CN109004235B - Carbon-based three-dimensional ordered lithium ion battery current collector, preparation method thereof and lithium ion battery - Google Patents
Carbon-based three-dimensional ordered lithium ion battery current collector, preparation method thereof and lithium ion battery Download PDFInfo
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- CN109004235B CN109004235B CN201810872903.7A CN201810872903A CN109004235B CN 109004235 B CN109004235 B CN 109004235B CN 201810872903 A CN201810872903 A CN 201810872903A CN 109004235 B CN109004235 B CN 109004235B
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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
- H01M4/663—Selection of materials containing carbon or carbonaceous materials as conductive part, e.g. graphite, carbon fibres
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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
- H01M10/052—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
- 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
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
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Abstract
The invention discloses a carbon-based three-dimensional ordered lithium ion battery current collector, a preparation method thereof and a lithium ion battery, wherein the current collector consists of a polymer carrier, an ordering regulator and conductive particles; the polymer carrier is natural vegetable gum, the mass ratio of the natural vegetable gum to the conductive particles is 1:1, and the mass ratio of the natural vegetable gum to the ordering regulator is 100 (1-2). The electrode can be free from using metal foil in the preparation process of the battery, so that the weight of the electrode is obviously reduced, and the electrode can store several times of electric quantity compared with the electrode using a metal foil current collector under the condition that the electrode active substance is not changed again with the same electrode quality.
Description
Technical Field
The invention belongs to the field of lithium ion battery manufacturing, and particularly relates to a carbon-based three-dimensional ordered lithium ion battery current collector, a preparation method thereof and a lithium ion battery.
Background
The current collector is an important component of the lithium ion battery, and the current collector mainly has the function of collecting the current generated by the active materials of the battery so as to form larger current to be output to the outside. Usually a metal foil, usually a copper foil for the negative electrode and an aluminum foil for the positive electrode. After the battery is assembled, the electrode active substance is uniformly fixed on the surface of the current collector, so that electrons are gathered on the metal foil during chemical reaction. The metal foil itself does not participate in chemical reactions, but merely provides a lamellar carrier for the electrode active material and facilitates the collection of current. In the preparation process of the battery, in order to ensure that the electrode active material can be fully contacted with the electrolyte, the current collector can be coated with the electrode material with the thickness of several microns. This results in the mass of the current collector occupying a large portion of the electrode mass. Therefore, in order to reduce the weight of the battery, the thickness of the metal foil is generally reduced, but the fact that the current collector occupies most of the weight of the battery cannot be changed. In order to improve the utilization rate of the current collector, battery technologists have proposed an improvement direction of the three-dimensional current collector, and hope that the current collector can develop towards high porosity and high specific surface area, if the electric conductivity and the bearing capacity of the active material of the current collector are ensured. The three-dimensional current collector appearing in the current research comprises two directions of a metal base and a carbon base, and the metal base current collector is made of a porous material by utilizing a metal material represented by foamed nickel, so that the bearing capacity of the current collector with unit mass to an electrode active substance can be effectively improved. However, when the metal material is used in a battery, the weight ratio is still high. The carbon-based current collector is made of a conductive thin-layer material represented by graphene into a spongy substance, so that the conductivity is ensured, and the mass ratio of the current collector is greatly reduced. However, the current collector prepared by using graphene needs to be oxidized to change the dispersibility and then restored with conductivity through reduction. The preparation process is complicated and also inevitably results in high cost.
Disclosure of Invention
The invention aims to provide a carbon-based three-dimensional ordered lithium ion battery current collector, a preparation method thereof and a lithium ion battery, which can avoid using metal foil in the battery preparation process, thereby realizing the purpose of reducing the weight of the battery.
In order to achieve the above purpose, the technical scheme provided by the invention is as follows:
in order to achieve the purpose, the invention adopts the following technical scheme:
a carbon-based three-dimensional ordered lithium ion battery current collector is composed of a polymer carrier, an order regulator and conductive particles; the polymer carrier is natural vegetable gum, the mass ratio of the natural vegetable gum to the conductive particles is 1:1, and the mass ratio of the natural vegetable gum to the ordering regulator is 100 (1-2).
The natural vegetable gum solution is natural vegetable gum with non-ionic characteristics, and is selected from guanidine gum or xanthan gum; the order regulator is a cross-linking agent with reversible cross-linking capability on natural vegetable gum, and is selected from borax or an organic boron cross-linking agent; the conductive particles are carbon powder selected from super-p or acetylene black.
A preparation method of a carbon-based three-dimensional ordered lithium ion battery current collector comprises the following steps:
the method comprises the following steps: firstly, preparing a natural plant gum solution, standing and swelling for later use after the preparation is finished; preparing a boron-containing order regulator solution;
step two: mixing the natural vegetable gum solution with the conductive particles to ensure that the mass ratio of the natural vegetable gum to the conductive particles is 1:1, and then performing ball milling to obtain mixed liquid;
step three: adding an ordering regulator into the mixed liquid obtained in the step two to ensure that the mass ratio of the natural vegetable gum solution to the ordering regulator solution is 100 (1-2), and then performing ball milling to obtain viscous slurry;
step four: and pouring the slurry obtained in the step three into a mould, transferring to a cold trap, cooling to-40 ℃, carrying out constant temperature treatment, and transferring to a freeze dryer to ensure complete drying to obtain the carbon-based three-dimensional ordered current collector.
The natural vegetable gum solution is natural vegetable gum with non-ionic characteristics, and is selected from guanidine gum or xanthan gum.
The order regulator is a cross-linking agent with reversible cross-linking capability on natural vegetable gum, and is selected from borax or an organic boron cross-linking agent.
The conductive particles are carbon powder selected from super-p or acetylene black.
The concentration of the natural plant gum solution is 0.5-2%; the content of boron element in the ordering regulator solution is 0.4-2%.
In the fourth step, the temperature is adjusted to-40 ℃ in a cold trap, and the constant temperature is kept for 3 hours; adjusting the pressure in the freeze dryer to 5-10Pa, and the duration is 12-24 h.
A lithium ion battery based on a carbon-based three-dimensional ordered lithium ion battery current collector is characterized in that an electrode material with the same mass as that of conductive particles is added into the current collector.
The electrode material is nano Fe3O4Or graphite.
Compared with the prior art, the invention has the following advantages:
the invention can avoid the potential risk of difficult adsorption of the charged electrode active substances caused by charge repulsion because of using the nonionic polymer. The non-ionic polymer has a slow unfolding speed during dissolution and swelling, but the unfolding degree and the flatness can be controlled by the order regulator. The sedimentation of the conductive particles in the viscous slurry can be intercepted by the strip-shaped nonionic polymer, so that the conductive particles are spread on the strip-shaped sheet to form a conductive layer, and the conductive layer is more convenient to prepare by a particle sedimentation method than by using graphene. The order regulator with reversible crosslinking capacity can ensure that the arrangement of the strip-shaped sheets is orderly and orderly in a certain range. The electrolyte passing capacity is improved. The three-dimensional current collector can conveniently provide an attachment carrier for the electrode active substance and facilitate the reaction of the active substance and the electrolyte, so that the utilization rate of the electrode material is high. Because no metal foil is used, the weight of the electrode is obviously reduced, and under the condition that the electrode quality is the same and the electrode active substance is not changed, the electrode can store multiple times of electric quantity compared with the electrode using a metal foil current collector.
The preparation method of the invention adopts the polymer carrier, the order regulator and the conductive particles as raw materials, so that the processing steps are effectively reduced, and the obtained viscous slurry is poured into a grinding tool through conventional operation, put into a cold trap to be cooled to minus 40 ℃ and kept at the constant temperature for 3 hours, and then transferred to a freeze dryer to be regulated at the pressure of 5-10Pa until being completely dried, so that the spongy substance is the three-dimensional current collector. Meanwhile, the characteristics of the thin-layer material are utilized to carry out ordered control, so that the arrangement of the current collectors is more regular, and better electrolyte passing capacity is obtained. When the electrode active material carries out lithium ion exchange reaction on the surface of the conductive network, the electrode active material can conveniently provide the inflow and outflow of electrons, and plays the role of a current collector.
Drawings
Fig. 1 is a porous structure diagram of a carbon-based three-dimensional ordered current collector;
FIG. 2 carbon-based three-dimensional ordered current collector surface Fe3O4A distribution diagram;
FIG. 3 Fe3O4A CV curve of reaction at the surface of the three-dimensional current collector;
FIG. 4 Fe when using three-dimensional current collectors3O4And (4) cycle performance.
Detailed Description
The invention relates to a carbon-based three-dimensional ordered lithium ion battery current collector which comprises a polymer carrier, an ordering regulator and conductive particles. By polymeric carrier is meant natural vegetable gums having non-ionic character such as guar gum and xanthan gum. The order regulator is a cross-linking agent with reversible cross-linking capability on natural vegetable gum, such as borax and an organic boron cross-linking agent. The conductive fine particles refer to extremely fine carbon powder such as super-p or acetylene black.
The flow of the three-dimensional current collector preparation is as follows. The carrier is first dissolved in water, and the granular natural vegetable gum is stretched into belt shape in the solution. Mixing the conductive particles with the natural plant gum solution, grinding uniformly, adding the order regulator, and grinding uniformly. Pouring the obtained viscous slurry into a grinding tool, placing into a cold trap, cooling to-40 deg.C, keeping the temperature for 3h, transferring to a freeze dryer, and adjusting pressure to 5-10Pa until completely drying. The obtained spongy substance is the three-dimensional current collector.
The idea of the invention is as follows: the surface of the thin layer material with the nanometer thickness is covered with a conductive substance, and a three-dimensional conductive network is formed by utilizing the mutual interweaving of the thin layer material. Meanwhile, the characteristics of the thin-layer material are utilized to carry out ordered control, so that the arrangement of the current collectors is more regular, and better electrolyte passing capacity is obtained. When the electrode active material carries out lithium ion exchange reaction on the surface of the conductive network, the electrode active material can conveniently provide the inflow and outflow of electrons, and plays the role of a current collector. The specific preparation method is as follows.
The preparation method of the invention specifically comprises the following operations: firstly, preparing natural plant gum solution with the concentration of 0.5-2%, and standing for swelling for 4-6 h. Preparing an order regulator solution to ensure that the content of boron element is 0.4-2%. The natural vegetable gum solution is mixed with the conductive particles to ensure that the mass ratio of the natural vegetable gum to the conductive particles is 1: 1. And (3) after ball milling for 5min, adding an ordering regulator to ensure that the mass ratio of the natural vegetable gum solution to the ordering regulator solution is 100: 1-2. And then ball milling is carried out for 5min to obtain viscous slurry. Pouring the slurry into a mold, adjusting the temperature to-40 ℃ in a cold trap, keeping the temperature constant for 3h, transferring the slurry into a freeze dryer, adjusting the pressure to 5-10Pa, and keeping the pressure for 12-24h to ensure complete drying, thereby obtaining the carbon-based three-dimensional ordered current collector. When the three-dimensional ordered current collector is applied to a lithium ion battery cathode, the conductive particles are added in the preparation process, and simultaneously electrode active substances with the same mass are added. The three-dimensional ordered current collector with the electrode active material can be used as an electrode.
Example 1
A carbon-based three-dimensional ordered lithium ion battery current collector is prepared by firstly preparing a guanidine gum solution with the concentration of 0.5 percent and standing for swelling for 4 hours. Preparing a borax solution as an ordering regulator, wherein the concentration is 3.5%, the content of boron element is 0.4% in conversion, mixing a guanidine gum solution and super-p according to a mass ratio of 100:0.5 to ensure that the mass ratio of guanidine gum to super-p is 1:1, adding the ordering regulator after ball milling for 5min to ensure that the mass ratio of the guanidine gum solution to the ordering regulator is 100:2, and then ball milling for 5min to obtain viscous slurry. Pouring the slurry into a mold, adjusting the temperature to-40 ℃ in a cold trap, keeping the temperature constant for 3 hours, transferring the slurry into a freeze dryer, adjusting the pressure to 5Pa, and keeping the pressure for 12 hours to ensure complete drying, thereby obtaining the carbon-based three-dimensional ordered current collector.
When the nano Fe is required3O4When the Fe-P-Fe-B alloy is used as an electrode material, only the super-p is added in the preparation process of a current collector, and the nano Fe with the same mass is added3O4That is, the Fe can be stably circulated for 500 times or more when used as an electrode3O4The capacity of more than 600mAh/g is exerted. The three-dimensional porous structure is shown in figure 1, active substances are embedded on the surface of a current collector as shown in figure 2, and the structure can enable Fe3O4Fully contacts with the electrolyte and conveniently collects the current to the current collector. FIG. 3 shows Fe3O4The CV curve of the current collector surface during charging and discharging shows that the current collector is opposite to Fe3O4Has no effect on the chemical changes of (a). FIG. 4 shows Fe with a three-dimensional current collector3O4Electrode cycle performance diagram, according to the data in the diagram, Fe3O4Can still keep effective contact with the current collector after 500 cycles, so that Fe3O4The capacity of more than 600mAh/g is exerted.
Example 2
A carbon-based three-dimensional ordered lithium ion battery current collector is prepared by firstly preparing a xanthan gum solution with the concentration of 2 percent and standing for 6 hours for swelling. Preparing a borax solution as an ordering regulator, wherein the concentration is 3.5%, the content of boron element is 0.4% in conversion mode, mixing a xanthan gum solution and acetylene black according to a mass ratio of 100:2, enabling the mass ratio of the xanthan gum to the acetylene black to be 1:1, adding the ordering regulator after ball milling for 5min, enabling the mass ratio of the xanthan gum solution to the ordering regulator to be 100:1, and then ball milling for 5min to obtain viscous slurry. Pouring the slurry into a mold, adjusting the temperature to-40 ℃ in a cold trap, keeping the temperature constant for 3 hours, transferring the slurry into a freeze dryer, adjusting the pressure to 5Pa, and keeping the pressure for 24 hours to ensure complete drying, thereby obtaining the carbon-based three-dimensional ordered current collector.
When graphite is used as an electrode material, only acetylene black is added in the preparation process of the current collector, and the graphite with the same quality is added, so that the graphite can be stably circulated for more than 1000 times when used as an electrode, and the graphite can exert the capacity of 360 mAh/g. Since no copper foil is used in the current collector, the reduction in electrode mass is more than 50%.
Example 3
A carbon-based three-dimensional ordered lithium ion battery current collector is prepared by firstly preparing a guanidine gum solution with the concentration of 1% and standing for swelling for 5 hours. Preparing a borax solution as an ordering regulator, wherein the concentration is 3%, the content of boron element is 1% in conversion, mixing a guanidine gum solution and acetylene black according to a mass ratio of 100:1.5, enabling the mass ratio of guanidine gum to acetylene black to be 1:1, adding the ordering regulator after ball milling for 5min, enabling the mass ratio of the guanidine gum solution to the ordering regulator to be 100:1.5, and then ball milling for 5min to obtain viscous slurry. Pouring the slurry into a mold, adjusting the temperature to-40 ℃ in a cold trap, keeping the temperature constant for 3 hours, transferring the slurry into a freeze dryer, adjusting the pressure to 5Pa, and keeping the pressure for 24 hours to ensure complete drying, thereby obtaining the carbon-based three-dimensional ordered current collector.
When graphite is used as an electrode material, only acetylene black is added in the preparation process of the current collector, and the graphite with the same quality is added, so that the graphite can be stably circulated for more than 1000 times when used as an electrode, and the graphite can exert the capacity of 360 mAh/g. Since no copper foil is used in the current collector, the reduction in electrode mass is more than 50%. The electrode material is selected for lithium ion batteries.
Example 4
A carbon-based three-dimensional ordered lithium ion battery current collector is prepared by firstly preparing a xanthan gum solution with the concentration of 0.5 percent and standing for swelling for 4 hours. Preparing a borax solution as an ordering regulator, wherein the concentration is 3.5%, the content of boron element is 0.4% in conversion, mixing a xanthan gum solution and super-p according to a mass ratio of 100:0.5, enabling the mass ratio of the xanthan gum to the super-p to be 1:1, adding the ordering regulator after ball milling for 5min, enabling the mass ratio of the xanthan gum solution to the ordering regulator to be 100:2, and then ball milling for 5min to obtain viscous slurry. Pouring the slurry into a mold, adjusting the temperature to-40 ℃ in a cold trap, keeping the temperature constant for 3 hours, transferring the slurry into a freeze dryer, adjusting the pressure to 5Pa, and keeping the pressure for 12 hours to ensure complete drying, thereby obtaining the carbon-based three-dimensional ordered current collector.
When the nano Fe is required3O4When the Fe-P-Fe-B alloy is used as an electrode material, only the super-p is added in the preparation process of a current collector, and the nano Fe with the same mass is added3O4And (4) finishing. The electrode material is selected for lithium ion batteries.
The foregoing is a more detailed description of the invention and it is not intended that the invention be limited to the specific embodiments described herein, but that various modifications, alterations, and substitutions may be made by those skilled in the art without departing from the spirit of the invention, which should be construed to fall within the scope of the invention as defined by the appended claims.
Claims (8)
1. A carbon-based three-dimensional ordered lithium ion battery current collector is characterized in that: the current collector consists of a polymer carrier, an order regulator and conductive particles; wherein the polymer carrier is natural vegetable gum, the mass ratio of the natural vegetable gum to the conductive particles is 1:1, and the mass ratio of the natural vegetable gum to the ordering regulator is 100 (1-2);
the natural vegetable gum is natural vegetable gum with nonionic characteristics and is selected from guanidine gum or xanthan gum; the order regulator is a cross-linking agent with reversible cross-linking capability on natural vegetable gum, and is selected from borax or an organic boron cross-linking agent.
2. The current collector of claim 1, wherein the conductive particles are carbon powder selected from super-p or acetylene black.
3. A preparation method of a carbon-based three-dimensional ordered lithium ion battery current collector is characterized by comprising the following steps: the method comprises the following steps:
the method comprises the following steps: firstly, preparing a natural plant gum solution, standing and swelling for later use after the preparation is finished; preparing a boron-containing order regulator solution;
step two: mixing the natural vegetable gum solution with the conductive particles to ensure that the mass ratio of the natural vegetable gum to the conductive particles is 1:1, and then performing ball milling to obtain mixed liquid;
step three: adding an ordering regulator into the mixed liquid obtained in the step two to ensure that the mass ratio of the natural vegetable gum solution to the ordering regulator solution is 100 (1-2), and then performing ball milling to obtain viscous slurry;
step four: pouring the slurry obtained in the step three into a mold, transferring to a cold trap, cooling to-40 ℃, carrying out constant temperature treatment, and transferring to a freeze dryer to ensure complete drying to obtain a carbon-based three-dimensional ordered current collector;
the natural vegetable gum solution is natural vegetable gum with non-ionic characteristics, and is selected from guanidine gum or xanthan gum;
the order regulator is a cross-linking agent with reversible cross-linking capability on natural vegetable gum, and is selected from borax or an organic boron cross-linking agent.
4. The method for preparing the current collector of the carbon-based three-dimensional ordered lithium ion battery according to claim 3, wherein the conductive particles are carbon powder selected from super-p or acetylene black.
5. The preparation method of the carbon-based three-dimensional ordered lithium ion battery current collector according to claim 3, wherein the concentration of the natural vegetable gum solution is 0.5-2%; the content of boron element in the ordering regulator solution is 0.4-2%.
6. The preparation method of the current collector of the carbon-based three-dimensional ordered lithium ion battery according to claim 3, wherein in the fourth step, the temperature is kept constant in a cold trap for 3 hours; adjusting the pressure in the freeze dryer to 5-10Pa, and the duration is 12-24 h.
7. A lithium ion battery based on the carbon-based three-dimensional ordered lithium ion battery current collector of claim 1, wherein an electrode material having the same mass as the conductive fine particles is added to the current collector.
8. The lithium ion battery based on the carbon-based three-dimensional ordered lithium ion battery current collector of claim 7, wherein the electrode material is nano Fe3O4Or graphite.
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN106328940A (en) * | 2016-09-21 | 2017-01-11 | 南昌大学 | Method for preparing high-porosity carbon-based current collector anode pieces of lithium ion batteries |
| JP2017224407A (en) * | 2016-06-13 | 2017-12-21 | 東洋インキＳｃホールディングス株式会社 | Conductive composition, backing layer-attached current collector for nonaqueous electrolyte secondary battery, electrode for nonaqueous electrolyte secondary battery, and nonaqueous electrolyte secondary battery |
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| WO2015127224A1 (en) * | 2014-02-21 | 2015-08-27 | Hercules Incorporated | Cross-linked binder for lithium ion batteries |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| JP2017224407A (en) * | 2016-06-13 | 2017-12-21 | 東洋インキＳｃホールディングス株式会社 | Conductive composition, backing layer-attached current collector for nonaqueous electrolyte secondary battery, electrode for nonaqueous electrolyte secondary battery, and nonaqueous electrolyte secondary battery |
| CN106328940A (en) * | 2016-09-21 | 2017-01-11 | 南昌大学 | Method for preparing high-porosity carbon-based current collector anode pieces of lithium ion batteries |
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