CN113540437A - Low-temperature lithium ion battery with improved cycle performance - Google Patents

Low-temperature lithium ion battery with improved cycle performance Download PDF

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Publication number
CN113540437A
CN113540437A CN202110704760.0A CN202110704760A CN113540437A CN 113540437 A CN113540437 A CN 113540437A CN 202110704760 A CN202110704760 A CN 202110704760A CN 113540437 A CN113540437 A CN 113540437A
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lithium ion
cycle performance
ion battery
improved cycle
low temperature
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卢孟萍
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Changzhou Gaotai Information Technology 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
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
    • H01M4/50—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese
    • H01M4/505—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese of mixed oxides or hydroxides containing manganese for inserting or intercalating light metals, e.g. LiMn2O4 or LiMn2OxFy
    • 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
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
    • H01M10/0566—Liquid materials
    • H01M10/0567—Liquid materials characterised by the additives
    • 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
    • H01M10/058—Construction or manufacture
    • 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
    • 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
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
    • H01M4/483—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides for non-aqueous cells
    • 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
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
    • H01M4/583—Carbonaceous material, e.g. graphite-intercalation compounds or CFx
    • H01M4/587—Carbonaceous material, e.g. graphite-intercalation compounds or CFx for inserting or intercalating light metals
    • 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
    • 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
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Abstract

The invention discloses a low-temperature lithium ion battery with improved cycle performance, which comprises a positive electrode, a negative electrode, electrolyte and an isolating membrane, wherein the positive electrode is connected with the negative electrode; the positive electrode comprises lithium manganate, a conductive agent, a dispersing agent and a binder; the negative electrode comprises titanium dioxide, graphite, a conductive agent, a dispersing agent and a binder; preferably, the positive electrode further comprises NCM coated with polystyrene; wherein the total amount of the NCM coated with polystyrene and the lithium manganate is 100 parts, and the lithium manganate accounts for 50-80 parts; the invention effectively improves the cycle performance of the battery at low temperature by matching the anode and the cathode materials.

Description

Low-temperature lithium ion battery with improved cycle performance
Technical Field
The invention relates to the technical field of lithium ion batteries, in particular to a low-temperature lithium ion battery with improved cycle performance.
Background
The vast country of China has obvious difference in the north and south climates, so that the electric automobile faces severe tests of different climatic environments in the use process. Particularly, in the aspect of temperature, the temperature of cold winter in the north is often reduced to-30 ℃, and the temperature has obvious influence on the performance, the service life, the safety and the like of the lithium ion battery.
The low-temperature environment can seriously affect the dynamic performance of the lithium ion battery, and macroscopically, the cycle performance is poor, and even the lithium ion battery can not be charged and discharged at low temperature.
Disclosure of Invention
The invention aims to provide a low-temperature lithium ion battery with improved cycle performance.
In order to solve the technical problem, the technical scheme of the invention is as follows: a low-temperature lithium ion battery with improved cycle performance comprises a positive electrode, a negative electrode, electrolyte and an isolating membrane; the positive electrode comprises lithium manganate, a conductive agent, a dispersing agent and a binder;
the negative electrode includes titanium dioxide, graphite, a conductive agent, a dispersant, and a binder.
Preferably, the positive electrode further comprises NCM coated with polystyrene;
wherein the total amount of the NCM coated with polystyrene and the lithium manganate is 100 parts, and the lithium manganate accounts for 50-80 parts.
According to the invention, the lithium manganate is matched with NCM coated with polystyrene, so that the overall capacity of the positive electrode is improved, meanwhile, at a low temperature, the lithium ion de-intercalation resistance is smaller, and the lithium ion de-intercalation resistance is matched with the negative electrode with smaller lithium ion de-intercalation resistance at the same low temperature, when lithium ions are intercalated and deintercalated between the two electrodes in a reciprocating manner, the resistance is smaller, the SEI film consumes less lithium ions, and the macroscopic expression is that the cycle performance is enhanced. The invention further limits the dosage proportion of the lithium manganate and the NCM coated with polystyrene, mainly because the dosage of the lithium manganate influences the capacity of the anode, the low-temperature performance of the lithium manganate is better than that of the coated ternary lithium, the lithium manganate has large proportion and good low-temperature performance.
The negative electrode preferably includes, in mass fraction:
10 to 30 percent of titanium dioxide;
graphite 61% to 87%;
1% to 3% of a conductive agent;
1% to 2% of a dispersant;
1 to 5 percent of binder.
The higher the proportion of doped titanium dioxide of the negative electrode is, the better the low-temperature cycle performance is.
Preferably the graphite has a D50 of between 5 μm and 15 μm. The graphite particle size is small, the obtained low-temperature battery has good dynamics, and the battery is beneficial to running at low temperature.
Preferably, the conductive agent is one or more of graphene, SP, carbon nanotubes and carbon fibers. The conductive agent is added to improve the low-temperature dynamic performance of the system.
Preferably, the binder is one or more of polyvinyl alcohol, polytetrafluoroethylene and polyvinylidene fluoride. Further preferably, PVDF is preferred, which has a glass transition temperature of-42 ℃ and is suitable for use in low temperature systems above-40 ℃.
In the invention, the dispersant is sodium carboxymethyl cellulose (CMC); the diaphragm selects a polyethylene coating ceramic layer diaphragm, wherein a ceramic layer is coated on two surfaces of the diaphragm, the total thickness of the ceramic layer is 1-3 mu m, the ceramic layer can improve the liquid retention capacity, the ion conducting capacity of the diaphragm at low temperature is facilitated, and the ceramic layer is too thick and reduces the energy density of a system.
Preferably, the electrolyte comprises a solvent and a lithium salt; wherein the solvent comprises ethylene carbonate and methyl formate, and the mass ratio of the ethylene carbonate to the methyl formate is 1-3: 1. the melting point of Methyl Formate (MF) reaches-99 ℃, the Methyl Formate (MF) is an ideal low-temperature solvent, salts and additives can be better dissolved by matching with Ethylene Carbonate (EC), the low-temperature ionic conductivity of the electrolyte can be improved by the MF, but the addition amount is too large, and the dissolution of lithium salts and additives is influenced.
Preferably, the lithium salt is LiAsF6The lithium salt accounts for 1 to 2 percent of the electrolyte by mass. LiAsF6The addition amount of the lithium salt is 1-2% (mass percentage), and the lithium salt improves the dynamic performance of the electrolyte and the low-temperature cycle life.
Preferably, the electrolyte further comprises an additive, the additive is propyl sulfite, and the dosage of the additive accounts for 1-3% of the mass of the electrolyte. According to the invention, propyl sulfite accounting for 1-3% of the electrolyte by mass is matched with lithium manganate, so that the circulation performance of the system at low temperature can be improved, too many additives are added, the impedance of the electrolyte is improved, and the low-temperature circulation performance of the system is reduced.
By adopting the technical scheme, the invention has the beneficial effects that:
according to the invention, the positive electrode is made of a lithium manganate material with good low-temperature performance, and is matched with the negative electrode containing graphene and titanium dioxide with good low-temperature performance to form a system with good low temperature; at low temperature, Li+The two electrodes are embedded and de-embedded back and forth, the required resistance is small, the SEI film consumption is small, and the macroscopic expression is that the cycle performance is enhanced;
the negative electrode of the invention adopts titanium dioxide mixed graphite, improves the low-temperature performance of the negative electrode, improves the working capacity of the electrolyte at low temperature by optimizing the composition of the electrolyte solvent, the additive and the lithium salt, and simultaneously, the proper isolating membrane is matched to comprehensively optimize the low-temperature performance of the battery, so that the battery in the system can complete charging and discharging at the temperature of minus 30 ℃, and the cycle life is longer than 200 weeks.
Thereby achieving the above object of the present invention.
Drawings
FIG. 1 is a cycle curve at-30 ℃ of lithium ion batteries obtained in examples 1 to 5 of the present invention and a comparative example.
Detailed Description
In order to further explain the technical solution of the present invention, the present invention is explained in detail by the following specific examples.
Example 1
The invention discloses a low-temperature lithium ion battery with improved cycle performance, wherein the composition of the lithium ion battery and the using amount of each substance are shown in table 1 in detail;
the embodiment also discloses a manufacturing process of the lithium ion battery, which comprises the following steps:
stirring a main material by a positive electrode or a negative electrode, coating, cold pressing, slitting, and preparing a sheet to obtain a pole piece;
and (3) preparing the positive and negative pole pieces and the diaphragm into a bare cell through a lamination or winding process, and preparing the bare cell into the 2Ah flexible package battery after packaging, liquid injection, standing and formation.
Example 2
The main differences between this example and example 1 are detailed in table 1.
Example 3
The main differences between this example and example 1 are detailed in table 1.
Example 4
The main differences between this example and example 1 are detailed in table 1.
Example 5
The main differences between this example and example 1 are detailed in table 1.
Watch (A)
Figure 370903DEST_PATH_IMAGE002
Components and amounts (in mass%) of lithium ion batteries obtained in comparative example and examples 1 to 5
Figure 619481DEST_PATH_IMAGE004
The pouch cells prepared in examples 1 to 5 and comparative example were placed at-30C and tested for cycle data of 0.5C charge and 1C discharge, and a 200-cycle curve was recorded, as shown in fig. 1.
The energy densities of the batteries obtained in examples 1 to 5 and comparative example were calculated as shown in table 2, wherein the energy densities were calculated by: first cycle capacity is compared to the overall mass of each cell.
Table 2 mass energy density of lithium ion batteries obtained in examples 1 to 5 and comparative example at low temperature
Figure 749111DEST_PATH_IMAGE006
As can be seen from fig. 1 and table 2, the comparative example is a conventional battery system, and energy density at low temperature is advantageous, but cycle performance is extremely poor; the low-temperature batteries obtained in the embodiments 1 to 5 are slightly lower in energy density than the conventional battery system, but the cycle performance is greatly improved, and the low-temperature batteries are in accordance with the development principle of the low-temperature batteries as a whole.
According to the invention, the lithium manganate is matched with NCM coated with polystyrene, so that the overall capacity of the positive electrode is improved, meanwhile, at a low temperature, the lithium ion de-intercalation resistance is smaller, and the lithium ion de-intercalation resistance is matched with the negative electrode with smaller lithium ion de-intercalation resistance at the same low temperature, when lithium ions are intercalated and deintercalated between the two electrodes in a reciprocating manner, the resistance is smaller, the SEI film consumes less lithium ions, and the macroscopic expression is that the cycle performance is enhanced. The invention further limits the dosage proportion of the lithium manganate and the NCM coated with polystyrene, mainly because the dosage of the lithium manganate influences the capacity of the anode, the low-temperature performance of the lithium manganate is better than that of the coated ternary lithium, the lithium manganate has large proportion and good low-temperature performance. Compared with the energy density comparison data of the embodiment 1 and the embodiment 5, the energy density of the system is improved by the anode mixed modified ternary material, but the low-temperature performance is slightly reduced.
As can be seen from the comparison of the data in the examples 1 to 3, the higher the proportion of doped titanium dioxide in the negative electrode is, the thicker the isolating membrane ceramic layer is, the liquid retention amount is improved, the better the low-temperature cycle performance is, but the energy density of the system is reduced;
it can be seen from the battery cycle data obtained in comparative examples 1 to 5 that the larger the ratio of the electrolyte MF and the more the lithium salt, the better the cycle performance of the system.
According to the invention, the positive electrode is made of a lithium manganate material with good low-temperature performance, and is matched with the negative electrode containing graphene and titanium dioxide with good low-temperature performance to form a system with good low temperature; at low temperature, Li+The two electrodes are embedded and de-embedded back and forth, the required resistance is small, the SEI film consumption is small, and the macroscopic expression is that the cycle performance is enhanced;
the negative electrode of the invention adopts titanium dioxide mixed graphite, improves the low-temperature performance of the negative electrode, improves the working capacity of the electrolyte at low temperature by optimizing the composition of the electrolyte solvent, the additive and the lithium salt, and simultaneously, the proper isolating membrane is matched to comprehensively optimize the low-temperature performance of the battery, so that the battery in the system can complete charging and discharging at the temperature of minus 30 ℃, and the cycle life is longer than 200 weeks. Therefore, the battery system is suitable for low-temperature environment.

Claims (9)

1. A low-temperature lithium ion battery with improved cycle performance comprises a positive electrode, a negative electrode, electrolyte and an isolating membrane; the method is characterized in that:
the positive electrode comprises lithium manganate, a conductive agent, a dispersing agent and a binder;
the negative electrode includes titanium dioxide, graphite, a conductive agent, a dispersant, and a binder.
2. A low temperature lithium ion battery of claim 1 having improved cycle performance, wherein: the positive electrode further comprises NCM coated with polystyrene;
wherein the total amount of the NCM coated with polystyrene and the lithium manganate is 100 parts, and the lithium manganate accounts for 50-80 parts.
3. A low temperature lithium ion battery of claim 1 having improved cycle performance, wherein: the negative electrode comprises the following components in percentage by mass:
10 to 30 percent of titanium dioxide;
graphite 61% to 87%;
1% to 3% of a conductive agent;
1% to 2% of a dispersant;
1 to 5 percent of binder.
4. A low temperature lithium ion battery of claim 3 having improved cycle performance, wherein: the graphite has a D50 of between 5 μm and 15 μm.
5. A low temperature lithium ion battery of claim 1 having improved cycle performance, wherein: the conductive agent is one or more of graphene, SP, carbon nanotubes and carbon fibers.
6. A low temperature lithium ion battery of claim 1 having improved cycle performance, wherein: the binder is one or more of polyvinyl alcohol, polytetrafluoroethylene and polyvinylidene fluoride.
7. A low temperature lithium ion battery of improved cycle performance according to any one of claims 1 to 6 wherein: the electrolyte includes a solvent and a lithium salt; wherein the solvent comprises ethylene carbonate and methyl formate, and the mass ratio of the ethylene carbonate to the methyl formate is 1-3: 1.
8. a low temperature lithium ion battery of claim 7 having improved cycle performance, wherein: the lithium salt is LiAsF6The lithium salt accounts for 1 to 2 percent of the electrolyte by mass.
9. A low temperature lithium ion battery of claim 7 having improved cycle performance, wherein: the electrolyte also comprises an additive, wherein the additive is propyl sulfite, and the dosage of the additive accounts for 1-3% of the mass of the electrolyte.
CN202110704760.0A 2021-06-24 2021-06-24 Low-temperature lithium ion battery with improved cycle performance Withdrawn CN113540437A (en)

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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN114005954A (en) * 2021-10-28 2022-02-01 珠海冠宇电池股份有限公司 Negative electrode sheet and electrochemical device
CN115312748A (en) * 2022-10-13 2022-11-08 雅迪科技集团有限公司 Preparation method of negative electrode material, negative electrode material and sodium ion battery

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN114005954A (en) * 2021-10-28 2022-02-01 珠海冠宇电池股份有限公司 Negative electrode sheet and electrochemical device
CN115312748A (en) * 2022-10-13 2022-11-08 雅迪科技集团有限公司 Preparation method of negative electrode material, negative electrode material and sodium ion battery

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Application publication date: 20211022