CN106784623A - A kind of multitube lithium-sulfur cell - Google Patents
A kind of multitube lithium-sulfur cell Download PDFInfo
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- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0561—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of inorganic materials only
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- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
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Abstract
The present invention provides a kind of multitube lithium-sulfur cell, including positive pole, positive pole shell, negative pole and anode coat, the negative pole is extended in positive pole by multiple Compound Negative pole pipes of array arrangement, the Compound Negative pole pipe includes the porous metallic layers of internal layer and is attached to the solid electrolyte layer supported by porous metallic layers of outer layer, the porous metallic layers are connected with anode coat, negative collector electrode is collectively formed, the positive pole shell is contacted with the carbon material in positive pole, collectively forms positive collector electrode.Be applied to Compound Negative pole pipe in lithium-sulfur cell to solve the potential safety hazard that polysulfide " shuttle effect " and Li dendrite are caused by the present invention;The easily rupturable phenomenon of conventional batteries earthenware is solved by the design of porous metallic layers, so as to lift battery safety;Battery structure is further improved simultaneously, multiple Compound Negative pole pipe array arrangements and both positive and negative polarity active material space quarantine measures are taken, the purpose for improving cell power density and battery security is reached.
Description
Technical field
The present invention relates to technical field of lithium batteries, and in particular to a kind of multitube lithium-sulfur cell.
Background technology
Lithium ion battery is a kind of new type of energy storage device developed in recent years, in past more than 20 years, lithium-ion electric
Pond leads portable electric appts to move towards new change with the characteristic of its high-energy-density.But, with various Novel portables
Formula electronic equipment and new-energy automobile are developed rapidly, and people it is also proposed higher energy density, preferably peace to energy-storage battery
The full requirement such as performance and lower cost.All kinds of battery systems are contrasted, specific energy, security and cost performance tripartite is considered
Face key element, with lithium metal as negative pole, a kind of new chemical battery of the elemental sulfur as positive pole(Lithium-sulfur cell)It is current battery industry
Main development direction.
In lithium-sulfur cell, the theoretical specific capacity of active material sulphur is 1675mAh/Kg, and theoretical specific energy reaches 2600Wh/
Kg, is 5-8 times of conventional lithium ion battery, 3.4 times of sodium-sulphur battery, and with low cost, environment-friendly.Nearly ten years, people
Carry out largely the aspects such as electrode structure stability, the utilization rate of raising security and sulphur, extension battery cycle life are maintained
Research work.However, lithium-sulfur cell cannot also be applied on a large scale still in the laboratory development stage at present, mainly deposit
In following technical bottleneck problem:(One)Potential safety hazard aspect:Principal element is to use organic polymer barrier film, is filled in battery
Negative metal lithium superficial growth Li dendrite when electric, easily pierces through organic membrane for polymer and causes both positive and negative polarity short circuit;Another factor
It is to use liquid state organic electrolyte, burning, blast is easily triggered in both positive and negative polarity short circuit or high temperature;(Two)Cycle life aspect:Shadow
The principal element for ringing cycle performance is capacitance loss that lithium polysulfide " shuttle effect " is caused, battery when being operated, its
Intermediate product lithium polysulfide is dissolved in organic electrolyte, and through the hole of organic porous polymer film, in battery just
There are shuttles between negative pole(Referred to as shuttle effect), make the irreversible loss of active material elemental sulfur, reduce battery
Coulombic efficiency.In addition, the lithium polysulfide shuttled to negative pole can chemically react with lithium anode, inside battery is triggered to put
Electrical phenomena, and the lithium sulfide insoluble in electrolyte of reaction generation can be deposited on cathode of lithium surface, so as to trigger lithium metal table
Face deteriorates, and reduce further battery cycle life.In this several defects, shuttle effect is that lithium-sulfur cell performance is destroyed most
A bit big, is very scabrous using existing organic polymer membrane technique.
The content of the invention
Based on the weak point that existing lithium-sulfur cell technology is present, the present invention provides a kind of multitube lithium-sulfur cell, to solve
Certainly " shuttle effect " forms the potential safety hazard brought to the destruction of lithium-sulfur cell performance and Li dendrite.
In order to solve the above technical problems, the present invention is adopted the following technical scheme that:
A kind of multitube lithium-sulfur cell, including positive pole, positive pole shell, negative pole and anode coat, it is described just extremely to contain active sulfur
S/C composite reactive things, the negative electrode active material of the negative pole including lithium metal, the negative pole by array arrangement several
Compound Negative pole pipe is extended in positive pole, the porous metallic layers of the Compound Negative pole pipe including internal layer and be attached to outer layer by porous
The solid electrolyte layer of metal level support, the porous metallic layers are connected in spout part with anode coat, collectively form negative pole current collection
Pole, the positive pole shell is contacted with the carbon material in positive pole, collectively forms positive collector electrode.
Dead ring is provided between the positive pole and negative pole, the dead ring is closely connected with solid electrolyte layer.
Ionic liquid is adsorbed with the porous metallic layers.
The thickness of the porous metallic layers is 0.2~1.5mm.
Porous metals average pore size is 0.1~5um in the porous metallic layers, and porosity is 50~80%.
The thickness of the solid electrolyte layer is 0.015~0.060mm.
1~the 4mm of lumen diameter of the Compound Negative pole pipe.
10~the 300mm of length of the Compound Negative pole pipe.
From above technical scheme, be applied to Compound Negative pole pipe in lithium-sulfur cell by the present invention, and in Compound Negative pole pipe
Porous metals in adion liquid, improve the interface compatibility of motlten metal lithium and solid electrolyte film, make lithium-sulfur cell
Can be in the boiling point of sulphur(444℃)250 ~ 350 DEG C of temperature range work below.The dense solid electrolyte matter layer of composite negative pole outer tube layer
The potential safety hazard that polysulfide " shuttle effect " and Li dendrite are caused can be solved;Biography is solved by the design of porous metallic layers
The easily rupturable phenomenon of system cell ceramic tube, so as to lift battery performance and safe class;Further improve battery knot simultaneously
Structure, takes with multiple Compound Negative pole pipe array arrangements and both positive and negative polarity active material space quarantine measures, reaches the raising power of battery
The purpose of density and battery security, and the technical scheme of the full technical strategies of lithium-sulfur cell and practicality is constituted with this.
Brief description of the drawings
Fig. 1 is the longitudinal sectional view of multitube lithium-sulfur cell of the present invention, and shows that the part of dead ring region is put
Big figure;
Fig. 2 is the structural representation of Compound Negative pole pipe in the present invention;
Fig. 3 blocks formation mechenism schematic diagram for automatic when breakdown point occurs in solid electrolyte layer of the present invention.
In figure:1st, positive pole, 2, positive pole shell, 3, negative pole, 4, anode coat, 5, Compound Negative pole pipe, 51, porous metallic layers,
52nd, solid electrolyte layer, 6, dead ring.
Specific embodiment
A kind of preferred embodiment of the invention is described in detail below in conjunction with the accompanying drawings.
As shown in figure 1, the lithium-sulfur cell includes positive pole 1, positive pole shell 2, negative pole 3, anode coat 4, and with electricity
The Compound Negative pole pipe 5 of solution matter and barrier film function.
The positive pole 1 is the S/C active materials containing active sulfur, and the negative pole 3 includes the negative electrode active of lithium metal
Material.
The negative pole is extended in positive pole by Compound Negative pole pipe, increases contact area, improves charge and discharge efficiency.It is described
The internal diameter r of Compound Negative pole pipe is 1~4mm, and external diameter R is 1.43~7.12mm, and composite negative pole length is 10~300mm.Compound Negative
The less intracavity diameter of pole pipe, it is to avoid the possibility that negative pole motlten metal lithium is largely contacted with positive electrode active material sulphur, significantly carries
The security of battery high.
250 ~ 350 DEG C of multitube lithium-sulfur cell operating temperature range of the present invention.
As shown in Fig. 2 the Compound Negative pole pipe 5 includes being adsorbed with the porous metallic layers 51 and solid electrolyte of ionic liquid
Layer 52, wherein solid electrolyte layer is attached to porous metallic layers outer layer, and the porous metallic layers are played a supporting role.By porous gold
The solid electrolyte layer of the supporting body surface composite conducting that category layer is constituted, it is high with mechanical strength, it is not easily broken, is broken, antidetonation
The characteristics of property is strong.Porous metallic layers 51 are connected with anode coat 4, collectively form negative collector electrode, wherein exposed on the outside of the mouth of pipe
Porous metallic layers are welded with anode coat, increased electronic conductivity, and positive pole shell 2 is contacted with positive pole carbon material, collectively formed
Positive collector electrode.Dead ring 6 is additionally provided between positive pole and negative pole, the dead ring is closely connected with solid electrolyte layer, plays
Both positive and negative polarity isolation, insulating effect, preferably Ai2O3 (aluminum oxide) ceramic ring, its intensity is larger and high temperature resistant.
The thickness of porous metallic layers 51 is 0.2~1.5mm, with stainless steel, titanium, nickel, bronze, nickel alloy, titanium alloy
A kind of metal dust is mixed and made into shape embryo with adhesive, pore creating material, sintering aid, and shape embryo is formed after firing through chemical washing, porous
In 0.1~5um, porosity is 50~80% to porous metals average pore size in metal level.The thickness of the solid electrolyte layer 52 is
0.015~0.060mm, relatively thin conducting solid electrolyte ceramic membrane improves the conductance of ion, consolidates so that ionic conductivity is high
Body electrolyte glass ceramics are material, are formed using sol-gel processing or using dip-coating film sintering.The present embodiment
Middle solid electrolyte layer uses inorganic material, such as ceramics, glass.The solid electrolyte non-refractory of organic material, is not suitable for
This programme.
Take many Compound Negative pole pipes to collectively form the Integration Design of negative pole in the present invention, cell work(can be improved
Rate density and efficiency for charge-discharge.
As shown in Fig. 2 solid electrolyte layer 52 is arranged on the outer layer of porous metallic layers 51 by the present invention, a pipe is collectively formed
Formula structure, is internally formed a tube chamber 53 for filling negative electrode active material molten state lithium, the solid electricity under the support of porous metallic layers
Solution matter layer can be made relatively thin compact film, and be easy to the negative pole lithium that encapsulation is melted, and external surface area is big, and electrical efficiency is high.
Next to that considering the perishable solid electrolyte of negative pole lithium, the perishable metal of positive pole sulphur, the design arrangement of such ectonexine can keep away
Exempt from mutual directly contact.
A kind of ionic liquid is also adsorbed with the hole of porous metallic layers 51, the ionic liquid high temperature resistant(450 DEG C of >), energy
Quick conducting lithium ions, and be in a liquid state in battery operating temperature scope, stable chemical nature.180 DEG C of the fusing point of lithium, lithium is to electrolysis
The moistening temperature of matter ceramics tube wall is 550 DEG C, and the boiling point of positive pole sulphur is 444 DEG C, it is clear that simple by cathode of lithium and sulphur positive pole
The lithium-sulfur cell cisco unity malfunction of composition.Composite negative pole tubular construction of the invention effectively solves the technical barrier, porous
Metal as inorganic solid electrolyte supporter, while significantly increasing body mechanical strength, a kind of adsorbable ion of filling
Liquid, ionic liquid has the function of surface-active, has good compatibility with inorganic solid electrolyte surface, while can be notable
The surface tension of molten lithium metal is reduced, molten lithium metal and inorganic solid electrolyte interface compatibility is effectively improved, so that
Interface resistance is reduced, battery is worked at a lower temperature.In the present embodiment, lithium-sulfur cell operating temperature 250 ~ 350
℃。
In the present embodiment, ionic liquid is preferably LiAlCl4.
As shown in figure 3, the tube wall film layer that solid electrolyte layer 52 and porous metallic layers 51 are constituted is only by Li+, other
What material does not pass through including electronics, if because the factors such as battery strenuous vibration, collision make solid electrolyte layer burst apart, tube wall has
Certain self-healing function.The principle of self-healing function is as follows:
Motlten metal lithium has larger surface tension, and molten sulfur has larger viscosity and vapour pressure higher, when solid electricity
When solution matter layer bursts apart, the lithium of melting, sulphur slowly enter porous metals under the retardance of porous metallic layers from porous metallic layers both sides
Layer hole, and lithium sulfide solid particle is quickly generated in hole, until lithium sulfide solid particle is fully filled with porous metallic layers
Hole and formed obstruction untill, locally obstruction under the negative pole still can normal work.Self-healing repair function, solves from source
Determine safety problem, had battery safety and substantially lifted.
The above implementation method is only that the preferred embodiment of the present invention is described, not to model of the invention
Enclose and be defined, on the premise of design spirit of the present invention is not departed from, those of ordinary skill in the art are to technical side of the invention
Various modifications and improvement that case is made, all should fall into the protection domain of claims of the present invention determination.
Claims (8)
1. a kind of multitube lithium-sulfur cell, including positive pole (1), positive pole shell (2), negative pole (3) and anode coat (4), it is described just
S/C composite reactive things extremely containing active sulfur, the negative pole includes the negative electrode active material of lithium metal, it is characterised in that institute
State during negative pole (3) extends to positive pole (1) by several Compound Negative pole pipes (5) of array arrangement, Compound Negative pole pipe (5) bag
The porous metallic layers (51) for including internal layer and the solid electrolyte layer (52) supported by porous metallic layers for being attached to outer layer, this is porous
Metal level is connected with anode coat (4), collectively forms negative collector electrode, and the positive pole shell (2) connects with the carbon material in positive pole
Touch, collectively form positive collector electrode.
2. multitube lithium-sulfur cell according to claim 1, it is characterised in that set between the positive pole (1) and negative pole (3)
Dead ring (6) is equipped with, the dead ring is connected with solid electrolyte layer.
3. multitube lithium-sulfur cell according to claim 1, it is characterised in that be adsorbed with the porous metallic layers (51)
Ionic liquid.
4. multitube lithium-sulfur cell according to claim 1, it is characterised in that the thickness of the porous metallic layers (51) is
0.2~1.5mm.
5. multitube lithium-sulfur cell according to claim 1, it is characterised in that porous gold in the porous metallic layers (51)
Category average pore size is 0.1~5um, and porosity is 50~80%.
6. multitube lithium-sulfur cell according to claim 1, it is characterised in that the thickness of the solid electrolyte layer (52)
It is 0.015~0.060mm.
7. multitube lithium-sulfur cell according to claim 1, it is characterised in that the lumen diameter 1 of the Compound Negative pole pipe
~4mm.
8. multitube lithium-sulfur cell according to claim 1, it is characterised in that the pipe range 10 of the Compound Negative pole pipe~
300mm。
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Cited By (4)
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---|---|---|---|---|
WO2019072028A1 (en) * | 2016-10-12 | 2019-04-18 | Prologium Technology Co., Ltd. | Current collector |
CN109980291A (en) * | 2019-04-01 | 2019-07-05 | 浙江工业大学 | A kind of battery core and its preparation method and application of cylindrical type lithium-sulfur cell |
WO2019170074A1 (en) * | 2018-03-08 | 2019-09-12 | Yi Cui | Solid electrolyte-based molten lithium electrochemical cells |
JP2021526286A (en) * | 2018-05-17 | 2021-09-30 | ビサーズ バッテリー コーポレーション | Molten fluid system with non-brittle solid electrolyte |
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Cited By (6)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
WO2019072028A1 (en) * | 2016-10-12 | 2019-04-18 | Prologium Technology Co., Ltd. | Current collector |
WO2019170074A1 (en) * | 2018-03-08 | 2019-09-12 | Yi Cui | Solid electrolyte-based molten lithium electrochemical cells |
CN112514136A (en) * | 2018-03-08 | 2021-03-16 | 崔屹 | Solid electrolyte based molten lithium electrochemical cell |
JP2021526286A (en) * | 2018-05-17 | 2021-09-30 | ビサーズ バッテリー コーポレーション | Molten fluid system with non-brittle solid electrolyte |
CN109980291A (en) * | 2019-04-01 | 2019-07-05 | 浙江工业大学 | A kind of battery core and its preparation method and application of cylindrical type lithium-sulfur cell |
CN109980291B (en) * | 2019-04-01 | 2021-07-13 | 浙江工业大学 | Battery cell of cylindrical lithium-sulfur battery and preparation method and application thereof |
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CN106784623B (en) | 2023-07-28 |
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