CN111342116A - Safety lithium ion battery - Google Patents

Safety lithium ion battery Download PDF

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Publication number
CN111342116A
CN111342116A CN202010187142.9A CN202010187142A CN111342116A CN 111342116 A CN111342116 A CN 111342116A CN 202010187142 A CN202010187142 A CN 202010187142A CN 111342116 A CN111342116 A CN 111342116A
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molecular sieve
lithium ion
ion battery
coating
safety lithium
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CN202010187142.9A
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Chinese (zh)
Inventor
曹迎倩
张越超
李天龙
高秀玲
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Tianjin EV Energies Co Ltd
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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
    • 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
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
    • H01M10/4235—Safety or regulating additives or arrangements in electrodes, separators or electrolyte
    • 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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  • Chemical & Material Sciences (AREA)
  • Manufacturing & Machinery (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Materials Engineering (AREA)
  • Secondary Cells (AREA)
  • Battery Electrode And Active Subsutance (AREA)

Abstract

The invention provides a safety lithium ion battery, wherein the outer surface of a negative current collector at the outermost layer in a battery core of the battery is coated with a molecular sieve coating, and the molecular sieve coating comprises the following components in percentage by weight: 70-90% of molecular sieve, 10-30% of conductive agent and 10-20% of binder. According to the lithium ion battery, the outer surface of the cathode plate on the outermost layer of the battery cell is coated with the molecular sieve coating which is selectively adsorbed, and the molecular sieve coating is arranged on the surface of the first cathode plate which does not participate in the chemical reaction of the battery and is far away from the side of the anode plate, so that the electrochemical performance of the battery cell is not reduced, the gas generated by the battery cell can be effectively adsorbed, and the safety performance of the battery cell is obviously improved.

Description

Safety lithium ion battery
Technical Field
The invention belongs to the field of lithium ion batteries, and particularly relates to a safety lithium ion battery.
Background
With the continuous innovation of new energy material research and development technology, the lithium ion battery with the advantages of low carbon, environmental protection, high energy density, wide working temperature range and the like is widely concerned. In recent years, together with the vigorous promotion of national policies, the lithium ion battery industry gradually becomes the main force of the electric automobile energy storage market. Therefore, the market puts forward the requirements of higher energy density, higher endurance mileage, higher power density and the like for the lithium battery. However, the safety performance of the high-energy-density battery cell is greatly reduced, and the new energy electric vehicle has a few ignition accidents in the market. This requires us to improve the safety performance of lithium ion batteries.
In order to improve the safety performance of the lithium ion battery, researchers have devised many schemes. Some technologies are to add flame retardant, anti-overcharge additive and the like into the electrolyte to improve the safety performance of the battery cell, but the technology is expensive, and the internal resistance of the electrolyte is generally higher, so that the electrochemical performance of the battery cell is improved.
Some technologies utilize the PTC principle, a layer of PTC high polymer material is coated on a current collector, and when the temperature of a battery core rises, the current is quickly blocked by utilizing the principle that the resistance of the material suddenly increases, so that further thermal expansion reaction is avoided. Although the technology solves the problem of resistance increase by adding the conductive agent, the coating thickness is generally 2-4um, which affects the coating area of the active material and is contrary to the aim of pursuing higher cell energy density. Therefore, this technique also has certain drawbacks.
In the existing technologies, a diaphragm with a high melting point, such as aramid fiber, is adopted, or the surface of the diaphragm is modified by flame retardant additives, so that when heat accumulation occurs in a battery cell, short circuits of a positive electrode and a negative electrode caused by thermal contraction of the diaphragm are avoided. However, the technology also has the disadvantages that the internal resistance of the diaphragm is too large, the self-discharge risk is large, the lithium ion transmission is influenced, and meanwhile, when a large amount of gas is produced from the battery cell, the further thermal runaway cannot be avoided.
In other technologies, oxygen is added into the positive electrode material to absorb the oxygen, so that when the positive electrode active material is decomposed at high temperature and releases oxygen, ambient oxygen is captured quickly, the internal oxygen concentration of the lithium battery in thermal runaway is reduced, the lithium battery cannot meet the ignition condition, and the thermal runaway of the lithium battery is avoided. The molecular sieve disclosed in patent application CN201810712193, an internal oxygen self-absorption safety lithium battery, is mainly used for adsorbing oxygen generated in a battery cell, and an oxygen absorbent is mixed with a positive electrode material, so that the mixing not only causes the reduction of energy density of the battery cell and the increase of complexity of a homogenate mixing process, but also causes the reduction of electrical properties of the battery cell, such as high-temperature storage performance, rate capability, high-temperature and low-temperature performances.
Therefore, it is necessary to find a method for improving the safety of the battery cell without affecting the electrochemical properties of the battery cell.
Disclosure of Invention
In view of the above, the present invention provides a safety lithium ion battery, which can improve the safety of the battery without affecting the electrochemical properties of the battery.
In order to achieve the purpose, the technical scheme of the invention is realized as follows:
a safety lithium ion battery is characterized in that the outer surface of a negative current collector at the outermost layer in a battery cell of the battery is coated with a molecular sieve coating, and the molecular sieve coating comprises the following components in percentage by weight: 70-90% of molecular sieve, 10-30% of conductive agent and 10-20% of binder.
Preferably, the weight percentage of the molecular sieve is 75-85%.
Preferably, the molecular sieve has a pore diameter of 0.5-1nm and a specific surface area of 300-500m2/g。
Further, the thickness of the molecular sieve coating is 2um-20um, preferably 5-7 um.
Due to the 'shape selection effect', the molecular sieve with small pore diameter is limited by the pore diameter, and can only allow the entry and adsorption of small molecular gas molecules such as oxygen, hydrogen, carbon monoxide, carbon dioxide, methane, ethylene, ethane, propane, propylene and the like, but not allow the entry of electrolyte components such as solvent macromolecules such as dimethyl carbonate (DMC), Ethylene Carbonate (EC) and the like. Therefore, the molecular sieve with high specific surface area and high adsorption capacity can selectively adsorb the gas generated by the electric core after being heated and decomposed, and effectively reduces the risk of overlarge pressure and even explosion caused by gas generation.
Further, the molecular sieve is one or a composite of more than two of a 3A molecular sieve, a 4A molecular sieve, a 5A molecular sieve, a NaY molecular sieve, a 13X molecular sieve, a SAPO molecular sieve, an ALPO molecular sieve and a metal modified molecular sieve of any one of the molecular sieves.
Further, the conductive agent is one or a composite of more than two of Cu particles, conductive carbon black, carbon nano tubes and acetylene black.
Further, the binder may be CMC and/or SBR.
Further, the preparation process of the molecular sieve coating comprises the following steps: dispersing a molecular sieve raw material in a solvent, adding a conductive agent after uniform dispersion, then adding a uniformly dispersed binder into the solvent, stirring the mixture at a low speed for 10-70min, then stirring the mixture at a high speed for 2-5h, mixing the mixture uniformly to obtain a molecular sieve coating slurry, coating the molecular sieve coating slurry on the surface of a negative current collector, drying the coating at 80-150 ℃, and removing solvent molecules to obtain the catalyst.
Further, the solvent is one or a mixture of more than two of ammonia water, triethylamine, tetraethyl ammonium hydroxide, morphine and the like.
The solvent is adopted because the alkaline group-hydroxyl of solute molecules in the alkaline solvent can be combined with L acid and B acid in a molecular sieve framework to accelerate the dispersion of the molecular sieve, and a water system can be effectively combined with a binder, so that the bonding effect of the molecular sieve coating and the Cu current collector is improved.
Compared with the prior art, the safety lithium ion battery provided by the invention has the following advantages:
(1) the invention can improve the safety performance of the battery and simultaneously does not influence the electrochemical performance of the battery. Compared with the traditional methods of compounding the molecular sieve and the anode material and the like, the molecular sieve coating is arranged on the outermost negative electrode plate and is arranged on the surface of the first negative electrode plate which does not participate in the chemical reaction of the battery and is far away from the side of the anode plate, and because substances of the molecular sieve coating do not participate in the reaction, the use area of the effective coating of the anode and cathode active materials in the battery core cannot be reduced, and because the molecular sieve with small pore size selectively adsorbs, the adsorption consumption of the electrolyte cannot be caused, so the transmission of lithium ions in the battery cannot be influenced. When the electrolyte is decomposed to generate gas due to abuse conditions such as heating or overcharging of the battery cell, the molecular sieve coating can adsorb the generated gas by virtue of the larger specific surface area of the molecular sieve coating, so that risks such as breaking an aluminum plastic film and the like caused by overlarge internal pressure of the battery cell are avoided. It is possible to improve safety without affecting the electrochemical performance of the battery.
(2) The invention directly coats the molecular sieve coating on the negative plate, and needs to overcome the problems of the adhesion of the copper current collector and the molecular sieve coating and the dispersion of the molecular sieve;
(3) the invention has simple process, easy realization, basically no need of modifying and adjusting the prior equipment, simple coating process, low material cost and suitability for large-scale popularization.
Drawings
FIG. 1 is a schematic view of a pole piece comprising a molecular sieve coating.
In the figure: 100: a negative current collector; 110: coating a molecular sieve; 120: a negative electrode active material layer; 130: a diaphragm; 140: a positive current collector; 150: a positive electrode active material layer.
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 invention is described in detail below with reference to embodiments and the accompanying drawings.
Example 1
A safety lithium ion battery: the lithium ion battery comprises a positive plate, a first negative plate, a second negative plate, a diaphragm and electrolyte.
Preparing a first negative plate by a conventional method, wherein the first negative plate is a plate coated with negative active material coatings on two sides, the negative active material coatings are prepared from active materials, conductive agents, binders and solvents, the active materials are selected from graphite, the conductive agents are selected from acetylene black, the binders are selected from a mixture of SBR and CMC, and the active materials are as follows: conductive agent: the mass ratio of the binder is 95: 5: and 5, selecting a copper foil as a current collector, and using water as a solvent.
The positive plate is prepared by a conventional method, a coating of the positive plate is prepared from a positive active material, a conductive agent binder and a solvent, the positive active material is NMC811, the conductive agent is carbon black, the binder is PVDF, the solvent is NMP, and the active material: conductive agent: the mass ratio of the binder is 95: 5: and 5, adopting Al foil as a current collector.
The electrolyte is prepared according to EC: PC: EMC: VC: PS 35: 5: 60: 1: 1, 1mol of lithium salt LiPF6 was added thereto, and the mixture was stirred sufficiently. The diaphragm adopts a polypropylene PP diaphragm.
The second negative pole piece is a pole piece with a molecular sieve coating on one side and a negative active material coating on the other side, and the preparation method comprises the following steps: dispersing 70 parts of 4A molecular sieve in 150 parts of aqueous solution of tetraethylammonium hydroxide, then adding 10 parts of dispersed CMC and SBR binder and 10 parts of conductive agent carbon black into the molecular sieve solution, uniformly stirring, vacuumizing to prepare slurry, then coating the slurry on a single-side Cu current collector, and coating the other side of the current collector with an active material which is the same as that of the first negative plate. And then placing a molecular sieve coating layer provided with selective adsorption on the outermost layer of the battery cell according to the sequence shown in figure 1, preparing the prepared positive plate, negative plate and diaphragm into the battery cell in a Z-shaped lamination way, packaging the battery cell in an aluminum-plastic packaging bag, baking at high temperature, injecting liquid, standing, and pre-charging into a component volume to obtain the battery cell.
Example 2
The difference from the embodiment 1 is that the component proportion of the molecular sieve coating in the second negative plate is different, and the specific proportion is as follows: molecular sieve: adhesive: 80 parts of conductive agent: 10: 10.
example 3
This example is substantially the same as example 1, except that the conductive agent used in the molecular sieve coating in the second negative electrode sheet is elemental Cu particles, and the molecular sieve: adhesive: the proportion of the conductive agent is 70: 10: 10.
comparative example 1
Comparative example 1 is substantially the same as example 1 except that the number of the 2 nd negative electrode sheets in the battery cell of comparative example 1 is 1, one second negative electrode sheet is replaced by a first negative electrode sheet, and then zigzag lamination, packaging, high-temperature baking, liquid injection, standing and pre-charging are carried out to form the component capacity.
Comparative example 2
Comparative example 1 is substantially the same as example 1, except that the number of the 2 nd negative electrode sheets in the battery cell of comparative example 1 is 0, the two second negative electrode sheets at the outermost side are completely replaced by the first negative electrode sheets, and then zigzag lamination, packaging, high-temperature baking, liquid injection, standing and pre-charging are carried out to form the component capacity.
Comparative example 3
The cell of comparative example 3 is substantially similar to that of example 1, except that the molecular sieve used in the example is added to the positive active material and uniformly distributed in the positive active material coating, and it should be noted that the molecular sieve and the amount of the molecular sieve in the whole cell are the same as those in example 1, i.e. the molecular sieves used in the first and last negative electrode sheets of example 1 are uniformly distributed in the positive active material coating of the positive electrode sheet of comparative example 3. The negative plate used is the first negative plate.
Test example: safety testing
The battery cell prepared in the above examples 1 to 3 and comparative examples 1 to 3 was filled with a 1C constant current and a constant voltage at room temperature, and then left to stand for 3 hours, the battery cell was placed in an oven at a temperature of 130 ℃ for heating, the temperature was raised from room temperature to 130 ℃ at a rate of 5 ℃/min, and then kept at a constant temperature at 130 ℃ for 3 hours; the results are shown in Table 1 below.
Compared with the comparative example 2, the safety performance of the battery cell can be effectively improved by adding the molecular sieve coating in a certain proportion; compared with the comparative example 3 (namely the traditional method for mixing the molecular sieve and the cathode material), the method can effectively reduce the internal resistance of the cell.
TABLE 1
Group of Battery cell Cell internal resistance/m omega Failure time at 130 ℃ Whether or not to pass
Example 1 1# 1.32 Does not fail for 3h By passing
Example 1 2# 1.34 Does not fail for 3h By passing
Example 2 1# 1.25 Does not fail for 3h By passing
Example 2 2# 1.28 Does not fail for 3h By passing
Example 3 1# 1.40 Does not fail for 3h By passing
Example 3 2# 1.45 Does not fail for 3h By passing
Comparative example 1 1# 1.28 Does not fail for 3h By passing
Comparative example 1 2# 1.26 2.8h failure Failure of
Comparative example 2 1# 1.25 1.2h failure Failure of
Comparative example 2 2# 1.30 1.1h failure Failure of
Comparative example 3 1# 2.89 Does not fail for 3h By passing
Comparative example 3 2# 2.36 Does not fail for 3h By passing
Test example: electrical Performance testing
The cells prepared in the above examples 1-3 and comparative examples 1-3 were subjected to low/normal temperature 3C rate discharge and 55 ℃ high temperature storage performance test, and the capacity retention rate/nuclear power retention rate thereof was recorded, and the results are shown in table 2 below.
TABLE 2
Figure BDA0002414591150000071
Figure BDA0002414591150000081
As seen from table 2, the rate capability and storage performance of inventive examples 1-3 are comparable to those of comparative sample 2 (conventional cell), while the rate capability and storage performance of comparative example 3 (conventional molecular sieve and positive electrode material blending scheme) are somewhat degraded.
Therefore, when the electrolyte is decomposed to generate gas due to abuse conditions such as heating or overcharging in the battery cell of the safety lithium ion battery provided by the embodiment of the invention, the molecular sieve coating can adsorb the generated gas by virtue of the larger specific surface area of the molecular sieve coating, so that risks such as breaking an aluminum plastic film and the like caused by overlarge internal pressure of the battery cell are avoided. The safety performance of the battery core can be improved without influencing the internal resistance and the electrochemical performance of the battery.
The above description is only for the purpose of illustrating the preferred embodiments of the present invention and should not be taken as limiting the invention, so that any modifications, equivalents, improvements and the like, which are within the spirit and principle of the present invention, should be included in the scope of the present invention.

Claims (10)

1. A safety lithium ion battery, characterized by: the outer surface of the outermost negative current collector in the battery core of the battery is coated with a molecular sieve coating, and the molecular sieve coating comprises the following components in percentage by weight: 70-90% of molecular sieve, 10-30% of conductive agent and 10-20% of binder.
2. The safety lithium ion battery according to claim 1, wherein: the weight percentage of the molecular sieve is 75-85%.
3. The safety lithium ion battery according to claim 1, wherein: the pore diameter of the molecular sieve is 0.5-1nm, and the specific surface area is 300-500m2/g。
4. The safety lithium ion battery according to claim 1, wherein: the thickness of the molecular sieve coating is 2um-20 um.
5. The safety lithium ion battery according to claim 1, wherein: the thickness of the molecular sieve coating is 5-7 um.
6. The safety lithium ion battery according to claim 1, wherein: the molecular sieve is one or a composite of more than two of a 3A molecular sieve, a 4A molecular sieve, a 5A molecular sieve, a NaY molecular sieve, a 13X molecular sieve, a SAPO molecular sieve, an ALPO molecular sieve and a metal modified molecular sieve of any one of the molecular sieves.
7. The safety lithium ion battery according to claim 1, wherein: the conductive agent is one or a composite of more than two of Cu particles, conductive carbon black, carbon nano tubes and acetylene black.
8. The safety lithium ion battery according to claim 1, wherein: CMC and/or SBR of the binder.
9. The safety lithium ion battery according to claim 1, wherein: the preparation process of the molecular sieve coating comprises the following steps: dispersing a molecular sieve raw material in a solvent, adding a conductive agent after uniform dispersion, then adding a uniformly dispersed binder into the solvent, stirring the mixture at a low speed for 10-70min, then stirring the mixture at a high speed for 2-5h, mixing the mixture uniformly to obtain a molecular sieve coating slurry, coating the molecular sieve coating slurry on the surface of a negative current collector, drying the coating at 80-150 ℃, and removing solvent molecules to obtain the catalyst.
10. The safety lithium ion battery of claim 9, wherein: the solvent is one or more of mixed aqueous solution of ammonia water, triethylamine, tetraethyl ammonium hydroxide, morphine and the like.
CN202010187142.9A 2020-03-17 2020-03-17 Safety lithium ion battery Pending CN111342116A (en)

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Cited By (8)

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CN112234245A (en) * 2020-10-20 2021-01-15 天津市捷威动力工业有限公司 Internal heat insulation lithium ion battery
CN112271341A (en) * 2020-10-23 2021-01-26 珠海冠宇动力电池有限公司 Laminated battery core and lithium ion battery
CN112290098A (en) * 2020-10-19 2021-01-29 江苏智泰新能源科技有限公司 Anti-flatulence polymer lithium ion battery and preparation method thereof
CN112467270A (en) * 2020-11-03 2021-03-09 浙江锋锂新能源科技有限公司 Composite air suction element, preparation method thereof and flatulence-preventing self-repairing soft-package lithium battery
CN113871687A (en) * 2021-09-26 2021-12-31 蜂巢能源科技有限公司 Low-gas-production battery and preparation method thereof
US20220085432A1 (en) * 2020-09-15 2022-03-17 Sk Innovation Co., Ltd. Lithium secondary battery
CN114335689A (en) * 2021-12-30 2022-04-12 远景动力技术(江苏)有限公司 Electrochemical device and method for manufacturing electrochemical device
CN115498356A (en) * 2022-09-30 2022-12-20 峰谷动力(深圳)新能源技术有限公司 Lithium ion battery

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Cited By (9)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20220085432A1 (en) * 2020-09-15 2022-03-17 Sk Innovation Co., Ltd. Lithium secondary battery
US12009491B2 (en) * 2020-09-15 2024-06-11 Sk On Co., Ltd. Lithium secondary battery
CN112290098A (en) * 2020-10-19 2021-01-29 江苏智泰新能源科技有限公司 Anti-flatulence polymer lithium ion battery and preparation method thereof
CN112234245A (en) * 2020-10-20 2021-01-15 天津市捷威动力工业有限公司 Internal heat insulation lithium ion battery
CN112271341A (en) * 2020-10-23 2021-01-26 珠海冠宇动力电池有限公司 Laminated battery core and lithium ion battery
CN112467270A (en) * 2020-11-03 2021-03-09 浙江锋锂新能源科技有限公司 Composite air suction element, preparation method thereof and flatulence-preventing self-repairing soft-package lithium battery
CN113871687A (en) * 2021-09-26 2021-12-31 蜂巢能源科技有限公司 Low-gas-production battery and preparation method thereof
CN114335689A (en) * 2021-12-30 2022-04-12 远景动力技术(江苏)有限公司 Electrochemical device and method for manufacturing electrochemical device
CN115498356A (en) * 2022-09-30 2022-12-20 峰谷动力(深圳)新能源技术有限公司 Lithium ion battery

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Application publication date: 20200626