CN107039633A - A kind of energy-density lithium ion battery composite negative pole pole piece and its lithium ion battery - Google Patents
A kind of energy-density lithium ion battery composite negative pole pole piece and its lithium ion battery Download PDFInfo
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- CN107039633A CN107039633A CN201710181864.1A CN201710181864A CN107039633A CN 107039633 A CN107039633 A CN 107039633A CN 201710181864 A CN201710181864 A CN 201710181864A CN 107039633 A CN107039633 A CN 107039633A
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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
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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
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/058—Construction or manufacture
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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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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
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Abstract
The invention belongs to lithium ion battery preparation field, a kind of energy-density lithium ion battery composite negative pole pole piece, layer structure is presented in composite negative pole pole piece, and netted copper foil current collector is followed successively by from inside to outside（1）, be coated in the active material layer on reticulated collectors surface（2）, netted precoating lithium layer（3）And it is sprayed at outermost protective layer（4）, it is characterised in that：Described netted copper foil current collector（1）Porosity be 40~60%, mesh form is circular or rhombus, and thickness is 10~30 μm.The present invention, its cathode pole piece prepared, which is applied to lithium ion battery, has the advantages that to possess that excellent processing performance, high rate performance be high, energy density is high, and is applied to pure electric automobile.
Description
Technical field
The invention belongs to lithium ion battery preparation field, specifically a kind of energy-density lithium ion battery composite negative pole
Pole piece and its lithium ion battery.
Background technology
As the fast development of electric automobile and digital electric is, it is necessary to which more Large Copacity, more robust lithium ion battery should
For electric automobile and its electronics field.The energy density of current commercialized batteries of electric automobile is about 130Wh/kg,
Cycle-index is about 2000 times, and general distance travelled is 100~200 kilometers, causes electric automobile to be difficult to popularization；Therefore grind
Hair higher energy density, the electrokinetic cell of more long circulation life seem very necessary.And the density master of electrokinetic cell is improved at present
Have：1）Using high power capacity, the positive and negative pole material of high-pressure solid, such as ternary material, NCA, nickelic ternary material, silicon-carbon cathode；
2）Using high-voltage electrolyte；3）Using thinner copper aluminum foil current collector；4）Newest benefit lithium technology is introduced, gram appearance of material is improved
Amount performance and its first efficiency, so as to significantly improve the energy density of lithium ion battery.Although and the method 1-3 country has big
Quantifier elimination and improvement, but being difficult to have in a short time significantly improves, and method 4 is then a kind of newest benefit lithium
Technology, i.e., because lithium ion battery forms SEI consumption lithium ions in charge and discharge process, cause its first efficiency it is relatively low so as to dropping
The gram volume of its low material is played, and the gram volume performance of material can be significantly improved by mending lithium by material or pole piece.Although state
Interior researcher has research to mend lithium to improve the energy density and its other performance of lithium ion battery by pole piece.Such as patent is disclosed
Number be CN1290209C Chinese patent application, metallic lithium powder, negative material, non-aqueous media are mixed to form slurry, then applied
Cover and negative pole is made to collector.Exist because metallic lithium powder surface generally has nonconducting passivation layer, so needing to pass through
The methods such as roll-in are crushed the Li for discharging inside.But with it, can be left very inside pole piece after the dissolving of lithium powder
Many holes, or make pole piece become uneven, not only reduce compacted density, and electronics also can be by the conduction of negative pole
To large effect (impedance increase), cause effect to reduce while lithium powder is exposed in air easily water suction and bring safety hidden
Suffer from, and it is poor using lithium powder benefit lithium homogeneity, process is difficult to control to, and causes its actual effect to be difficult to meet design requirement.And pass through
The potential safety hazard that can then avoid lithium powder to cause using lithium piece, but be due to that the lithium content of lithium ion battery can be caused using lithium piece
It is too high, cause its structural stability difference and its tap density relatively low, unfavorable shadow can be caused to the chemical property of lithium ion battery
Ring.
The content of the invention
For at present in terms of lithium ion battery energy density is improved the cathode pole piece that uses mend deficiency that lithium powder is present and
Defect in terms of security performance, the purpose of the present invention is by supplementing netted lithium paper tinsel in cathode pole piece, on the one hand to negative pole pole
Piece carries out appropriate benefit lithium, in the case where not influenceing its energy density, improves the efficiency first of its lithium ion battery；On the other hand, pass through
Lithium paper tinsel and surface spraying safe floor are suppressed in negative terminal surface, makes that its process is controllable, preparation process is simple, it is easy to industrialization,
And applied to lithium ion battery.
The technical scheme is that be accomplished by the following way：A kind of energy-density lithium ion battery composite negative pole pole
Layer structure is presented in piece, composite negative pole pole piece, and netted copper foil current collector is followed successively by from inside to outside, reticulated collectors surface is coated in
Active material layer, netted precoating lithium layer and be sprayed at outermost protective layer, it is characterised in that：Described netted copper foil afflux
The porosity of body is 40~60%, and mesh form is circular or rhombus, and thickness is 10~30 μm.
Described active material layer is made up of active material, conductive agent, binding agent, and its mass ratio is, active material：It is conductive
Agent：Binding agent=90~95：1~5：1~5；Wherein conductive agent is one kind in CNT, graphene, super carbon black, is bonded
Agent is one kind in LA132 or sodium alginate；Active material is one kind in silicon-carbon cathode, hard carbon, soft carbon.
Described netted precoating lithium layer is made up of latticed lithium piece, and its porosity is 70~90%, and mesh shape is pros
Shape type；Thickness is 0.1~10mm；
Described protective layer is made up of 40~80% high molecular polymer and 20~60% functional materials.
Described high molecular polymer is zinc-containing solid catalyst, polyalkylene oxides, polyalkylsiloxane, polypropylene
One kind in acid alkyl ester and polyalkyl methacrylate.
Described functional materials are Melamine pyrophosphate, ammonium polyphosphate (APP), melamine polyphosphoric acids
One kind in ester, triphenyl phosphorus, phenyl phosphorus diamides, diphenylphosphine.
A kind of energy-density lithium ion battery composite negative pole pole piece is applied to lithium ion battery, in parts by weight, its feature
It is：Comprise the following steps：
1）, weigh 1~5g binding agents and be dissolved in after 150g redistilled waters are uniformly dispersed, addition 1~5g conductive agent redisperses are uniform
Afterwards, 90~95g active materials are added and active material slurry A are obtained after being uniformly dispersed at a high speed, with standby；
2nd, weigh 40~80g high molecular polymer be dissolved in be uniformly dispersed in 500ml carbon tetrachloride after add 20~60g features
Material obtains protecting liquid B after simultaneously ultrasonic disperse is uniform, with standby；
3）, by active material slurry A by high-precision coater in netted copper foil surface, dry after finishing, obtain pole volume
C；Preheated using roll squeezer, be heated to 80~150 DEG C, and latticed lithium piece and pole are rolled up into C by roll squeezer, by grid
Shape lithium piece is suppressed rolls up C intermediate surface in pole, dries and pole volume D is obtained after finishing；Liquid B sprayings will be protected finally by spraying technology
In pole volume D surfaces, dry and pole volume E is obtained after finishing, cathode pole piece is obtained after cutting.
4）, the cathode pole piece prepared using above-mentioned steps, ceramic diaphragm, ternary material anode pole piece, using up- coiler
Winding battery core is prepared, lithium ion battery is prepared by welding, drying, fluid injection, chemical conversion constant volume.
Beneficial effects of the present invention：Using in the netted lithium paper tinsel of cathode pole piece surface rolling, lithium, tool are mended compared with cathode pole piece lithium powder
There is the potential safety hazard that lithium paper tinsel activity is low, security performance is high, process is simple, process control avoids the splash zone of lithium powder from, together
The pole piece that Shi Caiyong lithium paper tinsels are prepared has the characteristics such as compacted density height；The spray coating liquor on lithium paper tinsel surface can avoid lithium paper tinsel straight simultaneously
Connect the service efficiency and security performance that its lithium paper tinsel is improved with air contact.While netted lithium paper tinsel, which has, mends lithium in right amount, activity is low, add
The features such as work is easy, and improve the chemical properties such as the energy density, multiplying power, circulation of its lithium ion battery.
Brief description of the drawings
The structural representation for the composite negative pole pole piece that Fig. 1, embodiment are prepared.
Wherein：1-collector, 2-active material layer, 3-netted precoating lithium layer, 4-protective layer.
Embodiment
Known by Fig. 1, a kind of energy-density lithium ion battery composite negative pole pole piece, layer structure is presented in composite negative pole pole piece,
Netted copper foil current collector 1, the active material layer 2 for being coated in reticulated collectors surface, netted precoating lithium layer 3 are followed successively by from inside to outside
And outermost protective layer 4 is sprayed at, the porosity of described netted copper foil current collector 1 is 40~60%, and mesh form is circle
Or rhombus, thickness is 10~30 μm.
Embodiment 1：
A kind of preparation method of energy-density lithium ion battery composite negative pole pole piece, step is：
1st, weigh 3g LA132 binding agents first to be dissolved in after 150g redistilled waters are uniformly dispersed, addition 3g CNTs simultaneously disperse
After uniform, 94g hard carbons are added, and obtain active material slurry A after being uniformly dispersed at a high speed, with standby；
2nd, weigh 60g zinc-containing solid catalyst be dissolved in be uniformly dispersed in 500ml carbon tetrachloride after the burnt phosphorus of addition 40g Melamines
Hydrochlorate obtains protecting liquid B after simultaneously ultrasonic disperse is uniform, with standby；
3rd, by active material slurry A by high-precision coater in netted copper foil（Porosity 50%, 20 μm of thickness）Surface,
Dry after finishing, obtain pole volume C；Preheated afterwards using roll squeezer, be heated to 120 DEG C, and by latticed lithium piece（Hole
Rate 80%, thickness 5mm）C is rolled up by roll squeezer with pole, and latticed lithium piece is suppressed and rolls up C intermediate surface in pole, is dried after finishing
Obtain pole volume D；Finally by spraying technology liquid B will be protected to be sprayed at pole volume D surfaces, dry and pole volume E is obtained after finishing, after cutting
Obtain anode pole piece.
3）The cathode pole piece finally prepared using above-mentioned steps, ceramic diaphragm, ternary material anode pole piece, and using volume
Prepare and made the test around battery core around machine, afterwards by welding, drying, fluid injection, be melted into constant volume and prepare lithium ion battery A1.
Embodiment 2：
1st, weigh 1g sodium alginate binding agents first to be dissolved in after 150g redistilled waters are uniformly dispersed, addition 4g graphenes simultaneously disperse
After uniform, 95g hard carbons are added, and obtain active material slurry A after being uniformly dispersed at a high speed, with standby；
Weigh simultaneously 40g polyalkylene oxides be dissolved in be uniformly dispersed in 500ml carbon tetrachloride after addition 60g ammonium polyphosphates simultaneously
Obtain protecting liquid B after ultrasonic disperse is uniform, with standby；
2nd, afterwards by active material slurry A by high-precision coater in netted copper foil（Porosity 40%, 30 μm of thickness）Table
Face, is dried after finishing, and obtains pole volume C；Preheated afterwards using roll squeezer, be heated to 80 DEG C, and by latticed lithium piece（Hole
Gap rate 70%, thickness 10mm）C is rolled up by roll squeezer with pole, and latticed lithium piece is suppressed and rolls up C intermediate surface in pole, drying is finished
After obtain pole volume D；Finally by spraying technology liquid B will be protected to be sprayed at pole volume D surfaces, dry and pole volume E, cutting are obtained after finishing
After obtain anode pole piece.
3rd, the cathode pole piece finally prepared using above-mentioned steps, ceramic diaphragm, ternary material anode pole piece, and using volume
Prepare and made the test around battery core around machine, afterwards by welding, drying, fluid injection, be melted into constant volume and prepare lithium ion battery A2.
Embodiment 3：
1st, 5gLA132 binding agents are weighed first to be dissolved in after 150g redistilled waters are uniformly dispersed, and add 5gSP conductive agent redisperses
After uniform, 90g hard carbons are added, and obtain active material slurry A after being uniformly dispersed at a high speed, with standby；
2nd, while the polyalkyl methacrylate for weighing 80g is dissolved in addition 20g trimerizations after being uniformly dispersed in 500ml carbon tetrachloride
Cyanamide condensed phosphate obtains protecting liquid B after simultaneously ultrasonic disperse is uniform, with standby；
3rd, by active material slurry A by high-precision coater in netted copper foil（Porosity 60%, 10 μm of thickness）Surface,
Dry after finishing, obtain pole volume C；Preheated afterwards using roll squeezer, be heated to 150 DEG C, and by latticed lithium piece（Hole
Rate 90%, thickness 1mm）C is rolled up by roll squeezer with pole, and latticed lithium piece is suppressed and rolls up C intermediate surface in pole, is dried after finishing
Obtain pole volume D；Finally by spraying technology liquid B will be protected to be sprayed at pole volume D surfaces, dry and pole volume E is obtained after finishing, after cutting
Obtain anode pole piece.
4th, the cathode pole piece finally prepared using above-mentioned steps, ceramic diaphragm, ternary material anode pole piece, and using volume
Prepare and made the test around battery core around machine, afterwards by welding, drying, fluid injection, be melted into constant volume and prepare lithium ion battery A3.
Comparative example：
Weigh 3g LA132 binding agents to be dissolved in after 150g redistilled waters are uniformly dispersed, addition 3g CNTs are simultaneously uniformly dispersed
Afterwards, 94g hard carbons are added（Producer：Shenzhen Bei Terui new energy materialses limited company, model：HC-1）, and it is scattered equal at a high speed
Active material slurry A is obtained after even, slurry A is coated on by copper foil (thickness is 20 μm) surface, dry, roller by coating machine afterwards
Cathode pole piece is obtained after pressure；The cathode pole piece prepared afterwards with above-mentioned steps, ceramic diaphragm, ternary material anode pole piece, and
Winding battery core is prepared using up- coiler, afterwards by welding, drying, fluid injection, be melted into constant volume and prepare lithium ion battery.
1）, button cell：
This test example detects discharge capacity first, first efficiency and the compacted density of the cathode pole piece of each embodiment and comparative example.
Using molar concentration as 1.3mol/l LiPF6Solution is electrolyte, and metal lithium sheet is that, to electrode, barrier film uses polyethylene (PE),
Polypropylene (PP) or poly- second propylene (PEP) composite membrane, simulated battery are assemblied in the glove box for be flushed with hydrogen gas and carried out, chemical property
Carried out on the blue electricity CT2001A type cell testers in Wuhan, charging/discharging voltage scope is 0.005V to 2.0V, and charge-discharge velocity is
0.1C。
The discharge capacity first of the cathode pole piece of each embodiment of table 1 and comparative example, first efficiency and compacted density experiment knot
Really
| Project | Embodiment 1 | Embodiment 2 | Embodiment 3 | Comparative example |
| Discharge capacity first（mAh/g） | 495.5 | 486.6 | 487.1 | 410.3 |
| Efficiency first（%） | 92.1 | 91.3 | 90.1 | 82.4 |
As can be seen from Table 1, embodiment prepares pole piece and is substantially better than comparative example in terms of gram volume and its first efficiency, and it is former
Because：By carrying out benefit lithium to hard carbon composite, the efficiency first of its material can be improved, and improve its gram volume.
2）, electrochemical property test
Respectively with embodiment 1, embodiment 2, the pole piece that embodiment 3 and comparative example are prepared is as negative material, with LiFePO4
For positive electrode, using LiPF6/EC+DEC（Volume ratio 1: 1）For electrolyte, the films of Celgard 2400 are barrier film, prepare 5Ah
Soft-package battery A1, A2, A3 and B1, and test the high rate performance and security performance of its soft-package battery.
This test example detects the imbibition liquid-keeping property of the lithium ion battery negative electrode of each embodiment and comparative example and its soft
The cycle performance of bag battery, as a result as shown in table 2 and table 3.
The imbibition liquid-keeping property result of the test of the cathode pole piece of each embodiment of table 2 and comparative example
| Sequence number | Rate of liquid aspiration（mL/min） | Protect liquid rate（24h electrolyte contents/0h electrolyte contents） |
| Embodiment 1 | 7.2 | 95.3% |
| Embodiment 2 | 6.5 | 94.2% |
| Embodiment 3 | 6.4 | 94.4% |
| Comparative example | 3.1 | 83.7% |
There is good imbibition compared with comparative example by the lithium ion battery negative electrode of the results showed that present invention of table 2
Liquid-keeping property, its reason has preferable compatibility to mend lithium layer and electrolyte, so that liquid is protected in the imbibition for improving cathode pole piece
Ability.
Test example：
By the lithium ion battery in embodiment 1-3 and comparative example at 25 ± 3 DEG C, entered for 500 times with 1.0C/1.0C circulation
Row cycle performance is tested.
According to lithium ion battery discharge capacity and the quality of battery first, the mass-energy for calculating lithium ion battery is close
Degree.
Test result is shown in Table 3.
The embodiment 1-3 of table 3 and the lithium ion battery in comparative example cycle performance and energy density
| Project | Cycle performance（500 conservation rates） | Energy density（Wh/kg） |
| Embodiment 1 | 96.9% | 122.5 |
| Embodiment 2 | 96.2% | 121.4 |
| Embodiment 3 | 95.9% | 120.9 |
| Comparative example | 91.5% | 113.5 |
As can be seen from Table 3, the cycle performance of lithium ion battery in embodiment is substantially better than comparative example, and its reason is that battery fills
The SEI films consumption lithium ion formed in discharge process, causes inside battery lithium ion not enough, and the lithium added in the present invention is compound
Piece can supplement the lithium ion in electrolyte in time due to forming lithium ion in charge and discharge process, improve in electrolyte lithium from
The transmission rate of son, improves its cycle performance.Further, using reticulated collectors, battery shared by collector can be reduced
Mass ratio, so as to improve the energy density of lithium ion battery.
Claims (7)
1. a kind of energy-density lithium ion battery composite negative pole pole piece, layer structure is presented in composite negative pole pole piece, from inside to outside according to
Secondary is netted copper foil current collector（1）, be coated in the active material layer on reticulated collectors surface（2）, netted precoating lithium layer（3）And spray
It is applied to outermost protective layer（4）, it is characterised in that：Described netted copper foil current collector（1）Porosity be 40~60%, net
Hole shape is circular or rhombus, and thickness is 10~30 μm.
2. a kind of energy-density lithium ion battery composite negative pole pole piece according to claim 1, it is characterised in that：Described
Active material layer（2）It is made up of active material, conductive agent, binding agent, its mass ratio is, active material：Conductive agent：Binding agent=
90~95：1~5：1~5；Wherein conductive agent be CNT, graphene, super carbon black in one kind, binding agent be LA132 or
One kind in sodium alginate；Active material is one kind in silicon-carbon cathode, hard carbon, soft carbon.
3. a kind of energy-density lithium ion battery composite negative pole pole piece according to claim 1, it is characterised in that：Described
Netted precoating lithium layer（3）It is made up of latticed lithium piece, its porosity is 70~90%, mesh shape is square type；Thickness is
0.1~10mm.
4. a kind of energy-density lithium ion battery composite negative pole pole piece according to claim 1, it is characterised in that：Described
Protective layer is（4）It is made up of 40~80% high molecular polymer and 20~60% functional materials.
5. a kind of energy-density lithium ion battery composite negative pole pole piece according to claim 4, it is characterised in that：Described
High molecular polymer is zinc-containing solid catalyst, polyalkylene oxides, polyalkylsiloxane, polyalkyl acrylate and poly- first
One kind in base alkyl acrylate.
6. a kind of energy-density lithium ion battery composite negative pole pole piece according to claim 4, it is characterised in that：Described
Functional materials are Melamine pyrophosphate, ammonium polyphosphate (APP), melamine condensed phosphate, triphenyl phosphorus, phenyl
One kind in phosphorus diamides, diphenylphosphine.
7. a kind of energy-density lithium ion battery composite negative pole pole piece as claimed in claim 1 is applied to the system of lithium ion battery
Preparation Method, in parts by weight, it is characterised in that：Comprise the following steps：
1）, weigh 1~5g binding agents and be dissolved in after 150g redistilled waters are uniformly dispersed, addition 1~5g conductive agent redisperses are uniform
Afterwards, 90~95g active materials are added and active material slurry A are obtained after being uniformly dispersed at a high speed, with standby；
2）, weigh 40~80g high molecular polymer be dissolved in be uniformly dispersed in 500ml carbon tetrachloride after add 20~60g functions
Property material and ultrasonic disperse it is uniform after obtain protect liquid B, with standby；
3）, by active material slurry A by high-precision coater in netted copper foil surface, dry after finishing, obtain pole volume
C；Preheated using roll squeezer, be heated to 80~150 DEG C, and latticed lithium piece and pole are rolled up into C by roll squeezer, by grid
Shape lithium piece is suppressed rolls up C intermediate surface in pole, dries and pole volume D is obtained after finishing；Liquid B sprayings will be protected finally by spraying technology
In pole volume D surfaces, dry and pole volume E is obtained after finishing, cathode pole piece is obtained after cutting.
4）, cathode pole piece and ceramic diaphragm, the ternary material anode pole piece prepared using above-mentioned steps, prepared using up- coiler
Make the test around battery core, lithium ion battery is made by welding, drying, fluid injection, chemical conversion constant volume.
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| CN201710181864.1A CN107039633A (en) | 2017-03-24 | 2017-03-24 | A kind of energy-density lithium ion battery composite negative pole pole piece and its lithium ion battery |
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