CN114204032B - Adhesive for lithium ion battery anode slurry - Google Patents
Adhesive for lithium ion battery anode slurry Download PDFInfo
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- CN114204032B CN114204032B CN202111610619.0A CN202111610619A CN114204032B CN 114204032 B CN114204032 B CN 114204032B CN 202111610619 A CN202111610619 A CN 202111610619A CN 114204032 B CN114204032 B CN 114204032B
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- component
- adhesive
- positive electrode
- formula
- lithium ion
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- 230000001070 adhesive effect Effects 0.000 title claims abstract description 40
- 239000000853 adhesive Substances 0.000 title claims abstract description 38
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 15
- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 15
- 239000006256 anode slurry Substances 0.000 title description 2
- 239000011267 electrode slurry Substances 0.000 claims abstract description 21
- 239000003795 chemical substances by application Substances 0.000 claims abstract description 8
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 claims description 25
- 239000003292 glue Substances 0.000 claims description 18
- 239000011230 binding agent Substances 0.000 claims description 13
- 229910052739 hydrogen Inorganic materials 0.000 claims description 9
- 239000001257 hydrogen Substances 0.000 claims description 9
- 125000004435 hydrogen atom Chemical group [H]* 0.000 claims description 9
- 125000000217 alkyl group Chemical group 0.000 claims description 6
- 125000003178 carboxy group Chemical group [H]OC(*)=O 0.000 claims description 4
- 239000007787 solid Substances 0.000 claims description 3
- 125000004093 cyano group Chemical group *C#N 0.000 claims description 2
- 125000001183 hydrocarbyl group Chemical group 0.000 claims description 2
- 125000002496 methyl group Chemical group [H]C([H])([H])* 0.000 claims description 2
- 125000001424 substituent group Chemical group 0.000 claims description 2
- 239000002002 slurry Substances 0.000 abstract description 12
- 230000015572 biosynthetic process Effects 0.000 abstract description 3
- 235000015110 jellies Nutrition 0.000 abstract description 3
- 239000008274 jelly Substances 0.000 abstract description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 abstract description 3
- 238000010521 absorption reaction Methods 0.000 abstract description 2
- 238000004062 sedimentation Methods 0.000 abstract description 2
- 239000002033 PVDF binder Substances 0.000 description 14
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 14
- 239000006245 Carbon black Super-P Substances 0.000 description 8
- 239000006258 conductive agent Substances 0.000 description 7
- 239000000203 mixture Substances 0.000 description 7
- 229910004764 HSV900 Inorganic materials 0.000 description 5
- 239000011248 coating agent Substances 0.000 description 4
- 238000000576 coating method Methods 0.000 description 4
- 238000003756 stirring Methods 0.000 description 4
- HFCVPDYCRZVZDF-UHFFFAOYSA-N [Li+].[Co+2].[Ni+2].[O-][Mn]([O-])(=O)=O Chemical compound [Li+].[Co+2].[Ni+2].[O-][Mn]([O-])(=O)=O HFCVPDYCRZVZDF-UHFFFAOYSA-N 0.000 description 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 2
- 229910012851 LiCoO 2 Inorganic materials 0.000 description 2
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 2
- 239000013543 active substance Substances 0.000 description 2
- 239000006185 dispersion Substances 0.000 description 2
- 239000011883 electrode binding agent Substances 0.000 description 2
- 229910052744 lithium Inorganic materials 0.000 description 2
- GELKBWJHTRAYNV-UHFFFAOYSA-K lithium iron phosphate Chemical compound [Li+].[Fe+2].[O-]P([O-])([O-])=O GELKBWJHTRAYNV-UHFFFAOYSA-K 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 2
- 239000007774 positive electrode material Substances 0.000 description 2
- 230000001105 regulatory effect Effects 0.000 description 2
- 230000000087 stabilizing effect Effects 0.000 description 2
- PXGOKWXKJXAPGV-UHFFFAOYSA-N Fluorine Chemical compound FF PXGOKWXKJXAPGV-UHFFFAOYSA-N 0.000 description 1
- NIXOWILDQLNWCW-UHFFFAOYSA-N acrylic acid group Chemical group C(C=C)(=O)O NIXOWILDQLNWCW-UHFFFAOYSA-N 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 239000004020 conductor Substances 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- QHGJSLXSVXVKHZ-UHFFFAOYSA-N dilithium;dioxido(dioxo)manganese Chemical compound [Li+].[Li+].[O-][Mn]([O-])(=O)=O QHGJSLXSVXVKHZ-UHFFFAOYSA-N 0.000 description 1
- 238000007580 dry-mixing Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000003912 environmental pollution Methods 0.000 description 1
- 239000011737 fluorine Substances 0.000 description 1
- 229910052731 fluorine Inorganic materials 0.000 description 1
- 229910021389 graphene Inorganic materials 0.000 description 1
- 229910000625 lithium cobalt oxide Inorganic materials 0.000 description 1
- DVATZODUVBMYHN-UHFFFAOYSA-K lithium;iron(2+);manganese(2+);phosphate Chemical compound [Li+].[Mn+2].[Fe+2].[O-]P([O-])([O-])=O DVATZODUVBMYHN-UHFFFAOYSA-K 0.000 description 1
- BFZPBUKRYWOWDV-UHFFFAOYSA-N lithium;oxido(oxo)cobalt Chemical compound [Li+].[O-][Co]=O BFZPBUKRYWOWDV-UHFFFAOYSA-N 0.000 description 1
- 230000014759 maintenance of location Effects 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 238000000034 method Methods 0.000 description 1
- 229920000915 polyvinyl chloride Polymers 0.000 description 1
- 239000004800 polyvinyl chloride Substances 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- 238000011084 recovery Methods 0.000 description 1
- 239000002904 solvent Substances 0.000 description 1
- 238000003860 storage Methods 0.000 description 1
- 238000004804 winding Methods 0.000 description 1
Classifications
-
- 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
- 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
- H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
- H01M2004/028—Positive electrodes
Landscapes
- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Manufacturing & Machinery (AREA)
- Battery Electrode And Active Subsutance (AREA)
Abstract
The invention discloses an adhesive for positive electrode slurry of a lithium ion battery, which comprises a component A serving as a main adhesive and a component B serving as a flexible agent, wherein the component A is shown as a formula (I),The component B is shown as a formula (II) or a formula (III),The adhesive is oily and fluorine-free, has the advantages of small adhesive dosage, stable slurry, difficult water absorption and jelly formation or sedimentation, and has the advantages of good flexibility and low battery impedance after being used for pole pieces.
Description
Technical Field
The invention relates to an adhesive, in particular to an adhesive for positive electrode slurry of a lithium ion battery.
Background
Since the application of the invention to lithium ion batteries in the 90 s of the last century, the binder in the positive electrode has been essentially polyvinylidene fluoride (PVDF). With the rapid development of lithium ion batteries, the demand for PVDF has increased dramatically, but PVDF has good adhesive properties, but because of fluorine, the production process is very serious to environmental pollution and is very unfavorable to human and other animal health.
In recent years, attempts have been made to develop aqueous acrylic positive electrode binders, but since the lithium battery performance is most susceptible to moisture, and the positive electrode materials are mostly hydrolyzed to some extent; the pole piece made of the water-based positive electrode binder is very hard, and is also greatly limited in winding process. So the positive electrode aqueous binder is also hardly popularized at present.
Disclosure of Invention
The invention aims to solve the technical problem of providing a novel adhesive which is an oily fluorine-free adhesive, is environment-friendly and is beneficial to popularization and application while ensuring good adhesive effect.
The invention discloses an adhesive for positive electrode slurry of a lithium ion battery, which comprises a component A serving as a main adhesive and a component B serving as a flexible agent,
The component A is shown as a formula (I),
In formula (I), R1 is selected from hydrogen, methyl, -COOR, linear or branched alkyl of C1-C50000 with-CN and/or-COOR 'substituents, R, R' are each independently selected from hydrogen, linear or branched alkyl of C1-C100; r2 is selected from hydrogen, C1-C100 linear or branched alkyl; x and z are natural numbers, and y is 0 or a natural number;
The component B is shown as a formula (II) or a formula (III),
In the formula (III), R3 and R4 are independently selected from hydrogen, -CN, -COOH, C1-C100 straight-chain or branched hydrocarbon groups with-CN and/or-COOH, and in the formula (II), m and n are natural numbers;
the component A accounts for 20-98% of the total mass of the adhesive, and the component B accounts for 2-80% of the total mass of the adhesive.
Further, the relative molecular weight of the component A is 30-180 ten thousand, and the relative molecular weight of the component B is 3-50 ten thousand.
Further, when the adhesive is used for preparing positive electrode slurry, the component A is directly added in a solid state or is added after being prepared into a glue solution, and the component B is added after being prepared into the glue solution.
Further, the component A or the component B is prepared into a glue solution by using N-methyl pyrrolidone.
The component A of the invention is a main binder, and the component B is a flexible agent, and can be added in two ways when the component A is used for preparing the positive electrode slurry of the lithium ion battery: 1. after the component A, the conductive agent and the positive electrode active material are fully dispersed and mixed, adding a solvent NMP (N-methyl pyrrolidone), adjusting the fluidity, adding a flexible agent component which is dissolved into glue solution by NMP, stirring, and adjusting the proper viscosity by NMP, thus being capable of being coated on the positive electrode plate. 2. Firstly dissolving the component A into glue solution by using NMP, then adding a conductive agent and a positive electrode active substance, adding proper NMP according to the requirement, fully dispersing, adding a flexible agent component which is dissolved into glue solution by using NMP, stirring, and adjusting proper viscosity by using NMP, thus being capable of being coated on a positive electrode plate.
The conductive agent is conductive material used in conventional lithium ion battery systems such as conductive carbon black, graphene, conductive carbon tube CNT and the like; the active substance can be one or a mixture of a plurality of lithium cobaltate, nickel cobalt lithium manganate ternary material, lithium manganate, lithium iron phosphate and lithium manganese iron phosphate.
The adhesive main body is made of two-component materials, wherein the component A serving as a main adhesive plays a main role in stabilizing slurry in positive electrode slurry and plays a main role in bonding in a pole piece; the component B serving as the flexible agent plays an auxiliary role in stabilizing slurry in the positive electrode slurry, and mainly improves the flexibility of the pole piece in the pole piece and has an auxiliary binding effect. The component A and the component B synergistically form the oily fluorine-free adhesive. The modified polyvinyl chloride positive electrode slurry is used in positive electrode slurry of a lithium ion battery, has the advantages of small binder dosage (only 40-60% of PVDF HSV900 dosage is needed to be added), stable slurry, difficult water absorption and jelly formation or sedimentation, and good flexibility and low battery impedance after being used in a pole piece. The preparation process is environment-friendly, and has great value in popularization and application. To date, oily fluorine-free adhesives have not been disclosed.
Drawings
Fig. 1 is a schematic diagram of experimental results of charge and discharge cycle with 1C current after further obtaining a positive electrode sheet for a lithium ion battery using the battery positive electrode slurry prepared by the adhesive of example 1 of the present invention.
Detailed Description
The invention is further explained below with reference to examples. The following examples are only illustrative of the present invention and are not intended to limit the scope of the invention.
Example 1
Nickel cobalt lithium manganate NCM622 system positive electrode slurry:
Dry matter mass ratio according to NCM622: super-P (conductive carbon black): binder = 97.3:1.6:1.1 (wherein the mass of component A and component B in the adhesive each account for 98% and 2% of the total mass of the adhesive).
In this embodiment, component A has the formula shown below, R1 is hydrogen, and R2 is-C 2H5:
The structural formula of the component B is shown as follows:
the component A is dissolved by NMP to prepare a glue solution with the mass concentration of about 4%, then the conductive agent Super-P and NCM622 with the formula amount and proper NMP are added according to the conventional component dosage of the positive electrode slurry, after the mixture is fully dispersed, the flexible agent component glue solution dissolved in NMP is added, and after the mixture is uniformly stirred, the viscosity of the slurry is regulated to be proper by NMP, so that the mixture is used for coating a pole piece and assembling a battery.
Test results:
Under the relative humidity RH60%, the slurry of the sample system is stable, the solid content is 78.5% (mass percent) and the viscosity is 7500mPa.s; and the bonding force of PVDF HSV900 adhesive system with the added amount of PVDF of 1.8 percent (mass percent) can be ensured, and the slurry is placed for two hours to generate the phenomenon of jelly formation.
The adhesive force of the pole piece of the tested system is normal, and powder cannot fall off when the pole piece passes through a round bar with the diameter of 2 mm; the obtained pole piece has good flexibility; the battery charge-discharge cycle is as shown in fig. 1 (charge-discharge curves almost overlap), normal; the storage is carried out at 70 ℃ for 48 hours, the capacity retention rate is 99.3%, and the capacity recovery rate is 99.9%.
Example 2
Nickel cobalt lithium manganate NCM622 system positive electrode slurry:
Dry matter mass ratio according to NCM622: super-P: binder = 97.3:1.6:1.1 (wherein the mass of the component A and the mass of the component B in the adhesive respectively account for 60% and 40% of the total mass of the adhesive).
In this example, component A has the following structural formula, R1 is- (CH 2)4 CN) and R2 is-CH 3:
The structural formula of the component B is as follows, R3 is- (CH 2)2 CN), and R4 is-C 4H9:
The component A is dissolved by NMP to prepare a glue solution with the mass concentration of about 4%, then the conductive agent Super-P and NCM622 with the formula amount and proper NMP are added according to the conventional component dosage of the positive electrode slurry, after the mixture is fully dispersed, the glue solution of the component B dissolved in NMP is added, and after the mixture is uniformly stirred, the viscosity of the slurry is adjusted to be proper by NMP, so that the mixture is used for coating a pole piece and assembling a battery. The test comparison results are comparable to example 1.
Example 3
High-voltage lithium cobalt oxide LiCoO 2 system positive electrode slurry:
Dry matter mass ratio is LiCoO 2: super-P: binder = 97.6:1.5:0.9 (wherein the mass of component A and component B in the adhesive each account for 90% and 10% of the total mass of the adhesive).
In this example, component A has the following structural formula, R1 is-CH 2 CHCN(CH2)2 CN, and R2 is-C 3H7:
The structural formula of the component B is as follows, R3 is H, and R4 is- (CH 2)2 CN):
Adding the component A, the conductive agent Super-P and the NCM622 into a stirrer, dry-mixing uniformly, gradually and properly adding NMP, adding the glue solution of the component B dissolved in NMP when the slurry has fluidity after full dispersion, stirring uniformly, and then adjusting the viscosity of the slurry to be proper by NMP for coating the pole piece and assembling the battery.
The control group was PVDF HSV900. Test results are compared, and the slurry and pole piece data are shown in the following table:
It can be seen that the binder addition of the present invention is less than that of PVDF addition, and the peel force of the pole piece is higher than that of the PVDF group.
The battery performance data tested were as follows:
| positive electrode adhesive | Capacity/mAh | Gram Capacity/mAh/g | Internal resistance/mΩ | Average cell thickness/mm |
| A+B | 3150 | 165.3 | 27.9 | 4.08 |
| PVDF HSV900 | 3135 | 165.1 | 27.1 | 4.04 |
It can be seen that the electrical performance data of the two groups are substantially unchanged.
Example 4
Lithium iron phosphate LFP system positive electrode slurry:
dry matter mass ratio is as follows: super-P: binder = 95.9:2.5:1.6 (wherein the mass of component A and component B in the adhesive are 82% and 18% of the total mass of the adhesive, respectively).
In this example, component A has the following structural formula, R1 is- (CH 2)5CHCN(CH2)3CH2COO C2H5) and R2 is-CN:
The structural formula of the component B is as follows, R3 is- (CH 2)9CH2 CN), and R4 is-CH 2 CH2 CN:
The component A is dissolved by NMP to prepare a glue solution with the mass concentration of about 4%, then the conductive agent Super-P and LFP and proper NMP are added, after the dispersion is complete, the glue solution of the component B dissolved in NMP is added, after the uniform stirring, the viscosity of the glue solution is regulated to be proper by NMP, and the glue solution is used for coating pole pieces and assembling batteries. The slurry and pole piece were compared as follows:
It can be seen that the binder addition of the present invention is much less than that of PVDF addition, and the peel force of the pole piece is comparable to that of the PVDF group.
The battery data are as follows:
| positive electrode adhesive | Gram Capacity/mAh/g | Internal resistance/mΩ |
| A+B | 145.1 | 4.5 |
| PVDF HSV900 | 144.9 | 4.6 |
It can be seen that the capacity exertion and the impedance of the two groups are almost indistinguishable.
Claims (4)
1. An adhesive for positive electrode slurry of a lithium ion battery, which is characterized in that: the adhesive consists of a component A serving as a main adhesive and a component B serving as a flexible agent,
The component A is shown as a formula (I),
In formula (I), R1 is selected from hydrogen, methyl, -COOR, linear or branched alkyl of C1-C50000 with-CN and/or-COOR 'substituents, R, R' are each independently selected from hydrogen, linear or branched alkyl of C1-C100; r2 is selected from hydrogen, C1-C100 linear or branched alkyl; x and z are natural numbers, and y is 0 or a natural number;
The component B is shown as a formula (II) or a formula (III),
In the formula (III), R3 and R4 are independently selected from hydrogen, -CN, -COOH, C1-C100 straight-chain or branched hydrocarbon groups with-CN and/or-COOH, and in the formula (II), m and n are natural numbers;
the component A accounts for 20-98% of the total mass of the adhesive, and the component B accounts for 2-80% of the total mass of the adhesive.
2. The binder for positive electrode slurry for lithium ion batteries according to claim 1, wherein: the relative molecular mass of the component A is 30-180 ten thousand, and the relative molecular mass of the component B is 3-50 ten thousand.
3. The binder for positive electrode slurry for lithium ion batteries according to claim 1, wherein: when the adhesive is used for preparing positive electrode slurry, the component A is directly added in a solid state or is added after being prepared into a glue solution, and the component B is added after being prepared into the glue solution.
4. The binder for positive electrode slurry for lithium ion batteries according to claim 3, wherein: the component A or the component B is prepared into a glue solution by using N-methyl pyrrolidone.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202111610619.0A CN114204032B (en) | 2021-12-27 | 2021-12-27 | Adhesive for lithium ion battery anode slurry |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202111610619.0A CN114204032B (en) | 2021-12-27 | 2021-12-27 | Adhesive for lithium ion battery anode slurry |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CN114204032A CN114204032A (en) | 2022-03-18 |
| CN114204032B true CN114204032B (en) | 2024-06-07 |
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| CN114204032A (en) | 2022-03-18 |
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