CN113036147B - Composite binder system suitable for silicon-containing battery, preparation method and application - Google Patents

Composite binder system suitable for silicon-containing battery, preparation method and application Download PDF

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CN113036147B
CN113036147B CN202110327831.XA CN202110327831A CN113036147B CN 113036147 B CN113036147 B CN 113036147B CN 202110327831 A CN202110327831 A CN 202110327831A CN 113036147 B CN113036147 B CN 113036147B
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binder
silicon
modulus
composite
stirring
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CN113036147A (en
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韩帅帅
张越超
高秀玲
从长杰
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Tianjin EV Energies Co Ltd
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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
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • H01M4/621—Binders
    • 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
    • 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
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • H01M4/621—Binders
    • H01M4/622—Binders being polymers
    • 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
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • H01M4/624—Electric conductive fillers
    • 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
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • H01M4/624—Electric conductive fillers
    • H01M4/625—Carbon or graphite
    • 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

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Abstract

The invention provides a composite binder system suitable for a silicon-containing battery, a preparation method and application thereof, wherein the composite binder system comprises a high-strength high-modulus binder, a flexible binder, a system stabilizer and an electron directing agent. The composite binder system disclosed by the invention is added with at least one flexible binder and one system stabilizer besides the high-strength high-modulus binder, so that the binding effect of silicon is ensured, the processing characteristics of the system are improved, wrinkles, edge material falling and the like are avoided, a good electronic path is formed in the system, the electric connection of the whole system is ensured, and the impedance of a battery is reduced.

Description

Composite binder system suitable for silicon-containing battery, preparation method and application
Technical Field
The invention belongs to the field of battery production processes, and particularly relates to a composite binder system suitable for a silicon-containing battery, a preparation method and application.
Background
With the development of new energy automobiles, the existing power battery system cannot meet the requirements of high-endurance, high-safety and quick-charging new energy automobiles. Particularly, the theoretical capacity of the graphite system commonly used at present is only 372mAh/g, and the improvement of the energy density of the power battery is greatly limited. The theoretical capacity of silicon can reach 4200mAh/g, so that the silicon-based material becomes a next generation negative extremely high potential material and is expected to present explosive application. However, the silicon material is different from graphite in intrinsic characteristics, and the material is easy to pulverize due to huge volume expansion in the charging and discharging processes, so that the electric connection is easily lost in a pole piece, and the battery is rapidly disabled. The expansion characteristics of silicon limit the use of silicon-based materials in lithium ion batteries. The current industry uses a novel binder, namely a high-strength high-modulus binder to restrict the expansion of silicon and improve the overall performance of the battery. However, the high-strength high-modulus adhesive has many problems in practical use, and a pole piece made of the adhesive is hard and brittle, is easy to wrinkle, is easy to drop materials at the edge, is difficult to process and is not easy to use in a large scale. The prepared battery has high internal resistance and high impedance.
Disclosure of Invention
In view of the above, the present invention is directed to a composite binder system for silicon-containing batteries, a preparation method and an application thereof, so as to inhibit the expansion of silicon, improve the processing characteristics of the system and reduce the internal resistance of the system.
In order to achieve the purpose, the technical scheme of the invention is realized as follows:
a composite adhesive system suitable for silicon-containing batteries comprises a high-strength high-modulus adhesive, a flexible adhesive, a system stabilizer and an electron guiding agent.
Preferably, the high-strength and high-modulus binder comprises one or more of PAM (polyacrylamide), PAN (polyacrylonitrile), PAA (polyacrylic acid), PMMA (polymethyl methacrylate), PI (polyimide), and modifications thereof.
Preferably, the flexible binder includes one or more of SBR (styrene butadiene rubber), PVDF (polyvinylidene fluoride), PTFE (polytetrafluoroethylene), and modifications thereof.
Preferably, the system stabilizer comprises CMC (carboxymethyl cellulose) or a CMC (carboxymethyl cellulose) modification.
Preferably, the electron guide agent includes one or more of carbon nanotubes, carbon nanofibers, graphene, polythiophene, and polypyrrole.
A method of making a composite binder system suitable for use in a silicon-containing battery, comprising the steps of:
(1) Mixing and stirring part of the high-strength high-modulus binder and all the electron guide agent to form a conductive-binder mixed solution;
(2) adding a system stabilizer and a negative main material into the conductive-binder mixed solution, and stirring to obtain first pre-slurrying;
(3) adding the rest high-strength high-modulus binder into the first pre-pulping, and stirring to obtain a second pre-pulping;
(4) and adding the flexible adhesive into the second pre-pulping and stirring to obtain the required composite adhesive system.
Preferably, the dosage ratio of the high-strength high-modulus binder, the electron directing agent, the system stabilizer and the flexible binder is 20:1:5: 15.
Preferably, the stirring speed in step (1) is 3000r/min 2500-.
A battery comprising a composite binder system as described in any preceding claim suitable for use in a silicon-containing battery.
A preparation method of a battery comprises the steps of homogenizing, coating, rolling, slitting, die cutting, laminating, welding, packaging, injecting liquid, pre-filling, corner shearing, air exhausting and capacity grading, wherein the homogenizing comprises any one of the preparation methods of the composite binder system suitable for the silicon-containing battery.
Compared with the prior art, the composite binder system suitable for the silicon-containing battery, the preparation method and the application have the following advantages:
(1) the composite binder system disclosed by the invention is added with at least one flexible binder and one system stabilizer besides the high-strength high-modulus binder, so that the binding effect of silicon is ensured, the processing characteristic of the system is improved, and wrinkles, edge falling and the like are avoided;
(2) the composite binder system disclosed by the invention is added with a special electronic guiding agent, a good electronic path is formed in the system, the electric connection of the whole system is ensured, and the impedance of the battery is reduced.
Drawings
The accompanying drawings, which are incorporated in and constitute a part of this specification, illustrate an embodiment of the invention and, together with the description, serve to explain the invention and not to limit the invention. In the drawings:
FIG. 1 is a schematic structural view of a pole piece prepared in comparative example 2 of the present invention;
fig. 2 is a schematic structural diagram of a pole piece prepared in embodiment 1 of the present invention.
Detailed Description
Unless defined otherwise, technical terms used in the following examples have the same meanings as commonly understood by one of ordinary skill in the art to which the present invention belongs. The test reagents used in the following examples, unless otherwise specified, are all conventional biochemical reagents; the experimental methods are conventional methods unless otherwise specified.
The present invention will be described in detail with reference to the following examples and accompanying drawings.
Comparative example 1 the homogenization procedure was as follows: at room temperature, 60% of CMC and 100% of ordinary conductive agent sp are added into a homogenizing tank and stirred, and the mixture is stirred for 60min at the rotating speed of 3000r/min to form a conductive-adhesive mixed solution. Adding the main material of the active substance, stirring for 150min at the rotating speed of 2500r/min, adding the rest 40% of the CMC into a homogenizing tank, stirring for 90min at the rotating speed of 3000r/min, adding 100% of the SBR after the viscosity and the solid content are proper, stirring uniformly at the rotating speed of 600r/min for 30min, and taking out of the tank for coating. Wherein the use amounts of the CMC as the system stabilizer and the SBR as the flexible binder are respectively 1.5 percent and 2.5 percent. The coating effect is good, and the edge has no folds. After the electricity core preparation was accomplished, charge to the state of full electricity with electric core, disassemble electric core, measure the thickness of negative pole piece under the full electricity state, compare with the thickness when initially rolling, reach negative pole full electricity inflation 42%.
Comparative example 2 the homogenization procedure was as follows: at room temperature, 50% of high-strength high-modulus binder PAA and 100% of common conductive agent sp are added into a homogenizing tank and stirred, and the mixture is stirred for 90min at the rotating speed of 2800r/min to form conductive-binder mixed solution. Adding active substance main material, stirring at 2000r/min for 180min, adding the rest 50% of high-strength high-modulus binder PAA into a homogenizing tank, stirring at 2500r/min for 120min, adjusting viscosity and solid content with solvent, and coating. Wherein the dosage of the high-strength and high-modulus binder PAA is 4 percent. The coating effect is poor, and the edge has obvious wrinkles. After the electricity core preparation was accomplished, charge to the state of full electricity with electric core, disassemble electric core, measure the thickness of negative pole piece under the full electricity state, compare with the thickness when initially rolling, reachs the full electricity inflation of negative pole 31%.
Comparative example 3 the homogenization procedure was as follows: at room temperature, 50% of high-strength high-modulus binder PAA and 100% of common conductive agent sp are added into a homogenizing tank and stirred, and the mixture is stirred for 90min at the rotating speed of 2800r/min to form conductive-binder mixed solution. And adding an active substance main material, stirring for 150min at the rotating speed of 3000r/min, adding the remaining 50% of the high-strength high-modulus binding agent PAA into a homogenizing tank, stirring for 130min at the rotating speed of 2800r/min, adjusting the viscosity and the solid content by using a solvent, adding 100% of flexible binding agent SBR after the viscosity and the solid content are proper, stirring uniformly for 30min at the rotating speed of 600r/min, and taking out of the tank for coating. Wherein the dosage of the high-strength and high-modulus binder PAA and the dosage of the flexible binder SBR are respectively 3 percent and 1 percent. The coating effect is good, and the edge has no folds. After the electricity core preparation was accomplished, charge to the state of full electricity with electric core, disassemble electric core, measure the thickness of negative pole piece under the full electricity state, compare with the thickness when rolling initially, reachs negative pole full electricity inflation 33%.
Comparative example 4 the homogenization procedure was as follows: at room temperature, 50% of high-strength high-modulus binder PAA and 100% of common conductive agent sp are added into a homogenizing tank and stirred, and the mixture is stirred for 90min at the rotating speed of 2800r/min to form conductive-binder mixed solution. Adding an active substance main material and 100% of system stabilizer CMC, stirring for 200min at the rotating speed of 2500r/min, adding the remaining 50% of high-strength high-modulus binder PAA into a homogenizing tank, stirring for 90min at the rotating speed of 3000r/min, adjusting the viscosity and the solid content by using a solvent, adding 100% of flexible binder SBR after the viscosity and the solid content are proper, stirring for 30min at the rotating speed of 500r/min, uniformly stirring, and taking out of the tank for coating. Wherein the dosage of the high-strength and high-modulus binder PAA, the dosage of the system stabilizer CMC and the dosage of the flexible binder SBR are respectively 2 percent, 0.5 percent and 1.5 percent. The coating effect is good, and the edge has no folds. After the electricity core preparation was accomplished, charge to the state of full electricity with electric core, disassemble electric core, measure the thickness of negative pole piece under the full electricity state, compare with the thickness when the initial rolling, reachs negative pole full electricity inflation 35%.
Example 1 homogenization procedure was as follows: at room temperature, 50% of high-strength high-modulus binder PAA, 100% of electron-guiding agent single-walled carbon nanotube and 100% of common conductive agent sp are added into a homogenizing tank and stirred, and the mixture is stirred for 120min at the rotating speed of 3000r/min to form conductive-binder mixed solution. Adding an active substance main material and 100% of system stabilizer CMC, stirring for 200min at the rotating speed of 2500r/min, adding the remaining 50% of high-strength high-modulus binder PAA into a homogenizing tank, stirring for 120min at the rotating speed of 2800r/min, adjusting the viscosity and the solid content by using a solvent, adding 100% of flexible binder SBR after the viscosity and the solid content are proper, stirring uniformly at the rotating speed of 600r/min for 30min, and taking out of the tank for coating. Wherein the dosage of the high-strength and high-modulus binder PAA, the dosage of the electron guiding agent single-walled carbon nanotube, the dosage of the system stabilizer CMC and the dosage of the flexible binder SBR are respectively 2 percent, 0.1 percent, 0.5 percent and 1.5 percent. The coating effect is good, and the edge has no folds. After the electricity core preparation was accomplished, charge to the state of full electricity with electric core, disassemble electric core, measure the thickness of negative pole piece under the full electricity state, compare with the thickness when the initial rolling, reachs negative pole full electricity inflation 35%.
Example 2 homogenization procedure was as follows: at room temperature, 50% of high-strength high-modulus binder PAA-PAN copolymer, 100% of electronic directing agent single-walled carbon nanotube and 100% of common conductive agent sp are added into a homogenizing tank to be stirred, and the mixture is stirred for 150min at the rotating speed of 3000r/min to form conductive-binder mixed solution. Adding an active substance main material and 100% of system stabilizer CMC, stirring for 150min at the rotating speed of 2800r/min, adding the remaining 50% of high-strength high-modulus binder PAA into a homogenizing tank, stirring for 150min at the rotating speed of 2500r/min, adjusting the viscosity and the solid content by using a solvent, adding 100% of flexible binder SBR after the viscosity and the solid content are proper, stirring for 30min at the rotating speed of 600r/min, uniformly stirring, and taking out of the tank for coating. Wherein the dosage of the high-strength and high-modulus binder PAA-PAN copolymer, the dosage of the electron guide agent single-walled carbon nanotube, the dosage of the system stabilizer CMC and the dosage of the flexible binder SBR are respectively 2%, 0.1%, 0.5% and 1.5%. The coating effect is good, and the edge has no folds. After the electricity core preparation was accomplished, charge to the state of full electricity with electric core, disassemble electric core, measure the thickness of negative pole piece under the full electricity state, compare with the thickness when the initial rolling, reachs negative pole full electricity inflation 34%.
The compositions and performance parameters of comparative examples 1-4 and examples 1-2 are shown in Table 1:
Figure BDA0002995285730000061
TABLE 1 Binder System and negative Pole piece Performance parameters
In the homogenizing process of the system, the high-strength high-modulus binder and the electronic guiding agent are mixed and stirred to form conductive slurry, and at the moment, the high-strength high-modulus binder and the electronic guiding agent are combined together in various modes such as crosslinking, adsorption, bridging, winding and the like to form a stable conductive-binder network, wherein the network forms a main body of the bound silicon material, so that high binding force is ensured, and high conductivity is also ensured. And finally, adding a flexible binder, and connecting the flexible binder into the previously formed conductive-binder network, thereby improving the subsequent processing performance.
The preparation process of the power battery comprises the processes of homogenizing, coating, rolling, slitting, die cutting, laminating, welding, packaging, injecting liquid, pre-filling, corner shearing, air suction, capacity grading and the like. The specific homogenization procedure is as follows: firstly, adding a part of high-strength high-modulus binder and an electronic guiding agent into a homogenizing tank, stirring to form a conductive-binder network, then adding a part of negative main material and a system stabilizer into the homogenizing tank, stirring for a period of time, then adding the rest of high-strength high-modulus binder and negative main material into the homogenizing tank, stirring, adding a flexible binder after the viscosity and the solid content are suitable, stirring uniformly, and taking out of the tank for coating. Compared with the embodiment 1, the scheme of only adding the high-strength high-modulus adhesive in the comparative example 2 has obviously different coating effects, the edge of the scheme of only adding the high-strength high-modulus adhesive has obvious wrinkles during coating, and as shown in fig. 1, the manufactured pole piece is a defective product. While example 1 coated with good edge without wrinkles as shown in fig. 2.
The above description is only for the purpose of illustrating the preferred embodiments of the present invention and is not to be construed as limiting the invention, and any modifications, equivalents, improvements and the like that fall within the spirit and principle of the present invention are intended to be included therein.

Claims (7)

1. A preparation method of a composite binder system suitable for a silicon-containing battery is characterized by comprising the following steps: the composite binder system comprises a high-strength high-modulus binder, a flexible binder, a system stabilizer and an electron directing agent, wherein the system stabilizer comprises CMC or a CMC modifier,
the preparation method comprises the following steps:
(1) mixing and stirring part of the high-strength high-modulus binder and all the electron guide agent to form a conductive-binder mixed solution;
(2) adding a system stabilizer and a negative main material into the conductive-binder mixed solution, and stirring to obtain first pre-slurrying;
(3) adding the rest high-strength high-modulus binder into the first pre-pulping, and stirring to obtain a second pre-pulping;
(4) adding the flexible adhesive into the second pre-pulping and stirring to obtain a required composite adhesive system,
the high-strength high-modulus binder comprises one or more of PAM, PAN, PAA, PMMA, PI and a modifier of the high-strength high-modulus binder.
2. The method of claim 1, wherein the composite binder system comprises: the flexible binder comprises one or more of SBR, PVDF, PTFE and a modified substance of the flexible binder.
3. The method of claim 1, wherein the composite binder system for silicon-containing batteries is prepared by: the electron guiding agent comprises one or more of carbon nano tubes, carbon nano fibers, graphene, polythiophene and polypyrrole.
4. The method of claim 1, wherein the composite binder system for silicon-containing batteries is prepared by: the dosage ratio of the high-strength high-modulus binder, the electronic guiding agent, the system stabilizer and the flexible binder is 20: 1: 5: 15.
5. The method of claim 1, wherein the composite binder system for silicon-containing batteries is prepared by: the stirring speed in the step (1) is 2500-.
6. A battery comprising a composite binder system suitable for use in a silicon-containing battery prepared by the method of any one of claims 1 to 5.
7. A preparation method of a battery comprises the steps of homogenizing, coating, rolling, slitting, die cutting, laminating, welding, packaging, injecting liquid, pre-filling, corner shearing, air exhausting and capacity grading, and is characterized in that: the homogenate comprising a method of preparing a composite binder system suitable for use in a silicon-containing cell as claimed in any one of claims 1 to 5.
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Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN104766944A (en) * 2015-03-30 2015-07-08 深圳市斯盛能源股份有限公司 Lithium ion secondary battery negative pole piece and preparation method thereof
CN109244386A (en) * 2018-08-17 2019-01-18 广西卓能新能源科技有限公司 A kind of siliceous lithium battery of high-energy and preparation method
CN111834623A (en) * 2020-07-27 2020-10-27 江西远东电池有限公司 Homogenizing method of lithium ion battery silicon-based negative electrode slurry
US10840512B1 (en) * 2019-12-18 2020-11-17 Enevate Corporation Method and system for multiple carbon precursors for enhanced battery electrode robustness

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN104766944A (en) * 2015-03-30 2015-07-08 深圳市斯盛能源股份有限公司 Lithium ion secondary battery negative pole piece and preparation method thereof
CN109244386A (en) * 2018-08-17 2019-01-18 广西卓能新能源科技有限公司 A kind of siliceous lithium battery of high-energy and preparation method
US10840512B1 (en) * 2019-12-18 2020-11-17 Enevate Corporation Method and system for multiple carbon precursors for enhanced battery electrode robustness
CN111834623A (en) * 2020-07-27 2020-10-27 江西远东电池有限公司 Homogenizing method of lithium ion battery silicon-based negative electrode slurry

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