CN110729470A - Positive electrode material of liquid or semi-liquid metal battery, preparation method and application - Google Patents
Positive electrode material of liquid or semi-liquid metal battery, preparation method and application Download PDFInfo
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- CN110729470A CN110729470A CN201911005166.1A CN201911005166A CN110729470A CN 110729470 A CN110729470 A CN 110729470A CN 201911005166 A CN201911005166 A CN 201911005166A CN 110729470 A CN110729470 A CN 110729470A
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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
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- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C1/00—Making non-ferrous alloys
- C22C1/08—Alloys with open or closed pores
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- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C11/00—Alloys based on lead
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- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C12/00—Alloys based on antimony or bismuth
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- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C13/00—Alloys based on tin
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- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C28/00—Alloys based on a metal not provided for in groups C22C5/00 - C22C27/00
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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
- H01M10/39—Accumulators not provided for in groups H01M10/05-H01M10/34 working at high temperature
- H01M10/399—Cells with molten salts
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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 positive electrode material of a liquid or semi-liquid metal battery, a preparation method and application thereof, and belongs to the field of electrode materials of energy storage batteries. The invention adopts Ga alloy formed by metal Ga or Ga and one or more than one simple substance in Sb, Bi, Sn and Pb as the anode material, can be alloyed with the existing cathode material (Li, Na, K, Ca and Mg), and has good electrochemical performance. The metal Ga has extremely low melting point (29.8 ℃), the Ga alloy preparation process is simple, and Ga or Ga alloy is used for a liquid or semi-liquid metal battery, so that the working temperature of the battery can be reduced, the polarization of the battery can be reduced, the discharge voltage of the battery can be improved or stabilized, and the charge and discharge performance of the battery under high current density can be improved on the basis of keeping the advantages of high capacity, long service life and the like of the liquid or semi-liquid metal battery.
Description
Technical Field
The invention belongs to an electrode material of an energy storage battery, and particularly relates to a positive electrode material for a liquid or semi-liquid metal battery and a preparation method thereof, which can be used for solving the problems of low working voltage and low energy efficiency of the liquid or semi-liquid metal battery under high current density.
Background
The rapid development and utilization of renewable energy technologies such as wind energy and solar energy effectively relieve the problems of environmental deterioration caused by fossil fuel combustion, but the renewable energy still has the problems of intermittency in time and space, low efficiency of integration into a power grid and the like. The large-scale efficient energy storage technology can obviously improve the grid-connected efficiency and reliability of the intermittent renewable energy sources and ensure the stability, reliability and safety of a power grid. Among various energy storage technologies, liquid metal batteries have become one of the most promising technologies in large-scale energy storage technologies due to their low cost and long cycle life.
The liquid metal battery is a high-temperature molten salt battery, the working temperature is 300-700 ℃, and the liquid metal battery has the potential of solving the problems of renewable energy source intermittency, low grid connection efficiency and the like. The liquid metal battery consists of a molten metal anode, a molten metal cathode and a molten salt electrolyte, and the molten metal anode, the molten metal cathode and the molten salt electrolyte are automatically layered due to density difference and mutual immiscibility. The unique design of the full liquid state can not only avoid the degradation of the internal microstructure of the electrode in the charging and discharging process, but also enable the liquid metal battery to work under higher current density, thereby realizing the ultra-long cycle life and excellent rate capability. In addition, the liquid metal battery also has the advantages of easy amplification and the like, so that the liquid metal battery becomes a large-scale energy storage technology with great potential.
Since 2012, the professor of the national institute of technology and technology, d.r.sadoway, usa proposed "all-Liquid Metal batteries", many research efforts on Liquid Metal batteries were undertakenThe reports include Li | | Sb-Sn, Li | | | Sb-Pb, etc. The systems have the advantages of low cost, high coulombic efficiency, long cycle life and the like, but the charge-discharge polarization is large under the condition of large current density, the discharge voltage is low, and the energy efficiency and the energy density of the systems under the condition of large current density are influenced. In the above report, the Li | | | Sb-Sn system is at 1000mAcm-2The discharge voltage under the current density is only 0.3V, and the Li I Sb-Pb system is 1000mAcm-2The discharge voltage at current density is also only 0.4V. The lower discharge voltage at high current densities can severely impact the energy efficiency of the energy storage system. (Li H, Wang K, Cheng S, et al. high Performance Liquid Metal batteries with environmental Friendly friend inorganic-Tin Positive Materials&Interfaces,2016,8(20):12830-12835.Wang K, Jiang K, Chung B, et al, lithium-atom-lead metal base for grid-level energy storage Nature,2014,514(7522):348-3Sb has high melting point (1150 deg.C), is solid in the working temperature range of liquid metal battery, and in the discharge process, the discharge product Li3The Sb is low in density and is positioned at the interface between the electrolyte and the positive electrode, and the Sn or Pb of the other metal phase is high in density and is positioned at the bottom of the positive electrode material. Solid phase Li at the electrolyte/cathode interface due to the low transport velocity of ions in the solid phase3Sb, limits the kinetics of the electrode reaction. Therefore, how to solve the problems of slow electrode reaction kinetics and large electrode polarization at the positive electrode interface is a technical key for realizing large-current charge and discharge of the liquid metal battery and improving the charge and discharge energy efficiency of the liquid metal battery.
Disclosure of Invention
The invention provides a positive electrode material of a liquid or semi-liquid metal battery and a preparation method thereof, which are applied to an energy storage battery and solve the problems of low working voltage, low energy efficiency and the like caused by large polarization of the existing liquid or semi-liquid metal battery under high current density.
The invention provides a positive electrode material of a liquid or semi-liquid metal battery, which is characterized in that:
the anode material is metal Ga or Ga alloy formed by metal Ga and one or more than one simple substance of metal Sb, Bi, Sn and Pb.
The mole percentage of the anode material is as follows: ga5-50Sb95-50、Ga5-50Bi95-50、Ga5-50Pb95-50、Ga5- 50Sn95-50、Ga5-50Sn95-50Pb0-45、Ga5-50Sn95-50Sb0-45、Ga5-50Pb95-50Sb0-45、Ga5-50Bi95-50Sb0-45、Ga5- 50Bi95-50Sn0-45、Ga5-50Bi95-50Pb0-45Wherein the lower right hand corner of the formula indicates the mole percent of each component and the mole percent of each component in each alloy add up to 100%.
The invention also provides a preparation method of the cathode material, metal Ga and other required metal raw materials are weighed according to the molar ratio, the mixture is heated to 50-100 ℃ above the melting point of the alloy in the proportion under the protection of inert atmosphere or vacuum condition, and the temperature is kept for 5-24h, so that the mixed metal raw materials are fully alloyed, and the cathode alloy material can be obtained.
The invention provides an energy storage battery applying a liquid or semi-liquid metal battery anode material, which comprises a shell, an anode, a cathode, an electrolyte, a cathode lead and a ceramic seal, wherein the cathode is formed by a current collector adsorbing a cathode liquid metal material, and the anode is made of the anode material.
The current collector in the energy storage battery is made of porous foam metal material.
The anode material and the cathode material of the energy storage battery are both in a liquid state at the working temperature, and the electrolyte material may be in a liquid state or a semi-liquid state due to different types of the electrolyte material.
The battery test result prepared according to the invention shows that compared with the existing anode material, the invention has the following specific advantages and beneficial effects:
firstly, the melting point of metal Ga is extremely low (29.8 ℃), the melting point of the obtained alloy can be reduced when the metal Ga is alloyed with one or more simple substances of metals Sb, Bi, Sn and Pb, and if Ga is alloyed with Sn, the melting point of an alloy phase in the composition range can be below 200 ℃, so that a liquid or semi-liquid metal battery is more stable in the operation process and has longer cycle life. And secondly, when Ga is alloyed with metals Sb, Bi, Sn and Pb and then is used as a positive electrode material of a liquid or semi-liquid metal battery, the polarization of the battery under high current density can be reduced, and the working voltage and the energy efficiency of the battery are improved. Thirdly, when Ga is alloyed with Sb, Bi, Sn and Pb and then used as the anode material of the liquid or semi-liquid metal battery, the utilization rate of the anode material can be improved, and the battery cost is reduced. Fourthly, the preparation method of the cathode material provided by the invention is very simple, does not need special equipment, has high yield and is very suitable for assembling large-scale liquid or semi-liquid metal batteries.
In summary, the metal Ga or the Ga alloy formed by the metal Ga and one or more of the metals Sb, Bi, Sn, and Pb as the positive electrode material has good electrochemical performance when assembled with the existing negative electrode material into a liquid or semi-liquid metal battery for testing. The metal Ga has extremely low melting point (29.8 ℃), the Ga alloy preparation process is simple, the metal Ga and the Ga alloy are used in a liquid or semi-liquid metal battery, the working temperature of the battery can be reduced, the polarization of the battery is reduced, the voltage of the battery is improved or stabilized, the charge and discharge performance of the battery under high current density is improved, the battery has higher energy efficiency under high current density, and the competitiveness of the liquid and semi-liquid metal batteries in the energy storage field is improved on the basis of keeping the advantages of high capacity, long service life and the like of the liquid or semi-liquid metal battery.
Drawings
FIG. 1 is a schematic cross-sectional view of a liquid metal battery using the present invention as the positive electrode material, in which 1-case, 2-positive electrode, 3-electrolyte, 4-negative electrode, 5-negative electrode lead, 6-ceramic seal;
fig. 2 is a charge-discharge performance curve of a liquid metal energy storage battery using example 2 of the present invention;
fig. 3 is a charge-discharge performance curve of a liquid metal energy storage battery using example 3 of the present invention;
fig. 4 is a cycle performance curve for a liquid metal energy storage cell employing example 3 of the present invention;
fig. 5 is a charge-discharge performance curve for different current densities for a liquid metal energy storage battery according to example 3 of the present invention.
Detailed Description
In order to make the technical problems, technical solutions and advantages of the present invention more apparent, the present invention will be further described with reference to the accompanying drawings and examples. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not limiting of 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.
The invention provides a positive electrode material for a liquid or semi-liquid metal battery, aiming at the problems of large polarization, low discharge voltage, low energy efficiency and the like of the existing liquid or semi-liquid metal battery under high current density, wherein the positive electrode material is Ga alloy formed by metal Ga or metal Ga and one or more than one elementary substances of Sb, Bi, Sn and Pb, and the chemical formula of the Ga alloy is as follows:
Ga5-50Sb95-50、Ga5-50Bi95-50、Ga5-50Pb95-50、Ga5-50Sn95-50、Ga5-50Sn95-50Pb0-45、Ga5- 50Sn95-50Sb0-45、Ga5-50Pb95-50Sb0-45、Ga5-50Bi95-50Sb0-45、Ga5-50Bi95-50Sn0-45、Ga5-50Bi95-50Pb0-45wherein the lower right hand corner of the formula indicates the mole percent of each component and the mole percent of each component in each alloy add up to 100%.
When the Ga alloy is prepared, metal Ga and other required metal raw materials are weighed according to the molar ratio and are placed into a graphite crucible, a ceramic crucible or a metal crucible to be uniformly mixed, then the crucible containing the mixed metal raw materials is placed into a tubular furnace or other heating furnaces or is directly placed into a metal shell, then the metal shell containing the mixed metal raw materials is placed into the tubular furnace or other heating furnaces, the mixture is heated to 50-100 ℃ above the melting point of the alloy in the ratio under the protection of inert atmosphere or vacuum condition, and the temperature is kept for 5-24 hours, so that the mixed metal raw materials are fully alloyed, and the anode alloy material can be obtained.
The liquid or semi-liquid metal energy storage battery using the invention as the anode material comprises a shell, an anode, a cathode, an electrolyte, a cathode lead and a ceramic seal, wherein the shell is made of a metal material, the anode, the electrolyte and the cathode are sequentially placed in the shell from bottom to top at a working temperature, the cathode is formed by a current collector adsorbing the cathode liquid metal material, the cathode lead connected with the current collector penetrates through a center hole at the top end of the shell and is insulated from the shell through the insulating ceramic seal, and the battery assembly is completed. The current collector is made of porous foam metal material. A schematic cross-sectional structure of a liquid metal battery is shown in fig. 1.
Table 1 lists 10 embodiments of the present invention, and a schematic structural diagram of a liquid or semi-liquid metal energy storage battery adopting each embodiment is shown in fig. 1, and includes a case 1, a positive electrode 2, an electrolyte 3, a negative electrode 4, a negative electrode lead 5 and a ceramic seal 6, where the case 1 is made of a metal material, the positive electrode 2, the electrolyte 3 and the negative electrode 4 are sequentially placed inside the case from bottom to top, the negative electrode 4 is formed by a current collector adsorbing a negative electrode liquid metal material, and the negative electrode lead 5 connected to the current collector passes through a central hole at the top end of the case and is insulated from the case 1 by the insulating ceramic seal 6.
TABLE 1
The assembly process of the energy storage battery of each embodiment described in table 1 is as follows: and placing the current collector in the molten negative electrode material, and preserving heat for a certain time to enable the negative electrode metal in the proportion to be adsorbed in the current collector, thereby completing the preparation of the negative electrode. And then, heating the battery shell to the working temperature, sequentially adding the positive electrode and the electrolyte into the shell, putting the current collector adsorbing the negative metal on the upper part of the electrolyte after the electrolyte is completely melted, cooling to the room temperature, and finishing the sealing of the battery, thus finishing the assembly of the battery. The test results are shown in Table 1.
Fig. 2 is a charge-discharge performance curve of the liquid metal energy storage battery in example 2 of the present invention, wherein the operating temperature is 500 ℃, the discharge voltage is 0.6V, the coulombic efficiency is 91.5%, and the energy efficiency is 65%.
Fig. 3 is a charge-discharge performance curve of the liquid metal energy storage battery of example 3 using the present invention, with an operating temperature of 500 ℃, a discharge voltage of 0.65V, a coulombic efficiency of 95%, and an energy efficiency of 73%.
FIG. 4 is a graph of the cycling performance of a liquid metal energy storage cell using example 3 of the present invention, operating at 500 ℃ at 600mAcm-2The coulombic efficiency is always kept above 98% after 53 cycles of charge and discharge under the current density, and the capacity attenuation rate is only 0.15% per cycle.
FIG. 5 is a graph showing the charging and discharging performance of the liquid metal energy storage battery of example 3 of the present invention at different current densities, wherein the operating temperature is 500 ℃, and the polarization of the battery increases very little at 1200mAcm with the increase of the current density-2The discharge voltage under the current density is about 0.5V, and the energy efficiency is as high as 45%.
The test results show that: the electrode material disclosed by the invention is used for a liquid or semi-liquid metal battery, so that the melting point of the anode material is reduced, the polarization of the battery is reduced, better voltage performance and higher energy efficiency are obtained, and the long cycle performance of the battery is good.
The above description is of the preferred embodiment of the invention and is not intended to limit the invention. It should be noted that the present invention is well understood by those skilled in the art, and therefore, many alternatives, modifications, and improvements based on the principles of the present invention are also considered to be within the scope of the present invention.
Claims (6)
1. A positive electrode material for a liquid or semi-liquid metal battery, characterized by: the anode material is Ga alloy formed by metal Ga or metal Ga and one or more than one simple substance of Sb, Bi, Sn and Pb.
2. The positive electrode material according to claim 1, wherein: the chemical formula of the Ga alloy is as follows: ga5-50Sb95-50、Ga5-50Bi95-50、Ga5-50Pb95-50、Ga5-50Sn95-50、Ga5-50Sn95-50Pb0-45、Ga5-50Sn95-50Sb0-45、Ga5-50Pb95- 50Sb0-45、Ga5-50Bi95-50Sb0-45、Ga5-50Bi95-50Sn0-45、Ga5-50Bi95-50Pb0-45Wherein the lower right hand corner of the formula indicates the mole percent of each component and the mole percent of each component in each alloy add up to 100%.
3. A preparation method of a positive electrode material of a liquid or semi-liquid metal battery is characterized by comprising the following steps: weighing metal Ga and other required metal raw materials according to the molar ratio of the metal Ga and the other required metal raw materials in the claims 1-2, heating to 50-100 ℃ above the melting point of the alloy in the ratio under the protection of inert atmosphere or vacuum, and preserving heat for 5-24 hours to fully alloy the mixed metal raw materials to obtain the cathode alloy material.
4. The utility model provides an use energy storage battery of liquid or semi-liquid metal battery cathode material, its constitution includes casing, positive pole, negative pole, electrolyte, negative pole lead wire and ceramic seal, and the negative pole comprises the mass flow body that adsorbs negative pole liquid metal material, its characterized in that: the positive electrode is made of the positive electrode material of claims 1-2.
5. An energy storage battery using a liquid or semi-liquid metal battery positive electrode material as claimed in claim 4, wherein: the current collector is made of porous foam metal material.
6. An energy storage battery using a liquid or semi-liquid metal battery positive electrode material as claimed in claim 4, wherein: the anode material and the cathode material are both in a liquid state at the working temperature, and the electrolyte material is in a liquid state or a semi-liquid state.
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| CN111705337A (en) * | 2020-06-23 | 2020-09-25 | 超威电源集团有限公司 | Method for preparing lead-calcium master alloy by molten salt galvanic cell method |
| CN113193179A (en) * | 2021-03-29 | 2021-07-30 | 西安交通大学 | Liquid metal battery and preparation method thereof |
| CN113745492A (en) * | 2021-08-26 | 2021-12-03 | 西安交通大学 | Liquid metal battery with prefabricated multi-pore structure positive electrode and preparation method thereof |
| CN113809409A (en) * | 2021-08-16 | 2021-12-17 | 北京科技大学 | Low-melting-point molten salt electrolyte of liquid or semi-liquid metal battery, preparation and application |
| CN113809317A (en) * | 2021-08-16 | 2021-12-17 | 北京科技大学 | Positive electrode material of liquid or semi-liquid metal battery and application |
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