CN108242530A - A kind of lithium slurry battery and its negative plate - Google Patents
A kind of lithium slurry battery and its negative plate Download PDFInfo
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- CN108242530A CN108242530A CN201611202373.2A CN201611202373A CN108242530A CN 108242530 A CN108242530 A CN 108242530A CN 201611202373 A CN201611202373 A CN 201611202373A CN 108242530 A CN108242530 A CN 108242530A
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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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- 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
- H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
- H01M10/4235—Safety or regulating additives or arrangements in electrodes, separators or 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
- H01M2220/00—Batteries for particular applications
- H01M2220/20—Batteries in motive systems, e.g. vehicle, ship, plane
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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
Abstract
The present invention provides a kind of negative plate of lithium slurry battery, which includes：Body containing lithium metal, can embedding lithium layers of foil and leakproof separation layer, body containing lithium metal, positioned at the both sides of body containing lithium metal can embedding lithium layers of foil and leakproof separation layer positioned at outermost both sides form sandwich composite construction, the edge of sandwich composite construction carries out insulated enclosure.Wherein, can embedding lithium layers of foil can in lithium slurry battery charge and discharge process in situ dusting formed can embedding lithium porous layer, can the embedding lithium reaction of embedding lithium porous layer can avoid the formation of the face of body surface containing lithium metal Li dendrite；In addition, can embedding lithium layers of foil dusting partially due to increase the surface area of material and therefore can reduce the real current density of electrode, can equally avoid the formation of the face of body surface containing lithium metal Li dendrite in this way.In addition, can embedding lithium porous layer be formed in situ in inside battery, without additionally prepare it is porous can embedding lithium layer process, therefore can effectively simplify the preparation process of pole piece, save cost and improve production efficiency.
Description
Technical field
The invention belongs to electrochemical kinetics battery technology field, more particularly to a kind of lithium slurry battery and its negative plate.
Background technology
Lithium ion battery is the novel high-energy battery using lithium intercalation compound as positive and negative pole material, with lead-acid battery, ni-mh
Battery is compared to having the advantages that higher than energy, voltage is high, self discharge is small, good cycle and long lifespan etc. are a series of, increasingly
It is concerned by people.In recent years, lithium ion battery technology achieves fast development, has started to be applied in electric vehicle.
Lithium slurry battery include electrode slice and electrolyte, inject electrolyte after battery positive plate and/or negative plate inside
Electrocondution slurry is formed with, electrocondution slurry contains the conductive particle that certain proportion suspends or precipitates in the electrolytic solution.When battery by
When external impact or concussion, since this partially electronically conductive particle is not adhesively fixed, it can move in the electrolytic solution, and formed
Dynamic conductive network.Conductive particle is led for carbon black, Ketjen black, graphene, carbon nanotube, carbon fiber or metallic conduction particle etc.
One or more of electric agent mixture or conductive particle for electrode active material and above-mentioned conductive agent compound or mix
Object, compound or mixing mode include surface cladding, bonding or mechanical mixture etc..
In the lithium slurry battery mentioned in Chinese invention patent CN201610074921.1, the negative current collector of electronic conduction
It is close to the separation layer of battery so that battery is in high rate charge-discharge and lithium ion is easily deposited on negative current collector when overcharging
Surface pierces through separation layer so as to there is " Li dendrite " and leads to the danger of internal short-circuit of battery.Chinese invention patent
CN201610621508.2 propose by set between separation layer and body containing lithium metal it is porous can embedding lithium current collector layer avoid
The surface that lithium is deposited on the body containing lithium metal forms Li dendrite, so as to improve the safety of battery.But it needs additionally to prepare porous
Can embedding lithium current collector layer process, therefore manufacture cost it is higher.
Invention content
For the problem present on, the present invention provides a kind of negative plate of lithium slurry battery.The negative plate is included containing lithium
Metallic object, can embedding lithium layers of foil and leakproof separation layer.Wherein, can embedding lithium layers of foil can lead in charge and discharge process several times before battery
Cross lithium ion embedded abjection reaction it is in situ be pulverized into can embedding lithium porous layer, can the embedding lithium reaction of embedding lithium porous layer can avoid containing
The formation of lithium metal body surface face Li dendrite；In addition, can embedding lithium layers of foil dusting partially due to increase the surface area of material and because
This can reduce the real current density of electrode, can equally avoid the formation of the face of body surface containing lithium metal Li dendrite in this way, so as to
Increase battery security.In addition, can embedding lithium porous layer be formed in situ in inside battery, without additionally prepare it is porous can embedding lithium
The process of layer, therefore can effectively simplify the preparation process of pole piece, save cost and improve production efficiency.In addition, containing lithium metal
Body is simultaneously as negative electrode active material and lithium source, and pair is anti-during can effectively supplementing the formation of cathode SEI films and circulating battery
Cope with the consumption of anode lithium.
Technical solution provided by the invention is as follows：
A kind of negative plate of lithium slurry battery is provided according to the present invention, which includes：Body containing lithium metal, can embedding lithium foil
Layer and leakproof separation layer, body containing lithium metal, positioned at the both sides of body containing lithium metal can embedding lithium layers of foil and positioned at outermost both sides
Leakproof separation layer forms sandwich composite construction, and the edge of the sandwich composite construction carries out insulated enclosure.It can embedding lithium layers of foil energy
Enough dusting formation in situ in lithium slurry battery charge and discharge process can embedding lithium porous layer.It wherein, can embedding lithium layers of foil original position dusting shape
Into can embedding lithium porous layer be to realize in the following way：Before lithium slurry battery during charge and discharge several times, lithium ion exists
Embedded abjection reaction that can be in the material of embedding lithium layers of foil so that can embedding lithium layers of foil original position dusting formation can embedding lithium porous layer.
Body containing lithium metal can be single layer structure or multilayered structure, and the material of the body containing lithium metal can be lithium metal or lithium base
Alloy.Lithium-base alloy can be Li-Al, Li-Si, Li-Mg, Li-Sn, Li-Bi, Li-Sb etc., can be binary, ternary or
It is multicomponent alloy, may include that Mg, Ca, Al, Si, Ge, Sn, Pb, As, Sb, Bi, Pt, Ag, Au, Zn, Cd, Hg etc. can be in alloy
Lithium is dissolved and/or the element of addition reaction, wherein the content of non-elemental lithium is not more than 50%.It is multilayer in body containing lithium metal
In the case of structure, the material of each layer can be identical or can be different.Body containing lithium metal can by welding, spraying, being bonded, electrification
The mode of plating, chemical plating or machinery press-in is fixed on current collector layer and/or can embedding lithium layers of foil.
Being respectively equipped in the both sides of the body containing lithium metal can embedding lithium layers of foil.Can embedding lithium layers of foil material it is reversible de- for that can carry out
Embedding lithium reaction, volume change is apparent during removal lithium embedded and is easy to the material of dusting in situ.Can the material of embedding lithium layers of foil can be with
Including：Aluminium and acieral, tin and kamash alloy, zinc and zinc-containing alloy, silicon and silicon-base alloy etc., above-mentioned material contain Mg, Ca,
Si, Ge, Sn, Pb, As, Sb, Bi, Pt, Ag, Au, Zn, Cd, Hg etc. can be dissolved with lithium and/or the element of addition reaction.It can
The thickness of embedding lithium layers of foil for 0.01 μm~1000 μm, preferably 5 μm~200 μm, each can embedding lithium layers of foil can be single layer structure
Or multilayered structure.Can embedding lithium layers of foil in the case of multilayered structure, the material of each layer can be identical or different.In multilayered structure
Each layer can only stack together or can be by welding, spraying, being bonded, electrochemical plating, chemical plating, vacuum vapor deposition
Or the modes such as machinery press-in link together.In addition, can embedding lithium layers of foil body containing lithium metal and/or collection can be adhered to by binding agent
Fluid layer so that sheet or powdery after dusting can intercalation materials of li ions be still bonded in it is not easily to fall off on body containing lithium metal, in this way
Can be further ensured that by can after embedding lithium layers of foil dusting obtained sheet or powdery can intercalation materials of li ions and can embedding lithium it is porous
The electrical connection properties of layer.
Will be described in detail below can embedding lithium layers of foil be pulverized into situ in charge and discharge process can embedding lithium porous layer process.
Before lithium slurry battery during charge and discharge several times, in charging process, lithium ion can embedding lithium layers of foil surface obtain electronics and it is embedded or
Deposit to can in the material of embedding lithium layers of foil and with can the material of embedding lithium layers of foil solid solution and/or addition reaction occurs；In discharge process
In, the lithium of solid solution and/or addition reaction occurs from can deviate from the material of embedding lithium layers of foil.Due to aluminium and acieral, tin and tin
It is larger that the materials such as based alloy, zinc and zinc-containing alloy, silicon and silicon-base alloy in embedding lithium take off the front and rear volume change of lithium reaction, therefore will
Cause can embedding lithium layers of foil dusting, can embedding lithium porous layer so as to be formed.This can embedding lithium porous layer in battery assembling pressure, binding agent
The effects that under continue to keep being electrically connected with current collector layer and/or body containing lithium metal.When lithium slurry battery high current charge-discharge and mistake
When filling, under identical apparent area and apparent electric current, can embedding lithium porous layer can effectively reduce electrode current density, reduce electricity
It polarizes in pond；In addition, can enter partially into the dusting in negative plate electrolyte inside can the stream of intercalation materials of li ions in the electrolytic solution
Change effect prevents the growth of Li dendrite, therefore can be effectively prevented from formation of the Li dendrite in the face of body surface containing lithium metal, so as to increase
Power up the safety in pond.
Leakproof separation layer positioned at outermost both sides may be single layer structure or multilayered structure.Each layer in multilayered structure
Material, thickness, aperture and porosity can be identical or different.The material of leakproof separation layer can be that electronics is nonconducting porous poly-
Close object material；It is answered alternatively, the material of leakproof separation layer can be the nonconducting inorganic non-metallic material of electronics with organic polymer
The porous material of conjunction；Alternatively, the material of leakproof separation layer can be the nonconducting polymeric matrix of electronics, liquid organic plasticizers
With the gel polymer electrolyte composite material of the compound composition of lithium salts three parts；Alternatively, the material of leakproof separation layer can be
In the hole of the nonconducting porous polymer material of electronics or in inorganic non-metallic material and the compound porous material of organic polymer
The electrolyte of ionic conduction or polymeric colloid material are impregnated in the hole of material.Leakproof separation layer is in addition to playing insulating electron
Except effect, also act as after preventing dusting can the effect that is leaked from negative plate of intercalation materials of li ions.Preferably, the hole of leakproof separation layer
Diameter is 10 μm~800 μm, and thickness is 0.01 μm~1000 μm, and through-hole porosity is 10%~90%.
Leakproof separation layer, can embedding lithium layers of foil, body containing lithium metal, it is another can embedding lithium layers of foil and another leakproof separation layer form folder
Heart composite construction.The edge of sandwich composite construction can be realized exhausted by the stickup for the leakproof separation layer for being located at outermost both sides
Edge seals.Herein it should be pointed out that by the winding of single leakproof separation layer and cathode can also be realized in edge stickup
The leakproof isolation of piece and insulated enclosure.In addition, sandwich composite construction can be by being set to the insulated enclosure of its edge
Frame realizes insulated enclosure.Insulated enclosure frame can be connected to sandwich composite construction by way of hot pressing or stickup.Insulated enclosure
The material of frame can be the polymer material of insulation electrolyte resistance, and the polymer material for the electrolyte resistance that insulate is polyvinyl chloride, gathers
Ethylene, polypropylene, polystyrene, polytetrafluoroethylene (PTFE), polyester terephthalate, polyamide, polyimides, polyethers nitrile, polypropylene
One kind in sour methyl esters, Kynoar, polyurethane, polyacrylonitrile, butadiene-styrene rubber, sodium carboxymethylcellulose and improved polyalkene
It is or several.
Negative plate can also include one or more current collector layers.Current collector layer can be set to such as one in lower portion or more
It is a：Between two layers in the multilayered structure of the body containing lithium metal, body containing lithium metal and can be between embedding lithium layers of foil and can embedding lithium layers of foil
Multilayered structure in two layers between.In other words, current collector layer can be set to two layers in the multilayered structure of the body containing lithium metal
Between and/or the body containing lithium metal both sides and/or can be in the multilayered structure of embedding lithium layers of foil two layers between.Current collector layer can be to lead
Metal layer, the conductive metal layer are metal mesh or woven wire cloth, and mesh is rectangular, diamond shape, rectangle or polygon etc.；
Alternatively, the conductive metal layer can be the porous foam metal layer with porous structure；Alternatively, the conductive metal layer is metallic plate
Or metal foil is formed through mechanical stamping or chemical attack；Alternatively, it is set among the multilayered structure of the body containing lithium metal in current collector layer
When, conductive metal layer can also be metallic plate or metal foil.The material of conductive metal layer is stainless steel, nickel, titanium, silver, tin, tin plating
Copper or nickel-clad copper etc..In addition, current collector layer can be electric conduction of carbon fiber cloth, wire and organic fiber silk hybrid conductive cloth.In addition,
Current collector layer can be that surface coats conductive coating or is coated with the porous organic material of metallic film, and porous organic material includes natural
Linen-cotton, terylene, aramid fiber, nylon, polypropylene fibre, polyethylene and polytetrafluoroethylene (PTFE) etc..
Negative plate can also be equipped with negative lug.Negative lug can be electrically connected with body containing lithium metal；Alternatively, negative lug can be with
Current collector layer is electrically connected；Alternatively, negative lug can be electrically connected with body containing lithium metal and is electrically connected with current collector layer.That is, afflux
Layer and body containing lithium metal can play the role of collector.When current collector layer and the afflux simultaneously of body containing lithium metal, catchment effect
Uniformly, fever caused by high rate charge-discharge can be avoided.
A kind of lithium slurry battery is provided according to the present invention, lithium slurry battery includes：The negative plate of above-mentioned lithium slurry battery,
Positive plate, battery case, positive terminal, negative terminal, liquid injection port and the electrolyte of lithium slurry battery, wherein, negative plate with
Positive plate intersects stacked composition battery core, which is set in battery case.The positive pole ear of battery core is electrically connected to positive terminal,
The negative lug of battery core is electrically connected to negative terminal.Positive terminal and negative terminal are stretched out from battery case and and battery case
Between Fluid Sealing, electrolyte battery core is injected into battery case by liquid injection port and is placed in electrolyte.
The structure of the positive plate of lithium slurry battery can be sandwich anode composite piece.It provides by way of example sandwich multiple
The structure of positive plate is closed, in order to more fully understand the present invention.Sandwich anode composite piece can include porous afflux anode layer and
Anode sizing agent, porous afflux anode layer are made of the single or double coating porous anode material layer of porous anode collector, and two
The anode sizing agent of 0~5mm thickness is filled between a porous afflux anode layer, part or all of anode sizing agent penetrates into porous collection
In the hole for flowing anode layer, sandwich anode composite piece is formed；Sandwich anode composite piece is surrounded by insulated enclosure frame, and insulation is close
Frame is sealed in " returning " shape, and with porous afflux anode layer edge fixing seal, prevent anode sizing agent from sandwich four side of anode composite piece
Leakage.It should be pointed out that positive plate herein can be any positive plate for lithium slurry battery, structure is not limited to above-mentioned
Example.
Above-mentioned anode sizing agent can include electrolyte and the positive conductive particle that can be flowed in the electrolytic solution,
In, the mass ratio that positive conductive particle accounts for anode sizing agent is 5%~80%, and average grain diameter is 0.5 μm~500 μm.Positive conductive
Particle can be the one of the conductive agents such as carbon black, Ketjen black, graphene, carbon nanotube, carbon fiber and all kinds of metallic conduction particles
Kind is several compound, and compound mode includes surface cladding, bonding or mechanical mixture etc.；Alternatively, positive conductive particle can be
The compound or mixture of positive electrode active materials and above-mentioned all kinds of conductive agents, wherein, the quality of positive electrode active materials and conductive agent
Than being 0~98：100~2, compound or mixing mode includes surface cladding, bonding or mechanical mixture etc..Positive electrode active materials are
LiFePO4, lithium manganese phosphate, lithium metasilicate, ferric metasilicate lithium, sulphate cpd, sulphur carbon complex, sulphur simple substance, titanium sulphur compound,
Molybdenum sulfur compound, iron sulphur compound, doped lithium manganese oxide, lithium and cobalt oxides, Li-Ti oxide, lithium-barium oxide, lithium nickel manganese
Oxide, lithium nickel cobalt oxides, lithium nickel cobalt aluminum oxide, lithium nickel aluminum oxide, lithium nickel cobalt manganese oxide, lithium iron Ni, Mn oxide
In it is one or more.
It should be pointed out that positive plate herein can be any positive plate for lithium slurry battery, structure and material is simultaneously
It is not limited to above-mentioned example.
Advantage of the invention is that：
(1) in lithium slurry battery cathode sheet can embedding lithium layers of foil can in charge and discharge original position dusting formed can embedding lithium it is porous
Layer, without extraly prepare it is porous can embedding lithium layer, therefore can effectively simplify the preparation process of negative plate, saving cost simultaneously
Improve production efficiency；
(2) dusting in situ formed can embedding lithium porous layer can be effectively reduced the current density of electrode, reduce battery pole
Change, and can by can embedding lithium porous layer atomized particles material rheology of the non-adhesive fixed part in negative plate electrolyte inside
The growth to prevent Li dendrite is acted on, so as to be effectively prevented from formation of the Li dendrite in the face of body surface containing lithium metal, therefore is increased
The safety of battery is added；
(3) body containing lithium metal in lithium slurry battery cathode sheet, can be effective simultaneously as negative electrode active material and lithium source
Consumption of the side reaction to lithium during ground supplement cathode SEI films formation and circulating battery, it is close so as to improve the energy of battery
It spends and improves cycle performance.
Description of the drawings
Fig. 1 is the schematic diagram of the lithium slurry battery of the present invention；
Fig. 2 be according to the present invention can embedding lithium layers of foil original position dusting schematic diagram, wherein, Fig. 2 (a) is lithium ion and not
Embedded lithium ion can embedding lithium layers of foil schematic diagram；Fig. 2 (b) is schematic diagram when lithium ion insertion can be in embedding lithium layers of foil；Fig. 2
(c) for can embedding lithium layers of foil original position dusting formed can embedding lithium porous layer schematic diagram；
Fig. 3 is the charging and discharging curve figure of lithium slurry battery, wherein, cell positive material is starched for LiFePO4 in Fig. 3 (a)
Material, cathode be lithium metal, can embedding lithium layers of foil be aluminium foil；Cell positive material is LiFePO4 slurry in Fig. 3 (b), cathode only wraps
Include can embedding lithium layers of foil, can embedding lithium layers of foil be aluminium foil；
Fig. 4 is the schematic cross-section according to the negative plate of the lithium slurry battery of an embodiment of the present invention；
Fig. 5 is the schematic cross-section according to the negative plate of the lithium slurry battery of another embodiment of the present invention.
Reference numerals list
1 --- sandwich anode composite piece
101 --- porous afflux anode layer
102 --- anode sizing agent
2 --- negative plate
201st, 201' --- separation layer
202nd, 202' --- it can embedding lithium layers of foil
203rd, 203' --- body containing lithium metal
204 --- sandwich composite construction
205th, 205' --- current collector layer
206' --- insulated enclosure frame
3 --- separate cavities
Specific embodiment
Below in conjunction with attached drawing, by embodiment, the present invention will be further described.
Fig. 1 is the schematic diagram according to the lithium slurry battery of the present invention.The battery core of lithium slurry battery includes several and alternately sets
The sandwich anode composite piece 1 and negative plate 2 put, it is 0.1mm~1mm that height is equipped between sandwich anode composite piece 1 and negative plate 2
Separate cavities 3, electrolyte is full of in separate cavities 3.Sandwich anode composite piece 1 includes porous afflux anode layer 101 and anode sizing agent
102, porous afflux anode layer 101 is made of the single or double coating porous anode material layer of porous anode collector, two
It is oozed between porous afflux anode layer 101 filled with the anode sizing agent 102 that thickness is 0~5mm, part or all of anode sizing agent 102
It arrives thoroughly in the hole of porous afflux anode layer 101, forms sandwich anode composite piece 1.Negative plate 2 include leakproof separation layer 201, can
Embedding lithium layers of foil 202 and body containing lithium metal 203, wherein leakproof separation layer 201, can embedding lithium layers of foil 202 and body containing lithium metal 203 form
Sandwich composite construction 204.When over-charging of battery or big multiplying power fast charge, lithium ion will not largely be deposited on body containing lithium metal 203
Surface, but will be embedded into and can avoid and form Li dendrite in the face of body surface containing lithium metal in embedding lithium layers of foil 202；In addition contain lithium
Cathode SEI films form the consumption to lithium ion when metallic object 203 can supplement battery charge and discharge process, particularly initial charge.
Fig. 2 be according to the present invention can embedding lithium layers of foil original position dusting schematic diagram.Wherein, Fig. 2 (a) is lithium ion and not
Embedded lithium ion can embedding lithium layers of foil schematic diagram；Fig. 2 (b) is schematic diagram when lithium ion insertion can be in embedding lithium layers of foil；Fig. 2
(c) for can embedding lithium layers of foil original position dusting formed can embedding lithium porous layer schematic diagram.It in the following, can embedding lithium layers of foil original position dusting by explanation
Formed can embedding lithium porous layer process.Herein, can embedding lithium layers of foil material using aluminium as example.In charging process, lithium ion exists
Can embedding lithium layers of foil surface obtain electronics and it is embedded or deposit to can in the material of embedding lithium layers of foil and with can be in embedding lithium layers of foil aluminium it is former
Solid solution or addition reaction occur for son；In discharge process, the lithium of solid solution or addition reaction occurs from can be in the material of embedding lithium layers of foil
Abjection.Since aluminium takes off in embedding lithium, the front and rear volume change of lithium reaction is larger, by cause can embedding lithium layers of foil can intercalation materials of li ions
Dusting, can embedding lithium porous layer and the powdered material of powdery or sheet so as to be formed.The powdered material of a powdery or sheet part
Body containing lithium metal and/or current collector layer can be adhered to by binding agent, and another part can enter the electrolyte in negative plate
In.Being adhered to the powdered material of metallic object and/or current collector layer can continue to be electrically connected with current collector layer and/or the holding of body containing lithium metal
And it can continue to occur the reaction of removal lithium embedded.Also can into the powdery in the electrolyte in negative plate or the powdered material of sheet
It is enough to play the role of inhibiting lithium dendrite growth under the theomorphism of electrolyte.
Fig. 3 is the charging and discharging curve figure of lithium slurry battery, wherein, cell positive material is starched for LiFePO4 in Fig. 3 (a)
Material, cathode be lithium metal, can embedding lithium layers of foil be aluminium foil；Cell positive material is LiFePO4 slurry in Fig. 3 (b), cathode only wraps
Include can embedding lithium layers of foil, can embedding lithium layers of foil be aluminium foil.Show occur two charging platforms during initial charge in Fig. 3 (a),
It can thus be seen that having completed embedding lithium alloyage (2.85V) in first charge-discharge, lithium ion will not be hindered to pass through, after battery
It is continuous to show as discharge and recharge reaction of the LiFePO4 to lithium metal.Embedding lithium alloyage reaction electricity occurs in Fig. 3 (b) during aluminium foil charge and discharge
Position is 3.28V, and it is 2.85V to take off lithium current potential.It can be seen from the figure that cathode only include aluminium foil in the case of battery performance compared with
Difference, this is because dusting is serious after aluminum material alloying reaction, capacity attenuation is quickly.
Fig. 4 is the schematic cross-section according to the negative plate of the lithium slurry battery of an embodiment of the present invention.Negative plate includes
The body containing lithium metal 203 of individual layer.Current collector layer 205 is respectively equipped in the both sides of body containing lithium metal 203.Body containing lithium metal passes through welding
Mode be fixed on current collector layer.Being equipped on the side not contacted with body containing lithium metal 203 of current collector layer 205 can embedding lithium layers of foil
202.Can embedding lithium layers of foil 202 can be by conductive adhesive in current collector layer 205.Lithium slurry battery is in preceding charge and discharge process several times
In, lithium ion can in embedding lithium layers of foil 202 it is embedded deviate from and cause can embedding lithium layers of foil be pulverized into situ can embedding lithium porous layer.It can be embedding
Lithium porous layer can either allow lithium ion is smooth to pass through, and can overcharge or greatly in the case of multiplying power fast charge so that lithium ion is embedding
Entering can be in intercalation materials of li ions to it.In this way, the lithium ion insertion reaction occurred on cathode will not become lithium ion containing lithium metal
The deposition in body surface face, therefore avoid and form Li dendrite on the surface of the body containing lithium metal.Can the outside of embedding lithium layers of foil 202 set
There is leakproof separation layer 201, the end of two leakproof separation layers 201 links together to form negative plate by way of stickup
The insulated enclosure of edge.Can embedding lithium layers of foil 202 dusting can intercalation materials of li ions part be adhered to current collector layer 205 and part
Enter in the electrolyte in negative plate, leakproof separation layer 201 can prevent dusting can intercalation materials of li ions leak into outside negative plate
In the electrolyte in face.
Fig. 5 is the schematic cross-section according to the negative plate of the lithium slurry battery of another embodiment of the present invention.Negative plate packet
Include the 203' of body containing lithium metal with double-layer structure.Current collector layer 205' is equipped between the double-layer structure of the 203' of body containing lithium metal.
Body containing lithium metal is fixed on current collector layer by way of bonding.Do not contacted with current collector layer 205' the one of the 203' of body containing lithium metal
Side be equipped with double-layer structure can embedding lithium layers of foil 202'.Can embedding lithium layers of foil 202' double-layer structure have different thickness simultaneously
By conductive adhesive together.Can embedding lithium layers of foil 202' can be by conductive adhesive in the 203' of body containing lithium metal.Lithium slurry electricity
Chi Qian is several times in charging process, lithium ion can in embedding lithium layers of foil it is embedded deviate from and cause can embedding lithium layers of foil be pulverized into situ can
Embedding lithium porous layer.Can embedding lithium porous layer can either allow lithium ion is smooth to pass through, and can overcharge or the feelings of big multiplying power fast charge
Under condition so that lithium ion be embedded into it can be in intercalation materials of li ions.In this way, the lithium ion insertion reaction occurred on cathode will not become
Lithium ion therefore is avoided and forms Li dendrite on the surface of the body containing lithium metal in the deposition in the face of body surface containing lithium metal.Can be embedding
The outside of lithium layers of foil 202' is equipped with leakproof separation layer 201'.Entire sandwich composite construction is sealed by insulated enclosure frame 206'
Connection.Can embedding lithium layers of foil 202' dusting can intercalation materials of li ions part be adhered to the 203' of body containing lithium metal and part enter it is negative
In electrolyte in pole piece, leakproof separation layer 201' and insulated enclosure frame 206' can prevent dusting can intercalation materials of li ions leak into
In electrolyte outside negative plate.
The specific embodiment of the invention is not limited to the present invention.Any those skilled in the art are not departing from
Under technical solution of the present invention ambit, all technical solution of the present invention is made using the methods and technical content of the disclosure above
Many possible changes and modifications or the equivalent embodiment for being revised as equivalent variations.Therefore, it is every without departing from the technology of the present invention side
The content of case, technical spirit any simple modifications, equivalents, and modifications made to the above embodiment according to the present invention,
Still fall within technical solution of the present invention protection in the range of.
Claims (16)
1. a kind of negative plate of lithium slurry battery, which is characterized in that the negative plate includes：Body containing lithium metal, can embedding lithium layers of foil
And leakproof separation layer, the body containing lithium metal embedding lithium layers of foil and can be located at positioned at described in the both sides of body containing lithium metal
The leakproof separation layer of outermost both sides forms sandwich composite construction, and the edge of the sandwich composite construction insulate close
Envelope, wherein, it is described can embedding lithium layers of foil can in situ dusting formation can embedding lithium porous layer in lithium slurry battery charge and discharge process.
2. the negative plate of lithium slurry battery according to claim 1, wherein, it is described can the thickness of embedding lithium layers of foil be 0.01 μm
~1000 μm.
3. the negative plate of lithium slurry battery according to claim 2, wherein, it is described can embedding lithium layers of foil thickness for 5 μm~
200μm。
4. the negative plate of lithium slurry battery according to any one of claim 1 to 3, wherein, the body containing lithium metal, institute
State can embedding lithium layers of foil and the leakproof separation layer be able to as single layer structure or multilayered structure；
In the case of the multi-layer structure, the layers of material in the multilayered structure of the body containing lithium metal and thickness are identical or different；
The layers of material that can be in the multilayered structure of embedding lithium layers of foil and thickness are identical or different；Each layer material in the leakproof separation layer
Material, thickness, aperture and porosity are identical or different.
5. the negative plate of lithium slurry battery according to any one of claim 1 to 3, wherein, the body containing lithium metal
Material is lithium metal or lithium-base alloy；
Wherein, it is described can embedding lithium layers of foil material for can carry out reversible removal lithium embedded reaction, during removal lithium embedded volume occur
Change and generate the material of dusting in situ, it is described can the material of embedding lithium layers of foil include aluminium and acieral, tin and kamash alloy, zinc
And zinc-containing alloy, silicon and silicon-base alloy.
6. the negative plate of lithium slurry battery according to any one of claim 1 to 3, wherein, the sandwich composite construction
Edge by be located at outermost both sides the leakproof separation layer stickup realize insulated enclosure.
7. the negative plate of lithium slurry battery according to any one of claim 1 to 3, wherein, the sandwich composite construction
Edge be equipped with insulated enclosure frame, the insulated enclosure frame is connected to described sandwich compound by way of hot pressing or stickup
Structure, the material of the insulated enclosure frame are the polymer material of insulation electrolyte resistance, the polymer of the insulation electrolyte resistance
Material is polyvinyl chloride, polyethylene, polypropylene, polystyrene, polytetrafluoroethylene (PTFE), polyester terephthalate, polyamide, polyamides are sub-
Amine, polyethers nitrile, polymethyl acrylate, Kynoar, polyurethane, polyacrylonitrile, butadiene-styrene rubber, sodium carboxymethylcellulose and change
One or more of property polyolefin.
8. the negative plate of lithium slurry battery according to any one of claim 1 to 3, wherein, the leakproof separation layer
Material is the nonconducting porous polymer material of electronics；Alternatively, the material of the leakproof separation layer is nonconducting inorganic for electronics
Nonmetallic materials and the compound porous material of organic polymer；Alternatively, the material of the leakproof separation layer is nonconducting for electronics
The gel polymer electrolyte composite material of polymeric matrix, liquid organic plasticizers and the compound composition of lithium salts three parts；Alternatively,
The material of the leakproof separation layer is in the hole of the nonconducting porous polymer material of electronics or in inorganic non-metallic material
The electrolyte of ionic conduction or polymeric colloid material are impregnated in the hole of compound porous material with organic polymer.
9. the negative plate of lithium slurry battery according to any one of claim 1 to 3, wherein, the leakproof separation layer
Aperture is 10 μm~800 μm, and thickness is 0.01 μm~1000 μm, and through-hole porosity is 10%~90%.
10. the negative plate of lithium slurry battery according to claim 4, wherein, the negative plate further includes multiple current collector layers,
The multiple current collector layer be set to the body containing lithium metal and it is described can embedding lithium foil between embedding lithium layers of foil and/or described in being set to
Between two layers in the multilayered structure of layer.
11. the negative plate of lithium slurry battery according to claim 10, wherein, the current collector layer is conductive metal layer, institute
Conductive metal layer is stated as metal mesh or woven wire cloth, mesh is rectangular, diamond shape, rectangle or polygon；Alternatively, described lead
Metal layer is the porous foam metal layer with porous structure；Alternatively, the conductive metal layer is passed through for metallic plate or metal foil
Mechanical stamping or chemical attack form, and the material of the conductive metal layer is stainless steel, nickel, titanium, silver, tin, tin-coated copper or nickel plating
Copper；Or
The current collector layer is electric conduction of carbon fiber cloth, wire and organic fiber silk hybrid conductive cloth；Or
The current collector layer coats conductive coating for surface or is coated with the porous organic material of metallic film, the porous organic material
Including natural linen-cotton, terylene, aramid fiber, nylon, polypropylene fibre, polyethylene and polytetrafluoroethylene (PTFE).
12. the negative plate of lithium slurry battery according to claim 10, wherein, it is described can embedding lithium layers of foil pass through conductive bond
Agent is adhered to the body containing lithium metal and/or is adhered to the current collector layer.
13. the negative plate of lithium slurry battery according to claim 4, wherein, the negative plate further includes current collector layer, described
Between current collector layer be set in the multilayered structure of the body containing lithium metal two layers and/or it is set to the multiple current collector layer setting
In the body containing lithium metal and it is described can between embedding lithium layers of foil and/or be set to it is described can be in the multilayered structure of embedding lithium layers of foil two
Between layer.
14. the negative plate of lithium slurry battery according to claim 13, wherein, the current collector layer is conductive metal layer, institute
Conductive metal layer is stated as metal mesh or woven wire cloth, mesh is rectangular, diamond shape, rectangle or polygon；Alternatively, described lead
Metal layer is the porous foam metal layer with porous structure；Alternatively, the conductive metal layer is passed through for metallic plate or metal foil
Mechanical stamping or chemical attack form；Or the conductive metal layer be metallic plate or metal foil, the material of the conductive metal layer
Expect for stainless steel, nickel, titanium, silver, tin, tin-coated copper or nickel-clad copper；Or
The current collector layer is electric conduction of carbon fiber cloth, wire and organic fiber silk hybrid conductive cloth；Or
The current collector layer coats conductive coating for surface or is coated with the porous organic material of metallic film, the porous organic material
Including natural linen-cotton, terylene, aramid fiber, nylon, polypropylene fibre, polyethylene and polytetrafluoroethylene (PTFE).
15. the negative plate of the lithium slurry battery according to any one of claim 10 to 14, wherein, the negative plate is equipped with
Negative lug, the negative lug are electrically connected with the body containing lithium metal；Alternatively, the negative lug is electrically connected with the current collector layer
It connects；Alternatively, the negative lug is electrically connected with the body containing lithium metal and is electrically connected with the current collector layer.
16. a kind of lithium slurry battery, which is characterized in that the lithium slurry battery includes：According to any one of claim 1 to 15
The negative plate of lithium slurry battery, the positive plate of lithium slurry battery, battery case, positive terminal, negative terminal, liquid injection port
And electrolyte, wherein, the negative plate intersects stacked composition battery core with the positive plate, and the battery core is set to the battery
In housing, the positive pole ear of the battery core is electrically connected to the positive terminal, and the negative lug of the battery core is electrically connected to described
Negative terminal, the positive terminal and negative terminal are stretched out from the battery case and fluid is close between the battery case
Envelope, injects the electrolyte battery core into the battery case by the liquid injection port and is placed in electrolyte.
Priority Applications (3)
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|---|---|---|---|
| CN201611202373.2A CN108242530B (en) | 2016-12-23 | 2016-12-23 | Lithium slurry battery and negative plate thereof |
| PCT/CN2017/075925 WO2017152836A1 (en) | 2016-03-08 | 2017-03-08 | Cell for lithium paste battery, and lithium paste battery module |
| US16/082,838 US10868337B2 (en) | 2016-03-08 | 2017-03-08 | Cell-core for lithium slurry battery, and lithium slurry battery module |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201611202373.2A CN108242530B (en) | 2016-12-23 | 2016-12-23 | Lithium slurry battery and negative plate thereof |
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| CN111193074A (en) * | 2019-12-11 | 2020-05-22 | 国网经济技术研究院有限公司 | Detachable lithium slurry battery's compound unit and contain its lithium slurry battery |
| CN112216812A (en) * | 2019-07-10 | 2021-01-12 | 比亚迪股份有限公司 | Lithium ion battery repeating unit, lithium ion battery, using method of lithium ion battery, battery module and automobile |
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| CN109904539A (en) * | 2019-03-05 | 2019-06-18 | 广州徽一电子科技有限公司 | A kind of lithium battery anode slurry leakage-proof structure and its anti-leaking method |
| CN109904539B (en) * | 2019-03-05 | 2022-02-11 | 深圳市飞鹏新能源科技有限公司 | Lithium battery positive electrode slurry leakage-proof structure and leakage-proof method thereof |
| CN112216812A (en) * | 2019-07-10 | 2021-01-12 | 比亚迪股份有限公司 | Lithium ion battery repeating unit, lithium ion battery, using method of lithium ion battery, battery module and automobile |
| CN111193074A (en) * | 2019-12-11 | 2020-05-22 | 国网经济技术研究院有限公司 | Detachable lithium slurry battery's compound unit and contain its lithium slurry battery |
| CN111193074B (en) * | 2019-12-11 | 2021-06-29 | 国网经济技术研究院有限公司 | Detachable lithium slurry battery's compound unit and contain its lithium slurry battery |
| CN113871558A (en) * | 2020-06-30 | 2021-12-31 | 松山湖材料实验室 | Closed metal negative electrode, winding type battery and preparation method |
| CN114284463A (en) * | 2020-09-27 | 2022-04-05 | 北京好风光储能技术有限公司 | Composite lithium supplementing sheet, and battery cell and battery with same |
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