CN112838193A - Method for improving overcharge and overdischarge performance of lithium ion battery - Google Patents

Method for improving overcharge and overdischarge performance of lithium ion battery Download PDF

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CN112838193A
CN112838193A CN202110327807.6A CN202110327807A CN112838193A CN 112838193 A CN112838193 A CN 112838193A CN 202110327807 A CN202110327807 A CN 202110327807A CN 112838193 A CN112838193 A CN 112838193A
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hard carbon
lithium ion
ion battery
battery
overcharge
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于树凯
宋文娥
李鹏辉
张涛
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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
    • 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
    • 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
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H01M4/139—Processes of manufacture
    • H01M4/1393—Processes of manufacture of electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
    • 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
    • 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
    • H01M2004/021—Physical characteristics, e.g. porosity, surface area
    • 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
    • H01M2004/027—Negative electrodes
    • 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

Abstract

The invention provides a method for improving the overcharge and overdischarge performance of a lithium ion battery, which comprises the steps of mixing graphite serving as a main active substance and hard carbon serving as a secondary active substance with a conductive agent, a binder and a solvent, uniformly mixing the two substances in a stirring manner, coating the mixture on a current collector foil, and then baking, rolling and cutting the current collector foil to prepare a negative pole piece for the lithium ion battery. The invention takes graphite as a main active substance, a certain amount of hard carbon is doped as a secondary active substance, and the characteristic that the voltage of a hard carbon material changes slowly at the last stage of charging and discharging is utilized to buffer the voltage drop of the whole battery to a certain extent, so that the voltage drop rate of the battery is slowed, and the deep overdischarge of the battery is avoided. Meanwhile, the hard carbon has very large graphite layer spacing, so that the lithium ions can be rapidly inserted and removed, and the rate capability of the battery can be effectively improved by doping a certain amount of hard carbon.

Description

Method for improving overcharge and overdischarge performance of lithium ion battery
Technical Field
The invention belongs to the technical field of lithium ion batteries, and particularly relates to a method for improving the overcharge and overdischarge performances of a lithium ion battery.
Background
The current patent proposes some new methods aiming at improving the overcharge and overdischarge performance of the battery, and mainly adds special additives into electrolyte to establish a self-protection mechanism in the battery. And the high-safety composite diaphragm is adopted, so that the diaphragm is closed at high temperature, and the deep thermal runaway of the battery is prevented. The diaphragm with the protective coating is adopted, so that the diaphragm has a high heat-resistant function, and the heat shrinkage of the diaphragm is reduced.
Patent CN 104037453A discloses a functional electrolyte for preventing overcharge of lithium battery and a production method thereof, wherein the electrolyte is added with functional additives including 2,3, 4-trifluorobiphenyl and 1, 3-propylene sulfonic acid ethyl ester on the basis of a basic electrolyte. When the battery is overcharged and overdischarged, the additive in the electrolyte can be decomposed to form a polymeric film or a passivation film SEI on the surface of an electrode, so that the internal resistance of the battery is increased, the battery is prevented from being further charged and discharged, and the ignition and explosion of the battery are effectively prevented. The patent CN107819095A discloses a high-safety composite lithium battery diaphragm and a preparation method thereof, the composite diaphragm mainly comprises core-shell functional microspheres and a fibrous skeleton, the core-shell functional microspheres can be converted into molten state at high temperature, so that the pores of the diaphragm are closed, the battery is prevented from further thermal runaway, the core-shell functional microspheres can be converted into electronic conductive state at high potential, and micro short circuit is formed in the battery to prevent the battery from deep overcharge. Patent CN103035866A discloses that a protective layer is coated on the surface of a base material of a diaphragm material, and the main component of the protective layer is a core-shell structure compound using an inorganic substance as a core and an acrylate-based polymer as a shell. The core of the core-shell structure composite is selected from one or more of aluminum oxide, titanium dioxide, silicon dioxide, zirconium dioxide, tin dioxide, magnesium oxide, zinc oxide, barium sulfate, boron nitride, aluminum nitride and magnesium nitride, and on the basis of ensuring the original basic characteristics of the polyolefin microporous membrane, the membrane is endowed with a high heat-resistant function, and the heat shrinkage of the membrane is reduced, so that the internal short circuit of the lithium ion battery is effectively reduced, and the thermal runaway of the battery caused by the internal short circuit of the battery is prevented.
In general, the prior art has the following disadvantages:
firstly, additives in the electrolyte are decomposed, a polymeric film or a passivation film SEI is formed on the surface of an electrode, so that the internal resistance of the battery is increased, the battery is powered off, and the safety of the battery is improved.
② the ionic conductivity of the ceramic powder is low, thereby leading to low high-rate charge-discharge capacity of the battery.
The electroactive material in the composite diaphragm is easy to block the nanometer pore canal of the porous base membrane, so that the porosity of the diaphragm is reduced, and the charge and discharge performance of the battery in a normal state is influenced.
Disclosure of Invention
In view of this, the present invention is directed to a method for improving the overcharge and overdischarge performance of a lithium ion battery, so as to change the charge and discharge curve of the negative electrode material of the battery, especially the non-plateau curve at the end of charge and discharge, and reduce the abrupt change of voltage, thereby increasing the overcharge and overdischarge capacity of the battery and improving the safety of the battery.
In order to achieve the purpose, the technical scheme of the invention is realized as follows:
a method for improving the overcharge and overdischarge performance of a lithium ion battery comprises the steps of mixing graphite serving as a main active substance and hard carbon serving as a secondary active substance with a conductive agent, a binder and a solvent, uniformly mixing the two substances in a stirring manner, coating the mixture on a current collector foil, and baking, rolling and cutting the current collector foil to prepare a negative pole piece for the lithium ion battery.
Preferably, the main active material graphite is natural graphite, artificial graphite or a mixture of the natural graphite and the artificial graphite.
Preferably, the secondary active material hard carbon is at least one of asphalt-based hard carbon, biomass hard carbon and polymer-based hard carbon.
Preferably, the mass ratio of the main active material graphite to the secondary active material hard carbon to the conductive agent to the binder is 55.2-82.8: 36.8-9.2: 6-4: 2-4, preferably 73.6: 18.4: 4:4.
preferably, the interlayer spacing d (002) of the secondary active material hard carbon is in the range of 0.3-0.4nm, preferably 0.38-0.39 nm.
Preferably, the specific surface area of the secondary active material hard carbon is 2.0-10.0 m2A particle size of less than 20 μm, preferably 5.0 to 7.5 m/g2(g) the particle size is less than 10 mu m.
Preferably, the conductive agent is at least one of SPUERLI, CNT, KS-6, KS-15, SFG-6, Acetylene Black (AB), Ketjen Black (KB), and Vapor Grown Carbon Fiber (VGCF).
Preferably, the binder is at least one of polyvinylidene fluoride (PVDF), sodium carboxymethylcellulose (CMC), Styrene Butadiene Rubber (SBR), polyacrylic acid (PAA), polyvinyl alcohol (PVA), Polyamide (PAI), and Polyethyleneimine (PEI).
Preferably, the solvent is Nitrogen Methyl Pyrrolidone (NMP) or deionized water.
The invention also aims to provide a negative electrode material prepared by the method for improving the overcharge and overdischarge performances of the lithium ion battery.
Compared with the prior art, the method for improving the overcharge and overdischarge performances of the lithium ion battery has the following beneficial effects:
(1) the performance of the material used by the lithium ion battery is not changed, and from the characteristics of material charge and discharge, the change of the potential of a non-platform area of the battery in the process of removing lithium and inserting lithium, particularly the curve of the non-platform area at the end of charge and discharge, is changed by adding a small amount of hard carbon, so that the rapid change of voltage is reduced, the overcharge and overdischarge capabilities of the battery are fundamentally improved, and the safety of the battery is improved.
(2) The hard carbon has very large interlayer spacing (d (002)) compared with graphite, is beneficial to the intercalation and deintercalation of lithium ions, and can obviously improve the rate capability and the cycle performance of the battery by doping a small amount of hard carbon.
(3) The hard carbon has small particle size and large specific surface area, and the conductivity of the material can be improved and the internal resistance of the battery can be reduced by doping a small amount of hard carbon in the negative graphite material, so that the rate capability and the cycle performance of the lithium ion battery are improved.
Principle analysis:
the voltage of the full battery is determined by the difference value of the voltage of the anode material and the voltage of the cathode material, and the cathode active material graphite in the lithium ion battery obviously changes the voltage value of the lithium during the lithium intercalation and lithium deintercalation processes to form a voltage plateau area and a non-plateau area, so that the discharge curve of the full battery consisting of the ternary material and the graphite has obvious voltage plateau areas and non-plateau areas. In the voltage plateau stage, the voltage is kept stable, and the potential changes rapidly in the non-plateau region, so that the voltage of the battery changes greatly due to very small charge and discharge changes at the end of the plateau region. The invention takes graphite as a main active substance, a certain amount of hard carbon is doped as a secondary active substance, the voltage of the hard carbon material changes along with the change of the capacity, the invention is different from a charging and discharging platform of the graphite material, the charging and discharging curve of the hard carbon has no obvious platform area, and the whole charging and discharging curve is an oblique line area, so that the voltage changes steadily and does not change sharply in the charging and discharging process. Therefore, a small amount of hard carbon material is doped in the graphite, and the characteristic that the voltage of the hard carbon material changes slowly at the last stage of charging and discharging is utilized to buffer the voltage drop of the whole battery to a certain extent, so that the voltage drop rate of the battery is slowed, the charging and discharging curve of the negative electrode material of the battery is changed, particularly the non-plateau curve at the last stage of charging and discharging, the rapid voltage drop can be relieved, the deep over-discharging of the battery is avoided, the over-charging and over-discharging capacity of the battery is increased, and the safety of the battery is improved.
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 full cell discharge curve of example 1, example 2 and comparative example 1;
FIG. 2 is a charge-discharge curve of the battery of comparative example 2;
FIG. 3 is a charge-discharge curve of a battery of comparative example 3;
FIG. 4 is a battery rate discharge curve of example 1;
fig. 5 is a full cell overcharge curve for example 1, example 2, and comparative example 1;
fig. 6 is a full cell overdischarge curve for example 1, example 2 and comparative example 1.
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.
Graphite: the model is CP5-M, and the manufacturer is Shanghai fir Techni GmbH;
hard carbon: BioHC, a product of the same manufacturer, Cola;
SP: the model is Super P Li, and the manufacturer is the limited responsibility company of the Beijing Haiwei industrial chemical products;
PVDF: the model is PVDF5130, and the manufacturer is Shenzhen Enshi high-tech company;
NMP: the purity is 99.99 percent, and the manufacturer is Mickey chemical Co., Ltd;
NCM 111: the model is RL03, and the manufacturer is Hunan Ruixiang New Material GmbH.
The present invention will be described in detail with reference to the following examples and accompanying drawings.
Example 1
Graphite is used as a main active material, hard carbon is used as a secondary active material, and the ratio of the graphite to the conductive agent (SP) to the binder (PVDF) is 73.6: mixing at a ratio of 18.4:4.0:4.0, uniformly mixing by taking NMP as a solvent in a stirring manner, coating on a current collector foil, and baking, rolling and cutting to prepare the negative pole piece for the lithium ion battery. Mixing the ternary material (NCM111), a conductive agent (SP) and a binder (PVDF) at a ratio of 91.5:6:2.5, uniformly mixing the mixture in a stirring manner by taking NMP as a solvent, coating the mixture on a current collector foil, and baking, rolling and cutting the mixture to prepare the positive pole piece for the lithium ion battery. And assembling the prepared negative pole piece and positive pole piece into a full cell for performance test.
Example 2
Graphite is used as a main active material, hard carbon is used as a secondary active material, and the ratio of the graphite to the hard carbon to the conductive agent (SP) and the binder (PVDF) is 82.8: and (3) mixing at a ratio of 9.2:4.0:4.0, uniformly mixing by taking NMP as a solvent in a stirring manner, coating on a current collector foil, and baking, rolling and cutting to prepare the negative pole piece for the lithium ion battery. Mixing the ternary material (NCM111), a conductive agent (SP) and a binder (PVDF) at a ratio of 91.5:6:2.5, uniformly mixing the mixture in a stirring manner by taking NMP as a solvent, coating the mixture on a current collector foil, and baking, rolling and cutting the mixture to prepare the positive pole piece for the lithium ion battery. And assembling the prepared negative pole piece and positive pole piece into a full cell for performance test.
Comparative example 1
Graphite is used as an active substance, the active substance is mixed with a conductive agent (SP) and a binder (PVDF) at a ratio of 92:4.0:4.0, NMP is used as a solvent, the mixture is uniformly mixed in a stirring manner, then the mixture is coated on a current collector foil, and then the negative pole piece for the lithium ion battery is prepared by baking, rolling and cutting. Mixing the ternary material (NCM111), a conductive agent (SP) and a binder (PVDF) at a ratio of 91.5:6:2.5, uniformly mixing the mixture in a stirring manner by taking NMP as a solvent, coating the mixture on a current collector foil, and baking, rolling and cutting the mixture to prepare the positive pole piece for the lithium ion battery. And assembling the prepared negative pole piece and positive pole piece into a full cell for performance test.
Comparative example 2
And (3) taking a round metal lithium sheet as a positive electrode, cutting the negative electrode sheet in the comparative example 1 into a round sheet with the diameter of 10mm as a negative electrode, and performing charging and discharging tests.
Comparative example 3
And (3) taking a round metal lithium sheet as a positive electrode, replacing the graphite in the comparative example 1 with hard carbon to manufacture a negative electrode sheet, cutting the negative electrode sheet into a wafer with the diameter of 10mm as a negative electrode, and forming a charging circuit to carry out a charge and discharge test.
Table 1 table of full cell power performance test data for example 1, example 2 and comparative example 1
Figure BDA0002995279170000071
The full battery voltage is determined by the difference between the voltage of the anode material and the voltage of the cathode material, and as can be seen from the battery discharge curve in fig. 2, the graphite material has an obvious voltage platform in the charge and discharge process, and the voltage is kept stable in the voltage platform stage, but the voltage changes rapidly due to the small change of the capacity at the end of the charge and discharge platform. It can be seen from the charging and discharging curve of the battery in fig. 3 that the charging and discharging curve of the hard carbon has no obvious platform region, and the whole charging and discharging curve is an oblique line region, so that the voltage changes steadily and does not change sharply in the charging and discharging process. The incorporation of hard carbon in graphite can mitigate the sharp drop in voltage. As can be seen from fig. 1, the pure graphite cell without doped hard carbon has a sharp drop in cell voltage at the end of discharge, while the cells doped with 10% and 20% hard carbon have a buffer effect on the voltage drop of the whole cell due to the slow voltage change of the hard carbon material at the end of discharge, so that the voltage drop rate of the cell is slowed down, and deep over-discharge of the cell is avoided. However, as can also be seen from fig. 1, the battery capacity becomes lower as the hard carbon incorporation amount increases.
As can be seen from fig. 4, since hard carbon has a very large graphite layer interval, which facilitates rapid intercalation and deintercalation of lithium ions, the battery doped with a certain amount of hard carbon has very excellent rate performance. As can be seen from the overcharge and overdischarge curves of fig. 4 and 5, the temperature of the battery changes smoothly and the temperature rise is small in the overcharge and the overdischarge after a certain amount of hard carbon is doped. As can be seen from table 1, the cell voltage was still greater than 2.5V after discharging example 1 and example 2270A for 10s, whereas the cut-off voltage of 2.5V was reached after discharging comparative example 1 for 7.9 s. After discharging for 3s for example 1 and example 21150W, the cell voltage was greater than 2.8V, while the voltage of comparative example 1 was 2.5021V. The voltage of the battery is still less than 4.2V after the battery is charged for 3s by using the example 1 and the example 2845, while the cut-off voltage of the battery is reached by charging the battery for 2.85s by using the comparative example 1, and after a certain amount of hard carbon can be doped, the power performance of the battery can be improved, so that the battery has excellent high-power charging and discharging performance.
In the preparation process of the battery, a small amount of hard carbon is added into the negative electrode graphite material, so that the charge-discharge curve of the negative electrode material of the battery, particularly the non-plateau curve at the end of charge-discharge, is changed, and the rapid change of voltage is reduced, thereby increasing the overcharge and overdischarge capacity of the battery and improving the safety of the battery. And the addition of the hard carbon can reduce the internal resistance of the battery and improve the rate capability and the cycle performance of the battery.
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 (10)

1. A method for improving the overcharge and overdischarge performance of a lithium ion battery is characterized by comprising the following steps: graphite is used as a main active substance, hard carbon is used as a secondary active substance, the graphite and the hard carbon are mixed with a conductive agent, a binder and a solvent, the mixture is uniformly mixed in a stirring mode, then the mixture is coated on a current collector foil, and then the negative pole piece for the lithium ion battery is prepared by baking, rolling and cutting.
2. The method for improving the overcharge and overdischarge performance of a lithium ion battery according to claim 1, wherein: the main active substance graphite is natural graphite, artificial graphite or a mixture of the natural graphite and the artificial graphite.
3. The method for improving the overcharge and overdischarge performance of a lithium ion battery according to claim 1 or 2, wherein: the secondary active substance hard carbon is at least one of asphalt-based hard carbon, biomass hard carbon and polymer-based hard carbon.
4. The method for improving the overcharge and overdischarge performance of a lithium ion battery according to claim 1 or 2, wherein: the mass ratio of the main active substance graphite to the secondary active substance hard carbon to the conductive agent to the binder is 55.2-82.8: 36.8-9.2: 6-4: 2-4, preferably 73.6: 18.4: 4:4.
5. the method for improving the overcharge and overdischarge performance of a lithium ion battery according to claim 1 or 2, wherein: the interlayer spacing d (002) of the secondary active material hard carbon is 0.3-0.4nm, preferably 0.38-0.39 nm.
6. The method for improving the overcharge and overdischarge performance of a lithium ion battery according to claim 1 or 2, wherein: the secondary active substance hard carbon has a specific surface area of 2.0-10.0 m2A particle size of less than 20 μm, preferably 5.0 to 7.5 m/g2(g) the particle size is less than 10 mu m.
7. The method for improving the overcharge and overdischarge performance of a lithium ion battery according to claim 1 or 2, wherein: the conductive agent is at least one of SPUERLI, CNT, KS-6, KS-15, SFG-6, Acetylene Black (AB), Ketjen Black (KB) and Vapor Grown Carbon Fiber (VGCF).
8. The method for improving the overcharge and overdischarge performance of a lithium ion battery according to claim 1 or 2, wherein: the binder is at least one of polyvinylidene fluoride (PVDF), sodium carboxymethylcellulose (CMC), Styrene Butadiene Rubber (SBR), polyacrylic acid (PAA), polyvinyl alcohol (PVA), Polyamide (PAI) and Polyethyleneimine (PEI).
9. The method for improving the overcharge and overdischarge performance of a lithium ion battery according to claim 1 or 2, wherein: the solvent is N-methyl pyrrolidone (NMP) or deionized water.
10. An anode material, characterized in that: the lithium ion battery is prepared by adopting the method for improving the overcharge and overdischarge performances of the lithium ion battery as claimed in any one of claims 1 to 9.
CN202110327807.6A 2021-03-26 2021-03-26 Method for improving overcharge and overdischarge performance of lithium ion battery Pending CN112838193A (en)

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Application publication date: 20210525