CN115403033B - Conductive agent for lithium ion battery, negative electrode and preparation method thereof, and lithium ion battery - Google Patents
Conductive agent for lithium ion battery, negative electrode and preparation method thereof, and lithium ion battery Download PDFInfo
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- H01M10/4235—Safety or regulating additives or arrangements in electrodes, separators or electrolyte
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Abstract
The invention provides a conductive agent for a lithium ion battery, a negative electrode, a preparation method and the lithium ion battery, wherein the conductive agent is a single-walled carbon nanotube network structure formed by self-assembly of pure single-walled carbon nanotubes under Van der Waals force, namely, the conductive agent only contains the component of the single-walled carbon nanotubes, and additives such as a dispersing agent and the like are not required to be added in the preparation process, so that the purity of the conductive agent is effectively ensured, and meanwhile, the preparation process of the conductive agent is simplified; when the conductive agent is used for a negative electrode for a lithium ion battery, even if negative electrode active materials and electrolyte are subjected to side reaction in the process of charging and discharging the electrode, SEI films are generated on the surface of the negative electrode, the conductive agent with a single-arm carbon nano tube network structure and the negative electrode active materials have good electric contact performance, so that the problems of conductivity reduction, loss of electric contact and the like caused by side reaction of the electrode (generation of SEI films) can be effectively relieved.
Description
Technical Field
The invention relates to the technical field of new energy materials and preparation thereof, in particular to a conductive agent for a lithium ion battery, a negative electrode, a preparation method and the lithium ion battery.
Background
Along with the increase of global energy shortage and environmental protection consciousness, new energy becomes an important development direction at present, and the lithium ion battery becomes a hot spot of the energy industry by virtue of the advantages of high working voltage, no memory effect, small self-discharge, long cycle life and the like, and is widely applied to mobile electronic products such as mobile phones, computers and the like.
Lithium ion batteryThe silicon (Si) -based negative electrode material has theoretical specific capacity far higher than that of graphite (the theoretical specific capacity of pure silicon is 4200mAh/g, and the theoretical specific capacity of graphite is 372 mAh/g), and is a lithium ion battery negative electrode material with great prospect. However, the silicon negative electrode material has low conductivity, and silicon will react with LiPF in the electrolyte 6 The components undergo side reactions to generate Li 2 SiF 6 Resulting in failure of the electrical contacts at the electrode level, ultimately resulting in capacity loss, limiting its cycling stability and service life.
The silicon-carbon negative electrode material for the lithium ion battery becomes the first choice negative electrode material of the lithium ion battery with high specific capacity, wide material source and the like, but if the carbon layer is not strictly coated, the growth of the solid electrolyte can be thicker, and the poor electronic conductivity and the high material expansion rate greatly prevent the lithium ion battery from exerting the circulation and multiplying power performance.
Therefore, it is necessary to alleviate the adverse effects of the negative electrode for lithium ion batteries on the battery, enhance the electrical contact ability of the electrode, and improve the initial efficiency of the battery.
Disclosure of Invention
Aiming at the problems in the prior art, the invention provides a conductive agent for a lithium ion battery, which is a reticular conductive agent formed by self-assembly of single-wall carbon nanotubes and is applied to the lithium ion battery, and solves the problems of low initial efficiency and poor cycle performance of the silicon-carbon negative electrode system of the existing lithium ion battery. In addition, due to the ultra-strong van der Waals force effect between the single-wall carbon nano tube and the negative silicon carbon active particles, the influence of side reaction on electric contact can be reduced, so that the method has wide application prospect in the electrochemical industry. On the other hand, the invention also provides a negative electrode for the lithium ion battery, a preparation method and the lithium ion battery.
The specific invention comprises the following steps:
in a first aspect, the present invention provides a conductive agent for a lithium ion battery, where the conductive agent is composed of single-walled carbon nanotubes; the shape of the conductive agent is a netlike single-walled carbon nanotube structure formed by self-assembly of single-walled carbon nanotubes.
Optionally, the pipe diameter of the single-walled carbon nanotube is 2-3nm, and the thickness of the reticular single-walled carbon nanotube structure is 3-10000nm.
Optionally, the sheet resistance of the reticular single-walled carbon nanotube structure is 10-50Ω.
In a second aspect, the present invention provides a negative electrode for a lithium ion battery, the negative electrode comprising a negative electrode active material and the conductive agent according to the first aspect.
Optionally, the negative active material includes silicon @ carbon or silicon oxide @ carbon.
In a third aspect, the present invention provides a method for preparing a negative electrode for a lithium ion battery according to the second aspect, the method comprising the steps of:
s1, self-assembling a single-wall carbon nano tube by virtue of Van der Waals force to form a net structure;
s2, contacting the reticular single-walled carbon nanotube structure with a negative electrode active material, wherein the reticular single-walled carbon nanotube structure is combined with the negative electrode active material by virtue of van der Waals acting force;
s3, rolling the material prepared in the step 2 and a current collector into a whole to prepare the negative electrode for the lithium ion battery.
In a fourth aspect, the present invention provides a lithium ion battery, which includes the negative electrode for a lithium ion battery according to the second aspect.
Compared with the prior art, the invention has the following advantages:
the conductive agent for the lithium ion battery is a net-shaped single-walled carbon nanotube structure formed by self-assembly of pure single-walled carbon nanotubes under the action of Van der Waals force, namely, the conductive agent only contains the single-walled carbon nanotubes, and additives such as dispersing agents and the like are not needed to be added in the preparation process. The preparation process of the conductive agent is simplified while the purity of the conductive agent is effectively ensured.
The negative electrode for the lithium ion battery comprises a negative electrode active material and the conductive agent, and the conductive agent (the single-arm carbon nano tube network structure) with a network structure and the silicon carbon negative electrode material have stronger van der Waals acting force, so that the conductive agent (the single-arm carbon nano tube network structure) can be self-assembled to form the negative electrode of the battery under the action of the van der Waals force after being contacted with the silicon carbon negative electrode active material, and the preparation process of the electrode is simplified. In addition, in the process of charging and discharging the electrode, even though side reaction occurs between the anode active material and the electrolyte, an SEI film is generated on the surface of the anode, and the conductive agent with a single-arm carbon nano-tube network structure and the anode active material have good electric contact performance, so that the problems of conductivity reduction, loss of electric contact and the like caused by side reaction of the electrode (generation of the SEI film) can be effectively relieved.
Drawings
In order to more clearly illustrate the embodiments of the present application or the technical solutions in the prior art, the drawings that are required in the embodiments or the description of the prior art will be briefly described below, it being obvious that the drawings in the following description are only some embodiments of the present application, and that other drawings may be obtained according to these drawings without inventive effort for a person skilled in the art.
FIG. 1 shows a scanning electron micrograph of a conductive agent provided by an embodiment of the present invention;
fig. 2 shows a flowchart of a preparation method of a negative electrode for a lithium ion battery according to an embodiment of the present invention;
fig. 3 shows cycle performance diagrams of lithium ion batteries provided in example 1 and comparative example of the present invention.
Detailed Description
The following examples are provided for a better understanding of the present invention and are not limited to the preferred embodiments described herein, but are not intended to limit the scope of the invention, any product which is the same or similar to the present invention, whether in light of the present teachings or in combination with other prior art features, falls within the scope of the present invention.
Specific experimental steps or conditions are not noted in the examples and may be performed in accordance with the operation or conditions of conventional experimental steps described in the prior art in the field. The reagents used, as well as other instruments, are conventional reagent products available commercially, without the manufacturer's knowledge.
The existing conductive agent is usually stored and used in the form of conductive agent slurry, and the current carbon nanotube conductive agent for the lithium ion battery is not well dispersed due to large molecular acting force among carbon tubes, so that a plurality of additives such as dispersing agents and the like are required to be added in the preparation process of the conductive slurry, and the preparation difficulty and complexity of the conductive agent are increased to a certain extent. Meanwhile, the presence of the additive may increase the internal resistance (Re) and the charge transport resistance of the battery to some extent. Is unfavorable for the cycle and the first coulombic efficiency improvement of the battery.
In view of the above, a first object of the present invention is to provide a conductive agent for lithium ion batteries, the conductive agent having a composition of single-walled carbon nanotubes; the shape of the conductive agent is a netlike single-walled carbon nanotube structure formed by self-assembly of single-walled carbon nanotubes.
In specific implementation, the conductive agent is a single-wall carbon nanotube network structure formed by self-assembly of pure single-wall carbon nanotubes under van der Waals force, namely, the conductive agent only contains the single-wall carbon nanotubes, and the conductive agent and the single-wall carbon nanotubes are combined by physical force (van der Waals force), so that additives such as dispersing agents, binders and the like are not needed to be added in the preparation process. The preparation process of the conductive agent is simplified while the purity of the conductive agent is effectively ensured. Fig. 1 shows a scanning electron micrograph of a conductive agent provided in an embodiment of the present invention.
In some embodiments, the single-walled carbon nanotubes may have a tube diameter of 2-3nm and the reticulated single-walled carbon nanotube structure may have a thickness of 3-10000nm.
In some embodiments, the reticulated single-walled carbon nanotube structure has a sheet resistance of 10-50Ω.
A second object of the present invention is to provide a negative electrode for a lithium ion battery, which includes a negative electrode active material and the conductive agent described in the first aspect.
In specific implementation, the composition of the negative electrode for the lithium ion battery provided by the invention comprises the negative electrode active material and the conductive agent in the first aspect, and the conductive agent with a reticular structure (reticular single-arm carbon nano tube structure) and the silicon carbon negative electrode material have stronger van der Waals acting force, so that the conductive agent can be self-assembled to form the negative electrode of the battery under the van der Waals acting force after being contacted with the silicon carbon negative electrode active material, and the preparation process of the electrode is simplified. In addition, the single-walled carbon nanotube structure cannot be corroded by electrolyte, and in the cyclic charge and discharge process, even though negative electrode active materials and the electrolyte can generate side reaction, SEI films are generated on the surfaces of the negative electrodes, the problems of conductivity reduction, loss of electric contact and the like caused by electrode side reaction (SEI film generation) can be effectively relieved due to good electric contact performance between the conductive agents of the single-walled carbon nanotube network structure and the negative electrode active materials, and meanwhile, the electrodes still maintain good conductive and ionic capacities and can be endowed with certain flexibility.
In some embodiments, the negative electrode active material may be silicon @ carbon or silicon oxide @ carbon.
A third object of the present invention is to provide a method for preparing a negative electrode for a lithium ion battery according to the second aspect, fig. 2 shows a flowchart of a method for preparing a negative electrode for a lithium ion battery according to an embodiment of the present invention, and as shown in fig. 2, the method for preparing a negative electrode for a lithium ion battery includes the following steps:
s1, self-assembling a single-wall carbon nano tube by virtue of Van der Waals force to form a net structure;
s2, contacting the network structure formed by self-assembly of the single-walled carbon nanotubes with a negative electrode active material, wherein the network structure formed by self-assembly of the single-walled carbon nanotubes is combined with the negative electrode active material by virtue of van der Waals acting force;
s3, rolling the material prepared in the step 2 and a current collector into a whole to prepare the negative electrode for the lithium ion battery.
A fourth object of the present invention is a lithium ion battery including the negative electrode for a lithium ion battery according to the second aspect.
In specific implementation, the lithium ion battery provided by the invention has good electric contact performance between the conductive agent with the netlike single-arm carbon nanotube structure and the anode active material, and can effectively relieve the problems of conductivity reduction, loss of electric contact and the like caused by side reaction (generation of SEI film) between an electrode and electrolyte, thereby ensuring lower internal resistance (Re) and charge transmission resistance (Rct) of the battery, improving the cycle and first coulomb efficiency of the battery, and having wide application prospects in the electrochemical industry.
In order to make the present application more clearly understood to those skilled in the art, the conductive agent for lithium ion battery, the negative electrode and the preparation method thereof, and the lithium ion battery described in the present application will now be described in detail by the following examples.
Example 1
Self-assembling the single-wall carbon nano tube into a conductive network form by Van der Waals force at normal temperature;
binding silica @ carbon as an active component with a conductive network;
rolling the obtained material and a current collector into a whole, wherein the rolling thickness is 0.03mm, and preparing a pole piece;
assembling the obtained pole piece into a lithium ion battery;
electrochemical performance of the cells was tested using a LANDHE cell testing system and an electrochemical multifunction workstation (biological, VSP-300).
Example 2
The difference from example 1 is that: the active material is not silica @ carbon, but rather silicon @ carbon.
Comparative example 1
At normal temperature, commercial single-wall carbon nanotube slurry is mixed with a binder and silicon oxide@carbon in a certain ratio (5:5:90).
Coating and drying the copper foil current collector to obtain an electrode plate;
assembling a button cell;
electrochemical performance of the cells was tested using a LANDHE cell testing system and an electrochemical multifunction workstation (biological, VSP-300).
Fig. 3 shows cycle performance graphs of the lithium ion batteries provided in the embodiment 1 and the comparative example of the present invention, and as shown in fig. 3, the lithium ion battery provided in the embodiment 1 of the present invention uses a mesh-shaped single-arm carbon nanotube structure as a conductive agent, and in the comparative example, uses a single-wall carbon nanotube slurry as a conductive agent, and it can be seen that the cycle performance of the lithium ion battery provided in the embodiment 1 is significantly better than that of the comparative example 1.
Table 1 comparison of electrochemical properties of lithium ion batteries provided in example 1 and comparative example
| Battery cell | Example 1 | Contrast sample |
| First discharge capacity (mAh/g) | 1785.4 | 1513.6 |
| First coulombic efficiency (%) | 81.52 | 72.35 |
| Semi-cell internal resistance (omega) | 17.85 | 80.69 |
| Resistance to charge transfer (Ω) | 2.63 | 3.52 |
Table 1 shows the electrochemical performance results of the lithium ion batteries provided in example 1 and comparative example using the LANDHE battery test system and the electrochemical multifunctional workstation (biology, VSP-300), and as shown in table 1, the lithium ion battery provided in example 1 of the present invention using the single-arm carbon nanotube network structure as the conductive agent exhibited superior performance in terms of the first discharge capacity, the first coulombic efficiency, the half-cell internal resistance, and the charge transport resistance to the lithium ion battery using the single-wall carbon nanotube paste as the conductive agent in comparative example.
The invention has been described in detail with reference to the conductive agent for lithium ion battery, the negative electrode and the preparation method thereof, and the lithium ion battery, and specific examples are applied to illustrate the principle and the implementation of the invention, and the description of the examples is only used to help understand the method and the core idea of the invention; meanwhile, as those skilled in the art will have variations in the specific embodiments and application scope in accordance with the ideas of the present invention, the present description should not be construed as limiting the present invention in view of the above.
Claims (5)
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| US6790425B1 (en) * | 1999-10-27 | 2004-09-14 | Wiliam Marsh Rice University | Macroscopic ordered assembly of carbon nanotubes |
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| CN114944490A (en) * | 2022-01-21 | 2022-08-26 | 清华大学 | Integrated dry-process electrode material and preparation method thereof |
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