CN109659493A - It is a kind of comprising solid electrolyte, low porosity cathode and application the cathode lithium battery - Google Patents
It is a kind of comprising solid electrolyte, low porosity cathode and application the cathode lithium battery Download PDFInfo
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- CN109659493A CN109659493A CN201811604753.8A CN201811604753A CN109659493A CN 109659493 A CN109659493 A CN 109659493A CN 201811604753 A CN201811604753 A CN 201811604753A CN 109659493 A CN109659493 A CN 109659493A
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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
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/139—Processes of manufacture
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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
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
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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
- H01M2004/021—Physical characteristics, e.g. porosity, surface area
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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
- H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
- H01M2004/027—Negative electrodes
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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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Abstract
The present invention provides a kind of cathode comprising solid electrolyte, low porosity, it include: negative electrode active material, solid electrolyte, conductive agent, adhesive, preparation method includes: that negative electrode active material and solid electrolyte are at least divided into 3 grades according to granularity, is mixed according still further to certain proportion to realize grain size distribution;The material that grain size distribution obtains is mixed with conductive agent, adhesive and organic solvent in certain ratio, is stirred evenly, smear is simultaneously dried;Pole piece after drying is pressurizeed at normal temperature, is pressed into available electrode.The present invention is by adding solid electrolyte into cathode pole piece, solid electrolyte participates in negative electrode material gradation and by cold compaction for low porosity electrode, and the method for lithium ion tunnel is provided for low porosity cathode, it can be improved the energy density of lithium battery, reduce the dosage of electrolyte.
Description
Technical field
The invention belongs to technical field of lithium batteries, and in particular to it is a kind of comprising solid electrolyte, low porosity cathode and
Using the lithium battery of the cathode.
Background technique
With the fast development of the applications such as electric car and generation of electricity by new energy, develop advanced energy storage technology have become it is urgent
It is essential and asks, in numerous energy storage technologies, lithium ion battery is considered as most potential one of energy storage technology.It is general currently on the market
All over the lithium ion battery used, electrolyte uses organic electrolyte material, it is possible to create the problems such as revealing, is inflammable and explosive makes
Lithium ion battery generates security risk in use.In recent years, as the scale of electric car expands rapidly, cell safety
Unprecedented attention is even more obtained.For safety problem, development can replace the solid-state of conventional batteries lithium diaphragm and electrolyte electric
Xie Zhi has become maximally efficient one of solution route.
Solid lithium ion electrolyte there is also many deficiencies, is mainly shown as at present: lithium ion conductivity compares liquid electrolyte
Matter is low, and solid electrolyte and electrode material interface resistance are very big etc., these disadvantages limit the application of solid lithium battery.Mesh
Before, the polymer matrix composite solid electrolyte of inorganic electrolyte filler enhancing effectively improves the lithium-ion electric of solid electrolyte
Conductance and improve solid electrolyte and electrode material interface resistance (Nature, 1998,394,456;Solid State
Ionics, 2009,180,1267;Nano Energy, 2016,28,447), but still it is not able to satisfy solid lithium ion battery business
Change the requirement of development.
A kind of receiving for lithium ion battery or lithium-sulfur cell is disclosed in the patent document of Publication No. CN1050946A
Rice quasi- solid electrolyte of structure and its preparation method and application, which inhaled by inorganic-organic hybrid frame material
Macroscopical solid electrolyte material that attached ionic conductive agent is formed, wherein inorganic-organic hybrid frame material only serves adion
Function, without lithium ion transport performance, the ionic conductive agent only adsorbed plays the role of transmitting lithium ion, this quasi- solid-state for itself
Electrolyte replaces the electrolyte and diaphragm in lithium ion battery.It is disclosed in the patent document of 10107645013 A of Publication No. CN
A kind of compound quasi-solid electrolyte film and preparation method thereof, the compound quasi-solid electrolyte film include solid electrolyte, containing lithium
Liquid electrolyte, inorganic nanoparticles and the binder of salt.It is disclosed in the patent document of 108365260 A of Publication No. CN
A kind of quasi-solid electrolyte, raw material composition includes polymer, ceramic electrolyte, lithium salts and ionic liquid, for lithium metal electricity
Pond, lithium-air battery and lithium-sulfur cell.
Although the compound quasi- electrolyte in above-mentioned patent has high conductance, but still there are between electrolyte and electrode
Interface stability problem mainly have for the processing method of electrode and splashed using various and in current solid state battery research
It penetrates, membrane electrode (Journal of electrochemical society.1996,143 (10): 3203- is made in deposition approach
3213;Solid State Ionics.2000,135(3-4):41-42;Functional material .2008,39 (1): 91-94) it or uses
Method that PEO base polymer electrolyte coats electrode active material (Advanced Energy Materials.2017,
1701437;Angew.Chem.Int.Ed.2016,55,1-5), but there is the deficiency of itself in the two: the former energy density
It is limited, limit the use scope of hull cell;The latter's room-temperature conductivity is low, and electrochemistry, chemical stability are bad.It is multiple to reduce
Composite electrode impedance improves the energy density of battery.
Active material/solid electrolyte/conductive material complex solid of the porosity within 20% is made in present invention design
Electrode;By this application of electrode in lithium ion battery, the lithium ion battery of preparation includes the cathode (porosity containing solid electrolyte
Lower than 20%)/diaphragm/anode and a small amount of electrolyte.
Conventional electrodes, with the raising of compacted density, the ion channel in pole piece is also reduced, and influences active material appearance
The performance of amount causes the power characteristic of battery to deteriorate.Solid electrolyte is added in electrode material, electrode is in high compacted density
Under state, unobstructed ion transmission channel can be still constructed in the case where electrolyte additional amount is reduced.In addition, in order to continuous work
Industry metaplasia produces, and improves battery yield, and solid electrode should not be sintered processing.Under the premise of herein, the present invention is referring to modern cement slurry system
Method of completing the square prepares the cathode containing solid electrolyte using cold pressing-classification gradation mode;Using the preparation side of conventional lithium battery
Method prepares lithium battery.
According to closely packed model, closely the arrange gap of formation of bulky grain is filled by medium grain, and big or middle particle is formed
Gap again by small particles filled (as shown in figure), successively classification filling can greatly improve bulk density.However, such
Situation is only applicable in theory as swing ball filling, to practical particle-filled and be not suitable for.In actual operation, bulky grain, in
Particle, little particle include that nano sized particles can't be distributed in strict accordance with optimal alignment mathematically, therefore, between particles at different levels
It is differential should increase, short grained amount also can be much higher than the usage amount in closely packed model.Such method is in modern cement slurry
Prepare middle by numerous studies, Li Pengxiao et al. sums up at least 4 times or more of ratio of multicomponent system different component mean particle size
Preferable tightly packed effect (oil drilling technology .2017.Vol.39No.3.307-312) could be obtained;Zhou Shiming etc. also refers to
Out, the quantity of relatively fine particle should be filled in enough in the gap of close-packed arrays particle composition.The appropriate number for increasing coarse grain component
Amount, can be improved mixture bulk density, makes it close to closestpacking, but when component is greater than 3, then practical significance less (stone
Oily drilling technique .2007.Vol.35No.4.46-49.).And when preparing solid electrode, because material therefor granularity is smaller,
Interaction of particles is stronger, it more difficult to dense electrodes of the porosity within 20% are made, thus, the present invention prepares cement slurry work in reference
On the basis of skill, in conjunction with battery homogenate, pressed-disc technique, cold pressing-classification gradation method technique is more meticulously proposed.
The present invention compared with the electrode in current lithium ion battery, coating layer thickness close in the case where, active material carry
Amount significantly improves;Electrode porosity is substantially reduced;Electrode itself can play the role of transmitting ion, electronics;Make in lithium battery
Largely reduce the usage amount of liquid electrolyte.
Summary of the invention
It is an object of the invention to by adding solid electrolyte into cathode pole piece, solid electrolyte participates in negative electrode material
Gradation and by cold compaction for low porosity electrode, and provide the method for lithium ion tunnel for low porosity cathode, it is electric to improve lithium
The energy density in pond reduces the dosage of electrolyte, develops the low porosity comprising solid electrolyte, high-energy density cathode pole
The lithium battery of this cathode of piece and application.
In order to achieve the above objectives, the invention provides the following technical scheme:
A kind of cathode comprising solid electrolyte, low porosity, comprising: negative electrode active material, solid electrolyte, conduction
Agent, adhesive, the amount of solid electrolyte are not higher than the 30wt% of total amount, wherein the granularity of negative electrode active material and solid electrolyte
At least it is divided into 3 grades, porosity is between 10%-20%.
A kind of preparation method comprising solid electrolyte, the cathode of low porosity includes: by negative electrode active material and solid-state
Electrolyte is at least divided into 3 grades according to granularity, carries out mixing according still further to certain proportion and realizes grain size distribution;Grain size distribution is obtained
Material is mixed with conductive agent, adhesive and organic solvent in certain ratio, is stirred evenly, and smear is simultaneously dried;By the pole after drying
Piece pressurization, is pressed into available electrode.
Preferably, it is a kind of comprising solid electrolyte, low porosity cathode in, the solid electrolyte includes: polymer
It is at least one kind of in solid electrolyte, inorganic solid electrolyte.
Preferably, a kind of comprising in solid electrolyte, low porosity cathode, the negative electrode active material includes: that silicon substrate is negative
Pole material, carbon negative pole material, silicon oxocarbon group negative electrode material, lithium titanate anode material, tin base cathode material, the oxygen of transition metal containing lithium
One or more of compound negative electrode material, alloy type negative material.
Preferably, a kind of comprising in solid electrolyte, low porosity cathode, the carbon negative pole material include: conductive black,
One or more of carbon nanotube, graphene, graphene oxide and redox graphene etc..Preferably, the conductive charcoal
The black one or more for Super-P, KB, XC72.
Preferably, it is a kind of comprising solid electrolyte, low porosity cathode in, 3 grades of grade timings, large, medium and small grain graininess
Range is respectively D50 (0.4~20 μm), D50 (0.1~5 μm) D50 (0.02~1 μm), and the fineness ratio of two neighboring grade is greater than
Equal to 4.
Preferably, it is a kind of comprising solid electrolyte, low porosity cathode in, the volume Zhan of 3 grades of grade timings, bulky grain is total
60% or more of volume, short grained volume of the total volume 5% or more.
Preferably, it is a kind of comprising solid electrolyte, low porosity cathode in, 4 grades of grade timings, large, medium and small, minimum
The particle size range of grain is respectively D50 (1.5~32 μm), D50 (0.3~8 μm), D50 (0.08~2 μm), D50 (0.02~0.5 μ
M), the fineness ratio of two neighboring grade is more than or equal to 4.
Preferably, it is a kind of comprising solid electrolyte, low porosity cathode in, the volume Zhan of 4 grades of grade timings, bulky grain is total
50% or more of volume, the volume of nano sized particles of the total volume 3% or more.
Preferably, it is a kind of comprising solid electrolyte, low porosity cathode in, the dispersion of powder, mixing in a liquid into
Row, the liquid are N-Methyl pyrrolidone, propene carbonate, tetrahydrofuran, butyl butyrate.
Preferably, it is a kind of comprising solid electrolyte, low porosity cathode in, it is total that the content of adhesive is no more than each material
The 10wt% of amount, the solid content of mixed slurry is between 30%-65wt%.
Preferably, it is a kind of comprising solid electrolyte, low porosity cathode in, it is fully dispersed after slurry scratch in afflux
On body, the collector includes: aluminium foil, copper foil, stainless steel foil.
Preferably, it is a kind of comprising solid electrolyte, the cathode of low porosity preparation method in, the tabletting method can be adopted
With roll-in or hydraulic, tabletting carries out at normal temperature.
A kind of lithium battery, by it is described containing solid electrolyte, the cathode of low porosity and the compatible anode of electricity, positive and negative anodes it
Between interlayer and electrolyte be placed in container and form the lithium battery.
Preferably, the amount of the electrolyte is the 1.0-3 of pore volume total in the wall of cathode, anode and positive and negative anodes
Times.
The beneficial effects of the present invention are: the present invention is as adding electrode hole made from solid electrolyte into cathode pole piece
Gap rate is low, is conducive to reduce electrode impedance, improves the energy density of battery, while reducing the dosage of electrolyte;Solid electrolyte ginseng
It is classified gradation with negative electrode material, while reducing electrode porosity, increases the ion transmission channel of low porosity electrode, improves electricity
Pole ion transport capability.
Detailed description of the invention
Fig. 1: the graph of pore diameter distribution of different porosities (18%, 30%) SiC+LLZTO cathode
Fig. 2 a: the soft-package battery first charge-discharge for SiC+LLZTO cathode and NCM523 the anode assembling that porosity is 18%
Curve
Fig. 2 b: the soft-package battery first charge-discharge for SiC+LLZTO cathode and NCM523 the anode assembling that porosity is 30%
Curve
Fig. 3: the soft-package battery that different porosities (18%, 30%) SiC+LLZTO cathode is assembled with NCM523 anode follows
Ring performance curve
Specific embodiment
It below will present invention is described further combined with drawings and examples.It is further right that these descriptions are intended merely to
The present invention is illustrated, rather than is limited the invention.
Embodiment 1
A kind of preparation method comprising solid electrolyte, the cathode of low porosity, method are as follows:
(1) Si-C composite material of D50 (15.9 μm), the Si-C composite material and D50 of D50 (2.5 μm) are selected
The solid electrolyte LLZTO powder of (500nm), by bulky grain: middle particle: little particle=7:2:1 (actual volume ratio) carries out 3 grades
Gradation checks in the real density of each component, calculates mass ratio, weighs the powder body material that gross weight is 190g.
(2) by the N-Methyl pyrrolidone of 56g, the PVDF glue of 100g 6% and is weighed up the SP conductive agent of 1.5g
The mixing of 190g powder body material, is homogenized using homogenizer, disperses 5min, 5000 revs/min of revolving speed dispersions with 1000 revs/min of revolving speeds
5min, 7000 revs/min of revolving speed dispersion 5min are repeated 4 times, and after slurry is cooling, the viscosity of testing size is 3600Pas, test slurry
Expect that fineness is 35 μm, then, by slurry double spread in copper foil on coating machine, the surface density for testing electrode is 8.1mg/cm2。
(3) electrode is cut into wide 60mm, the pole piece of long 210mm carries out roll-in on roll squeezer, adjusts the roller of roll squeezer
Between spacing, each pole piece roll-in 3 times respectively obtains the pole that porosity is 18% and 30% by the way that different roller spacing is arranged
Piece (it is respectively 18%:0.046mL/g, 30%:0.12mL/g that the hole of pole piece, which holds), is cut into required size for pole piece, dry,
Weighing.
Embodiment 2
A kind of lithium ion battery, by it is described containing solid electrolyte, the cathode of low porosity and the compatible anode of electricity, every
Film, electrolyte, which are placed in container, forms the lithium ion battery, and method is as follows:
(1) according in embodiment 1 step (2) and (3), prepare NCM523 anode pole piece, according to P/N ratio be 1.15, system
The surface density of standby anode pole piece is 26.1mg/cm2, after roll-in, the pole piece that porosity is 30% one side coating anode is obtained, by pole
Piece is cut into required size, dry, weighing.
(2) using the anode pole piece and cathode pole piece cut out, and with a thickness of 32 μm of diaphragm, lamination is carried out, then
Anode pole piece and cathode pole piece soldering polar ear carry out fluid injection finally, staying mouth above aluminum plastic film by cell package in aluminum plastic film,
The amount of electrolyte is 2 times of anode pole piece, cathode pole piece and diaphragm total pore volume.
(3) it by the cell package after fluid injection, stands for 24 hours, then Vacuum Package, obtaining cathode porosity is 18% and 30%
Soft-package battery.
(4) soft-package battery is tested, and takes initial charge control capability, then chooses the side that blanking voltage carries out charge and discharge
Method.
(5) soft-package battery is tested, and initial charge capacity is the theoretical capacity of silicon-carbon cathode, and voltage at this time is set as charging
Blanking voltage, discharge cut-off voltage 2.8V, discharge-rate 0.1C, 0.3C, 0.5C, 1C.
The pore-size distribution for the electrode that porosity is 18% and 30% is shown in Fig. 1, the electrode of porosity 18%, aperture integrated distribution
At 0.7 μm, and pore-size distribution is relatively narrow, and the electrode of porosity 30%, aperture integrated distribution is at 1.8 μm, and pore-size distribution is wider;Pole
It is respectively 18%:0.046mL/g, 30%:0.12mL/g that the hole of piece, which holds, and the amount of electrolyte is hole in the pole piece of porosity 30%
2.6 times in 18% pole piece of gap rate.
The first charge-discharge curve and cycle performance curve of soft-package battery are shown in Fig. 2 a, Fig. 2 b and Fig. 3, it has been found that cathode
The electrode assembling Soft Roll that the discharge capacity for the first time and cathode porosity for the electrode assembling soft-package battery that porosity is 18% are 30%
The discharge capacity for the first time of battery is very close, and high rate performance and cycle performance are more excellent, illustrates LLZTO in low porosity electrode
Play the role of conducting lithium ions.
The present invention can also have other various embodiments, without departing substantially from the present invention and its essence, the skill of this field
Art personnel make corresponding changes and modifications according to invention, but these corresponding changes and modifications all should belong to right of the present invention and want
The protection scope asked.
Claims (16)
1. a kind of cathode comprising solid electrolyte, low porosity, it is characterised in that: include: negative electrode active material, solid state electrolysis
Matter, conductive agent, adhesive, the amount of solid electrolyte are not higher than the 30wt% of total amount, wherein negative electrode active material and solid state electrolysis
The granularity of matter is at least divided into 3 grades, and porosity is between 10%-20%.
2. the cathode comprising solid electrolyte, low porosity as described in claim 1, it is characterised in that: the solid state electrolysis
Matter includes: at least one of copolymer solid electrolyte, inorganic solid electrolyte.
3. the cathode comprising solid electrolyte, low porosity as described in claim 1, it is characterised in that: the negative electrode active
Material includes: silicon based anode material, carbon negative pole material, silicon oxocarbon group negative electrode material, lithium titanate anode material, tin base cathode material
One or more of material, the negative electrode material of transition-metal oxide containing lithium, alloy type negative material.
4. the cathode comprising solid electrolyte, low porosity as claimed in claim 3, it is characterised in that: the Carbon anode material
Material includes one or more of conductive black, carbon nanotube, graphene, graphene oxide and redox graphene.
5. the cathode comprising solid electrolyte, low porosity as claimed in claim 4, it is characterised in that: the conductive black
For the one or more of Super-P, KB, XC72.
6. as described in claim 1 including solid electrolyte, low porosity cathode, it is characterised in that: 3 grades of grade timings, big,
In, little particle particle size range be respectively 0.4~20 μm, 0.1~5 μm, 0.02~1 μm, the fineness ratio of two neighboring grade is greater than
Equal to 4, the grain graininess is D50 value.
7. the cathode comprising solid electrolyte, low porosity as claimed in claim 6, it is characterised in that: 3 grades of grade timings, greatly
The volume of particle of the total volume 60% or more, short grained volume of the total volume 5% or more.
8. the cathode comprising solid electrolyte, low porosity as described in claim 1, it is characterised in that: 4 grades of grade timings, big,
Middle or small, nano sized particles particle size ranges are respectively 1.5~32 μm, 0.3~8 μm, 0.08~2 μm, 0.02~0.5 μm, and adjacent two
The fineness ratio of a grade is more than or equal to 4, and the grain graininess is D50 value.
9. the cathode comprising solid electrolyte, low porosity as claimed in claim 8, it is characterised in that: 4 grades of grade timings, greatly
The volume of particle of the total volume 50% or more, the volume of nano sized particles of the total volume 3% or more.
10. the cathode comprising solid electrolyte, low porosity as described in claim 1, it is characterised in that: the dispersion of powder,
Mixing carries out in a liquid, and the liquid is N-Methyl pyrrolidone, propene carbonate, tetrahydrofuran, butyl butyrate.
11. the cathode comprising solid electrolyte, low porosity as described in claim 1, it is characterised in that: the content of adhesive
No more than the 10wt% of each total amount of material, the solid content of mixed slurry is between 30%-65wt%.
12. the cathode comprising solid electrolyte, low porosity as described in claim 1, it is characterised in that: after fully dispersed
Slurry scratches on a current collector, and the collector includes: aluminium foil, copper foil, stainless steel foil.
13. special such as the described in any item preparation methods comprising solid electrolyte, the cathode of low porosity of claim 1-12
Sign is: including: that negative electrode active material and solid electrolyte are at least divided into 3 grades according to granularity, carries out according still further to certain proportion
Grain size distribution is realized in mixing;The material that grain size distribution obtains is mixed with conductive agent, adhesive and organic solvent in certain ratio,
It stirs evenly, smear is simultaneously dried;By the pole piece pressurization after drying, it is pressed into available electrode.
14. the preparation method comprising solid electrolyte, the cathode of low porosity as claimed in claim 13, it is characterised in that:
Roll-in or hydraulic can be used in the tabletting method, and tabletting carries out at normal temperature.
15. a kind of lithium battery, by described in any item cathode and the electric phases containing solid electrolyte, low porosity of claim 1-12
Interlayer and electrolyte between the anode of appearance, positive and negative anodes are placed in container and form the lithium battery.
16. lithium battery as claimed in claim 15, it is characterised in that: the amount of the liquid electrolyte be cathode, anode and
1.0-3 times of total pore volume in the wall of positive and negative anodes.
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