CN103531776B - The lithium ion battery and its positive electrode and chemical synthesizing method of high security extra long life - Google Patents
The lithium ion battery and its positive electrode and chemical synthesizing method of high security extra long life Download PDFInfo
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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
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- 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
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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
- H01M10/058—Construction or manufacture
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- 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
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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
- H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
- H01M10/44—Methods for charging or discharging
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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
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/131—Electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
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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
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- H—ELECTRICITY
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- 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
- H01M4/52—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron
- H01M4/525—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron of mixed oxides or hydroxides containing iron, cobalt or nickel for inserting or intercalating light metals, e.g. LiNiO2, LiCoO2 or LiCoOxFy
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- 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
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
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Abstract
The present invention relates to a kind of main active material and its battery formation method as lithium ion cell positive, main active material includes spinel structure LiMn2O4 LiMn in the anode2O4, the nickeliferous lithium transition-metal oxide and subadditive of main additive in alkalinity metal or nonmetal oxide.The lithium ion battery of the high security extra long life is made up of above-mentioned the positive electrode, the negative electrode and the separator of lamination or winding process, and wherein negative electrode active material is lithium titanate, and battery is prepared by specific chemical synthesizing method.Present invention is characterized in that being added in LiMn2O4 using nickeliferous lithium transition-metal oxide and in the metal or nonmetal oxide of alkalinity as major and minor additive, simultaneously, after being specifically melted into preparation, the production gas phenomenon that battery is in use can effectively be inhibited, solves the problems, such as the inflatable of battery, thus the advantages of playing high security specific to its material and extra long life to greatest extent.
Description
Technical field
The present invention relates to anodes made of a kind of anode material for lithium-ion batteries, the material, the electricity comprising the anode
The chemical synthesizing method more particularly to a kind of setting for the lithium ion secondary battery of power and stored energy application of pond and the battery
Meter and manufacturing field.
Background technique
Lithium ion battery is the new generation of green after nickel-metal hydride battery developed rapidly in early 1990s
High-energy rechargeable battery.It has monomer voltage is high, energy density is big, self-discharge rate is low, efficiency for charge-discharge is high, have extended cycle life,
Memory-less effect and advantages of environment protection, it has also become the master of the portable electronic products such as mobile phone, digital camera, laptop
Mating power supply is led, and starts to show up prominently in electric bicycle, electric car power supply.In recent years, with lithium ion battery
The continuous decline of the improved day by day and production cost of energy, application field and the market share are still constantly expanding.
Lithium ion battery positive and negative electrode material be all made of lithium ion can be freely embeddable and deviate from have stratiform or tunnel knot
The lithium ion inlaid scheme of structure.When charging, lithium ion is deviate from from anode, is embedded in cathode；When electric discharge, lithium ion is then de- from cathode
Out, insertion anode.I.e. in charge and discharge process, lithium ion is embedded in abjection in positive and negative interpolar and moves back and forth, like swinging back and forth
Rocking chair or the shuttlecock of reciprocating motion, therefore visually it is known as " rocking chair (rocking chair) " or " shuttlecock
(shuttlecock) " battery.
Currently, lithium titanate (the Li of spinel structure4Ti5O12) as lithium ion battery negative material of new generation, it is more next
More it is valued by people.Lithium titanate has the advantages that not available for traditional carbon material.Firstly, lithium titanate belongs to zero strain material
Expect, its skeleton remains unchanged in charge and discharge process；Secondly, its charge and discharge platform height (1.5V vs Li/Li+), gold will not occur
Belong to the deposition of lithium；Again, with lithium ion three-dimensional diffusion channel, lithium ion diffusion coefficient 1 quantity higher than carbon negative pole material
Grade.Replace carbon material as the cathode of lithium ion battery using lithium titanate, cycle life, safety and the power of battery can be improved
Performance, in recent years, the novel anode material as power and energy-storage battery are got growing concern for.In addition, with tradition
Lithium ion cell anode material lithium cobaltate is compared, the LiMn2O4 (LiMn of spinel structure2O4) have that abundant raw material, price be low, nothing
Environmental pollution, easily recycling, the advantages that current potential is high and safety is good.Therefore, use LiMn2O4 for anode, the lithium that lithium titanate is cathode
Ion battery can take into account many advantages such as safety, long-life and low cost, it is considered to be power and the great prospect of energy storage field
Battery system.
However, under study for action it has been found that traditional lithium titanate/lithium manganate battery is easy to produce gas in cyclic process
Body so as to cause battery impedance increase, performance rapid decay, or even when inner pressure of battery reaches a certain level, causes battery case
Body rupture, occurs safety accident.This fatal disadvantage, before the development of lithium titanate/LiMn2O4 system lithium ion battery light
Scape has coverd with the shade for being difficult to disperse together.Flatulence problem becomes system lithium ion battery bottleneck problem urgently to be resolved.
Summary of the invention
In order to solve above-mentioned practical problem, the present invention provides a kind of improved lithium titanate/LiMn2O4 system lithium-ion electrics
Pond designs and manufactures method, and this method can efficiently solve the flatulence problem of the system battery, is produced with this method
Battery can give full play of the characteristics of high security possessed by the material system and extra long life.
First aspect of the present invention provides a kind of anode material for lithium-ion batteries, and the positive electrode includes main active material
Material, the main active material includes spinel structure LiMn2O4 LiMn2O4, main additive and subadditive.
The main additive refers to nickeliferous lithium transition-metal oxide；The subadditive refers to the metal or non-gold in alkalinity
Belong to oxide.
In first aspect of the present invention, in the main active material, the spinel structure LiMn2O4, main addition
Agent and subadditive mass percentage are preferably (60%-95%): (35%-5%): (5%-0%).
In first aspect of the present invention, the main additive is selected from lithium nickelate, lithium nickel cobalt dioxide, nickel ion doped and nickel cobalt
One or more of combinations of LiMn2O4.
In first aspect of the present invention, the subadditive is selected from aluminium oxide, calcium oxide, zirconium oxide, zinc oxide, oxygen
One or more of combinations of SiClx.
In first aspect of the present invention, the positive electrode further includes conductive agent and binder.
Wherein, main active material, conductive agent and binder mass percentage are preferably (60%-99%): (30%-0%):
(10%-1%).
Wherein, the conductive agent is selected from the combination of one or more of acetylene black, furnace black, VGCF, carbon nanotube.
Wherein, the binder is selected from the combination of one or more of SBR, PVDF.
The second aspect of the present invention provides a kind of lithium ion cell positive, and the anode includes the present invention first
Positive electrode described in aspect.
The lithium ion cell positive described in the second aspect of the present invention is coated on substrate by the positive electrode and is prepared
It obtains；Wherein the substrate can be any conductive material, such as Cu, Al, Ag or electrical conductivity alloy, and preferably Al.
Third aspect of the present invention provides a kind of lithium ion battery of high security extra long life, including the present invention second
Anode described in a aspect further includes cathode and diaphragm.
The cathode further includes lithium titanate, conductive agent and binder.
Wherein lithium titanate, conductive agent and binder mass percentage are preferably (60%~99%): (30%~0%): (10%
~1%).
Wherein, the conductive agent is selected from the combination of one or more of acetylene black, furnace black, VGCF, carbon nanotube.
Wherein, the binder is selected from the combination of one or more of SBR, PVDF.
Negative electrode of lithium ion battery described in third aspect of the present invention is coated on substrate by the negative electrode material and is prepared
It obtains；Wherein the substrate can be any conductive material, such as Cu, Al, Ag or electrical conductivity alloy, and preferably Al.
The 4th aspect of the present invention provides a kind of lithium ion battery production method of high security extra long life, battery by
Anode described in the second aspect of the present invention and cathode and diaphragm are made up of lamination or winding process.
In the 4th aspect of the present invention, the chemical synthesizing method of the lithium ion battery of the high security extra long life includes:
It shelves early period, no less than one charging process or charge and discharge cycles process and later period shelve three phases.
Wherein, finger is shelved early period before charge and discharge cycles, and battery is opened a way at 45 DEG C -80 DEG C and is shelved 12-48 hours.
Wherein, in one or more steps of charge or discharge process, electric current is the battery not less than 0.5C(C
Nominal capacity), more preferably scheme is: being made of constant current-constant-voltage charge/constant-current discharge cyclic process of one or more, constant current
Charging/constant-current discharge stage electric current is 1-5C.
Wherein, the later period shelves finger after charge and discharge cycles, and battery is opened a way at 45 DEG C -80 DEG C and is shelved 12-48 hours.
Above-mentioned various aspects of the invention and its various preferred embodiments in the absence of special restrictions can be by these
Field technical staff is unrestricted to be combined.
The present invention can efficiently solve the flatulence phenomenon that traditional lithium titanate/lithium manganate battery generates in cyclic process
Reason show themselves in that using nickeliferous lithium transition-metal oxide and in alkalinity metal or nonmetal oxide as major and minor addition
Agent is added in LiMn2O4, and additive material can consume the acidic corrosives substances such as moisture, free acid in electrolyte, protection electricity
Pond main material produces gas to reduce in battery process recycling；Meanwhile battery is joined in battery after specific fertilizer alleviant
It is sufficiently decomposed with the unstable material of battery producing gas, to reduce it in battery normal circulation use to the unfavorable shadow of battery
It rings, so that battery be inhibited to produce gas in use, solves the problems, such as the inflatable of battery.Using a process for preparing lithium titanate/manganese
Sour lithium system lithium ion battery can sufficiently eliminate inflatable to the adverse effect of battery, to play its material to greatest extent
The advantages of expecting specific high security and extra long life, sufficiently meets the requirement of power and stored energy application field.In addition,
The method is easy to operate, and effect is obvious, and existing lithium ion battery production equipment can be used completely and produced, do not increase any
Production cost and technology difficulty are highly suitable for being mass produced.
Detailed description of the invention
Fig. 1 is the cycle performance curve comparison figure of comparative example Yu embodiment lithium ion battery.
Fig. 2 is comparative example and appearance comparison diagram of the embodiment lithium ion battery after recycling for a long time.
Specific embodiment
It is conventional using pure LiMn2O4 as the main active material preparation of anode first in order to fully demonstrate implementation result of the invention
11198148 type laminated aluminum film rectangular lithium ion batteries.Specific step is as follows.
Comparative example
After LiMn2O4 is mixed with Supper P, Kynoar according to 92: 4: 4 weight ratio, it is dissolved in N- methyl
In pyrrolidones, anode sizing agent is made in uniform stirring, is then coated, is dried according to conventional lithium ion battery manufacture process
It does, roll, cutting positive plate is made；Lithium titanate is mixed with Supper P, Kynoar according to 92: 4: 4 weight ratio
Afterwards, it is dissolved in N-Methyl pyrrolidone, negative electrode slurry is made in uniform stirring, then manufactures work according to conventional lithium ion battery
Skill is coated, dries, rolling, cuts negative electrode tab is made；Positive and negative plate is separated with diaphragm, using zigzag lamination, is made
Battery core is passing through the processes such as welding, encapsulation, baking, fluid injection, battery is made.Battery is melted by conventional method, i.e., is filled with 0.1C
Electricity 1 time.Finally, battery is carried out vacuum evacuation sealing, final products are made.
Preparing lithium ion battery using method provided by the invention, specific step is as follows.
Embodiment 1
Using nickle cobalt lithium manganate LiNi1/3Co1/3Mn1/3O2And aluminium oxide Al2O3Respectively as major and minor additive, LiMn2O4
It is mixed with major and minor additive according to the ratio that mass percentage is 90%, 9%, 1% and constitutes main active material, by main active material
After being mixed with Supper P, Kynoar according to 92: 4: 4 weight ratio, it is dissolved in N-Methyl pyrrolidone, uniformly stirs
Then mixing is coated according to conventional lithium ion battery manufacture process, dries, rolling, cutting and be made just at anode sizing agent
Pole piece；After lithium titanate is mixed with Supper P, Kynoar according to 92: 4: 4 weight ratio, it is dissolved in N- methylpyrrole
In alkanone, negative electrode slurry is made in uniform stirring, is then coated, dries, is ground according to conventional lithium ion battery manufacture process
It presses, cut negative electrode tab is made；Positive and negative plate is separated with diaphragm, using zigzag lamination, battery core is made, by welding, envelope
The processes such as dress, baking, fluid injection, are made battery.The chemical synthesizing method of battery are as follows: battery is opened a way at 60 DEG C and is shelved 24 hours；With
1C charge and discharge cycles 5 times；Then battery is fully charged with 1C, it opens a way and shelves 24 hours at 70 DEG C.Finally, battery is carried out true
Empty exhaust sealing, is made final products.
Embodiment 2
Using nickle cobalt lithium manganate LiNi1/3Co1/3Mn1/3O2With calcium oxide CaO respectively as major and minor additive, LiMn2O4 with
The ratio mixing that major and minor additive is 90%, 8%, 2% according to mass percentage constitutes main active material, by main active material with
After Supper P, Kynoar are according to 92: 4: 4 weight ratio mixing, it is dissolved in N-Methyl pyrrolidone, uniform stirring
Anode sizing agent is made, is then coated, dries according to conventional lithium ion battery manufacture process, rolling, cutting anode is made
Piece；After lithium titanate is mixed with Supper P, Kynoar according to 92: 4: 4 weight ratio, it is dissolved in N- crassitude
In ketone, negative electrode slurry is made in uniform stirring, be then coated, dry according to conventional lithium ion battery manufacture process, rolling,
It cuts and negative electrode tab is made；Positive and negative plate is separated with diaphragm, using zigzag lamination, battery core is made, by welding, encapsulation,
The processes such as baking, fluid injection, are made battery.The chemical synthesizing method of battery are as follows: battery is opened a way at 60 DEG C and is shelved 36 hours；It is filled with 2C
Discharge cycles 5 times；Then battery is fully charged with 1C, it opens a way and shelves 24 hours at 70 DEG C.Finally, battery is carried out vacuum row
Sealing gland mouth, is made final products.
Safety is carried out with embodiment lithium ion battery to comparative example according to the requirement of national standard GB/T18287-2000 and is filled
Discharge cycle performance test, test result is as shown in table 1, Fig. 1 and Fig. 2.As it can be seen from table 1 comparative example and embodiment battery
It can be tested by security performance, and embodiment battery is in short circuit and considerably lower, this embodiment that overcharges temperature in test process
Lithium titanate/advantage of the LiMn2O4 system lithium ion battery in terms of safety；From figure 1 it appears that when having recycled 800 times
After, the capacity of embodiment battery is still in 20000mAh or so, and comparative example battery capacity is via under 20000mAh or so
16000mAh or so is dropped to, this illustrates that embodiment battery has excellent cycle performance；As shown in Fig. 2, being followed in long-term charge and discharge
During ring, after having recycled 800 times, comparative example cell thickness increasing degree is larger, increases to 21mm from 11mm, shows its hair
More serious flatulence has been given birth to, and embodiment cell thickness is always maintained within the scope of 11-12mm, does not find significant change, is shown
Embodiment battery flatulence phenomenon is significantly suppressed.
The safety test result of 1 comparative example of table and embodiment battery
It is from above-described embodiment as can be seen that provided by the present invention by spinel structure LiMn2O4 LiMn2O4, main additive
The master that nickeliferous lithium transition-metal oxide and subadditive is constituted by a certain percentage in the metal or nonmetal oxide of alkalinity
Active material and its battery formation method can effectively inhibit traditional lithium titanate/lithium manganate battery and generate in cyclic process
Flatulence phenomenon, so that the advantages of playing high security specific to its material and extra long life to greatest extent, sufficiently meets
The requirement of power and stored energy application field.
Specific embodiments of the present invention are described in detail above, but it is merely an example, the present invention is simultaneously unlimited
It is formed on particular embodiments described above.To those skilled in the art, any couple of present invention carries out equivalent modifications and
Substitution is also all among scope of the invention.Therefore, without departing from the spirit and scope of the invention made by equal transformation and
Modification, all should be contained within the scope of the invention.
Claims (5)
1. a kind of lithium ion battery, it is characterised in that: including anode, cathode and diaphragm；
Wherein, the anode includes main active material, and the main active material includes spinel structure LiMn2O4 LiMn2O4, master add
Add agent and subadditive；The main additive be selected from one of lithium nickelate, lithium nickel cobalt dioxide, nickel ion doped and nickle cobalt lithium manganate with
On；The subadditive is selected from one or more of aluminium oxide, calcium oxide, zirconium oxide, silica；Also, the spinelle knot
Structure LiMn2O4, main additive and subadditive mass percentage are (60%-95%): (35%-5%): (5%-1%)；
The cathode includes lithium titanate, conductive agent and binder；Wherein lithium titanate, conductive agent and binder mass percentage are
(60%-99%): (30%-0%): (10%-1%).
2. lithium ion battery according to claim 1, which is characterized in that the anode further includes conductive agent and binder.
3. lithium ion battery according to claim 1, which is characterized in that the main active material, conductive agent and binder
Mass percentage be (60%-99%): (30%-0%): (10%-1%)；The conductive agent be selected from acetylene black, furnace black,
One or more of VGCF, carbon nanotube；The binder is selected from one of SBR, PVDF.
4. a kind of chemical synthesizing method of lithium ion battery described in claim 1, characterized by comprising: shelve early period, no less than
One charging process or charge and discharge cycles process and later period shelve three phases.
5. the chemical synthesizing method of lithium ion battery according to claim 4, it is characterised in that: shelve finger early period and followed in charge and discharge
Before ring, battery is opened a way at 45 DEG C -80 DEG C and is shelved 12-48 hours；In at least one step of charge or discharge process,
Electric current is not less than 0.5C；Later period shelves finger after charge and discharge cycles, and battery is opened a way at 45 DEG C -80 DEG C, and it is small to shelve 12-48
When.
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| CN104934633A (en) * | 2014-03-21 | 2015-09-23 | 江苏海四达电源股份有限公司 | Cylindrical 2000 mAh lithium-ion power battery with large current rapid charging/discharging performance |
| CN105514326B (en) * | 2015-01-16 | 2018-02-13 | 万向一二三股份公司 | A kind of composite diaphragm and the power lithium titanate battery containing the composite diaphragm |
| CN105810887A (en) * | 2016-03-17 | 2016-07-27 | 苏州宇量电池有限公司 | Positive plate capable of improving lithium nickel manganese oxide battery capacity and lithium nickel manganese oxide battery applying positive electrode plate |
| CN107403908A (en) * | 2017-07-05 | 2017-11-28 | 天津普兰能源科技有限公司 | A kind of method for suppressing lithium titanate battery flatulence |
| CN109378520B (en) * | 2018-11-13 | 2021-03-26 | 上海电气国轩新能源科技有限公司 | Nickel cobalt lithium manganate and lithium titanate system battery and preparation method thereof |
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| CN101388448A (en) * | 2006-09-14 | 2009-03-18 | 日产自动车株式会社 | Positive electrode for non-aqueous electrolyte secondary battery and non-aqueous electrolyte secondary battery using the same |
| CN102263288A (en) * | 2011-06-29 | 2011-11-30 | 上海空间电源研究所 | High-power lithium ion storage battery and manufacturing method thereof |
| CN103187554A (en) * | 2011-12-28 | 2013-07-03 | 上海空间电源研究所 | Manganese-based composite electrode, lithium-ion battery containing manganese-based composite electrode, and preparation method |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101388448A (en) * | 2006-09-14 | 2009-03-18 | 日产自动车株式会社 | Positive electrode for non-aqueous electrolyte secondary battery and non-aqueous electrolyte secondary battery using the same |
| CN102263288A (en) * | 2011-06-29 | 2011-11-30 | 上海空间电源研究所 | High-power lithium ion storage battery and manufacturing method thereof |
| CN103187554A (en) * | 2011-12-28 | 2013-07-03 | 上海空间电源研究所 | Manganese-based composite electrode, lithium-ion battery containing manganese-based composite electrode, and preparation method |
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