CN115133109B - Water system copper ion battery - Google Patents
Water system copper ion battery Download PDFInfo
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- CN115133109B CN115133109B CN202210689373.9A CN202210689373A CN115133109B CN 115133109 B CN115133109 B CN 115133109B CN 202210689373 A CN202210689373 A CN 202210689373A CN 115133109 B CN115133109 B CN 115133109B
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- tellurium
- ion battery
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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
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/054—Accumulators with insertion or intercalation of metals other than lithium, e.g. with magnesium or aluminium
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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 belongs to the field of water-based batteries, and particularly relates to a water-based copper ion battery. Wherein, the simple substance tellurium composite electrode is taken as an anode, the aqueous solution of copper ion salt is taken as electrolyte, and the metal copper sheet is taken as a cathode. The tellurium composite anode is prepared by fully mixing simple substance tellurium powder with a conductive agent and a binder and adopting a pressing or coating mode to prepare an electrode slice. The charge and discharge process of the battery involves the oxidation-reduction reaction of the carrier metal copper ions and tellurium, and the transfer number of unit electrons can be up to 4, so the battery has the characteristics of high capacity and high energy. The water system copper ion battery has low cost of raw materials, simple and easy operation of the preparation process, high load per unit area of the electrode and suitability for large-scale production and application.
Description
Technical Field
The invention belongs to the field of water-based batteries, and particularly relates to a water-based copper ion battery.
Background
With the rapid development of technology, the demand of energy in the society is gradually increased, and related energy and chemical fields are rapidly developed. Batteries are receiving increasing attention as a high-efficiency, pollution-free energy storage device, which plays a role in energy regulation and use that is difficult to replace. Among them, electrochemical cells such as lithium ion cells have been developed very rapidly in recent years due to their advantages of high energy and high power. However, with the large-scale application of energy storage devices, the problem of lithium resource shortage is also manifested day by day. In addition, the organic electrolyte used in the current battery also brings about a plurality of safety accidents. Therefore, the current energy storage batteries face significant challenges, and there is a need to find more safe, low cost energy storage batteries.
Compared with the organic electrolyte used in the current lithium ion battery, the safety coefficient of the water-based electrolyte is much higher, and it is easy to understand that the water-based electrolyte is not flammable, so that the risk of combustion and explosion of the battery is greatly reduced. The safety is high, the preparation condition is loose, the cost is low, and the method is always the advantage of the water-based electrolyte.
In order to realize sustainable development of energy, people turn their eyes to water-based metal ion batteries. Particularly aqueous copper ion batteries have recently led to researchersThere is a great deal of attention. The copper resource is abundant, the purification process is simpler, the production cost is low, in addition, the aqueous copper ion battery uses a mild aqueous solution as an electrolyte, and the safety is extremely high. More importantly, copper ions can undergo multiple electron transfer in an electrochemical reaction, and thus can provide higher capacity, than lithium ion batteries with single electron transfer reactions. For example, a sulfur (S) electrode can provide 3044mAhg when storing copper ions -1 Is known (Angew. Chem.2019,131, 12770), while the self-supporting copper sulphide (CuS) electrode also has a specific capacity of 510mAh g -1 Is a specific capacity (ACS Nano 2021,15,5420). However, the sulfur electrode has problems of extremely low conductivity, poor cycle performance and the like, while the self-supporting copper sulfide electrode has problems of low loading amount and low specific area capacity.
Comparative zinc ion cell CN 110034342B, "an aqueous zinc-tellurium secondary cell", tellurium was used as the positive electrode material, wherein the positive electrode involved Te and TeO 2 4 electron transfer between the transitions, only Zn and Zn occur in the zinc cathode 2+ Is a transition of (2). However, in copper ion battery systems, copper will co-act with the positive electrode material during the reaction process, and Cu to Cu will occur 2+ To Cu + Is a characteristic reaction of copper electrodes. This completely different reaction relative to zinc ion batteries gives it the potential to achieve higher capacities. In addition, copper has very high reactivity, reversibility and stability as a negative electrode, is not easy to generate dendrite even under high current density, and is more stable and safer than a zinc negative electrode.
Disclosure of Invention
In order to solve the problems of poor cycle performance and low specific area capacity of the existing water-based copper ion battery, the invention provides a water-based copper ion battery which comprises an anode, a cathode, electrolyte and a diaphragm;
the positive electrode is a tellurium composite electrode;
the electrolyte is copper salt aqueous solution;
the negative electrode is copper foil.
Preferably, the preparation method of the tellurium composite electrode comprises the following steps:
s1: tellurium, a conductive agent and a binder are mixed and then added with a solvent to form slurry;
s2: and coating the slurry on a current collector, and drying to obtain the tellurium composite electrode.
Further, the conductive agent is one or more of acetylene black, ketjen black, active carbon, graphene, carbon nanotubes and carbon fibers.
Further, the binder is polyvinylidene fluoride, polytetrafluoroethylene, hydroxymethyl cellulose or polyvinyl alcohol.
Further, the solvent is water, ethanol or N-methylpyrrolidone.
Further, the mass ratio of tellurium to the conductive agent to the binder is 60-90:5-20:5-20.
Further, the current collector is made of titanium or carbon.
Preferably, the copper salt comprises one or more of copper sulfate, copper chloride, copper acetate and copper nitrate.
Preferably, the concentration of the copper salt in the copper salt aqueous solution is 0.1-2M.
Preferably, the separator is made of glass fiber, cellulose or porous polyolefin.
The invention aims to provide a novel water-based copper ion battery, which takes a simple substance tellurium composite electrode as an anode, takes an aqueous solution of copper ion salt as electrolyte and takes a metal copper sheet as a cathode. The tellurium composite anode is prepared by fully mixing simple substance tellurium powder with a conductive agent and a binder and adopting a pressing or coating mode to prepare an electrode slice. The charge and discharge process of the battery involves the oxidation-reduction reaction of the carrier metal copper ions and tellurium, and the transfer number of unit electrons can be up to 4, so the battery has the characteristics of high capacity and high energy. The water system copper ion battery has low cost of raw materials, simple and easy operation of the preparation process, high load per unit area of the electrode and suitability for large-scale production and application.
The invention relates to a copper ion battery system. Copper has very high reactivity, reversibility and stability as a cathode, and dendrite is not easy to generate even under high current density; the copper cathode and the tellurium anode co-act in the reaction process to generateRaw Cu to Cu 2+ To Cu + Is a characteristic reaction of copper electrodes. This reaction also results in a system of simple substance Te and negative divalent Te 2- But the system can produce a 4 electron transfer reaction.
Compared with the prior art, the technical scheme of the invention has the following advantages:
(1) The invention provides a novel water-based copper ion battery, copper ions are de-intercalated in a tellurium composite electrode and simultaneously undergo oxidation-reduction reaction, the number of unit electron transfer is up to 4, and the whole battery has the characteristics of high capacity and high energy density.
(2) The electrode unit area load in the battery manufactured by the invention is high, the operation is simple, the cost is low, and the battery is suitable for large-scale production and application.
(3) The materials used in the invention are safe and pollution-free, have environmental friendliness and have wide prospects in the energy storage field.
Drawings
FIG. 1 is an electron micrograph of a tellurium composite electrode prepared as in example 1.
Fig. 2 is a charge-discharge curve of the aqueous copper ion battery prepared in example 1.
FIG. 3 is an X-ray diffraction pattern of the tellurium composite electrode prepared as in example 2 before and after discharge.
Fig. 4 is a charge-discharge curve of the aqueous copper ion battery prepared in example 2.
Fig. 5 is a charge-discharge curve of the aqueous copper ion battery prepared in example 3.
Detailed Description
The present invention will be further described with reference to the accompanying drawings and specific examples, which are not intended to be limiting, so that those skilled in the art will better understand the invention and practice it.
Example 1
And weighing simple substance tellurium, activated carbon and polyvinylidene fluoride according to the mass ratio of 70:10:20, fully grinding and uniformly mixing in an agate mortar, and then adding N-methyl pyrrolidone for mixing and stirring to obtain uniformly dispersed slurry. Will beThe slurry is coated on the cleaned titanium foil in a scraping way, the coating amount of the slurry is 3mg per square centimeter based on the total mass of the slurry, and then the tellurium composite electrode is obtained by placing the slurry in a vacuum drying oven and drying the slurry for 2 hours at 60 ℃. Cutting tellurium composite electrode into 1cm area 2 As a positive electrode, polished and washed and 1cm in area 2 The copper foil of (2) is used as a negative electrode, a copper chloride aqueous solution with the concentration of 0.2M is used as an electrolyte, and cellulose is used as a diaphragm to assemble the 2032 button cell. The charge and discharge test results are shown in FIG. 2, at 0.05 and 0.05A g -1 At current density up to 550mAh g -1 Is a specific discharge capacity of (a).
Example 2
And weighing simple substance tellurium, acetylene black and polytetrafluoroethylene according to the mass ratio of 60:25:15, fully grinding and uniformly mixing in an agate mortar, gradually adding water, stirring and rolling to obtain plasticine-like mixed slurry. And rolling the slurry on a clean titanium net, wherein the slurry loading amount is 3mg per square centimeter, and then placing the titanium net in a vacuum drying oven and drying the titanium net at 100 ℃ for 8 hours to obtain the tellurium composite electrode. Cutting tellurium composite electrode into 1cm area 2 As a positive electrode, polished and washed and 1cm in area 2 The copper foil of (2) is used as a negative electrode, a copper sulfate aqueous solution with the concentration of 0.5M is used as electrolyte, and glass fiber is used as a diaphragm to assemble the 2032 button cell. Characterization is carried out on the composite anode before and after discharge, the obtained X-ray diffraction pattern is shown in figure 3, and the main simple substance tellurium before discharge can be seen from the X-ray diffraction pattern, and cuprous telluride is generated after discharge. The charge and discharge test results are shown in FIG. 4, at 0.05 and 0.05A g -1 At the highest current density, 564mAh g -1 Is a specific discharge capacity of (a).
Example 3
And weighing simple substance tellurium, carbon fiber and polyvinyl alcohol according to the mass ratio of 80:10:10, fully grinding and uniformly mixing in an agate mortar, and then adding N-methyl pyrrolidone for mixing and stirring to obtain uniformly dispersed slurry. The slurry is coated on the cleaned carbon cloth, the coating amount of the slurry is 3mg per square centimeter based on the total mass of the slurry, and then the tellurium composite electrode is obtained by placing the slurry in a vacuum drying oven and drying the slurry for 5 hours at 80 ℃. Cutting tellurium composite electrode into 1cm area 2 As a positive electrode, polished and washed and 1cm in area 2 Takes copper foil of 0.2M thick as a negative electrodeThe 2032 button cell was assembled with porous polyolefin as the separator, with a copper acetate aqueous solution of degree as the electrolyte. The charge and discharge test results are shown in FIG. 5, at 0.05 and 0.05A g -1 At the highest current density, 564mAh g -1 Is a specific discharge capacity of (a).
Example 4
And weighing simple substance tellurium, carbon nano tubes and polyvinyl alcohol according to the mass ratio of 75:15:15, fully grinding and uniformly mixing in an agate mortar, and then adding N-methyl pyrrolidone for mixing and stirring to obtain uniformly dispersed slurry. The slurry was coated on a cleaned titanium mesh in an amount of 3mg per square centimeter based on the total mass of the slurry, and then placed in a vacuum oven to be dried at 75 ℃ for 7 hours to obtain a tellurium composite electrode. Cutting tellurium composite electrode into 1cm area 2 As a positive electrode, polished and washed and 1cm in area 2 The copper foil of (2) is used as a negative electrode, a 1.5M concentration copper chloride aqueous solution is used as an electrolyte, and glass fiber is used as a diaphragm to assemble the 2032 button cell.
Example 5
And weighing simple substance tellurium, ketjen black and polyvinylidene fluoride according to a mass ratio of 84:8:8, fully grinding and uniformly mixing in an agate mortar, and then adding N-methyl pyrrolidone for mixing and stirring to obtain uniformly dispersed slurry. The slurry is coated on the cleaned carbon cloth, the coating amount of the slurry is 3mg per square centimeter based on the total mass of the slurry, and then the tellurium composite electrode is obtained by placing the slurry in a vacuum drying oven and drying the slurry for 4 hours at 82 ℃. Cutting tellurium composite electrode into 1cm area 2 As a positive electrode, polished and washed and 1cm in area 2 The copper foil of (2) is used as a negative electrode, a copper acetate aqueous solution with the concentration of 0.5M is used as an electrolyte, and cellulose is used as a diaphragm to assemble the 2032 button cell.
Example 6
And weighing simple substance tellurium, acetylene black and polyvinyl alcohol according to the mass ratio of 74:13:13, fully grinding and uniformly mixing in an agate mortar, and then adding N-methyl pyrrolidone for mixing and stirring to obtain uniformly dispersed slurry. The slurry is coated on the cleaned carbon cloth, the coating amount of the slurry is 3mg per square centimeter based on the total mass of the slurry, and then the tellurium composite electrode is obtained by placing the slurry in a vacuum drying oven and drying the slurry for 3 hours at 77 ℃. Cutting tellurium composite electrode into 1cm area 2 As a positive electrode, polished and washed and 1cm in area 2 The copper foil of (2) is used as a negative electrode, a copper acetate aqueous solution with the concentration of 0.4M is used as an electrolyte, and porous polyolefin is used as a diaphragm to assemble the 2032 button cell.
Example 7
And weighing simple substance tellurium, active carbon and polytetrafluoroethylene according to the mass ratio of 64:18:18, fully grinding and uniformly mixing in an agate mortar, gradually adding water, stirring and rolling to obtain plasticine-like mixed slurry. And rolling the slurry on a clean titanium net, wherein the slurry loading amount is 3mg per square centimeter, and then placing the titanium net in a vacuum drying oven and drying the titanium net at 110 ℃ for 6 hours to obtain the tellurium composite electrode. Cutting tellurium composite electrode into 1cm area 2 As a positive electrode, polished and washed and 1cm in area 2 The copper foil of (2) is used as a negative electrode, a copper acetate aqueous solution with the concentration of 0.4M is used as an electrolyte, and cellulose is used as a diaphragm to assemble the 2032 button cell.
Example 8
And weighing simple substance tellurium, acetylene black and polyvinyl alcohol according to the mass ratio of 66:14:20, fully grinding and uniformly mixing in an agate mortar, and then adding N-methyl pyrrolidone for mixing and stirring to obtain uniformly dispersed slurry. The slurry is coated on the cleaned carbon cloth, the coating amount of the slurry is 3mg per square centimeter based on the total mass of the slurry, and then the tellurium composite electrode is obtained by placing the slurry in a vacuum drying oven and drying the slurry for 7 hours at 78 ℃. Cutting tellurium composite electrode into 1cm area 2 As a positive electrode, polished and washed and 1cm in area 2 The copper foil of (2) is used as a negative electrode, a 1.7M concentration copper sulfate aqueous solution is used as an electrolyte, and glass fiber is used as a diaphragm to assemble the 2032 button cell.
Example 9
And weighing simple substance tellurium, activated carbon and polyvinylidene fluoride according to a mass ratio of 89:5:6, fully grinding and uniformly mixing in an agate mortar, and then adding N-methyl pyrrolidone for mixing and stirring to obtain uniformly dispersed slurry. The slurry is coated on the cleaned carbon cloth, the coating amount of the slurry is 3mg per square centimeter based on the total mass of the slurry, and then the tellurium composite electrode is obtained by placing the slurry in a vacuum drying oven and drying the slurry for 7 hours at 79 ℃. Cutting tellurium composite electrode into 1cm area 2 As a positive electrode, polished and washed and 1cm in area 2 Copper of (2)The foil is used as a negative electrode, a copper nitrate aqueous solution with the concentration of 0.2M is used as an electrolyte, and porous polyolefin is used as a diaphragm to assemble 2032 button cell.
Example 10
And weighing simple substance tellurium, active carbon and polyvinyl alcohol according to a mass ratio of 72:10:18, fully grinding and uniformly mixing in an agate mortar, and then adding N-methyl pyrrolidone for mixing and stirring to obtain uniformly dispersed slurry. The slurry is coated on the cleaned carbon cloth, the coating amount of the slurry is 3mg per square centimeter based on the total mass of the slurry, and then the tellurium composite electrode is obtained by placing the slurry in a vacuum drying oven and drying the slurry for 8 hours at 76 ℃. Cutting tellurium composite electrode into 1cm area 2 As a positive electrode, polished and washed and 1cm in area 2 The copper foil of (2) is used as a negative electrode, a copper acetate aqueous solution with the concentration of 0.5M is used as an electrolyte, and glass fiber is used as a diaphragm to assemble the 2032 button cell.
It is apparent that the above examples are given by way of illustration only and are not limiting of the embodiments. Other variations and modifications of the present invention will be apparent to those of ordinary skill in the art in light of the foregoing description. It is not necessary here nor is it exhaustive of all embodiments. And obvious variations or modifications thereof are contemplated as falling within the scope of the present invention.
Claims (10)
1. A water-based copper ion battery is characterized by comprising a positive electrode, a negative electrode, electrolyte and a diaphragm;
the positive electrode is a tellurium composite electrode, and tellurium is simple substance tellurium;
the electrolyte is copper salt aqueous solution;
the negative electrode is copper foil.
2. The aqueous copper ion battery of claim 1, wherein the method for preparing the tellurium composite electrode comprises the steps of:
s1: tellurium, a conductive agent and a binder are mixed and then added with a solvent to form slurry;
s2: and coating the slurry on a current collector, and drying to obtain the tellurium composite electrode.
3. The aqueous copper ion battery of claim 2 wherein the conductive agent is one or more of acetylene black, ketjen black, activated carbon, graphene, carbon nanotubes, and carbon fibers.
4. The aqueous copper ion battery of claim 2 wherein the binder is polyvinylidene fluoride, polytetrafluoroethylene, hydroxymethyl cellulose or polyvinyl alcohol.
5. The aqueous copper ion battery of claim 2 wherein the solvent is water, ethanol or N-methylpyrrolidone.
6. The aqueous copper ion battery according to claim 2, wherein the mass ratio of tellurium, the conductive agent and the binder is 60-90:5-20:5-20.
7. The aqueous copper ion battery of claim 2 wherein the current collector is titanium or carbon.
8. The aqueous copper ion battery of claim 1 wherein the copper salt comprises one or more of copper sulfate, copper chloride, copper acetate, and copper nitrate.
9. The aqueous copper ion battery of claim 1 wherein the concentration of copper salt in the aqueous copper salt solution is from 0.1M to 2M.
10. The aqueous copper ion battery according to claim 1, wherein the separator is made of glass fiber, cellulose or porous polyolefin.
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| CN115133109B true CN115133109B (en) | 2023-05-12 |
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| WO2021228001A1 (en) * | 2020-05-11 | 2021-11-18 | 湖南大学 | Four-electron conversion reaction-based aqueous zinc-iodine battery and electrolyte thereof |
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2022
- 2022-06-17 CN CN202210689373.9A patent/CN115133109B/en active Active
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