CN109659565B - Composite current collector, preparation method thereof, electrode and lithium ion battery - Google Patents
Composite current collector, preparation method thereof, electrode and lithium ion battery Download PDFInfo
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- H01—ELECTRIC ELEMENTS
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- 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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- 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
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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- H—ELECTRICITY
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- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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- H01M10/4235—Safety or regulating additives or arrangements in electrodes, separators or electrolyte
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- H01M4/02—Electrodes composed of, or comprising, active material
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Abstract
The invention relates to a composite current collector, a preparation method thereof, an electrode and a lithium ion battery, wherein the composite current collector comprises a current collector and a surface coating formed on the current collector, and the surface coating comprises nano bismuth, nano bismuth oxide, a binder and a conductive agent. The nano bismuth in the surface coating of the composite current collector is in a nano magnitude, so that the contact area between the current collector and an active material in an active material layer can be increased, the internal resistance of an interface is further reduced, and the stability of the battery capacity is improved; and the melting point of the nano bismuth is low, so that the nano bismuth can be fused when the lithium ion battery is heated, and the contact between the active substance and the current collector is cut off, so that a conductive path is cut off to avoid further thermal runaway. The nano bismuth and the nano bismuth oxide have good compatibility, and the nano bismuth oxide with the flame retardant function in the composite current collector can cooperate with the nano bismuth to inhibit the combustion of the battery and play a role in preventing the explosion of the lithium ion battery when the heating temperature of the lithium ion battery is increased, so that the safety performance of the battery is improved.
Description
Technical Field
The invention relates to the technical field of batteries, in particular to a composite current collector, a preparation method thereof, an electrode and a lithium ion battery.
Background
With the rapid development of new energy industry, the requirements for electrochemical equipment are increasing day by day. On one hand, the electrochemical properties such as higher energy density, rapid charge and discharge and the like are required; on the other hand, higher safety performance is pursued. The current collector is an important component of the lithium ion battery, and refers to a mechanical carrier for bearing active substances of a positive electrode or a negative electrode, and can provide a migration passage for electrons. Most current collectors of the existing lithium ion batteries are copper foils and aluminum foils, and the battery capacity stability of the lithium ion batteries prepared based on the current collectors needs to be improved; in addition, the conventional lithium ion battery has a problem of explosion tendency in a high temperature environment, and therefore, the temperature for storing the battery in the environment is preferably 35 ℃ or lower.
Disclosure of Invention
Accordingly, it is necessary to provide a current collector capable of improving the battery capacity stability and safety performance of a lithium ion battery.
In one aspect of the invention, a composite current collector is provided, which comprises a current collector and a surface coating formed on the current collector, wherein the surface coating comprises nano bismuth, nano bismuth oxide, a binder and a conductive agent.
In one embodiment, the mass ratio of the nano bismuth to the nano bismuth oxide to the binder to the conductive agent is (6-8): (0.5-1.5): (0.1-0.5).
In one embodiment, the nano bismuth has a particle size of 5nm to 100nm; the grain diameter of the nano bismuth oxide is 10 nm-100 nm. Preferably, the specific surface area of the nano bismuth and the nano bismuth oxide is 1 to 50m 2 /g。
In one embodiment, the surface coating has a thickness of no more than 2 microns.
In one embodiment, the binder is selected from at least one of styrene-butadiene rubber, acrylic resin, carboxymethyl cellulose, polytetrafluoroethylene emulsion, polyvinylidene fluoride and polyvinyl alcohol;
the conductive agent is at least one selected from carbon black, acetylene black, carbon fiber, carbon nanotube, graphene, ketjen black, SP and KS-6.
In one embodiment, the current collector is selected from at least one of aluminum foil, nickel foam, nickel foil, nickel mesh, copper foil, stainless steel mesh, stainless steel punch Kong Gangdai, stainless steel foil, titanium mesh, lead foil, lead cloth, graphitized carbon cloth, and graphene cloth material.
In another aspect of the present invention, a method for preparing a composite current collector is provided, which includes the following steps:
mixing nano bismuth, nano bismuth oxide, a binder and a conductive agent in a solvent to obtain slurry;
and coating the slurry on the surface of the current collector, and drying to obtain the composite current collector.
In another aspect of the invention, there is provided an electrode comprising the composite current collector of any one of the above and an active material layer formed on the surface coating of the composite current collector.
In one embodiment, the electrode is an electrode for a lithium ion battery; the electrode is a positive electrode, and the active material layer contains a ternary positive electrode material; or the electrode is a negative electrode, and the active material layer contains a graphite negative electrode material.
In another aspect of the present invention, there is provided a lithium ion battery, wherein at least one of a positive electrode and a negative electrode of the lithium ion battery is the electrode described in any one of the above.
The composite current collector can be used for a lithium ion battery, the nano bismuth in the surface coating of the composite current collector is in a nano level, the specific surface area is large, the contact area between the current collector and an active substance in an active material layer can be increased, and the internal resistance of an interface is further reduced, so that the cycle performance of the battery and the stability of the battery capacity are improved; and the melting point of the nano bismuth is low, so that the nano bismuth can be fused when the lithium ion battery is heated, and the contact between the active substance and the current collector is cut off, so that a conductive path is cut off, and further thermal runaway is avoided. Meanwhile, the compatibility of the nano bismuth and the nano bismuth oxide is good, and the nano bismuth oxide with the flame-retardant effect in the surface coating of the composite current collector can cooperate with the nano bismuth to inhibit the combustion of the battery and play a role in preventing the explosion of the lithium ion battery when the heating temperature of the lithium ion battery is increased, so that the safety performance of the battery is improved.
In addition, the superconducting performance of bismuth can reduce the internal resistance of the battery, and the composite current collector also has better battery capacity stability under the condition of low temperature.
Drawings
Fig. 1 is a schematic structural view of a composite current collector prepared in example 1;
fig. 2 is a graph of cycle test performance of the lithium ion batteries prepared in example 6 and comparative example 1.
Detailed Description
In order that the invention may be more fully understood, a more complete description of the invention, and a preferred embodiment of the invention, is now provided. This invention may, however, be embodied in many different forms and should not be construed as limited to the embodiments set forth herein. Rather, these embodiments are provided so that this disclosure will be thorough and complete.
Unless defined otherwise, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs. The terminology used in the description of the invention herein is for the purpose of describing particular embodiments only and is not intended to be limiting of the invention. As used herein, the term "and/or" includes any and all combinations of one or more of the associated listed items.
One embodiment of the invention provides a composite current collector, which comprises a current collector and a surface coating formed on the current collector, wherein the surface coating comprises nano bismuth, nano bismuth oxide, a binder and a conductive agent.
In one embodiment, the particle size of the nano bismuth is 5nm to 100nm; the grain diameter of the nano bismuth oxide is 10 nm-100 nm. Preferably, the specific surface area of the nano bismuth and the nano bismuth oxide is 1 to 50m 2 /g。
In one embodiment, the thickness of the surface coating is no more than 2 microns.
In one embodiment, the binder includes, but is not limited to, at least one of styrene-butadiene rubber, acrylic resin, carboxymethyl cellulose, polytetrafluoroethylene emulsion, polyvinylidene fluoride, and polyvinyl alcohol. The conductive agent includes, but is not limited to, at least one of carbon black, acetylene black, carbon fiber, carbon nanotube, graphene, ketjen black, SP, and KS-6. The current collector includes, but is not limited to, at least one of aluminum foil, nickel foam, nickel foil, nickel mesh, copper foil, stainless steel mesh, stainless steel punch Kong Gangdai, stainless steel foil, titanium mesh, lead foil, lead cloth, graphitized carbon cloth, and graphene cloth material.
The composite current collector can be used for a lithium ion battery, the nano bismuth in the surface coating of the composite current collector is in a nano level, the specific surface area is large, the contact area between the current collector and an active substance in an active material layer can be increased, and the internal resistance of an interface is further reduced, so that the cycle performance of the battery and the stability of the battery capacity are improved; and the melting point of the nano bismuth is low, so that the nano bismuth can be fused when the lithium ion battery is heated, and the contact between the active substance and the current collector is cut off, so that a conductive path is cut off, and further thermal runaway is avoided. Meanwhile, the compatibility of the nano bismuth and the nano bismuth oxide is good, and the nano bismuth oxide with the flame-retardant effect in the surface coating of the composite current collector can cooperate with the nano bismuth to inhibit the combustion of the battery and play a role in preventing the explosion of the lithium ion battery when the heating temperature of the lithium ion battery is increased, so that the safety performance of the battery is improved.
In addition, the superconducting performance of bismuth can reduce the internal resistance of the battery, and the composite current collector also has better battery capacity stability under the condition of low temperature.
In one embodiment, the mass ratio of the nano bismuth to the nano bismuth oxide to the adhesive to the conductive agent is (6-8): (0.5-1.5): (0.1-0.5): (0.1-0.5); the stability and the safety performance of the battery capacity can be further improved by controlling the proportion of the nano bismuth, the nano bismuth oxide, the binder and the conductive agent.
An embodiment of the present invention provides a method for preparing any one of the above composite current collectors, including the following steps S1 to S2.
Step S1: mixing nano bismuth, nano bismuth oxide, a binder and a conductive agent in a solvent to obtain slurry.
The raw materials are provided according to the composition of the surface coating of the above-mentioned one composite current collector. For example, in one embodiment, the mass ratio of the nano bismuth to the nano bismuth oxide to the binder to the conductive agent is (6-8): (0.5-1.5): (0.1-0.5).
Among them, the solvent is preferably an organic solvent such as N-methylpyrrolidone (NMP), DMF, ethanol, ethylene glycol, methanol, isopropanol, and the like.
It is understood that nano-bismuth can be obtained by reacting a soluble bismuth salt with a reducing agent. Specifically, for example, bismuth nitrate and sodium borohydride are reacted to obtain nano bismuth. Moreover, bismuth sources in China are rich, and the reactant concentration required by the method for preparing the nano bismuth is low, so that the cost is low.
Step S2: and coating the slurry on the surface of the current collector, and drying to obtain the composite current collector.
Further, the drying condition is that the mixture is dried in an oven at the temperature of 80-120 ℃ to constant weight.
The preparation method of the composite current collector is simple to operate and suitable for large-scale production and application; compared with the traditional method of directly growing graphene on the surface of the copper foil in a cladding manner by adopting a chemical vapor deposition method to improve the rate capability and the cycle life of the battery, the preparation method of the composite current collector has simple and easily realized conditions and low requirement on equipment; and the nano bismuth oxide are used as raw materials, so that the method has the advantage of low cost compared with a method adopting graphene and carbon nano tubes.
An embodiment of the present invention provides an electrode comprising the composite current collector of any one of the above and an active material layer formed on a surface coating of the composite current collector.
In one embodiment, the electrode is an electrode for a lithium ion battery.
Further, the above electrode is a positive electrode, and the active material layer contains a ternary positive electrode material for supplying lithium ions. Further, the ternary positive electrode material may be NCM (nickel cobalt manganese) or NCA (nickel cobalt aluminum), and the like, and then the positive electrode active material layer is formed on the composite current collector by using a conventional method. Specifically, a ternary cathode material, a binder and a conductive agent can be mixed in a solvent to prepare cathode slurry; and coating the positive slurry on the composite current collector, and drying.
In another embodiment, the electrode is a negative electrode, and the active material layer contains a graphite negative electrode material capable of co-intercalating lithium ions. Specifically, graphite, a binder and a conductive agent may be mixed in a solvent to prepare a negative electrode slurry; and coating the negative electrode slurry on the composite current collector, and drying.
Further, the conductive agent in the positive electrode slurry or the negative electrode slurry is at least one selected from carbon black, acetylene black, carbon fiber, carbon nanotube, graphene, ketjen black, SP, and KS-6. The binder is at least one selected from styrene butadiene rubber, acrylic resin, carboxymethyl cellulose, polyvinylidene fluoride and polyvinyl alcohol.
An embodiment of the present invention provides a lithium ion battery, wherein at least one of a positive electrode and a negative electrode of the lithium ion battery is an electrode of any one of the above.
In one embodiment, both the positive electrode and the negative electrode of the lithium ion battery are made of the above composite current collector. Other preparation methods are all realized by adopting conventional methods in the industry.
By adopting the electrode, the cycle performance and the safety performance of the lithium ion battery are obviously improved.
The following are specific examples.
The present invention is further illustrated by the following examples, which are not intended to limit the scope of the invention.
Example 1 preparation of composite current collector
(1) Respectively preparing 0.01M bismuth nitrate solution and 0.01M sodium borohydride solution;
(2) According to the molar ratio of sodium borohydride to bismuth nitrate 3:1, sodium borohydride is dropwise added into a bismuth nitrate solution, stirring is continued for 5min after dropwise addition is completed, the rotating speed is 1000rpm, and after a product is washed by deionized water, the product is dried in a drying oven at 100 ℃ to constant weight to prepare the nano bismuth.
(3) Mixing nano bismuth, nano bismuth oxide, a binder and a conductive agent in a solvent according to the mass ratio of 8.5. And coating the slurry on the surface of the copper foil, and drying in a 90 ℃ oven to constant weight to obtain the composite current collector. Wherein the coating thickness is less than 2 microns. Wherein, the binder is polytetrafluoroethylene emulsion, and the conductive agent is SP. The structural schematic diagram of the prepared composite current collector is shown in fig. 1, and the surface of the copper foil 101 is coated with a surface coating 102 containing nano bismuth and nano bismuth oxide.
Example 2 the steps of preparing a composite current collector are substantially the same as those of example 1, except that the mass ratio of the nano bismuth to the nano bismuth oxide to the binder to the conductive agent in step (3) is 6.5; the binder is styrene-butadiene latex and the carboxymethylcellulose sodium conductive agent is acetylene black.
Example 3 the steps of preparing a composite current collector are substantially the same as those of example 1, except that the mass ratio of the nano bismuth to the nano bismuth oxide to the binder to the conductive agent in step (3) is 8.5; the binder is polyvinylidene fluoride, and the conductive agent is carbon nano tubes.
Example 4 the steps of preparing a composite current collector are substantially the same as those of example 1, except that the mass ratio of the nano bismuth to the nano bismuth oxide to the binder to the conductive agent in step (3) is 7; the adhesive is polyvinyl alcohol alkene, and the conductive agent is carbon black.
The above examples 1 to 4 are preparation examples of composite current collectors; examples 5 to 8 are examples of the production of lithium ion batteries.
Example 5 preparation of lithium ion batteries
(1) Selecting a ternary material NCM as a positive electrode, and mixing the ternary material NCM with a binder and a conductive agent in an NMP solvent to prepare positive electrode slurry; and coating the positive electrode slurry on the composite current collector obtained in the embodiment 1, and drying in a vacuum drying oven at 120 ℃ to obtain a positive electrode piece.
(2) Selecting graphite as a negative electrode material, and mixing the graphite with a binder and a conductive agent in an ethylene glycol solvent to prepare negative electrode slurry; and coating the negative electrode slurry on the composite current collector obtained in the embodiment 1, and drying in a vacuum drying oven at 120 ℃ to obtain a negative electrode plate.
(3) And assembling the positive pole piece, the negative pole piece, the diaphragm and the lithium ion electrolyte into the lithium ion battery.
The steps for preparing the lithium ion batteries of examples 6 to 8 are substantially the same as those of example 5, except that the composite current collectors used in step (1) and step (2) are the composite current collectors prepared in examples 2 to 4, respectively.
Comparative example 1 preparation of lithium ion Battery
Comparative example 1 the procedure for preparing a lithium ion battery was substantially the same as in example 5, except that the composite current collector used in steps (1) and (2) was a copper foil that was not surface-coated with nano bismuth and nano bismuth oxide.
As shown in fig. 2, in which the abscissa is the cycle number (SOC) of the test and the ordinate is the remaining capacity (SOC), the capacity of the lithium ion battery using the modified composite current collector obtained in example 6 is maintained at about 91.7% after the lithium ion battery is subjected to a cycle test at room temperature at a current of 1C for 800 times; the lithium ion battery of comparative example 1 employs an unmodified copper foil, and after performing a cycle test at room temperature for 800 times at a current of 1C, the capacity retention rate is about 80%. Other examples were also tested for cycling performance in the same manner, and the capacity retention after 800 cycles at 1C at room temperature was obtained, as shown in table 1.
TABLE 1
| Group of | Example 5 | Example 6 | Example 7 | Example 8 | Comparative example 1 |
| Capacity retention rate | 88.7 | 91.7 | 90.3 | 91.1 | 83.285 |
The overcharge test was performed on the lithium ion batteries prepared in the above examples 5 to 8 and comparative example 1, and the specific operation was as follows: the method comprises the steps of discharging a battery cell to 3.0V at a constant current of 1C, and standing for 10min; then charging to 4.2V with a constant current and a constant voltage of 1C, stopping the current at 0.05C, and standing for 10min; and finally, charging to 6.3V with a constant current of 1C, standing for 1h, and observing the cell. If the battery cell does not explode or catch fire, the experiment is passed, otherwise, the experiment is not carried out. The statistical results obtained are shown in table 2.
TABLE 2
It can be seen from table 2 that 90% of the lithium ion batteries prepared in examples 6 to 8 can pass the overcharge experiment, and 10% of the comparative lithium ion batteries using unmodified foil as the current collector can pass the overcharge experiment, so that the current collector provided by the invention can improve the safety performance of the batteries.
The technical features of the embodiments described above may be arbitrarily combined, and for the sake of brevity, all possible combinations of the technical features in the embodiments described above are not described, but should be considered as being within the scope of the present specification as long as there is no contradiction between the combinations of the technical features.
The above-mentioned embodiments only express several embodiments of the present invention, and the description thereof is more specific and detailed, but not construed as limiting the scope of the invention. It should be noted that, for a person skilled in the art, several variations and modifications can be made without departing from the inventive concept, which falls within the scope of the present invention. Therefore, the protection scope of the present patent shall be subject to the appended claims.
Claims (10)
1. The lithium ion battery electrode is characterized by comprising a composite current collector and an active material layer, wherein the composite current collector comprises a current collector and a surface coating formed on the current collector, the active material layer is formed on the surface coating of the composite current collector, and the surface coating comprises nano bismuth, nano bismuth oxide, a binder and a conductive agent.
2. The lithium ion battery electrode of claim 1, wherein the mass ratio of the nano bismuth, the nano bismuth oxide, the binder and the conductive agent is (6-8), (0.5-1.5), (0.1-0.5) and (0.1-0.5).
3. The lithium ion battery electrode of claim 1, wherein the nano bismuth has a particle size of 5nm to 100nm; the grain diameter of the nano bismuth oxide is 10 nm-100 nm.
4. The lithium ion battery electrode of claim 1, wherein the surface coating has a thickness of no more than 2 microns.
5. The lithium ion battery electrode of claim 1, wherein the binder is selected from at least one of styrene-butadiene rubber, acrylic resin, carboxymethyl cellulose, polytetrafluoroethylene emulsion, polyvinylidene fluoride, and polyvinyl alcohol;
the conductive agent is selected from at least one of carbon black, carbon fiber, carbon nanotube and graphene.
6. The lithium ion battery electrode of claim 1, wherein the current collector is selected from at least one of aluminum foil, nickel foam, nickel foil, nickel mesh, copper foil, stainless steel mesh, stainless steel punch Kong Gangdai, stainless steel foil, titanium mesh, lead foil, lead cloth, graphitized carbon cloth, and graphene cloth materials.
7. The lithium ion battery electrode of any of claims 1-6, wherein the lithium ion battery electrode is a lithium ion battery positive electrode, and the active material layer comprises a ternary positive electrode material; or the lithium ion battery electrode is a lithium ion battery cathode, and the active material layer contains a graphite cathode material.
8. A preparation method of a lithium ion battery anode is characterized by comprising the following steps:
mixing nano bismuth, nano bismuth oxide, a binder and a conductive agent in a solvent to obtain coating slurry;
coating the slurry on the surface of a current collector, and drying to obtain a composite current collector;
mixing a ternary positive electrode material, a binder and a conductive agent in a solvent to prepare positive electrode slurry;
and coating the positive slurry on the composite current collector, and drying.
9. A preparation method of a lithium ion battery cathode is characterized by comprising the following steps:
mixing nano bismuth, nano bismuth oxide, a binder and a conductive agent in a solvent to obtain coating slurry;
coating the slurry on the surface of a current collector, and drying to obtain a composite current collector;
mixing graphite, a binder and a conductive agent in a solvent to prepare negative electrode slurry;
and coating the negative electrode slurry on the composite current collector, and drying.
10. A lithium ion battery, characterized in that at least one of the positive electrode and the negative electrode of the lithium ion battery is the lithium ion battery electrode according to any one of claims 1 to 7.
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| CN111048788B (en) * | 2019-12-26 | 2021-06-01 | 珠海冠宇电池股份有限公司 | Current collector and preparation method and application thereof |
| CN115440987B (en) * | 2021-06-01 | 2024-10-11 | 比亚迪股份有限公司 | Current collector, preparation method thereof, negative electrode and electrochemical energy storage device |
| CN114335557B (en) * | 2021-11-30 | 2023-07-14 | 蜂巢能源科技有限公司 | Composite foil and preparation method thereof, current collector and lithium ion battery |
| CN117038999A (en) * | 2023-08-23 | 2023-11-10 | 重庆市紫建新能源有限公司 | High-safety porous polymer composite current collector and lithium ion battery |
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| US5721068A (en) * | 1995-07-14 | 1998-02-24 | Rayovac Corporation | Electrochemical cell, gelled anode, and coated current collector therefor |
| US7976976B2 (en) * | 2007-02-07 | 2011-07-12 | Rosecreek Technologies Inc. | Composite current collector |
| CN101931072A (en) * | 2009-06-26 | 2010-12-29 | 能原材公司 | Anode active material and secondary lithium battery |
| CN101894682B (en) * | 2010-02-26 | 2012-07-04 | 上海奥威科技开发有限公司 | High-energy ultracapacitor |
| 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 |
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