CN106558726A - A kind of titanium system negative electrode lithium ion battery - Google Patents
A kind of titanium system negative electrode lithium ion battery Download PDFInfo
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- CN106558726A CN106558726A CN201510617992.7A CN201510617992A CN106558726A CN 106558726 A CN106558726 A CN 106558726A CN 201510617992 A CN201510617992 A CN 201510617992A CN 106558726 A CN106558726 A CN 106558726A
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- battery
- lithium ion
- ion battery
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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
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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
- H01M4/485—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of mixed oxides or hydroxides for inserting or intercalating light metals, e.g. LiTi2O4 or LiTi2OxFy
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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
- 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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- General Chemical & Material Sciences (AREA)
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- Manufacturing & Machinery (AREA)
- Inorganic Chemistry (AREA)
- Battery Electrode And Active Subsutance (AREA)
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Abstract
The present invention relates to a kind of titanium system negative electrode lithium ion battery.It is characterized in that：Titanium system negative pole includes Lix+4/3Ti5/3O4(0≤x≤1) and TiNb2-xO7(0≤x≤0.1) two kinds of active substances, prepare flexible packaged battery core according to laminated process using PVDF polymer coatings barrier film, and lithium ion battery is obtained using hot pressing integral process after fluid injection.The present invention can reduce the negative battery system impact of " gassing " to the internal resistance of cell and capacity under the high temperature conditions of titanium system, so as to improve the high temperature service life of titanium system negative battery.
Description
Technical field
The invention belongs to technical field of electrochemistry, and in particular to a kind of titanium system negative electrode lithium ion battery.
Background technology
At present the negative material of commercialization lithium battery is mainly carbon negative pole material, such as electrographite, native graphite,
MCMB etc., but carbon negative pole material is due to its architectural characteristic, during lithium ion repeatedly deintercalation
Its change in volume can be made big, its cycle life is had a strong impact on, and which is relatively low to lithium current potential, during use
Lithium metal precipitation is easily caused, there is potential safety hazard.
Lithium titanate anode due in 1.55V, forming SEI films to lithium current potential, and there is no lithium and separate out and ask
Topic, therefore security performance is excellent, and due to zero strain characteristic, material itself has excellent stability.
New niobium titanium oxide negative material voltage platform is equally 1.55V, with gram volume it is high the characteristics of, it is but stable
Property it is slightly poor, therefore two kinds of negative poles are used in mixed way and can have complementary advantages, and further lift the energy density of titanium system negative pole.
But titanium system negative material is higher due to its activity, battery system easily " gassing ", can be led in high temperature environments
Internal resistance increase, capacity is caused to decline, so as to affect the life-span, this limits its application to a certain extent.People are led to
Additive is added to the electrolyte in battery system often and coating modification process is carried out to negative material, both
Mode can play a part of to delay battery producing gas, but can't thoroughly solve lithium titanate battery aerogenesis at present and ask
Topic.But by change battery manufacturing process, prepare containing polymer battery, can make positive/negative plate with every
Film is bonded to one, even if battery producing gas, also will not produce impact to internal resistance and capacity attenuation, such that it is able to
Improve the high temperature service life of titanium system negative battery.
Chinese patent 201310593540.0 discloses a kind of gel polymer energy storage lithium ion battery and its preparation
Method, the invention limit positive electrode as cladded type high voltage LiNi0.5Mn1.5O4Material, lithium titanate are negative pole,
Prepare high voltage lithium titanate battery.But high voltage system is proposed higher wanting to electrode material, electrolyte
Ask, bring unstable factor.The present invention uses conventional voltage positive electrode, high power capacity mixed with titanium system negative pole material
Material and hot pressing integral method, lift the energy density of titanium system negative battery from another angle, while preparing
Containing polymer battery, the high-temperature cycle life of battery is further improved.
The content of the invention
In order to improve the high temperature service life of titanium system negative pole system battery, the present invention propose a kind of titanium system negative pole lithium from
Sub- battery.Specifically technical scheme is：
A kind of titanium system negative electrode lithium ion battery, in the battery, battery core prepares battery by hot pressing integral process.
Wherein, positive/negative plate (at least negative plate), barrier film can be bonded to one by hot pressing integral process with smooth.
Wherein the negative pole of battery is titanium system negative pole, and which includes Lix+4/3Ti5/3O4(0≤x≤1), and TiNb2-xO7(0
≤ x≤0.1) two kinds of active substances, wherein TiNb2-xO7Gross activity material mass hundred shared by (0≤x≤0.1)
Divide than being 10%～50%.The barrier film of battery is polymer coating barrier film, by basement membrane and the polymer containing PVDF
Coating two parts are constituted.Basement membrane is polypropylene (PP), polyethylene (PE), polypropylene-polyethylene-polypropylene
(PP-PE-PP), one kind in polyimides (PI) or polyethylene terephthalate (PET)；PVDF
Polymer coating one side thickness is 1～5 μm.It is preferred that, PVDF polymer coatings are coated towards the one of negative plate
Face.
Wherein, the PVDF polymer for coating basement membrane is commercially available.
The positive pole includes one or more work in cobalt acid lithium, LiMn2O4, lithium nickelate or nickle cobalt lithium manganate
Property material, the electrolyte of the nonaqueous electrolytic solution includes LiPF6、LiClO4、LiAsF6, or LiCF3SO3
In one or more.
Hot pressing integral process prepares above-mentioned lithium ion battery, specifically includes following steps：
(1) by made by, negative plate, PVDF polymer coating barrier films, positive plate are according to lamination or wind work
Skill makes naked battery core, and battery core is encapsulated with aluminum plastic film, is reserved liquid injection port, is prepared into flexible-packed battery；
(2) inject the electrolyte in battery, hot pressing is carried out to battery, coated separator polymer swollen-state polymerization will
Together with pole piece and barrier film bond, form integration, it is hot-forming after battery is melted into, that is, this is obtained
Bright lithium ion battery.
Wherein, the hot pressing integral process prepares the battery, and in step (2), hot pressing temperature is 40～100 DEG C,
Time is 2h～10h, pressure≤0.5MPa,.
The present invention's is mainly characterized by：
(1) two kind of titanium based material Lix+4/3Ti5/3O4(0≤x≤1), and TiNb2-xO7(0≤x≤0.1) conduct
When negative electrode active material is used, with very high safety, niobium titanium oxide TiNb2-xO7(0≤x≤0.1)
With higher theoretical capacity, the present invention preferably TiNb2O7Actual specific capacity is 300mAh/g, compares metatitanic acid
The actual specific capacity of lithium 165mAh/g is higher.Therefore, adulterate in lithium titanate TiNb2O7It is used in mixed way, can be with
Its energy density is improved further.But two kinds of titanium system negative materials be respectively provided with activity it is higher the characteristics of, easily with
Electrolyte reacts, and causes the phenomenon of battery system " gassing ", so as to affect high temperature service life.Therefore originally
Invention improves the high temperature cyclic performance of high power capacity titanium system negative battery by improving battery preparation technique.
(2) lithium ion battery prepared by the present invention is existed at a certain temperature using barrier film coating PVDF polymer
It is swelling in electrolyte, hot pressing integral process is carried out to the battery core after fluid injection, makes the positive/negative plate, barrier film can
It is bonded to one with smooth so that, after hot environment " gassing ", gas will not for titanium system negative battery system
Retain in-between the electrodes, so as to caused by solving the problems, such as gas, the internal resistance of cell increases life time decay.
Description of the drawings
Fig. 1 is the schematic appearance of 25Ah batteries made by the present invention；Wherein, 1 is the electricity of flexible-packed battery
Core main body, the ledge 2 of upper and lower both sides is lug.
Fig. 2 is 60 DEG C of high-temperature cycle life figures of battery prepared by embodiment one.
Specific embodiment
More detailed explanation is done to a kind of titanium system negative electrode lithium ion battery of the invention with reference to specific embodiment.
But the present invention is not limited to following examples.
Embodiment one：
With cobalt acid lithium as positive electrode active materials, according to 94% positive electrode active materials (be based on positive pole quality), 3%
Electrically conductive graphite (being based on positive pole quality), the ratio of 3%PVDF (being based on positive pole quality) are dissolved in N- methylpyrroles
In alkanone solvent, in Vacuum mixer, mixing dispersion, is prepared into uniform bubble-free slurry, is coated in aluminium foil
On be prepared into positive plate.
With Li4/3Ti5/3O4And TiNb2O7By 8:2 mixed proportions as negative active core-shell material, according to 90% negative pole
Active material (being based on negative pole quality), 5% conductive black (being based on negative pole quality), 5%PVDF are (based on negative
Pole quality) ratio be dissolved in N-Methyl pyrrolidone solvent, in Vacuum mixer mixing dispersion, prepare
Uniformly bubble-free slurry, is coated on aluminium foil and is prepared into negative plate.
From with double-deck PP as basement membrane, the composite diaphragm of two-sided each 1 μm of oiliness PVDF coating.
Negative plate, PVDF coated separators, positive plate are adopted into lamination process, after being encapsulated with aluminum plastic film, electricity is made
Core.
Battery core is injected into electrolyte, after standing 24h, battery core is entered under the conditions of 50 DEG C, 6h, 0.4Mpa
Row hot pressing polymerization integration, is melted into battery afterwards, that is, titanium system negative electrode lithium ion battery is obtained.
Embodiment two：
With Li in the present embodiment4/3Ti5/3O4And TiNb2O7By 5:5 mixed proportions as negative active core-shell material, its
It is with embodiment one.
Embodiment three：
From with double-deck PP as basement membrane, the composite diaphragm of two-sided each 2 μm of oiliness PVDF coatings, other are same
Embodiment one.
Example IV：
From with double-deck PP as basement membrane, the composite diaphragm of 2 μm of oiliness PVDF coatings of one side is applied laminated
Towards negative plate, flexible packaged battery core is prepared according to laminated process.Other are with embodiment one.
Embodiment five：
Battery core carries out hot pressing under the conditions of 70 DEG C, 2h, 0.2Mpa and is polymerized integration system for lithium ion battery, its
It is with embodiment one.
Comparative example one：
With Li4/3Ti5/3O4And TiNb2O7By 8:2 mixed proportions as negative active core-shell material, from double-deck PP
Uncoated barrier film, prepares flexible package laminated type battery core, after chemical conversion, obtains final product lithium ion battery.
Comparative example two：
With Li4/3Ti5/3O4As negative active core-shell material, from the uncoated barrier films of double-deck PP, Soft Roll folding is prepared
Piece type battery core, after chemical conversion, obtains final product lithium ion battery.
Table 1 below show the performance comparison of battery made by above-described embodiment, and embodiment one is to embodiment five
After the micro- aerogenesis of 60 DEG C of high temperature circulation middle and late stage batteries, gas is present in made 25Ah polymer batteries
Between battery core and aluminum plastic film, battery core is harder, and pole piece is tight with barrier film bonding, no gas between electrode, because
This capacity do not have rapid decay, and embodiment one in 60 DEG C of high temperature circulation can keep 1100 times following
The ring life-span.But, due to the PVDF polymer conductivities in coated separator it is poor, therefore containing polymer should
The internal resistance of battery is higher, and power-performance slightly can be affected, and the bigger impact of coating layer thickness is more obvious.And it is right
Conventional lithium-ion battery made by ratio one, after high temperature circulation aerogenesis, battery core softens, under capacity is quick
Drop, life-span are relatively poor.Comparative example two is used alone Li4/3Ti5/3O4For negative pole, due to Li4/3Ti5/3O4Stability
More preferably, therefore cycle performance is slightly more better than comparative example one, but energy density is relatively low.Therefore, containing polymerization
Thing lithium ion battery, in terms of the high-temperature cycle life of titanium system negative battery is improved, has a clear superiority.
Table 1
Claims (10)
1. a kind of titanium system negative electrode lithium ion battery, it is characterised in that negative pole is titanium system negative pole, comprising Lix+4/3Ti5/3O4
(0≤x≤1)、TiNb2-xO7(0≤x≤0.1) two kinds of active substances, wherein TiNb2-xO7Account for gross activity thing
Matter mass ratio is 10%～50%.
2. lithium ion battery according to claim 1, it is characterised in that the battery is by battery core fluid injection
Hot pressing integration is obtained afterwards.
3. lithium ion battery according to claim 1 and 2, it is characterised in that the barrier film of the battery is poly-
Compound coated separator, is made up of with the polymer coating two parts containing PVDF basement membrane.
4. lithium ion battery according to claim 3, it is characterised in that the basement membrane be polypropylene (PP),
Polyethylene (PE), polypropylene-polyethylene-polypropylene (PP-PE-PP), polyimides (PI) or poly- to benzene
One kind in dioctyl phthalate second diester (PET).
5. the lithium ion battery according to claim 3 or 4, it is characterised in that the PVDF polymer is applied
Layer one side thickness is 1～5 μm, and single or double is coated on membrane surface；Such as one side coating, have during assembling
The one of PVDF coatings is facing to negative plate.
6. lithium ion battery according to claim 1 and 2, it is characterised in that the positive pole of battery includes cobalt acid
One or more active materials in lithium, LiMn2O4, lithium nickelate or nickle cobalt lithium manganate.
7. the lithium ion battery according to any of the above-described claim, it is characterised in that the hot pressing integration system
The standby lithium ion battery is obtained by the method for comprising the following steps：
(1) by made by, negative plate, barrier film, positive plate make naked battery core according to lamination or winding process, and battery core is used
Aluminum plastic film is encapsulated, and is reserved liquid injection port, is prepared into flexible-packed battery；
(2) inject the electrolyte in battery, hot pressing is carried out to battery, the polymer swollen-state polymerization of coated separator will
At least cathode pole piece together with barrier film bonding forms integration, afterwards battery is melted into, and obtains final product described
Lithium ion battery.
8. hot pressing integral process according to claim 7 prepares lithium ion battery, it is characterised in that hot pressing temperature
Spend for 40～100 DEG C, the time is 2h～10h, pressure≤0.5MPa.
9. lithium ion battery according to claim 1, it is characterised in that the battery using voltage range is
1.5V～2.8V.
10. the preparation method of the lithium ion battery according to any of the above-described claim, it is characterised in that the side
Method comprises the steps：
(1) by made by, negative plate, barrier film, positive plate make naked battery core according to lamination or winding process, and battery core is used
Aluminum plastic film is encapsulated, and is reserved liquid injection port, is prepared into flexible-packed battery；
(2) inject the electrolyte in battery, hot pressing is carried out to battery, the polymer swollen-state polymerization of coated separator will
At least cathode pole piece together with barrier film bonding forms integration, afterwards battery is melted into, and obtains final product described
Lithium ion battery.
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| CN201510617992.7A CN106558726A (en) | 2015-09-24 | 2015-09-24 | A kind of titanium system negative electrode lithium ion battery |
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| CN201510617992.7A CN106558726A (en) | 2015-09-24 | 2015-09-24 | A kind of titanium system negative electrode lithium ion battery |
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN109841830A (en) * | 2019-02-14 | 2019-06-04 | 河南电池研究院有限公司 | A kind of lithium ion battery negative material and preparation method thereof |
| CN110518196A (en) * | 2019-07-11 | 2019-11-29 | 高芳 | A kind of negative electrode material of lithium battery |
| CN114388869A (en) * | 2021-12-23 | 2022-04-22 | 荣盛盟固利新能源科技股份有限公司 | Gel polymer battery and preparation method thereof |
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