CN112151805A - Negative electrode current collector and aqueous battery - Google Patents
Negative electrode current collector and aqueous battery Download PDFInfo
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- CN112151805A CN112151805A CN202010920027.8A CN202010920027A CN112151805A CN 112151805 A CN112151805 A CN 112151805A CN 202010920027 A CN202010920027 A CN 202010920027A CN 112151805 A CN112151805 A CN 112151805A
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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
- H01M4/64—Carriers or collectors
- H01M4/66—Selection of materials
- H01M4/665—Composites
- H01M4/667—Composites in the form of layers, e.g. coatings
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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
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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
- H01M4/64—Carriers or collectors
- H01M4/66—Selection of materials
- H01M4/661—Metal or alloys, e.g. alloy coatings
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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
- H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
- H01M2004/027—Negative electrodes
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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 negative electrode current collector and an aqueous battery. Wherein the negative electrode current collector includes: the metal plating layer is formed on at least part of the surface of the substrate, and the metal plating layer is formed by high hydrogen evolution potential metal. The surface of the negative current collector is provided with a coating formed by high hydrogen evolution potential metal, so that the problems of negative dendrite, hydrogen evolution, corrosion and the like can be effectively inhibited, the service life of the battery is prolonged, and the performance of the battery is improved.
Description
Technical Field
The present invention relates to the field of aqueous batteries, and more particularly, to a negative electrode current collector and an aqueous battery using the same.
Background
The water system battery has the advantages of high energy density, high power density, efficient and safe discharge process, non-toxic and cheap battery materials, simple preparation process and the like, and has good application value and development prospect in the fields of large-scale energy storage and the like.
In the existing water-based battery, a negative current collector mostly uses pure metal materials and alloy materials, such as stainless steel materials, nickel-based materials, titanium-based materials, copper-based materials, graphite materials and the like; the negative electrode adopts the materials as a current collector, so that the problems of dendrite, hydrogen evolution, corrosion, passivation and the like of the zinc negative electrode cannot be solved, and the cycle life of the battery is influenced. Even if a brass mesh is used as the negative electrode current collector, the above problems cannot be effectively solved. As can be seen, the conventional water-based battery has yet to be improved.
Disclosure of Invention
The present invention is directed to solving, at least to some extent, one of the technical problems in the related art. To this end, an object of the present invention is to propose a negative electrode current collector and an aqueous battery using the same. The surface of the negative current collector is provided with a coating formed by high hydrogen evolution potential metal, so that the problems of negative dendrite, hydrogen evolution, corrosion and the like can be effectively inhibited, the service life of the battery is prolonged, and the performance of the battery is improved.
In one aspect of the present invention, a negative electrode current collector is provided. According to an embodiment of the present invention, the negative electrode current collector includes: a substrate; a metal plating layer formed on at least a part of the surface of the base, the metal plating layer being formed of a high hydrogen evolution potential metal.
According to the negative current collector disclosed by the embodiment of the invention, the high hydrogen evolution potential metal coating on the surface of the negative current collector can increase the hydrogen evolution difficulty of the negative electrode, and the hydrogen evolution side reaction of the battery is effectively avoided. Meanwhile, the interface regulation is carried out by utilizing the metal coating, so that the uniform nucleation of zinc ions in the electrolyte during deposition can be promoted, the tip effect caused by uneven deposition is reduced, and the growth of zinc dendrite is effectively inhibited. On the other hand, the metal coating can be used as a transition layer between the negative active material and the current collector matrix, and plays a role in buffering and protecting the current collector matrix when the negative active material is dissolved. Under the condition that the battery is placed for a long time, the current collector matrix is separated from the electrolyte by the metal coating, and the current collector matrix can be effectively protected from being corroded. Therefore, the surface of the negative current collector is provided with the plating layer formed by the high hydrogen evolution potential metal, so that the problems of negative dendrite, hydrogen evolution, corrosion and the like can be effectively inhibited, the service life of the battery is prolonged, and the performance of the battery is improved.
In addition, the negative electrode current collector according to the above embodiment of the present invention may further have the following additional technical features:
in some embodiments of the invention, the substrate is a copper mesh.
In some embodiments of the invention, the substrate is a diagonal-drawn brass mesh.
In some embodiments of the invention, the high hydrogen evolution potential metal is selected from at least one of Zn, Sn, Pb, In, Bi.
In some embodiments of the present invention, the thickness of the metal coating is 0.1 to 500 μm.
In some embodiments of the present invention, the thickness of the metal coating is 0.1 to 3 μm.
In another aspect of the present invention, an aqueous battery is provided. According to an embodiment of the present invention, the water-based battery includes: a positive electrode, a negative electrode, and an aqueous electrolyte solution; wherein, the positive electrode comprises a positive electrode active material and a positive electrode current collector, and the negative electrode comprises a negative electrode active material and the negative electrode current collector of the embodiment. Therefore, the water-based battery can effectively overcome the problems of dendrite, hydrogen evolution, corrosion and the like of the negative electrode, and can obtain longer service life and higher electrochemical performance.
In addition, the water-based battery according to the above embodiment of the invention may further have the following additional technical features:
in some embodiments of the invention, the negative active material is zinc powder.
In some embodiments of the present invention, the positive electrode active material is lithium manganate, and the aqueous electrolyte is a mixed aqueous solution of lithium sulfate and zinc sulfate.
In some embodiments of the present invention, the positive electrode active material is manganese dioxide, and the aqueous electrolyte is a mixed aqueous solution of manganese sulfate and zinc sulfate.
Additional aspects and advantages of the invention will be set forth in part in the description which follows and, in part, will be obvious from the description, or may be learned by practice of the invention.
Drawings
The above and/or additional aspects and advantages of the present invention will become apparent and readily appreciated from the following description of the embodiments, taken in conjunction with the accompanying drawings of which:
fig. 1 is a pictorial view of a negative electrode current collector according to an embodiment of the present invention;
fig. 2 is a graph showing the results of cycle performance tests of the water-based batteries prepared in example 1 and comparative example.
Detailed Description
The following describes embodiments of the present invention in detail. The following examples are illustrative only and are not to be construed as limiting the invention. The examples, where specific techniques or conditions are not indicated, are to be construed according to the techniques or conditions described in the literature in the art or according to the product specifications. The reagents or instruments used are not indicated by the manufacturer, and are all conventional products commercially available.
In one aspect of the present invention, a negative electrode current collector is provided. According to an embodiment of the present invention, the negative electrode current collector includes: the metal plating layer is formed on at least part of the surface of the substrate, and the metal plating layer is formed by high hydrogen evolution potential metal.
According to the negative current collector disclosed by the embodiment of the invention, the high hydrogen evolution potential metal coating on the surface of the negative current collector can increase the hydrogen evolution difficulty of the negative electrode, and the hydrogen evolution side reaction of the battery is effectively avoided. Meanwhile, the interface regulation is carried out by utilizing the metal coating, so that the uniform nucleation of zinc ions in the electrolyte during deposition can be promoted, the tip effect caused by uneven deposition is reduced, and the growth of zinc dendrite is effectively inhibited. On the other hand, the metal coating can be used as a transition layer between the negative active material and the current collector matrix, and plays a role in buffering and protecting the current collector matrix when the negative active material is dissolved. Under the condition that the battery is placed for a long time, the current collector matrix is separated from the electrolyte by the metal coating, and the current collector matrix can be effectively protected from being corroded. Therefore, the surface of the negative current collector is provided with the plating layer formed by the high hydrogen evolution potential metal, so that the problems of negative dendrite, hydrogen evolution, corrosion and the like can be effectively inhibited, the service life of the battery is prolonged, and the performance of the battery is improved.
The negative electrode current collector according to an embodiment of the present invention is further described in detail below.
According to some embodiments of the invention, the substrate may be a copper mesh. The surface of the traditional copper mesh current collector is easy to generate hydrogen evolution side reaction, and the long-time contact with water can generate verdigris, so that the internal resistance is increased and the conductivity is reduced. According to the negative current collector provided by the invention, the metal coating is arranged on the surface of the substrate, so that the problems can be effectively solved, and the performance of the copper mesh current collector is ensured.
According to some embodiments of the invention, the substrate is preferably a wire-stayed brass net. This can further improve the electrochemical performance of the battery.
According to some embodiments of the present invention, the high hydrogen evolution potential metal may be selected from at least one of Zn, Sn, Pb, In, and Bi. The metal has high hydrogen evolution potential, and can effectively inhibit the generation of hydrogen evolution side reaction after a coating is formed on the surface of a negative electrode substrate. Meanwhile, the plating layer formed by the metal can promote the uniform nucleation of zinc ions in the electrolyte during deposition, reduce the tip effect caused by uneven deposition and effectively inhibit the growth of zinc dendrite.
According to some embodiments of the present invention, the thickness of the metal plating layer may be 0.1 to 500 μm, such as 0.1 μm, 0.5 μm, 1 μm, 1.5 μm, 2 μm, 2.5 μm, 3 μm, 5 μm, 10 μm, 50 μm, 80 μm, 100 μm, 200 μm, 300 μm, 400 μm, 500 μm, and the like. The inventors have found that by controlling the thickness of the metal plating layer within the above range, the performance can be further advantageously exhibited. If the thickness of the metal coating is too small, the local part of the current collector matrix can not be covered by the coating, so that the partial copper mesh generates hydrogen evolution and corrosion phenomena, and further the current at the part is unbalanced, thereby generating dendritic crystals and influencing the performance of the battery; if the thickness of the metal coating is too large, the flexibility of the current collector substrate is reduced, the brittleness is increased, the thickness is not uniform easily, and the processes such as slurry drawing and the like in the production process of the pole piece are affected.
According to some embodiments of the present invention, the thickness of the metal plating layer is preferably 0.1 to 3 μm.
The specific method for forming the metal plating layer is not particularly limited, and a method well known in the art, such as electroplating or electroless plating, may be used. Fig. 1 shows a physical diagram of a galvanized copper mesh according to an embodiment of the invention, and the light-colored part of the lower half of the copper mesh in fig. 1 is a galvanized layer.
In another aspect of the present invention, an aqueous battery is provided. According to an embodiment of the present invention, the water-based battery includes: a positive electrode, a negative electrode, and an aqueous electrolyte solution; wherein, the positive electrode comprises a positive electrode active material and a positive electrode current collector, and the negative electrode comprises a negative electrode active material and the negative electrode current collector of the above embodiment. Therefore, the water-based battery can effectively overcome the problems of dendrite, hydrogen evolution, corrosion and the like of the negative electrode, and can obtain longer service life and higher electrochemical performance.
According to some embodiments of the invention, the negative active material is zinc powder.
In the aqueous battery of the present invention, specific kinds of the aqueous electrolytic solution are not particularly limited, and an aqueous electrolytic solution commonly used in the art, for example, a sulfate solution, an acetate solution (for example, lithium acetate, manganese acetate, zinc acetate, or the like), a nitrate solution, a perchlorate solution, a methanesulfonate solution, a trifluoromethanesulfonate solution, or the like can be used, and a sulfate solution is preferable.
According to some embodiments of the present invention, the positive electrode active material is lithium manganate, and the aqueous electrolyte is a mixed aqueous solution of lithium sulfate and zinc sulfate. The inventors have found that when lithium manganate is used as a positive electrode active material, the aqueous electrolyte solution is a mixed aqueous solution of lithium sulfate and zinc sulfate, and the battery performance is further improved. Wherein the concentration of lithium sulfate is preferably 0.8-1.2 mol/L, and the concentration of zinc sulfate is preferably 1.6-2.0 mol/L. More preferably, when lithium manganate is used as the positive electrode active material, the concentration of lithium sulfate in the aqueous electrolyte is 1.0mol/L and the concentration of zinc sulfate is 1.8 mol/L.
According to some embodiments of the present invention, the positive electrode active material is manganese dioxide, and the aqueous electrolyte is a mixed aqueous solution of manganese sulfate and zinc sulfate. The inventors have found that when manganese dioxide is used as the positive electrode active material, the aqueous electrolyte solution uses a mixed aqueous solution of manganese sulfate and zinc sulfate, and the battery performance is better. The preferable concentration of manganese sulfate is 0.1-0.3 mol/L, and the preferable concentration of zinc sulfate is 1.6-2.0 mol/L. More preferably, when manganese dioxide is used as the positive electrode active material, the concentration of manganese sulfate in the aqueous electrolyte is 0.2mol/L and the concentration of zinc sulfate is 1.8 mol/L.
In addition, it should be noted that the water-based battery has all the features and advantages described above for the negative electrode current collector, and thus, detailed description thereof is omitted.
The invention will now be described with reference to specific examples, which are intended to be illustrative only and not to be limiting in any way.
Example 1
Firstly, preparing a galvanized copper net (electroplating):
1. soaking the brass net in 1mol/L sodium hydroxide solution for 5min, and removing oil and rust. Washed by deionized water and dried.
2. Adding a zinc plating solution into the plating bath, wherein the main component of the zinc plating solution is zinc sulfate of 1 mol/L. 0.5mol/L sodium sulfate and 0.5mol/L potassium chloride were added as conductive salts, 0.2mol/L boric acid was added as a buffer, and 0.05mol/L cetyltrimethylammonium bromide (CTAB) was added as a surfactant. The pH value of the solution is adjusted to 3.5 and the solution is stirred evenly. The reaction temperature was controlled to room temperature.
3. Electroplating is carried out by taking zinc foil as an anode and taking a brass net as a cathode. The current is 250mA/dm2The electroplating time is 5 h.
4. After the galvanized copper mesh is cleaned by deionized water, the galvanized copper mesh is soaked in 0.5 percent nitric acid solution for 5min so as to shine the coating. Then the copper mesh is washed by clean water and dried to obtain the galvanized copper mesh, and the thickness of the plating layer is about 1.2 mu m.
Secondly, preparing the water-based battery
The positive active material adopts lithium manganate, the water system electrolyte adopts a mixed aqueous solution of 1.0mol/L lithium sulfate and 1.8mol/L zinc sulfate, the prepared zinc-plated copper mesh is used as a negative current collector, and the zinc negative electrode is prepared by a slurry drawing process.
Example 2
A galvanized copper mesh and an aqueous battery were produced in substantially the same manner as in example 1, except that the plating time was 2 hours during the production of the galvanized copper mesh, and the thickness of the plated layer in the produced galvanized copper mesh was about 0.8 μm.
Example 3
A galvanized copper mesh and an aqueous battery were produced in substantially the same manner as in example 1, except that the plating time was 8 hours during the production of the galvanized copper mesh, and the thickness of the plated layer in the produced galvanized copper mesh was about 2 μm.
Example 4
Firstly, preparing a tin-plated copper mesh (chemical plating):
1. soaking the brass net in 1mol/L sodium hydroxide solution for 5min, and removing oil and rust. Washed by deionized water and dried.
2. Adding commercially available tin plating solution into the electroplating bath, immersing the brass net, and chemically plating tin for 5 min.
3. And cleaning the tin-plated copper mesh by using deionized water, wherein the thickness of the plated layer is about 1.0 mu m.
Secondly, preparing the water-based battery
The positive active material adopts lithium manganate, the water system electrolyte adopts a mixed aqueous solution of 1.0mol/L lithium sulfate and 1.8mol/L zinc sulfate, the prepared tinned copper net is used as a negative current collector, and the zinc negative electrode is prepared by a slurry drawing process.
Example 5
A tin-plated copper mesh and a water-based battery were produced in substantially the same manner as in example 4, except that the plating time was 2min during the production of the tin-plated copper mesh, and the thickness of the plating layer in the produced tin-plated copper mesh was about 0.2 μm.
Example 6
A tin-plated copper mesh and a water-based battery were produced in substantially the same manner as in example 4, except that the plating time was 20min during the production of the tin-plated copper mesh, and the thickness of the plating layer in the produced tin-plated copper mesh was about 1.8 μm.
Comparative example
An aqueous battery was prepared in substantially the same manner as in example 1, except that a commercially available brass mesh having no metal plating was used as the negative electrode current collector.
Test example
The water system batteries prepared in examples 1 to 6 and comparative example were respectively removed, and the initial specific capacity and the capacity retention rate after 150 cycles were tested. The test conditions included: the voltage range is 1.4-2.1V, the multiplying power is 0.2C, and the temperature is 45 ℃. The test results are shown in table 1 and fig. 2.
TABLE 1
The test result shows that the cycle retention rate of the water-based battery manufactured by the negative current collector with the metal coating is remarkably improved compared with that of the water-based battery manufactured by the traditional copper mesh current collector. The problems of dendritic crystal, hydrogen evolution, corrosion and the like of the negative electrode can be effectively inhibited due to the metal coating on the surface of the copper mesh, so that the service life of the battery is prolonged, and the performance of the battery is improved.
In the description herein, references to the description of the term "one embodiment," "some embodiments," "an example," "a specific example," or "some examples," etc., mean that a particular feature, structure, material, or characteristic described in connection with the embodiment or example is included in at least one embodiment or example of the invention. In this specification, the schematic representations of the terms used above are not necessarily intended to refer to the same embodiment or example. Furthermore, the particular features, structures, materials, or characteristics described may be combined in any suitable manner in any one or more embodiments or examples. Furthermore, various embodiments or examples and features of different embodiments or examples described in this specification can be combined and combined by one skilled in the art without contradiction.
Although embodiments of the present invention have been shown and described above, it is understood that the above embodiments are exemplary and should not be construed as limiting the present invention, and that variations, modifications, substitutions and alterations can be made to the above embodiments by those of ordinary skill in the art within the scope of the present invention.
Claims (10)
1. An anode current collector, comprising:
a substrate;
a metal plating layer formed on at least a part of the surface of the base, the metal plating layer being formed of a high hydrogen evolution potential metal.
2. The negative electrode current collector of claim 1, wherein the substrate is a copper mesh.
3. The negative electrode current collector of claim 2, wherein the substrate is a diagonal-drawn brass mesh.
4. The negative electrode current collector of claim 1, wherein the high hydrogen evolution potential metal is selected from at least one of Zn, Sn, Pb, In, Bi.
5. The negative electrode current collector as claimed in claim 1, wherein the metal plating layer has a thickness of 0.1 to 500 μm.
6. The negative electrode current collector as claimed in claim 5, wherein the metal plating layer has a thickness of 0.1 to 3 μm.
7. An aqueous battery, characterized by comprising: a positive electrode, a negative electrode, and an aqueous electrolyte solution; wherein the positive electrode comprises a positive electrode active material and a positive electrode current collector, and the negative electrode comprises a negative electrode active material and a negative electrode current collector as claimed in any one of claims 1 to 6.
8. The water-based battery according to claim 7, wherein the negative active material is zinc powder.
9. The aqueous battery according to claim 7, wherein the positive electrode active material is lithium manganate, and the aqueous electrolyte is a mixed aqueous solution of lithium sulfate and zinc sulfate.
10. The aqueous battery according to claim 7, wherein the positive electrode active material is manganese dioxide, and the aqueous electrolyte is a mixed aqueous solution of manganese sulfate and zinc sulfate.
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| CN107256946A (en) * | 2011-11-03 | 2017-10-17 | 苏州宝时得电动工具有限公司 | Battery |
| CN107403968A (en) * | 2016-05-20 | 2017-11-28 | 苏州宝时得电动工具有限公司 | Aqoue seconary battery |
| WO2018090161A1 (en) * | 2016-11-18 | 2018-05-24 | 深圳市寒暑科技新能源有限公司 | Rechargeable zinc ion battery employing copper metal as negative electrode current collector |
| CN111430819A (en) * | 2020-03-31 | 2020-07-17 | 恩力能源科技(安徽)有限公司 | Water-based ion battery and preparation method thereof |
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2020
- 2020-09-04 CN CN202010920027.8A patent/CN112151805A/en active Pending
Patent Citations (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2010153287A (en) * | 2008-12-26 | 2010-07-08 | Hitachi Maxell Ltd | Alkaline battery |
| CN107256946A (en) * | 2011-11-03 | 2017-10-17 | 苏州宝时得电动工具有限公司 | Battery |
| CN105810895A (en) * | 2014-12-30 | 2016-07-27 | 苏州宝时得电动工具有限公司 | Positive electrode, and battery containing same |
| CN107403968A (en) * | 2016-05-20 | 2017-11-28 | 苏州宝时得电动工具有限公司 | Aqoue seconary battery |
| WO2018090161A1 (en) * | 2016-11-18 | 2018-05-24 | 深圳市寒暑科技新能源有限公司 | Rechargeable zinc ion battery employing copper metal as negative electrode current collector |
| CN111430819A (en) * | 2020-03-31 | 2020-07-17 | 恩力能源科技(安徽)有限公司 | Water-based ion battery and preparation method thereof |
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