CN108539124A - With the secondary cell and preparation method thereof for mending lithium electrode - Google Patents
With the secondary cell and preparation method thereof for mending lithium electrode Download PDFInfo
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- CN108539124A CN108539124A CN201710116105.7A CN201710116105A CN108539124A CN 108539124 A CN108539124 A CN 108539124A CN 201710116105 A CN201710116105 A CN 201710116105A CN 108539124 A CN108539124 A CN 108539124A
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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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- 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
- H01M4/134—Electrodes based on metals, Si or alloys
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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
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
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- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Materials Engineering (AREA)
- Manufacturing & Machinery (AREA)
- Secondary Cells (AREA)
- Battery Electrode And Active Subsutance (AREA)
Abstract
The present invention relates to the secondary cell and preparation method thereof for mending lithium electrode.According to an exemplary embodiment, a kind of secondary cell may include：Positive plate and negative plate, are isolated from each other by diaphragm；And at least one benefit pole piece comprising lithium active layer, at least one benefit pole piece are kept apart also by diaphragm and the positive plate and negative plate.The secondary cell of the present invention can realize high capacity, and with pole piece is mended so as to supplement elemental lithium to negative plate or positive plate for the first time or in cyclic process, to realize high coulombic efficiency, and improve cycle characteristics.
Description
Technical field
Present invention relates in general to new energy fields, more specifically it relates to a kind of having the secondary cell for mending lithium electrode,
Elemental lithium can be supplemented to the negative plate of secondary cell or positive plate for the first time or in cyclic process, and further relate to prepare this
The method with the secondary cell for mending lithium electrode of sample.
Background technology
In recent years, fast-developing electric vehicle and energy storage industry are to using lithium ion battery, sodium-ion battery as representative
More stringent requirements are proposed for energy density, cost, cyclicity and the safety of secondary cell.It is conventional by taking lithium ion battery as an example
Lithium ion battery mainly to use graphite cathode, the theoretical capacity of graphite cathode be 372mAh/g, domestic main graphite at present
Cathode manufacturer has been realized in the capacity of 365mAh/g such as Jiangxi purple great mansion, Shenzhen Bei Terui, close to theoretical capacity
The limit.In order to realize that higher energy density and power density, people begin to focus on novel anode material, such as ungraphitised carbon
Material, silicium cathode, silicon-carbon composite cathode, the sub- silicium cathode of oxidation and the sub- silicon silicon-carbon composite cathode of oxidation etc..However, these materials
The serious problems such as that there are irreversible capacities is high for material, coulombic efficiency is low for the first time, are easy to cause capacity of lithium ion battery and are decreased obviously.
Currently, in order to solve the problems, such as lithium ion battery negative material, coulombic efficiency is low for the first time, proposing of researcher
It is pre- to learn reduction method, artificial SEI (Solid Electrolyte Interface, solid electrolyte interface) embrane methods and electrochemistry
Lithiumation method etc., wherein electrochemistry prelithiation method are that coulombic efficiency is low for the first time for a kind of most direct solution lithium ion battery negative material
The method of this problem.
In Chinese patent application the 200480021793.Xth, discloses and a kind of directly connecing lithium powder with electrode material
It touches, the method that electrode material prelithiation is then realized by galvanic interaction again.However, this method easy tos produce " dead lithium ", and
And reaction is violent, the structure for being easy to cause electrode material is destroyed, and is difficult to form SEI films that are fine and close and stablizing, finally
So that the cycle performance of electrode material declines.In addition, lithium powder is a kind of more dangerous material, it is easy burning, therefore implementing should
The process conditions of prelithiation method are more harsh, result in cost increase.
In Chinese patent application the 201210573270.2nd, for the big problem of lithiumation electric current, disclose a kind of low
Warm electrolyte filling method makes galvanic interaction carry out at a lower temperature to control the embedding lithium speed of material, to improve material
Coulombic efficiency and while capacity for the first time, improves the cycle performance of material.However, this method needs low-temperature operation, technique more multiple
It is miscellaneous, it is of high cost, and also the electrolysis fluid viscosity under low temperature increases, fluid injection operating difficulties.
In Chinese patent application the 201410839836.0th, lithium metal is coated on anode and cathode, is then applied again
Solid electrolyte is covered, to reduce reaction speed, but complex manufacturing technology, it is not easy large-scale industrial production.
Nano-silicon and carbon compound cathode or the sub- silicon of oxidation and carbon compound cathode are considered as third generation cathode, theoretical capacity
It can reach 4200mAh/g.Battery energy density can be increased to using such cathode by 300wh/kg, but such cathode is first all
It is relatively low compared with anode with cycle efficieny.Such as to realize long circulating, then there is still a need for carry out benefit lithium to battery.
Invention content
One aspect of the present invention is to provide a kind of novel secondary cell, can realize high capacity, and have
There is benefit pole piece so as to supplement elemental lithium to the negative plate of secondary cell or positive plate for the first time or in cyclic process, with
Realize high coulombic efficiency.
According to an exemplary embodiment, a kind of secondary cell may include：Positive plate and negative plate, by diaphragm each other every
It leaves；And at least one benefit pole piece comprising lithium active layer, at least one benefit pole piece also by diaphragm with it is described
Positive plate and negative plate are kept apart.
In some instances, the lithium active layer include pure metal lithium, Li-Si alloy, lithium-aluminium alloy, lithium boron alloy and
It is one or more in lithium magnesium alloy.
In some instances, the secondary cell further includes：Shell, for accommodating the positive plate, negative plate, mending lithium electrode
Piece and diaphragm；Anode ear is connected to the positive plate and extends to outside the shell；Negative electrode lug, be connected to the negative plate and
It extends to outside the shell；And lithium electrode ear is mended, it is connected to the benefit pole piece and extends to outside the shell.The benefit lithium electrode
Ear may include nickel or aluminium.
In some instances, multiple positive plates, diaphragm and negative plate are stacked to a stacking, at least one benefit pole piece
One or more of left side in the stacking, right side, front side, rear side and bottom side place is set, the anode ear, negative electrode lug and
It mends lithium electrode ear and the top sides in the stacking is set.
In some instances, when the anode ear is electrically connected to the benefit lithium electrode ear, the benefit pole piece to it is described just
Pole piece carries out benefit lithium.
In some instances, when the negative electrode lug is electrically connected to the benefit lithium electrode ear, the benefit pole piece is to described negative
Pole piece carries out benefit lithium.
In some instances, the benefit pole piece further includes collector, and the lithium active layer is arranged on the collector.
The collector may include one or more in copper foil, nickel foil, steel foil, carbon film.
In some instances, the secondary cell includes liquid lithium ionic cell, solid lithium ion battery, liquid metal lithium
Battery, solid metallic lithium battery or colloidal sol lithium ion battery.
In some instances, the secondary cell is sodium ion or metal sode cell, and the benefit pole piece is to mend sodium pole piece.
According to another exemplary embodiment, a kind of method preparing secondary cell may include：Prepare positive plate, negative plate and
Diaphragm；Preparation includes the benefit pole piece of lithium active layer；The positive plate, negative plate, benefit pole piece and diaphragm are assembled into battery core,
The wherein described positive plate, negative plate and benefit pole piece are separated from one another by the diaphragm；And the battery core is encapsulated into shell
In body.
In some instances, the method further includes：By anode ear, negative electrode lug and mend lithium electrode ear be welded to it is described just
In pole piece, negative plate and benefit pole piece.Wherein, after the encapsulation step, the anode ear, negative electrode lug and benefit lithium electrode ear point
It is not extended to except the shell from the battery core.
In some instances, the method further includes：Execute the chemical conversion step of secondary cell；And by the anode ear or
Negative electrode lug is electrically connected to the benefit lithium electrode ear, to supplement elemental lithium to the positive plate or negative plate by discharge process.
Other features and advantages of the present invention will become apparent the description of exemplary embodiment by following.
Description of the drawings
Attached drawing diagrammatically illustrates exemplary embodiment of the present invention.It should be understood that attached drawing was not drawn to scale.
Fig. 1 shows the structural schematic diagram of the secondary cell of the prior art.
Fig. 2 shows the structural schematic diagrams according to the secondary cell of an of the invention exemplary embodiment.
Fig. 3 shows the structural schematic diagram for the benefit pole piece that the secondary cell of Fig. 2 includes.
Fig. 4 shows the flow chart of the method for preparing secondary cell according to an exemplary embodiment of the invention.
Specific implementation mode
Fig. 1 shows the structural schematic diagram of the secondary cell 100 of the prior art.As shown in Figure 1, secondary cell 100 includes shell
The battery core 120 of body 110 and receiving in the housing.Battery core 120 includes the stacking of positive plate 122, diaphragm 121 and negative plate 124,
Middle positive plate 122 and negative plate 124 are isolated from each other by diaphragm 121.The stacking can have various structures, such as multiple
Shape layer is sequentially stacked or multiple layers bend or be wound into cylinder or flat pattern etc..Positive plate 122 is prolonged by anode ear 132
It reaches outside shell 110, negative plate 124 is extended to by negative electrode lug 134 outside shell 110, electrically operated in order to execute charge and discharge.Shell
110 can also have the opening (not shown) for injecting electrolyte.It should be understood that the secondary cell 100 of the prior art is various
Structure, material etc. are all known in the art, therefore are only briefly described here, are described in detail without another one.
Fig. 2 shows the structural schematic diagrams of secondary cell 200 according to an embodiment of the invention.As shown in Fig. 2, battery 200
The same battery core 220 for including shell 210 and being contained in shell 210.Shell 210 can be flexible shell, such as by plastic foil
Can also be stiff case, such as be made of metal or alloy such as aluminium, steel etc. being made.Shell 210 can be insulation, also may be used
To be conductive.When shell 210 is conductive, pole piece should be kept apart by diaphragm and shell.In some embodiments, it is described below
Positive plate, negative plate and mend one of pole piece and may be also electrically connected to conductive shell 210, to which conductive shell 210 can be used as
Its connection terminal, as in the prior art often by battery case as negative terminal.At this point it is possible to omit described below
One lug.Shell 210 can have variously-shaped, such as cylindrical shape, flat pattern, cubic shaped etc., to adapt to
The battery flat profile of its electronic equipment being applied to.
Battery core 220 may include the stacking of positive plate 222, negative plate 224 and diaphragm 221, wherein positive plate 222 and negative plate
224 is separated from one another by diaphragm 221.Positive plate 222, negative plate 224 and diaphragm 221 can with it is in the prior art identical.
The difference is that, battery core 220 further includes mending pole piece 226 with the secondary cell of the prior art.Mending pole piece 226 can be
It is flexibly set in shell 210.For example, mending pole piece 226 and can be arranged stacking is formed by positive plate, negative plate and diaphragm
One or more sides, such as left side, right side, front side, rear side and bottom side.In another example mending pole piece 226 can also be arranged
Positive plate, negative plate and diaphragm are formed by stacking.That is, mend pole piece 226 can with positive plate, negative plate and every
Film is stacked or winds together.In the figure 2 example, two benefit pole pieces 226 are separately positioned on positive plate, negative plate and diaphragm
It is formed by the left and right side of stacking.Mending pole piece 226 can also be separated by diaphragm 221 and positive plate 222, negative plate 224
It opens, and is also kept apart by diaphragm 221 and shell 210.Although it is not shown, it should be understood that multiple positive plates 222 can be
One, or be electrically connected to each other by connecting circuit；Multiple negative plates 224 can be integrated, or by connecting circuit
It is electrically connected to each other；Multiple benefit pole pieces 226 can also be integrated, or is electrically connected to each other by connecting circuit.
Positive plate 222 and negative plate 224 can be identical as the positive plate and negative plate used in the prior art.For example, just
Pole piece 222 may include cobalt acid lithium, LiMn2O4, nickle cobalt lithium manganate, nickel cobalt lithium aluminate, lithium-rich oxide, nickel ion doped, phosphoric acid
Iron lithium, lithium manganese phosphate, cobalt phosphate lithium, LiNiPO, lithium ferric manganese phosphate, ferric phosphate, manganese phosphate, cobalt phosphate, nickel phosphate, ferrosilite
Lithium, manganese silicate of lithium, cobaltous silicate lithium, silicic acid nickel lithium, ferrosilite, manganous silicate, cobaltous silicate, silicic acid nickel and their arbitrary combination.
In further embodiments, the material for forming positive plate 222 also can be selected from manganese dioxide, iron sulfide, manganese sulfide, cobalt sulfide, sulphur
Change nickel, titanium sulfide, ferric sulfate, ferric phosphate, sulphur carbon and oxyvanadium compound and their arbitrary combination.It can be used to form cathode
The example of the material of piece 224 include but not limited to for example natural graphite, artificial graphite, soft carbon, hard carbon, siliceous, tin, germanium, zinc,
Aluminium, boron, the material of magnesium elements, transition metal oxide, transient metal sulfide, transition metal fluorides, transitional metal nitride
Object, transition metal phosphide, wherein the transition metal can be in Cr, Cu, Fe, Co, Ni, Nb, V, Mo, W and Ru one
Kind is a variety of.
Diaphragm 221 may include polymer film.The example for being used to form the polymer material of diaphragm 221 includes but not limited to
Polypropylene, polyethylene, ethylene oxide, polypropylene oxide, Kynoar, Kynoar-hexafluoropropene, polymethylacrylic acid
Methyl esters, polyacrylonitrile, polyimides, polyetherimide, makrolon, poly- aramid fiber, cellulose and their arbitrary combination.
In some embodiments, the thickness of diaphragm 221 can be in 6-60 μm of range, preferably in 6-25 μm of range.In some realities
It applies in example, diaphragm 221 can be the porous circulation in favor of electrolyte, for example, diaphragm 221 can be with the hole of 30%-90%
Gap rate.
In the charge and discharge process of secondary cell 200, electron channel, lithium member are formed between positive plate 222 and negative plate 224
Element shifts back and forth between positive plate 222 and negative plate 224.Since " dead lithium " may be formed in cyclic process, lead to two
The capacity of primary cell 200 declines.The present invention mends pole piece 226 by offer, can be supplemented to positive plate 222 and negative plate 224
Elemental lithium.Fig. 3 shows the structural schematic diagram for mending pole piece 226.As shown in figure 3, mending pole piece 226 may include collector 227
With the lithium active layer 228 being formed on collector 227.Collector 227 can be copper foil, it is a kind of in nickel foil, steel foil, C film or
Person is a variety of, thickness can be such as 1 μm~20mm, preferably 2~8 μm.Collector 227 can be porous or fine and close
Foil.Lithium active layer 228 may include the materials such as lithium metal, Li-Si alloy, lithium-aluminium alloy, lithium boron alloy, lithium magnesium alloy, can be
Band, item, ring or point format are formed on collector 227.The thickness of lithium active layer 228 can be such as 20 μm~1mm, excellent
Selection of land is 20~700 μm.In some embodiments, if lithium active layer 228 has enough mechanical strengths, collection can also be omitted
Fluid 227.
Although Fig. 3 is shown is formed with lithium active layer 228 on a surface of collector 227, it will be understood that, another
In some embodiments, it can also all be formed with lithium active layer 228 on two surfaces up and down of collector 227.
With continued reference to Fig. 2, secondary cell 200 further includes anode ear 232, negative electrode lug 234 and mends lithium electrode ear 236, they
It is connected respectively to positive plate 222, negative plate 224 and mends pole piece 236, and extend to outside shell 210, in order to two
Primary cell 200 executes charge and discharge and mends lithium operation, this will be described in detail later.Anode ear 232 and negative electrode lug 234 can
With with it is in the prior art identical.It mends lithium electrode ear 236 and may include such as nickel or aluminium pole ears.
Secondary cell 200 shown in Fig. 2 can be various secondary cells, such as liquid lithium ionic cell, solid lithium ion
Battery, liquid metal lithium battery, solid metallic lithium battery or colloidal sol lithium ion battery etc..When secondary cell 200 is liquid electricity
Chi Shi can also include electrolyte in shell 210 to infiltrate positive plate 222, negative plate 224 and mend pole piece 226.
The operation of secondary cell 200 is described below.As the secondary cell of the prior art, by by 232 He of anode ear
Negative electrode lug 234 is connected to external equipment, and it is electrically operated to execute charge and discharge, is not detailed herein.Lithium electrode ear 236 will be mended to connect
To anode ear 232 or negative electrode lug 234, then positive plate 222 or negative plate 224 can be carried out mending lithium operation.For example, when mending lithium electrode
When ear 236 is connected to anode ear 232, lithium ion access is formed between positive plate 222 and benefit pole piece 226.It is anti-by discharging
It answers, the lithium metal mended in pole piece 226 loses electronics, becomes lithium ion, and moves to and form lithiumation conjunction in positive plate 222
Object.When benefit lithium electrode ear 236 is connected to negative electrode lug 234, lithium ion access is formed between negative plate 224 and benefit pole piece 226.
By exoelectrical reaction, the lithium metal mended in pole piece 226 loses electronics, becomes lithium ion, and move to shape in negative plate 224
At such as LixC6The lithium compound of (in the case of common graphite cathode) etc.
It is appreciated that the operation of the benefit lithium of any one of positive plate 222 and negative plate 224 can at any time into
Row, such as in the cycle for the first time of secondary cell 200, or in cyclic process；In charging, or in electric discharge, etc..
Preferably, such as when completing the charging of secondary cell 200, elemental lithium is all embedded into cathode.At this point, may be due to lithium member
Element is consumed or is formed reasons such as " dead lithiums ", and the lithium ion being embedded in cathode is insufficient, can supplement lithium to negative plate 224 at this time
Ion.In another example when completing the electric discharge of secondary cell 200, elemental lithium all moves to side of the positive electrode.At this point, moving to anode
Lithium ion may be still insufficient, then can supplement lithium ion to positive plate 222.Certainly, as previously mentioned, can also charging when to
Positive plate 222 mends lithium, or mends lithium to negative plate 224 in electric discharge.During above-mentioned benefit lithium, in order to control the speed for mending lithium
Degree, can control discharge process, mend lithium using constant current or constant voltage mends lithium.
Mending the amount of lithium can be determined by testing in advance.For example, the coulombic efficiency of positive half-cell can be measured in terms of
The amount of each cycle period inactivation lithium is calculated, and measures the coulombic efficiency of cathode half-cell and is lost with calculating each cycle period
The amount of lithium living, the difference between the two is the theoretical value that each cycle period requires supplementation with lithium amount.In view of the reality in lithium up process
Efficiency, the lithium amount actually supplemented can be more than theoretical value.On the other hand, when supplementing excessive lithium, lithium precipitation can can occur,
Cause safety issue, so the lithium amount actually supplemented is preferably smaller than theoretical value.In some embodiments, the lithium amount actually supplemented
It can be 0.5~5 times of range of theoretical value.The inventors discovered that, it is contemplated that the safety issues such as lithium efficiency and lithium precipitation are mended,
Preferably, the lithium amount actually supplemented can be 0.6~2.5 times of range of theoretical value, good cell performance to realize
Can, and can guarantee safety.
Fig. 4 shows the flow chart of the method 300 for preparing secondary cell according to an exemplary embodiment of the invention.Such as Fig. 4
Described, method 300 can start from step S310, prepare positive plate, negative plate and diaphragm.As previously mentioned, these elements can
With it is in the prior art identical, therefore be not repeated herein describe its set-up procedure.Then in step S320, this hair can be prepared
Bright benefit pole piece.The process for preparing to mend pole piece may include forming lithium active layer to afflux by techniques such as coating, roll-ins
On body, to form pole piece, then pole piece is cut into the benefit pole piece of required shapes and sizes, and may also include baking process
To obtain dry pole piece.Then in step S330, positive plate, negative plate, benefit pole piece and diaphragm can be assembled into battery core.
The assembling process may include positive plate, negative plate, mend pole piece and diaphragm and be sequentially stacked into stacked arrangement, can also include
By each pole piece and membrane winding at desired shape.As previously mentioned, positive plate, negative plate and diaphragm can be located at by mending pole piece
Stacking on the outside of, can also be located at stack in.It, can will be on tab welding to battery core in step S340.Specifically, by positive
Ear is welded to positive plate, and negative pole lug welding to negative plate mends lithium electrode ear and is welded to benefit pole piece.In this step, if battery core
Then can also include passing through including multiple individual positive plates, multiple individual negative plates and multiple individual benefit pole pieces
Multiple individual positive plates are welded together connection circuit, multiple individual negative plates are welded together, and will be multiple
Pole piece is individually mended to be welded together.
Next, in step S350, then battery core can be encapsulated into form secondary cell in shell, lug extends to shell
In vitro in order to being connected to external equipment.In this step, further include being noted into shell if secondary cell is liquid state batteries
Enter electrolyte.In this way, it has been basically completed the assembling of secondary cell, but in order to enable manufactured secondary cell normally work
Make, it is also necessary to chemical conversion step S360 is carried out to it.Being melted into step S360 can be identical as the chemical conversion step of the prior art, in the step
Part lithium may be consumed in rapid, therefore can also include mending lithium step S370, to be mended to the anode of secondary cell and/or cathode
Lithium is filled, as described previously.In this way, just completing the manufacture of secondary cell, being formed by secondary cell can directly supply
User uses.
The secondary cell of the present invention compared with prior art, has many advantages.For example, the secondary cell of the present invention with it is existing
There is technology to compare, structure change is less, increases only and mends pole piece and benefit lithium electrode ear.Lithium electrode ear is mended by being suitably set, this
The secondary cell of invention can be with completely compatible existing electronic equipment.And by properly modifying charging equipment, such as provide with
Mend the circuit of lithium electrode ear connection, you can benefit lithium is easy to carry out, to improve the performance of secondary cell.Manufacture the process of secondary cell
Need only assure that mend pole piece does not react with environment, this by keeping ambient dew point following in -40 degree, other aspects and
Preparing for existing lithium ion battery is identical.Therefore, manufacturing cost can be substantially reduced in this way.
In existing secondary cell, if directly bonding lithium piece in negative terminal surface, or lithium powder is mixed in cathode, when
When electrolyte is added, discharge chemistry response intensity in situ is very big, and the formation of negative terminal surface SEI can be caused uncontrollable, direct shadow
Ring the cycle characteristics of battery.And the present invention secondary cell in, inject electrolyte after first Zhou Huacheng be free of lithium metal
Formation process it is identical, the generation of SEI is controllable, be conducive to improve battery cycle characteristics.And benefit lithium is carried out again after chemical conversion,
And lithium up process can be controlled by controlling current or voltage, to which the cycle for being conducive to further improve battery is special
Property.
It is also an advantage of the present invention that lithium be stored in mend pole piece on, and and be not involved in normal battery charge and discharge process.
In each cycle period, it is only necessary to supplement a small amount of lithium, such lithium of mending can reduce the probability of cathode analysis lithium.Moreover, mending lithium electrode
The lithium of on piece is only deviate from, and it is not in Li dendrite to mend pole piece, greatly improves battery security.
Some examples of the present invention are described below, and are compared with comparative example to illustrate certain effects of the present invention.
Example 1
1Ah cobalt acid lithiums/graphite Soft Roll electricity is prepared by stirring, coating, roll-in, pole piece cutting, baking pole piece, lamination
The capacity ratio N/P of core, negative material and positive electrode is about 1, after winding one layer of diaphragm, is placed in the left side of dry battery core and mends lithium electrode
Piece mends the dry battery core of lithium to be made, and it includes the metallic lithium layer of copper foil current collector and formation on a current collector to mend pole piece.It is dry to mend lithium
Then battery core soldering polar ear is packaged, and inject electrolyte to form secondary cell wherein it is nickel lug to mend lithium electrode ear.
It is recycled at 0.5 DEG C, to the lithium of anode supplement 0.03Ah capacity after first week charging, first week efficiency is 95%.It is follow-up every
The lithium of 0.001425Ah capacity is supplemented after week charging to graphite cathode.Coulombic efficiency is 99.95% after recycling 20 weeks, and capacity is kept
Rate is 94%.
Example 2
1Ah cobalt acid lithiums/silicium cathode Soft Roll electricity is prepared by stirring, coating, roll-in, pole piece cutting, baking pole piece, lamination
Core, N/P ratios are about 1.1, and after winding one layer of diaphragm, the lithium-aluminium alloy band of steel mesh collector nickel lug is placed in the left side of dry battery core
Shape pole piece mends the dry battery core of lithium to be made.Battery core soldering polar ear is done to mend lithium, is encapsulated into shell to form secondary cell.0.5
It is recycled at DEG C, supplements the lithium of 0.1Ah capacity to cathode after first week charging.It is supplemented to silicium cathode after subsequently charging weekly
The lithium of 0.14Ah capacity.Coulombic efficiency is 99.87% after recycling 20 weeks, capacity retention ratio 87.5%.
Comparative example 1
1Ah cobalt acid lithiums/silicon-carbon Soft Roll electricity is prepared by stirring, coating, roll-in, pole piece cutting, baking pole piece, lamination
Core, N/P ratios are 1, and are assembled into secondary cell.It is recycled at 0.5 DEG C.First week efficiency is 82.31%, and cycle is after 20 weeks
Coulombic efficiency is 99.38%, capacity retention ratio 67.24%.
By comparing example 1 above -2 and comparative example 1 as it can be seen that the present invention secondary cell compared with the existing technology two
Primary cell has better coulombic efficiency and cycle characteristics.
Several embodiments of the present invention are described above for lithium ion/lithium metal battery, however, it is understood that the present invention
Principle also may be used on sodium ion/metal sode cell, be similar in all respects with lithium battery.At this point, mending pole piece can claim
To mend sodium pole piece comprising sodium active layer.Since the sedimentation potential of metallic sodium is higher than lithium, so mending sodium pole piece can be used aluminum material
Collector, such as aluminium foil, aluminium strip, aluminium net etc..It mends sodium lug and aluminium pole ears can also be used.In other words, it should be appreciated that run through this explanation
Book should be also covered by the embodiment of sodium when referring to lithium.
The present invention, however, the present invention is not limited thereto are described above with reference to exemplary embodiment.Those skilled in the art it is aobvious and
Be clear to, in the case where not departing from the scope of the present invention and thought, can carry out various change in form and details and
Modification.The scope of the present invention is only defined by appended claims and its equivalent.
Claims (11)
1. a kind of secondary cell, including：
Positive plate and negative plate, are isolated from each other by diaphragm；And
At least one benefit pole piece comprising lithium active layer, at least one benefit pole piece is also by diaphragm and the anode
Piece and negative plate are kept apart.
2. secondary cell as described in claim 1, wherein the lithium active layer includes pure metal lithium, Li-Si alloy, the conjunction of lithium aluminium
It is one or more in gold, lithium boron alloy and lithium magnesium alloy.
3. secondary cell as described in claim 1, further includes：
Shell, for accommodating the positive plate, negative plate, mending pole piece and diaphragm；
Anode ear is connected to the positive plate and extends to outside the shell；
Negative electrode lug is connected to the negative plate and extends to outside the shell；And
Lithium electrode ear is mended, the benefit pole piece is connected to and extends to outside the shell.
4. secondary cell as claimed in claim 3, wherein multiple positive plates, diaphragm and negative plate are stacked to a stacking, described
One or more of the left side in the stacking, right side, front side, rear side and bottom side place, institute is arranged at least one benefit pole piece
It states anode ear, negative electrode lug and mends lithium electrode ear and top sides in the stacking are set.
5. secondary cell as claimed in claim 3, wherein described when the anode ear is electrically connected to the benefit lithium electrode ear
It mends pole piece and benefit lithium is carried out to the positive plate, and
When the negative electrode lug is electrically connected to the benefit lithium electrode ear, the benefit pole piece carries out benefit lithium to the negative plate.
6. secondary cell as described in claim 1, wherein the benefit pole piece further includes collector, and the lithium active layer is set
It sets on the collector.
7. secondary cell as described in claim 1, wherein the secondary cell include liquid lithium ionic cell, solid-state lithium from
Sub- battery, liquid metal lithium battery, solid metallic lithium battery or colloidal sol lithium ion battery.
8. secondary cell as described in claim 1, wherein the secondary cell is sodium ion or metal sode cell, the benefit
Pole piece is to mend sodium pole piece.
9. a kind of method preparing secondary cell, including：
Prepare positive plate, negative plate and diaphragm；
Prepare to mend pole piece, the benefit pole piece includes lithium active layer；
The positive plate, negative plate, benefit pole piece and diaphragm are assembled into battery core, wherein the positive plate, negative plate and benefit lithium
Pole piece is isolated from each other by the diaphragm；And
The battery core is encapsulated into shell.
10. method as claimed in claim 9, further includes：
Anode ear, negative electrode lug and benefit lithium electrode ear are welded to the positive plate, negative plate and mended in pole piece, wherein in institute
After stating encapsulation step, the anode ear, negative electrode lug and benefit lithium electrode ear are extended to from the battery core except the shell respectively.
11. method as claimed in claim 10, further includes：
Execute the chemical conversion step of secondary cell；And
The anode ear or negative electrode lug are electrically connected to the benefit lithium electrode ear, with by discharge process to the positive plate or cathode
Piece supplements elemental lithium.
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