CN108110257A - A kind of bipolar current collector and the bipolarity solid lithium secondary cell by its assembling - Google Patents
A kind of bipolar current collector and the bipolarity solid lithium secondary cell by its assembling Download PDFInfo
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- CN108110257A CN108110257A CN201711477580.3A CN201711477580A CN108110257A CN 108110257 A CN108110257 A CN 108110257A CN 201711477580 A CN201711477580 A CN 201711477580A CN 108110257 A CN108110257 A CN 108110257A
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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
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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
- H01M4/64—Carriers or collectors
- H01M4/66—Selection of materials
- H01M4/663—Selection of materials containing carbon or carbonaceous materials as conductive part, e.g. graphite, carbon fibres
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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 invention belongs to field of chemical power source, and in particular to a kind of bipolar current collector and the bipolarity solid lithium secondary cell by its assembling.The bipolar current collector is made of polymer and carbon material, and polymer material used is polyethylene, polypropylene, polystyrene or polycarbonate resin, and carbon material used is carbon black, carbon nanotubes or Super P.Alternately superposition obtains bipolar electrode of the bipolarity solid lithium secondary cell by lithium battery solid electrolyte membrane and including above-mentioned bipolar current collector.The present invention is using polymer carbon material composite conductive film as bipolar current collector, easy large area prepares and regulation and control thickness, and is both low density material, in the case of same thickness, quality will be less than metallic aluminium and metallic copper, by the energy density higher of its battery obtained;In addition, the voltage of the bipolarity solid lithium secondary cell can adjust the lamination assembling number of plies to regulate and control as needed, it can further optimize the space of battery pile and reduce gross mass.
Description
Technical field
The invention belongs to field of chemical power source, and in particular to a kind of bipolar current collector and the bipolarity solid-state by its assembling
Lithium secondary battery.
Background technology
Lithium ion battery has high energy density and power density, thus as the first choice of automobile power cell.But
It is that Current commercial lithium ion battery uses inflammable volatile organic liquid electrolyte as ion conducting medium so that lithium ion
Battery is there are serious security risk, when battery easily causes the accidents such as the explosion on fire of battery under conditions of abuse.And it adopts
Inflammable organic electrolyte is substituted with solid electrolyte, is expected to thoroughly solve the safety issue of lithium battery.
Power battery needs multiple battery cells of connecting in order to ensure the big output power of battery, power battery heap.It is and electric
The small fan-out capability that impedance can be caused excessive and then reduce electric current of the connecting portion area of pond monomer, while external connection can occupy
The space of battery and the weight for increasing battery pile.Therefore, external series can reduce the energy density and power density of battery.Make
It is exactly that the internal series-connection of battery is realized using bipolar current collector for one of solution, because the solid-state that solid state battery uses
Electrolyte is not contained in electrolyte, the situation that no liquid flowing causes positive and negative anodes liquid to connect short circuit occurs.And bipolar current collector
Maximum difficult point is that needs meet stable to lithium anode at low voltage and positive electrode is stablized under high voltages
While, also to keep the condition of high electronic conductivity and ionic conductivity insulation, these harsh use conditions limitations
The development and application of bipolar current collector.
A kind of bipolar battery is also referred in the patent of invention of Publication No. CN101076915B, is adopted in embodiment
Bipolar current collector material is stainless steel foil, and mass area ratio is very big, can influence the specific energy density of battery.Though
It so also mentions and thermoplastic polymer may be employed and metal powder is compound prepares collector, but these most metals can
It reacts to form alloy with lithium, it is poor to the electrochemical stability of lithium metal.And the gel electrolyte used in invention be containing
A certain amount of organic solvent, the phenomenon that completely liquid can not being avoided to connect short circuit in actual battery, occur.In addition, Application No.
The conductive film of coating of high molecular polymer formed in the invention of CN200910101378 using polyurethane resin and carbon black, but in fact
It applies aromatic urethane material in example and its compound system is unstable to lithium, and without reference on polymer-carbon in patent
Application of the material as lithium battery collector.
The content of the invention
To solve the disadvantage that the prior art and shortcoming, primary and foremost purpose of the invention is to provide a kind of bipolarity afflux
Body, this bipolar current collector can realize that the function of collector afflux and internal series-connection connect simultaneously in solid state battery system
The function of connecing.
Another object of the present invention is to provide the bipolarity solid lithium secondary cell including the bipolar current collector.
The purpose of the present invention is achieved through the following technical solutions:
A kind of bipolar current collector, is made of polymer and conductive carbon material, polymer used for polyethylene, polypropylene,
Polystyrene or polycarbonate resin, conductive carbon material used are carbon black, carbon nanotubes or Super P, and its preparation method is public affairs
The melting known is compound, the modes such as casting film, and conductive carbon material content is 10~25wt%.
A kind of bipolarity solid lithium secondary cell, is prepared by following steps:
(1) electrode for containing only anode layer is prepared:Lithium battery anode slurry is coated to thickness as described in 10~100 μm
The electrode containing only anode layer is obtained in bipolar current collector, after drying, anode layer weight per unit area is 3~20mg/cm2, cut out
Piece is spare.Drying temperature is preferably 50~100 DEG C.
Wherein, the lithium battery anode slurry is by positive electrode, conductive agent, lithium salts, binding agent and solvent routinely ratio
Allotment is made.The positive electrode can be cobalt acid lithium (LiCoO2), LiMn2O4 (LiMn2O4), nickel cobalt lithium aluminate (NCA), nickel cobalt
LiMn2O4 (NCM) and lithium ferric manganese phosphate (LiFexMn1-xPO4(0≤x≤1)) and lithium titanate (Li4Ti5O12) etc. lithium-ion electrics
Pond positive electrode, the conductive agent can be Super P, and the binding agent can be polyethylene glycol oxide (PEO), and the lithium salts can
Think double (trifluoromethane sulfonic acid acid imide) lithiums (LiTFSI), the solvent can be tetrahydrofuran (THF) solution.Anode material
Material, conductive agent, lithium salts, binding agent and solvent are not limited to the selection, other common described reagents are also applicable.
(2) electrode for containing only negative electrode layer is prepared:Lithium cell cathode material is pressed into thickness as described in 10~100 μm
In bipolar current collector, cut-parts are spare.
(3) bipolar electrode is prepared:In the blank one side compacting for the electrode for containing only anode layer that step (1) is obtained
Thickness is 1~20 μm of lithium cell cathode material, and acquisition one side is anode layer, and opposite side is the bipolar electrode of negative electrode layer, standby
With.
Step (2) and (3) described lithium cell cathode material can be lithium metal or lithium boron alloy.Equally, cathode of lithium battery
Material is not limited to the selection, other common lithium cell cathode materials are also applicable.
(4) bipolarity solid lithium secondary cell is assembled:
Lithium battery solid electrolyte is alternately superimposed on the electrode anode side for containing only anode layer prepared by step (1)
Bipolar electrode prepared by film and step (3), the electrode for the only negative electrode layer for then preparing step (2) are pressed into lithium battery
With the bipolarity solid lithium secondary cell on the blank one side of solid electrolyte membrane, obtained two layers or multi-layer stacks assemble.
It is preferably 2~20MPa that the superposition, which applies pressure,.
The lithium battery solid electrolyte membrane can be following composite solid electrolyte film, mainly be consolidated by oxide
State electrolyte and organic polymer solid electrolyte composition, the wherein content of oxide solid electrolyte are 55%~95wt%;
Oxide solid electrolyte used can be NASICON types solid electrolyte (LAGP or LATP), Garnet-type solid electrolysis
Matter (LLZO) or Ca-Ti ore type solid electrolyte (LLTO);Organic polymer solid electrolyte used can be EO segments and Li
Ion ratio is (20~3):1, the polyethylene glycol oxide (PEO) that weight average molecular weight is 5~1,000,000/bis- (trimethyl fluoride sulfonyl Asia
Amine) lithium (LiTFSI).
The preparation method of the lithium battery solid electrolyte membrane is as follows:To having dissolved the PEO/LiTFSI organic polymers
The middle addition oxide solid electrolyte of tetrahydrofuran (THF) solution of object solid electrolyte, is mixed evenly, whipping temp
Preferably 40~90 DEG C;Then slurry is coated uniformly on above the support carrier that polytetrafluoroethylene (PTFE) is substrate, after drying again
Drying and processing removes support carrier and obtains solid electrolyte membrane;Drying temperature is preferably 50~100 DEG C.Likewise, the lithium electricity
Pond is not limited to the selection with solid electrolyte membrane, other common solid electrolyte membranes are also applicable.
The present invention is had the following advantages compared with the prior art and effect:
Bipolar current collector and its bipolarity solid lithium secondary cell of assembling are due to using the brand-new technical side of the present invention
Case, compared with prior art, the present invention have following evident characteristic:
1st, the present invention uses polymer-carbon material composite conductive film as bipolar current collector, since composite conductive film is adopted
It is combined with polymer and conductive carbon material, thus regulates and controls thickness after easily prepared by large area.And both it is low
Density material, in the case of same thickness, quality will be less than metallic aluminium and metallic copper, can be close in the energy for increasing battery
Degree.
2nd, the present invention, can be to avoid bipolarity electricity using transfer medium of the solid electrolyte without solution as lithium ion
Positive and negative anodes liquid caused by the infiltration or submergence of extremely middle solution connects short circuit.
3rd, the bipolarity solid lithium secondary cell that is assembled of the present invention, since there is conduction electronics using composite conductive film
The function of lithium ion insulation so that composite conductive film can either be used as collector, while again can be as realization internal series-connection
Conductor, thus the voltage of single battery can adjust the lamination assembling number of plies to regulate and control as needed, need not move through external series company
It connects, can further optimize the space of battery pile and reduces gross mass.
Description of the drawings
Fig. 1 is multi-layer stacks bipolarity solid lithium secondary cell model schematic;1 is anode portion in figure;2 be solid-state electricity
Solve matter part;3 be cathode portion;4 be bipolar current collector;5 be bipolar electrode.
Fig. 2 is the voltage capacity charging and discharging curve figure of bipolarity solid lithium secondary cell made from embodiment 2, tests electric current
Density is 30mA g-1, voltage range is 5.5~9.0V;
Fig. 3 is the voltage capacity charging and discharging curve figure of the bipolarity solid lithium secondary cell made from embodiment 3, and test is electric
Current density is 30mA g-1, voltage range is 5.5~9.0V;
Fig. 4 is the voltage capacity charging and discharging curve figure test electricity of the bipolarity solid lithium secondary cell made from embodiment 4
Current density is 30mA g-1, voltage range is 2.0~4.0V.
Specific embodiment
With reference to embodiment, the present invention is described in further detail, but the implementation of the present invention is not limited to this.
Embodiment 1
The assembling of bipolarity solid lithium secondary cell includes the preparation of bipolar electrode, the preparation of solid electrolyte and battery
Assembling, specific implementation process are as follows:
(1) preparation of polymer-carbon material composite conductive film:
Polyethylene and carbon black are pressed 85:15 ratios weigh, and then melting mixing is uniform, and casting film obtains composite conducting
Film, thickness are 30 μm.
(2) preparation of anode layer electrode is contained only
The composite conductive film prepared by step (1) is used as collector, is only applied in one side and is covered with anode sizing agent, opposite side is empty
In vain.
Specific manufacturing step is as follows:
Positive electrode used is lithium ferric manganese phosphate (LiFe0.8Mn0.2PO4), conductive agent used is Super P, is bonded
Agent is polyethylene glycol oxide (PEO), and lithium salts is double (trifluoromethane sulfonic acid acid imide) lithiums (LiTFSI), and solvent is tetrahydrofuran
(THF) solution
A) in proportion 70%:11%:9%:10% weighs LiMn0.8Fe0.2PO4, PEO, LiTFSI and Super P's answers
Object 2g is closed, is positioned in the bottle of the THF solvents containing 4g, the uniform stirring under conditions of 60 DEG C is prepared into slurry;
B) slurry prepared is coated uniformly on composite conductive film one side, then stays overnight it at a temperature of 70 DEG C
Drying, obtains the electrode for containing only anode layer, and mass area ratio is 6mg cm-2, cut-parts are spare.
(3) preparation of negative electrode layer electrode is contained only
Composite conductive film prepared by step (1) is used only to cover sheet metal lithium in one side for collector.
Specific manufacturing step is as follows:
Negative electrode uses sheet metal lithium, lithium metal is cut into required size, then using the pressure of 8MPa
Composite conductive film one side is overlaid on, is prepared into the electrode for containing only negative electrode layer, metallic lithium layer thickness is 10 μm, spare.
(4) preparation of bipolar electrode:
Using the electrode for containing only anode layer prepared by step (2), one layer of sheet metal lithium is covered in opposite side.Specifically
Preparation process is as follows:
The electrode for containing only anode layer prepared by step (2) is cut into required size, then cuts out metallic lithium foil
Required size is cut into, the one side of composite conductive film blank is then overlaid on using the pressure of 8Mpa, is prepared into compound
Conductive film one side is anode layer, and opposite side is the bipolar electrode of negative electrode layer, spare.
(5) preparation of solid electrolyte:
The organic principle of solid electrolyte uses the PEO of 100,000 weight average molecular weight, dissolves the solvent of PEO for THF, electrolyte
For LiTFSI;The inorganic constituents of solid electrolyte is less than the LAGP powder of 300 mesh for particle size.
Specific preparation process is as follows:
A. by EO segments and Li ions 8:1 ratio weighs PEO and LiTFSI (gross mass is about 200mg) and is placed into reagent
In bottle, then THF is used to be dissolved for solvent, condition stirs for the temperature of lower 60 DEG C of inert atmosphere, solid content 8%;
B. the LAGP powder of 1800mg and then is again weighed, is added into the solution containing PEO, then again by it at 60 DEG C
Under the conditions of be mixed evenly, obtain the slurry of solid electrolyte;
C. the slurry configured is coated uniformly on above the support carrier that polytetrafluoro is substrate, 70 DEG C of bakings again after drying
It is dry.Support carrier is finally peeled away, obtains solid electrolyte membrane.
(6) assembling of bipolarity solid lithium secondary cell:
A. consolidating prepared by one layer of step (5) of electrode anode side pressure system of anode layer will be contained only prepared by step (2)
State dielectric film, pressure used are 8MPa;
B. then the bipolar electrode negative side prepared by step (4) is pressed on solid electrolyte membrane;
C. then proceed to the solid electrolyte membrane prepared by step (5) being pressed into side of the positive electrode;
D. step b and c are alternately repeated more times;
E. the only electrode of negative electrode layer prepared by step (3) is pressed on electrolyte layer, obtain multi-layer stacks assembling and
Into bipolarity solid lithium secondary cell.
The bipolarity solid lithium secondary cell schematic diagram of multiple-layer stacked is as shown in Figure 1.
Embodiment 2
The assembling of bipolarity solid lithium secondary cell includes the preparation of bipolar electrode, the preparation of solid electrolyte and battery
Assembling, specific implementation process are as follows:
(1) preparation of polymer-carbon material composite conductive film:
Polypropylene and carbon black are pressed 85:15 ratios weigh, and then melting mixing is uniform, and casting film obtains composite conducting
Film.
The step of step (2)~(5) reference implementation example 1 (2)~(5).
(6) assembling of bipolarity solid lithium secondary cell:
A is by the solid-state contained only prepared by one layer of step (5) of electrode anode side pressure system of anode layer obtained by step (2)
Dielectric film, pressure used are 8MPa;
Bipolar electrode negative side obtained by step (4) is then pressed on electrolyte layer by b;
C then proceedes to the solid electrolyte membrane obtained by step (5) being pressed into side of the positive electrode;
The electrode of step (3) only negative electrode layer obtained is pressed on electrolyte layer by d, is obtained two layers of lamination assembling and is formed
Bipolarity solid lithium secondary cell, test acquired results chemical property as shown in Figure 2.
Embodiment 3
Step and condition are referring to embodiment 2, the difference is that the inorganic constituents of solid electrolyte is replaced with by LAGP
LATP。
It is as shown in Figure 3 that it tests the chemical property of acquired results.
Embodiment 4
Step and condition are referring to embodiment 2, the difference is that positive electrode active materials are by LiMn0.8Fe0.2PO4It replaces with
Li4Ti5O12。
It is as shown in Figure 4 that it tests the chemical property of acquired results.
The embodiment is the preferable embodiment of the present invention, but embodiments of the present invention and from the embodiment
Limitation, other any Spirit Essences without departing from the present invention with made under principle change, modification, replacement, combine, simplification,
Equivalent substitute mode is should be, is included within protection scope of the present invention.
Claims (9)
1. a kind of bipolar current collector, which is characterized in that be made of polymer and conductive carbon material, the polymer is poly- second
Alkene, polypropylene, polystyrene or polycarbonate resin, the conductive carbon material be carbon black, carbon nanotubes or Super P, conductive carbon
Material content is 10~25wt%.
2. a kind of bipolarity solid lithium secondary cell, which is characterized in that be prepared by following steps:
(1) electrode for containing only anode layer is prepared:Lithium battery anode slurry is coated to the claim that thickness is 10~100 μm
The electrode containing only anode layer is obtained in 1 bipolar current collector, after drying;Anode layer mass area ratio is 3~20mg.
(2) electrode for containing only negative electrode layer is prepared:By the lithium cell cathode material that thickness is 1~20 μm be pressed into thickness be 10~
Described in 100 μm of claim 1 in bipolar current collector;
(3) bipolar electrode is prepared:The upper thickness of blank one side compacting for the electrode for containing only anode layer that step (1) is obtained
For 1~20 μm of lithium cell cathode material, acquisition one side is anode layer, and opposite side is the bipolar electrode of negative electrode layer;
(4) bipolarity solid lithium secondary cell is assembled:
On the electrode anode side for containing only anode layer prepared by step (1) alternately superposition lithium battery solid electrolyte membrane and
Bipolar electrode prepared by step (3), the electrode for the only negative electrode layer for then preparing step (2) are pressed into lithium battery with admittedly
On the blank one side of state dielectric film, obtain two layers or bipolarity solid lithium secondary cell that multi-layer stacks assemble.
A kind of 3. bipolarity solid lithium secondary cell according to claim 2, which is characterized in that step (1) described drying
Temperature is 50~100 DEG C, and the pressure that step (4) superposition applies is 2~20MPa.
A kind of 4. bipolarity solid lithium secondary cell according to claim 2, which is characterized in that the lithium battery anode slurry
Material is made of positive electrode, conductive agent, lithium salts, binding agent and solvent;The positive electrode is LiCoO2、LiMn2O4、NCA、NCM
And LiFexMn1-xPO4Any one in (0≤x≤1), the conductive agent are Super P, and the binding agent is PEO, the lithium
Salt is LiTFSI, and the solvent is THF.
5. a kind of bipolarity solid lithium secondary cell according to claim 4, which is characterized in that the positive electrode is led
Electric agent, lithium salts, the mass ratio of binding agent and solvent are 70%:11%:9%:10%.
6. a kind of bipolarity solid lithium secondary cell according to claim 2, which is characterized in that step (2) and (3) are described
Lithium cell cathode material is lithium metal or lithium boron alloy.
A kind of 7. bipolarity solid lithium secondary cell according to claim 2, which is characterized in that the lithium battery solid-state
Dielectric film is mainly made of oxide solid electrolyte and organic polymer solid electrolyte, wherein oxide solid electrolyte
Content be 55%~95wt%;The oxide solid electrolyte is LAGP, LATP, LLZO or LLTO;The organic polymer
Object solid electrolyte is EO segments and Li ion ratios are (20~3):1, weight average molecular weight is 5~1,000,000 PEO/LiTFSI.
A kind of 8. bipolarity solid lithium secondary cell according to claim 7, which is characterized in that the lithium battery solid-state
The preparation method of dielectric film is as follows:To the THF solution for having dissolved the PEO/LiTFSI organic polymers solid electrolyte
Middle addition oxide solid electrolyte, is mixed evenly, and slurry then is coated uniformly on the branch that polytetrafluoroethylene (PTFE) is substrate
It supports above carrier, drying and processing, stripping support carrier obtain solid electrolyte membrane again after drying.
A kind of 9. bipolarity solid lithium secondary cell according to claim 8, which is characterized in that the lithium battery solid-state
In the preparation method of dielectric film, whipping temp is 40~90 DEG C, and drying temperature is 50~100 DEG C.
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Cited By (12)
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CN109768334A (en) * | 2018-12-25 | 2019-05-17 | 中国电子科技集团公司第十八研究所 | Preparation method of bipolar solid-state lithium secondary battery |
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CN109768334A (en) * | 2018-12-25 | 2019-05-17 | 中国电子科技集团公司第十八研究所 | Preparation method of bipolar solid-state lithium secondary battery |
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CN114552027A (en) * | 2021-09-14 | 2022-05-27 | 万向一二三股份公司 | Bipolar all-solid-state battery |
CN114552027B (en) * | 2021-09-14 | 2023-09-05 | 万向一二三股份公司 | Bipolar all-solid-state battery |
CN114024037A (en) * | 2021-10-28 | 2022-02-08 | 中国第一汽车股份有限公司 | Solid-state battery cell, preparation method thereof and energy storage device |
CN114597420A (en) * | 2022-03-04 | 2022-06-07 | 蔚来动力科技(合肥)有限公司 | Lithium ion battery, bipolar current collector and preparation method thereof |
CN114597420B (en) * | 2022-03-04 | 2024-01-12 | 蔚来动力科技(合肥)有限公司 | Lithium ion battery, bipolar current collector and preparation method thereof |
CN114784289A (en) * | 2022-04-18 | 2022-07-22 | 蔚来汽车科技(安徽)有限公司 | Bipolar current collector and preparation method thereof, lithium ion battery and vehicle |
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