the action of magnesium metal, not only can the crystal grains of the magnesium alloy be refined, but also the overpotential of the hydrogen evolution reaction of the magnesium alloy is increased, so that the self-corrosion speed is reduced; meanwhile, the structure of a passivation film generated in the discharging process of the magnesium alloy can be damaged, so that the complete and compact passivation film is changed into a loose, porous and easily-fallen corrosion product, the passivation problem of the magnesium alloy is reduced, and the electrochemical performance of the magnesium alloy is improved.
In one embodiment, the magnesium alloy contains [ 90% -100% by mass ] of magnesium, and the balance is the alloy element. Wherein [ 90% -100%) represents a mass content of 90% or more and less than 100%. In one specific implementation, the alloy elements are aluminum, zinc and manganese, and the mass content of magnesium is 96%, the mass content of aluminum is 3%, the mass content of zinc is 0.8% and the mass content of manganese is 0.2%. The proportion and the variety of the magnesium element and the alloy element are controlled to optimize and control, so that the crystal grains of the magnesium alloy can be optimized, the overpotential of the hydrogen evolution reaction of the magnesium alloy is increased, the self-corrosion speed is reduced, and the porous loose structure can be optimized.
In addition, according to SEM analysis of the metal-air battery metal electrode material, the pore diameter of the porous loose structure of the metal-air battery metal electrode material is nano and/or micron. The pore diameter of the porous loose structure is 100-200 nm. And the particle size of the magnesium particles in the magnesium alloy in the metal electrode material of the metal-air battery is 500nm-200 mu m. Therefore, the metal electrode material of the metal-air battery adopts the magnesium alloy which comprises the alloy elements and magnesium to form a porous loose structure, and the magnesium alloy is endowed with small crystal grains in the presence of the alloy elements and under the action of the alloy elements and magnesium metal, so that the overpotential of the hydrogen evolution reaction is increased, and the self-corrosion speed is reduced. Due to the existence of the positive alloy, the structure of a passive film generated by the magnesium alloy in the discharge process can be effectively destroyed, so that the problem of magnesium alloy passivation is reduced, and the electrochemical performance of the magnesium alloy is improved.
On the other hand, the embodiment of the invention also provides a preparation method of the metal electrode material of the metal-air battery. The process flow of the preparation method of the metal-air battery metal electrode material is shown in figure 1, and the preparation method comprises the following steps:
s01: carrying out smelting alloying treatment on magnesium metal and alloy metal to form magnesium alloy;
s02: and (3) carrying out casting and rolling treatment on the magnesium alloy by adopting auxiliary heating to the temperature of 300-500 ℃, and then continuously carrying out rolling and rolling treatment for a plurality of times.
The smelting alloying treatment in step S01 may be to melt the magnesium metal and the alloy metal according to the temperature and conditions for preparing the magnesium alloy, so as to form the magnesium alloy.
The alloy metal in this step S01 may be at least one metal including aluminum, zinc, lithium, zinc, indium, gallium, and manganese, as described above. In addition, it should be understood that before the smelting alloying treatment, the surfaces of the metals should be treated cleanly to avoid the impurities and the like from adversely affecting the performance of the finally prepared metal-air battery metal electrode material.
In the step S02, the magnesium alloy prepared in the step S01 is subjected to casting and rolling treatment at 500 ℃ and several times of rolling and rolling treatment, on one hand, the magnesium alloy is formed into a predetermined shape and state, and more importantly, the magnesium alloy is subjected to secondary modification treatment on the microscopic morphology, such as a porous loose structure, so that the formed metal-air battery metal electrode material retains the porous loose structure, has proper pore diameter, and has stable structure and good mechanical properties. Therefore, in a specific embodiment, the process conditions of the casting and rolling process should be that the magnesium alloy prepared in step S01 is cast and rolled until the mechanical performance requirements such as the size and the corresponding strength of the metal electrode of the metal-air battery are met. The rolling process can be 1 or more than 2 times, and the rolling process is combined with the casting process until the formed metal-air battery metal electrode material reaches the preset size, such as thickness and the like.
According to the preparation method of the metal-air battery metal electrode material, the alloy metal and the magnesium metal are subjected to smelting alloying treatment, casting rolling treatment and rolling treatment, so that the formed metal-air battery metal electrode material has refined magnesium alloy grains, large overpotential of hydrogen evolution reaction, low self-corrosion speed, a loose structure with proper pore diameter and excellent mechanical properties such as strength. In addition, the preparation method has easily controlled conditions, and the prepared metal air battery metal electrode material has stable performance and high efficiency.
On the other hand, based on the metal-air battery metal electrode material and the preparation method thereof, the embodiment of the invention also provides a metal-air battery metal electrode. The metal-air battery metal electrode is prepared from the metal-air battery metal electrode material or the metal-air battery metal electrode material prepared by the preparation method. The metal-air battery metal electrode material can be prepared by taking the metal-air battery metal electrode material as a material according to the requirements of the metal-air battery metal electrode. Based on the properties of the metal electrode material for the metal-air battery as described above, the metal electrode for the metal-air battery is excellent and stable in electrochemical properties.
The embodiment of the invention also provides a metal-air battery. The metal-air battery naturally includes necessary components of the metal-air battery, such as an air electrode, a metal electrode, an electrolyte, and the like, and of course, includes a case for containing the electrolyte. Wherein the metal electrode is the metal electrode of the metal-air battery. Thus, the metal-air battery has excellent and stable electrochemical performance.
The metal-air battery metal electrode material, the preparation method and the application thereof according to the embodiment of the invention are illustrated by a plurality of specific examples.
Example 1
The embodiment provides a metal-air battery metal electrode material and a preparation method thereof. The metal air battery metal electrode material is a magnesium alloy with a porous loose structure, and the magnesium alloy contains 96% of Mg, 3% of Al, 0.8% of Zn and 0.2% of Mn.
The preparation method of the metal electrode material of the metal-air battery comprises the following steps:
s11, preparing a magnesium alloy:
after the surfaces of the raw materials are cleaned, mixing Mg metal, Al metal, Zn metal and Mn metal, and carrying out smelting alloying treatment to obtain a magnesium alloy with 96% of Mg, 3% of Al, 0.8% of Zn and 0.2% of Mn;
s12, carrying out casting rolling treatment and rolling treatment on the magnesium alloy:
and carrying out casting rolling treatment on the magnesium alloy by adopting auxiliary heating to 400 ℃, and then continuously carrying out rolling treatment for multiple times, so that the magnesium alloy meets the relevant performance requirements of preparing metal electrodes of metal-air batteries, such as thickness, strength and the like.
Example 2
The embodiment provides a metal-air battery metal electrode material and a preparation method thereof. The metal air battery metal electrode material is a magnesium alloy with a porous loose structure, and the magnesium alloy contains 93% of Mg, 4% of aluminum, 1% of gallium, 1.5% of indium and 0.5% of manganese.
The preparation method of the metal electrode material of the metal-air battery comprises the following steps:
s11, preparing a magnesium alloy:
after the surfaces of the raw materials are cleaned, magnesium metal, aluminum metal, gallium metal, indium metal and manganese metal are mixed and subjected to smelting alloying treatment to obtain a magnesium alloy with 93% of magnesium, 4% of aluminum, 1% of gallium, 1.5% of indium and 0.5% of manganese;
s12, carrying out casting rolling treatment and rolling treatment on the magnesium alloy:
and carrying out casting rolling treatment on the magnesium alloy by adopting auxiliary heating to 300 ℃, and then continuously carrying out rolling treatment for multiple times, so that the magnesium alloy meets the relevant performance requirements of preparing metal electrodes of metal-air batteries, such as thickness, strength and the like.
Example 3
The embodiment provides a metal-air battery metal electrode material and a preparation method thereof. The metal air battery metal electrode material is a magnesium alloy with a porous loose structure, and the magnesium alloy contains 99% of Mg and 1% of indium.
The preparation method of the metal electrode material of the metal-air battery comprises the following steps:
s11, preparing a magnesium alloy:
after the surfaces of the raw materials are cleaned, mixing magnesium metal and indium metal and carrying out smelting alloying treatment to obtain magnesium alloy with 99% of magnesium and 1% of indium;
s12, carrying out casting rolling treatment and rolling treatment on the magnesium alloy:
and carrying out casting rolling treatment on the magnesium alloy by adopting auxiliary heating to 500 ℃, and then continuously carrying out rolling treatment for multiple times, so that the magnesium alloy meets the relevant performance requirements of preparing metal electrodes of metal-air batteries, such as thickness, strength and the like.
Metal air cell embodiments
The metal-air battery metal electrode materials provided in the above embodiments 1 to 3 are cut according to the requirements of the metal-air battery metal electrode, so as to obtain the metal-air battery metal electrode.
And assembling the metal electrode of each metal-air battery, the air electrode and the electrolyte into the metal-air battery. Wherein, the electrolyte is neutral sodium chloride solution, and the air electrode is a novel carbon-based three-phase diffusion oxygen electrode.
Correlation characteristic test
The metal-air battery metal electrode materials provided in the above examples 1 to 3 were subjected to X-ray diffraction (XRD), Scanning Electron Microscope (SEM) analysis and energy spectrum analysis (EDS), respectively, wherein the X-ray diffraction analysis result of the metal-air battery metal electrode material provided in example 1 is shown in fig. 2, the scanning electron microscope is shown in fig. 3, and the energy spectrum analysis result is shown in fig. 4. As is apparent from fig. 2, the magnesium alloy anode material prepared in this example 1 is mainly composed of characteristic peaks of α -Mg. As can be seen from fig. 3, the magnesium anode material prepared in example 1 has a uniform porous loose structure, and the pore size is mostly distributed around 100-200 nm. Fig. 4 elemental analysis shows that the elements of the alloy are mainly composed of magnesium, aluminum, zinc, manganese and the like. In addition, it is known from X-ray diffraction (XRD), Scanning Electron Microscope (SEM) analysis and energy spectrum analysis (EDS) performed on the metal-air battery metal electrode materials provided in other examples that all the metal-air battery metal electrode materials provided in the examples have porous and loose structures and uniform distribution of the pores, and the X-ray diffraction patterns and the energy spectrum analysis patterns of the metal-air battery metal electrode materials provided in the respective examples respectively show respective alloy characteristics.
Meanwhile, the metal-air batteries containing the metal electrode materials of the metal-air batteries of the embodiments are respectively subjected to relevant electrochemical performance experiments, and the final experiment results show that the metal-air batteries containing the metal electrode materials of the metal-air batteries of the embodiments 1 to 3 have high energy density and high capacity, and the stability of the electrochemical performance and the service life are obviously improved.
The overpotential of the hydrogen evolution reaction can be increased to reduce the self-corrosion speed, and the structure of the passivation film can be damaged, so that the problem of magnesium alloy passivation is reduced, the active dissolution of the electrode is promoted, the electrochemical performance of the magnesium alloy is improved, the corresponding metal-air battery is endowed with excellent electrochemical performance, and the service life is prolonged.
The above description is only for the purpose of illustrating the preferred embodiments of the present invention and is not to be construed as limiting the invention, and any modifications, equivalents and improvements made within the spirit and principle of the present invention are intended to be included within the scope of the present invention.
Claims (7)
1. The metal air battery metal electrode material is a magnesium alloy with a loose structure, wherein alloy elements in the magnesium alloy comprise at least one of aluminum, lithium, zinc, indium, gallium and manganese, magnesium particles in the alloy have a particle size of 500nm-200 mu m, and the metal air battery metal electrode material is prepared by the following method:
carrying out smelting alloying treatment on magnesium metal and alloy metal to form magnesium alloy; the alloy metal further comprises at least one metal of aluminum, zinc, lithium, indium, gallium and manganese;
and (3) carrying out casting and rolling treatment on the magnesium alloy by adopting auxiliary heating to the temperature of 300-500 ℃, and then continuously carrying out rolling and rolling treatment for a plurality of times.
2. The metal-air battery metal electrode material as claimed in claim 1, wherein the magnesium alloy contains 90-100% by mass of magnesium, and the balance is the alloy element.
3. The metal-air battery metal electrode material of any one of claims 1-2, wherein the pore size of the loose structure is in the nanometer and/or micrometer scale.
4. The metal-air battery metal electrode material as claimed in claim 3, wherein the pore diameter of the porous structure is 100-200 nm.
5. The metal-air battery metal electrode material of claim 1, characterized in that: in the step of the smelting alloying treatment, the magnesium metal is mixed with the alloy metal according to the proportion that the magnesium metal accounts for 90% -100% of the total amount of the magnesium metal and the alloy metal, and the smelting alloying treatment is carried out.
6. A metal-air battery metal electrode, characterized in that: the metal-air battery metal electrode is prepared from the metal-air battery metal electrode material of any one of claims 1-5.
7. The utility model provides a metal-air battery, includes air electrode, metal electrode and electrolyte, its characterized in that: the metal electrode is the metal-air battery metal electrode of claim 6.
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| JPH07147167A (en) * | 1993-11-24 | 1995-06-06 | Aisin Seiki Co Ltd | Aluminium electrode for aluminum-air battery |
| JP2015063742A (en) * | 2013-09-25 | 2015-04-09 | 国立大学法人東北大学 | Porous metal, method for producing the same, and lithium air battery |
| KR20160128039A (en) * | 2015-04-28 | 2016-11-07 | 삼성전자주식회사 | Metal-air battery and Metal-air battery module |
| CN105826544B (en) * | 2016-05-30 | 2018-06-19 | 中南大学 | A kind of high current efficiency magnesium-rare earth anode material and its preparation method and application |
| CN105925862B (en) * | 2016-06-22 | 2018-09-28 | 中南大学 | A kind of magnesium-alloy anode material and preparation method thereof |
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| CN107868921A (en) * | 2017-09-30 | 2018-04-03 | 广东工业大学 | A kind of magnesium alloy anode rolled plate and its preparation method and application |
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| CN109930042A (en) * | 2019-04-14 | 2019-06-25 | 太原理工大学 | A kind of magnesium-alloy anode material and the preparation method and application thereof |
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