CN110444803A - A kind of lithium ion battery structure of semisolid and preparation method thereof - Google Patents

A kind of lithium ion battery structure of semisolid and preparation method thereof Download PDF

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Publication number
CN110444803A
CN110444803A CN201810417141.1A CN201810417141A CN110444803A CN 110444803 A CN110444803 A CN 110444803A CN 201810417141 A CN201810417141 A CN 201810417141A CN 110444803 A CN110444803 A CN 110444803A
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lithium ion
semisolid
ion battery
negative electrode
polyolefin
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不公告发明人
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Suzhou Hua Qian Era Amperex Technology Ltd
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Suzhou Hua Qian Era Amperex Technology Ltd
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    • HELECTRICITY
    • H01BASIC ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00Secondary cells; Manufacture thereof
    • H01M10/05Accumulators with non-aqueous electrolyte
    • H01M10/052Li-accumulators
    • H01M10/0525Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • HELECTRICITY
    • H01BASIC ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00Secondary cells; Manufacture thereof
    • H01M10/05Accumulators with non-aqueous electrolyte
    • H01M10/058Construction or manufacture
    • YGENERAL 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
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02EREDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10Energy storage using batteries
    • YGENERAL 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
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02PCLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50Manufacturing or production processes characterised by the final manufactured product

Abstract

The invention discloses lithium ion battery structures of a kind of semisolid and preparation method thereof, the battery structure includes positive plate, polyolefin-based gel polymer electrolyte film and negative electrode tab, polyolefin-based gel polymer electrolyte film is set between positive plate and negative electrode tab, and lithium ion conducts between positive plate and negative electrode tab by polyolefin-based gel polymer electrolyte film.The coupled structure of polymer dielectric and liquid electrolyte forms gel electrolyte film layer, first polymer dielectric ionic conductivity with higher in the present invention, and electrochemical stability and thermal stability are good, good imbibition, water retainability;By using common polyalkene diaphragm as supporting base material, and gelatin polymer is coated on it, form gel polymer electrolyte film layer, so as to do not increase require higher production equipment under the premise of, produce safer, higher quality semisolid lithium ion battery, and simple process, production cost are low.

Description

A kind of lithium ion battery structure of semisolid and preparation method thereof
Technical field
The invention belongs to electrochemical fields, and in particular to a kind of lithium ion battery structure of semisolid and preparation method thereof.
Background technique
Lithium ion battery is a kind of Novel rechargeable battery to grow up nearly ten years, its energy density per unit volume and mass ratio Energy is high, and memory-less effect is environmentally protective, and discharge voltage is 3 times of ni-Cd and nickel-metal hydride battery, thus just receives once coming out People's is extensive note that development is very fast.
The lithium ion battery of domestic production at present is mostly soft-package battery, and this battery thermal stability is poor, and pressure resistance is impacted, again Power impact, needle thorn etc. are easy to happen applause or explosion, and security performance is low;And as lithium ion battery is to large-sized power power supply The demand of field application rapidly develops, and the capacity and energy density of battery constantly increase, and current ratio and power density are also continuous It improves, to keep the safety problem of lithium ion battery increasingly prominent.One most outstanding the problem of being exactly lithium dendrite growth at present: Using in the lithium ion battery of liquid electrolyte, when the content of lithium embedded in graphite has been more than the range that it is born, that Extra lithium ion will be combined with the electronics to shuttle in cathode, start to deposit in negative terminal surface, thus formed Dendritic metal lithium simple substance, growth will puncture diaphragm to a certain extent, cause internal short-circuit of battery, seriously threaten personal peace Entirely.The self stability of lithium ion internal material is not good enough also to directly result in batteries caught fire, explosion.
Have producer in the world and produced polymer battery (solid state battery), has well solved the above problem, But production equipment required for the above-mentioned solid polymer cell of production is expensive, and manufacturing process is complicated, results in cost It is relatively high.Since the oxide ion of anode layer is easier to attract lithium ion than the polymer Li-ion of solid electrolyte layer, because This will form the layer for lacking lithium ion in the region of the anode layer side of electrolyte, due to lacking lithium ion, depletion layer tool There is high resistivity, therefore the capacity of battery can be made to reduce.If preventing the capacity of lithium battery from reducing will definitely increase anode The thickness of layer, and manufacture difficulty also will increase.
Summary of the invention
In order to solve the above-mentioned technical problems, the present invention provides a kind of lithium ion battery structure of semisolid and its preparation sides Method.
In order to achieve the above object, technical scheme is as follows:
The present invention provides a kind of lithium ion battery structure of semisolid, including positive plate, polyolefin-based gelatin polymer electricity Solution plasma membrane and negative electrode tab, polyolefin-based gel polymer electrolyte film are set between positive plate and negative electrode tab, and lithium ion passes through Polyolefin-based gel polymer electrolyte film conducts between positive plate and negative electrode tab.
The present invention also provides a kind of preparation methods of the lithium ion battery structure of semisolid, comprising the following steps:
The preparation of S1, polyolefin-based gel polymer electrolyte film:
S11, PVDF-HFP copolymer is placed into freeze-day with constant temperature 10-12h in vacuum oven, removes moisture therein, it is close It seals spare;
S12, according to the ratio of mass ratio 5: 95~15: 85 PVDF-HFP is dissolved in organic solvent at room temperature, 60 DEG C Magnetic agitation 4-8h;
S13, pore creating material is slowly added into solution, above-mentioned coating solution is coated onto the two of PE diaphragm using dipping process Side is first dried at room temperature for placing into evaporate solvent and removing residual solvent in vacuum oven, it is porous to obtain composition polymer Film;
S14, composition polymer perforated membrane is cut into disk, is transferred to glove box, immersed electrolyte, fully absorb electrolysis to film Up to polyolefin-based gel polymer electrolyte film after liquid;
The preparation of S2, positive plate:
S21, positive active material is uniformly mixed first, in accordance with mass ratio 8: 1-7: 2 with conductive agent acetylene black, is added The Kynoar solution that mass fraction is 5%, stirring form uniform positive slurry;
S22, the slurry is uniformly coated on aluminium foil, is then dried at 100-140 DEG C, roll-in, punching is made just Pole piece;
The preparation of S3, negative electrode tab:
S31, negative electrode active material natural graphite is uniformly mixed with conductive agent acetylene black according to mass ratio 8: 1-7: 2, then The Kynoar solution that mass fraction is 10% is added, stirring forms uniform cathode slurry;
S32, cathode slurry is uniformly coated on copper foil, is then dried at 100-140 DEG C, roll-in, punching is made Negative electrode tab;
S4, assembling:
Positive plate obtained above, polyolefin-based gel polymer electrolyte film and negative electrode tab successively lamination and are packed into knob It detains in battery, ageing, sealing obtains the lithium ion battery structure of semisolid.
As a preferred option, organic solvent is acetone, N-Methyl pyrrolidone, N, N- dimethyl formyl in step S12 One of amine is a variety of.
As a preferred option, the pore creating material in step S13 is water, isopropanol or the butanol of 5-15%wt.
As a preferred option, the electrolyte in step S14 is PC the and EC electrolyte or 1mol/L of 1mol/L LiPF6 The volume ratio of EC, DEC and DMC electrolyte of LiPF6, PC and EC are 1: 1, and the volume ratio of EC, DEC and DMC are 1: 1: 1.
As a preferred option, the electrolyte in step S14 is one of LiClO4, LiBF4, LiAsF6.
As a preferred option, the positive active material in step S21 is LiFePO4、LiCoO2、LiMn2O4, Li (Ni, Co, Mn) O2One of.
The invention has the following advantages: the coupled structure of polymer dielectric and liquid electrolyte is formed in the present invention Gel electrolyte film layer, first polymer dielectric ionic conductivity with higher, electrochemical stability and thermal stability are good, Good imbibition, water retainability;The polymer and electrolyte of gelatinization are mixed into gelated electrolyte, so as to avoid organic electrolyte Leakage, improve the security performance of battery;By using common polyalkene diaphragm as supporting base material, and coating is solidifying on it Xanthan polymer, formed gel polymer electrolyte film layer, so as to do not increase require higher production equipment under the premise of, Safer, higher quality semisolid lithium ion battery is produced, and simple process, production cost are low.
Specific embodiment
The following detailed description of the preferred embodiment of the present invention.
In order to reach the purpose of the present invention, provided in one of embodiment of the invention the lithium of semisolid a kind of from Sub- battery structure, including positive plate, polyolefin-based gel polymer electrolyte film and negative electrode tab, polyolefin-based gelatin polymer electricity Solution plasma membrane is set between positive plate and negative electrode tab, lithium ion by polyolefin-based gel polymer electrolyte film in positive plate and It is conducted between negative electrode tab.
Embodiment 1
The present invention also provides a kind of preparation methods of the lithium ion battery structure of semisolid, comprising the following steps:
The preparation of S1, polyolefin-based gel polymer electrolyte film:
S11, PVDF-HFP copolymer is put into vacuum oven freeze-day with constant temperature 12h, removes moisture therein, sealed standby With;
S12, PVDF-HFP is dissolved in acetone (ratio according to 5: 95) at room temperature, 60 DEG C of magnetic agitation 6h;
S13, the water for being slowly added to 5%wt are pore creating material into solution;Above-mentioned coating solution is coated onto using dipping process The two sides of PE diaphragm are first dried at room temperature for that it is molten to place into vacuum oven (50 DEG C, 12h) removing residual to evaporate acetone Agent obtains composition polymer perforated membrane;
S14, the electrolyte after pore-creating is cut into disk, is transferred to glove box, immerse PC (the poly- carbonic acid of 1mol/L LiPF6 Ester)+EC (ethylene carbonate) (volume ratio 1: 1) electrolyte, it is poly- up to polyolefin-based gel after film fully absorbs electrolyte Polymer electrolyte membrane;
The preparation of S2, positive plate:
S21, first by 0.64 gram of positive active material LiFePO4It is uniformly mixed with 0.08 gram of conductive agent acetylene black, then plus Enter Kynoar (PVDF) solution (solvent is n-methyl-2-pyrrolidone) that 1.6 gram mass scores are 5%, stirring is formed Uniform anode slurry;
S22, the slurry is uniformly coated on aluminium foil, is then dried at 120 DEG C, roll-in, punching is made radius and is 12 millimeters and 80 microns of thickness of round positive plate;
The preparation of S3, negative electrode tab:
S31,1.00 grams of negative electrode active material natural graphites are uniformly mixed with 0.05 gram of conductive agent acetylene black, are added Kynoar (PVDF) solution (solvent is n-methyl-2-pyrrolidone) that 1.25 gram mass scores are 10%, stirring are formed Uniform cathode slurry;
S32, cathode slurry is uniformly coated on copper foil, is then dried at 120 DEG C, roll-in, radius is made in punching The round negative electrode tab for being 70 microns for 14 millimeters and thickness;
S4, assembling:
Positive plate obtained above, polyolefin-based gel polymer electrolyte film and negative electrode tab successively lamination and are packed into knob It detains in battery, is conventionally aged, sealing obtains the lithium ion battery structure of semisolid.
Embodiment 2
The present invention also provides a kind of preparation methods of the lithium ion battery structure of semisolid, comprising the following steps:
The preparation of S1, polyolefin-based gel polymer electrolyte film:
S11, PVDF-HFP copolymer is put into vacuum oven freeze-day with constant temperature 12h, removes moisture therein, sealed standby With;
S12, PVDF-HFP is dissolved in N-Methyl pyrrolidone (ratio according to 15: 85) at room temperature, 60 DEG C of magnetic force Stir 6h;
S13, the butanol for being slowly added to 5%wt are pore creating material into solution.Above-mentioned coating solution is applied using dipping process To the two sides of PE diaphragm, first it is dried at room temperature for placing into vacuum oven (50 DEG C, 12h) to evaporate acetone and removing residual Solvent obtains composition polymer perforated membrane;
S14, the electrolyte after pore-creating is cut into disk, is transferred to glove box, immerse PC (the poly- carbonic acid of 1mol/L LiPF6 Ester)+EC (ethylene carbonate) (volume ratio 1: 1) electrolyte, it is poly- up to polyolefin-based gel after film fully absorbs electrolyte Polymer electrolyte membrane;
The preparation of S2, positive plate:
S21, first by 0.64 gram of positive active material LiFePO4It is uniformly mixed with 0.08 gram of conductive agent acetylene black, then plus Enter Kynoar (PVDF) solution (solvent is n-methyl-2-pyrrolidone) that 1.6 gram mass scores are 5%, stirring is formed Uniform anode slurry;
S22, the slurry is uniformly coated on aluminium foil, is then dried at 120 DEG C, roll-in, punching is made radius and is 12 millimeters and 80 microns of thickness of round positive plate;
The preparation of S3, negative electrode tab:
S31,1.00 grams of negative electrode active material natural graphites are uniformly mixed with 0.05 gram of conductive agent acetylene black, are added Kynoar (PVDF) solution (solvent is n-methyl-2-pyrrolidone) that 1.25 gram mass scores are 10%, stirring are formed Uniform cathode slurry;
S32, cathode slurry is uniformly coated on copper foil, is then dried at 120 DEG C, roll-in, radius is made in punching The round negative electrode tab for being 70 microns for 14 millimeters and thickness;
S4, assembling:
Positive plate obtained above, polyolefin-based gel polymer electrolyte film and negative electrode tab successively lamination and are packed into knob It detains in battery, is conventionally aged, sealing obtains the lithium ion battery structure of semisolid.
Embodiment 3
The present invention also provides a kind of preparation methods of the lithium ion battery structure of semisolid, comprising the following steps:
The preparation of S1, polyolefin-based gel polymer electrolyte film:
S11, PVDF-HFP copolymer is put into vacuum oven freeze-day with constant temperature 12h, removes moisture therein, sealed standby With;
S12, PVDF-HFP is dissolved in n,N-Dimethylformamide (ratio according to 15: 85) at room temperature, 60 DEG C of magnetic Power stirs 6h;
S13, isopropanol (5%wt) is slowly added into solution as pore creating material.Using dipping process by above-mentioned coating solution The two sides of PE diaphragm are coated onto, are first dried at room temperature for that it is residual to place into vacuum oven (70 DEG C, 12h) removing to evaporate acetone Solvent is stayed, composition polymer perforated membrane is obtained;
S14, the electrolyte after pore-creating is cut into disk, is transferred to glove box, immerse PC (the poly- carbonic acid of 1mol/L LiPF6 Ester)+EC (ethylene carbonate) (volume ratio 1: 1) electrolyte, it is poly- up to polyolefin-based gel after film fully absorbs electrolyte Polymer electrolyte membrane;
The preparation of S2, positive plate:
S21, first by 0.64 gram of positive active material LiFePO4It is uniformly mixed with 0.08 gram of conductive agent acetylene black, then plus Enter Kynoar (PVDF) solution (solvent is n-methyl-2-pyrrolidone) that 1.6 gram mass scores are 5%, stirring is formed Uniform anode slurry;
S22, the slurry is uniformly coated on aluminium foil, is then dried at 120 DEG C, roll-in, punching is made radius and is 12 millimeters and 80 microns of thickness of round positive plate;
The preparation of S3, negative electrode tab:
S31,1.00 grams of negative electrode active material natural graphites are uniformly mixed with 0.05 gram of conductive agent acetylene black, are added Kynoar (PVDF) solution (solvent is n-methyl-2-pyrrolidone) that 1.25 gram mass scores are 10%, stirring are formed Uniform cathode slurry;
S32, cathode slurry is uniformly coated on copper foil, is then dried at 120 DEG C, roll-in, radius is made in punching The round negative electrode tab for being 70 microns for 14 millimeters and thickness;
S4, assembling:
Positive plate obtained above, polyolefin-based gel polymer electrolyte film and negative electrode tab successively lamination and are packed into knob It detains in battery, is conventionally aged, sealing obtains the lithium ion battery structure of semisolid.
Comparative example 1
As a comparison using commercialized polyalkene diaphragm Celgard2400, polyalkene diaphragm Celgard2400 is carried out Characterization, gained characterization result are listed in table 1.
The polyolefin-based gel polymer electrolyte film of table 1 and Celgard2400 membrane properties test result
From the results shown in Table 1, the polyolefin-based gel polymer electrolyte prepared using method provided by the invention Plasma membrane has high temperature resistant, higher conductivity and high mechanical strength, meets the requirement of lithium ion battery electrolyte, from embodiment 1- 3 and the test result of comparative example 1 can be seen that the resistance to shrinking percentage of commercialized polyalkene diaphragm and transverse tensile strength is all very poor.
In addition, being listed in Table 2 below to above-described embodiment progress battery high temperature resistance and life test, acquired results.
2 battery high temperature resistance of table and life test
From the results shown in Table 2, the semisolid prepared with polyolefin-based gel polymer electrolyte film of the invention Lithium ion battery has better security performance and longer service life.
What has been described above is only a preferred embodiment of the present invention, it is noted that for those of ordinary skill in the art For, without departing from the concept of the premise of the invention, various modifications and improvements can be made, these belong to the present invention Protection scope.

Claims (7)

1. a kind of lithium ion battery structure of semisolid, which is characterized in that including positive plate, polyolefin-based gel polymer electrolyte Plasma membrane and negative electrode tab, polyolefin-based gel polymer electrolyte film are set between positive plate and negative electrode tab, and lithium ion is by poly- Alkylene gel polymer electrolyte film conducts between positive plate and negative electrode tab.
2. a kind of preparation method of the lithium ion battery structure of semisolid as described in claim 1, which is characterized in that including with Lower step:
The preparation of S1, polyolefin-based gel polymer electrolyte film:
S11, PVDF-HFP copolymer is placed into freeze-day with constant temperature 10-12h in vacuum oven, removes moisture therein, sealed standby With;
S12, according to the ratio of mass ratio 5: 95~15: 85 PVDF-HFP is dissolved in organic solvent at room temperature, 60 DEG C of magnetic force Stir 4-8h;
S13, pore creating material is slowly added into solution, above-mentioned coating solution is coated onto the two sides of PE diaphragm using dipping process, first It is dried at room temperature for placing into evaporate solvent and removing residual solvent in vacuum oven, obtains composition polymer perforated membrane;
S14, composition polymer perforated membrane is cut into disk, is transferred to glove box, electrolyte is immersed, after film fully absorbs electrolyte Up to polyolefin-based gel polymer electrolyte film;
The preparation of S2, positive plate:
S21, positive active material is uniformly mixed first, in accordance with mass ratio 8: 1-7: 2 with conductive agent acetylene black, adds quality The Kynoar solution that score is 5%, stirring form uniform positive slurry;
S22, the slurry is uniformly coated on aluminium foil, is then dried at 100-140 DEG C, roll-in, positive plate is made in punching;
The preparation of S3, negative electrode tab:
S31, negative electrode active material natural graphite is uniformly mixed with conductive agent acetylene black according to mass ratio 20: 1-30: 1, then plus Enter the Kynoar solution that mass fraction is 10%, stirring forms uniform cathode slurry;
S32, cathode slurry is uniformly coated on copper foil, is then dried at 100-140 DEG C, roll-in, cathode is made in punching Piece;
S4, assembling:
By positive plate obtained above, polyolefin-based gel polymer electrolyte film and negative electrode tab successively lamination and be packed into button electricity Chi Zhong, ageing, sealing obtain the lithium ion battery structure of semisolid.
3. the preparation method of the lithium ion battery structure of semisolid according to claim 2, which is characterized in that step S12 Middle organic solvent is one of acetone, N-Methyl pyrrolidone, n,N-Dimethylformamide or a variety of.
4. the preparation method of the lithium ion battery structure of semisolid according to claim 3, which is characterized in that step S13 In pore creating material be 5-15%wt water, isopropanol or butanol.
5. the preparation method of the lithium ion battery structure of semisolid according to claim 4, which is characterized in that step S14 In electrolyte be 1mol/L LiPF6 PC and EC electrolyte or 1mol/L LiPF6 EC, DEC and DMC electrolyte, PC and The volume ratio of EC is 1: 1, and the volume ratio of EC, DEC and DMC are 1: 1: 1.
6. the preparation method of the lithium ion battery structure of semisolid according to claim 4, which is characterized in that step S14 In electrolyte be one of LiClO4, LiBF4, LiAsF6.
7. the preparation method of the lithium ion battery structure of semisolid according to claim 4, which is characterized in that step S21 In positive active material be LiFePO4、LiCoO2、LiMn2O4, Li (Ni, Co, Mn) O2One of.
CN201810417141.1A 2018-05-03 2018-05-03 A kind of lithium ion battery structure of semisolid and preparation method thereof Pending CN110444803A (en)

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