CN109037789A - A kind of lithium aluminium double ion rechargeable battery - Google Patents
A kind of lithium aluminium double ion rechargeable battery Download PDFInfo
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- CN109037789A CN109037789A CN201810839781.1A CN201810839781A CN109037789A CN 109037789 A CN109037789 A CN 109037789A CN 201810839781 A CN201810839781 A CN 201810839781A CN 109037789 A CN109037789 A CN 109037789A
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- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
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- H01M4/36—Selection of substances as active materials, active masses, active liquids
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- H01M4/40—Alloys based on alkali metals
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- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
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- H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
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- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
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Abstract
The present invention relates to a kind of lithium aluminium double ion rechargeable batteries, including anode pole piece, cathode pole piece, positioned at anode pole piece and cathode pole piece diaphragm and electrolyte, electrolyte solution is made of multivalence aluminium ion solute and non-aqueous solvent, anode pole piece is made of the active material that can reversibly deviate from and be embedded in polyvalent cation, cathode pole piece is made of the active material that can be embedded in and deviate from second of ion reversibly from above-mentioned solvent, and second of ion is alkali metal ion.Its septation has electronic isolation and ion permeability；Contain non-aqueous solvent in electrolyte and multivalence aluminium ion Al can be provided3+And the solute of electrochemical deposition will not be generated.Charge and discharge can be more effectively carried out, migration mechanism of the multivalent ion between positive/negative plate is changed, effectively improves the energy density of battery.
Description
Technical field
The present invention relates to a kind of high platform voltage, the rechargeable battery of high-energy density, especially a kind of lithium aluminium double ion
Rechargeable battery.
Background technique
In recent years, the application potential of the lithium ion secondary battery of high-energy density is increasing, but is constrained to lithium ion
The monovalent lithium ion that battery is relied on when working, there are severe bottlenecks for the promotion of the energy density of lithium ion secondary battery.There is mirror
In this, introducing multivalent ion theoretically can effectively promote energy density；But but difficulty has breakthrough always in practical applications.
Main cause is that the ionic radius of multivalent ion is big, and ion is caused to be difficult to be embedded in inside graphite or other carbon-based materials；While by
In the presence of solid electrolyte interface film (SEI), multivalent ion can not reach negative terminal surface by SEI restore in next step instead
It answers.
In face of these problems, needs to change migration mechanism of the multivalent ion between positive/negative plate, could effectively mention
The energy density of high battery.In addition to adding high active substance ion in cathode, such as alkali metal ion Li+；Non-aqueous electrolyte
In simultaneously also need addition polyvalent metal ion, such as yttrium (Y), lanthanum (La) or alkaline-earth metal；Containing in anode to be reversibly embedded in
Deviate from the transistion metal compound of polyvalent metal ion, it is anti-to balance reversible abjection insertion of the alkali metal ion in cathode with this
It answers.
Chinese patent notification number is that CN 103928659A discloses a kind of rechargeable copper-zinc electricity
Pond is made of anode, cathode, diaphragm, shell, and the positive solution including copper-containing compound contains one kind or more in solution
Kind lithium salts or sodium salt and collector；Cathode includes the solution of zinc compound, contains one or more lithium salts or sodium salt in solution
And collector；Diaphragm only allows sodium ion or lithium ion to pass through.The battery mainly completes electricity by copper-zinc battery system
The charging and discharging in pond, the cost that copper-zinc is put into the actual use process be not low.
Summary of the invention
The purpose of the present invention is to solve defects of the existing technology, provide a kind of chargeable electricity of lithium aluminium double ion
Pond.
To achieve the goals above, the technical solution adopted by the present invention is that:
A kind of lithium aluminium double ion rechargeable battery, including anode pole piece, cathode pole piece, positioned at anode pole piece and cathode pole piece
Diaphragm and the electrolyte in diaphragm, electrolyte solution are made of multivalence aluminium ion solute and non-aqueous solvent, positive pole
Piece is made of the active material that can reversibly deviate from and be embedded in polyvalent cation, and cathode pole piece is by can be reversibly from above-mentioned molten
The active material composition of second of ion is embedded in and deviate from agent, and second of ion is alkali metal ion.Its septation has electricity
Insulating sublayer and ion permeability；Contain non-aqueous solvent in electrolyte and multivalence aluminium ion Al can be provided3+And electricity will not be generated
The solute of chemical deposition, such as: aluminum fluoride [ AlF3, lithium perchlorate [ Al (ClO4)3, tetrafluoro boric acid aluminium [ Al (BF4)3, hexafluoro
Aluminum phosphate [ Al (PF6)3Etc..
The active material of anode pole piece is one of transition metal oxide, sulfide, fluoride, carbon fluoride or more
Kind.
A kind of above-mentioned lithium aluminium double ion rechargeable battery, the active material of anode pole piece be the oxide of vanadium, sulfide,
One of the oxide of molybdenum, sulfide are a variety of, and the active material of anode pole piece is specifically as follows V2O5Or MoS x 。
A kind of above-mentioned lithium aluminium double ion rechargeable battery, the cathode pole piece active material be can be embedded in alkali metal from
Alkali metal, alkali metal alloy, one of the carbonaceous material or a variety of of son, specifically: the active material of cathode pole piece is metal
One of lithium, metallic sodium, lithium alloy, sodium alloy are a variety of.
A kind of above-mentioned lithium aluminium double ion rechargeable battery, the polyvalent cation of anode pole piece are Al3+, second of ion be
Li+、Na+、K+、Rb+、Cs+One of or it is a variety of.
The specific technical solution of the present invention is as follows: containing V in a kind of lithium aluminium double ion rechargeable battery2O5Anode,
LixSi cathode, formula are 0.5M Al (ClO4)3, EC(ethylene carbonate): DMC(dimethyl carbonate)=2: 1 electrolyte and
Borosilicate fiberglass diaphragm.In the discharge process for the first time of battery, the Al in electrolyte3+It migrates to anode and reacts, together
When cathode in Li+ be discharged into electrolyte.Due to high concentration Al3+Closer to anode, and overall insertion current potential is higher, above-mentioned anti-
It should occur mainly in corresponding pole piece.
In the charging process of battery, backward reaction occurs: the Al in anode3+With the Li in electrolyte+It migrates to cathode
Carry out reduction reaction.But since passivating film that negative terminal surface is quickly formed can only allow Li+By and -3.0V(standard hydrogen electricity
Position) it is reduced, so while charging voltage rises, the passivating film and electrolyte component of negative terminal surface can prevent Al3+Also
Original, to guarantee relatively low cathode potential and higher operating voltage.
The winding-structure of current maturation can be used in battery；Can anode formula for reference it is as follows: the nano-scale of 35-60%
Vanadium oxide/sulfide or molybdenum oxide/sulfide, the conductive carbon black of 5-10% and the Kynoar of 15-25%
(PVDF) dibutyl phthalate (DBP) plasticizer of binder and 20-30% are dissolved in the acetone solvent of 25-35%.
Slurry can coat on a current collector, and film is formed after being dried at room temperature for, and then cut into suitable width, and with
Diaphragm and to electrode carry out lamination assembling, the battery core after assembling needed before fluid injection first with polymer atent solvent (such as
Ether etc.) plasticizer before is extracted.
It is had excellent performance the invention has the benefit that disclosing one kind in the present invention, the secondary electricity of economic and practical double ion
Pond；Polyvalent metal ion does not include the alkaline-earth metal ions referred in background technique completely in its used electrolyte, can
Charge and discharge are more effectively carried out, migration mechanism of the multivalent ion between positive/negative plate is changed, effectively improves the energy of battery
Metric density.In addition to adding high active substance ion in cathode, such as alkali metal ion Li+；Containing in anode can be reversibly embedding
Enter to deviate from the transistion metal compound of polyvalent metal ion, be embedded in this to balance reversible abjection of the alkali metal ion in cathode
Reaction.
Detailed description of the invention
Fig. 1 is the Structure of cross section schematic diagram of laminated batteries in embodiment of the present invention；
Fig. 2 is that discharge voltage is to the indicatrix comparison diagram of gram volume for the first time, and which includes existing lithium ion battery (Li+)
With Dual-ion cell (yttrium Y3+With aluminium Al3+)；
Fig. 3 is curve graph of the cyclical voltage to relative capacity of existing lithium ion battery；
Fig. 4 is the Dual-ion cell (Y of embodiment of the present invention3+) cyclical voltage to the curve graph of relative capacity；
Fig. 5 is the Dual-ion cell (Al of embodiment of the present invention3+) cyclical voltage to the curve graph of relative capacity；
Fig. 6 is existing lithium ion battery and aluminium Al in comparison embodiment3+Dual-ion cell discharges and gram volume for the first time
Extraordinary curve comparison figure；
Fig. 7 is the cyclical voltage indicatrix in the embodiment in Fig. 6.
Specific embodiment
The present invention is further illustrated with specific example with reference to the accompanying drawing.
In Fig. 1, a kind of battery of lamination (lithium aluminium double ion rechargeable battery) 10 include anode 13, cathode 17,
Contain electrolyte in the diaphragm 15 to fall between.Plus plate current-collecting body 11, negative current collector 19 and positive pole ear 12 are born
Pole tab 16 is used to provide complete electrical circuit connection for battery.It is tested in order to facilitate the half-cell in laboratory, it can be in diaphragm
The silver wire 14 of a built-in class reference cell in 15.
Usually, anode 13 includes one layer of inclined divinyl copolymer matrix plasma membrane, is inserted into or inhales wherein being scattered with
Receive transition metal oxide/sulfide of polyvalent cation, such as V2O5Or MoS x (nano particle is best)；Corresponding cathode 17 wraps
Containing one layer of similar copolymer matrix plasma membrane or metal foil, it can reversibly be inserted into or be reacted with monovalent alkali metal ions.Diaphragm 15
It can be as it was noted above, being one layer of high molecule micropore film or glass fibre that can absorb non-aqueous electrolyte.Electrolyte
A small amount of alkali metal salt that can promote negative reaction rate can additionally be added.Reference cell 14 can be used to easily measurement pair
The electro-chemical activity of pole piece component is answered, to effectively determine the combination of electrode and electrolyte.
Actual cell assembling processes are as follows: anode, the diaphragm for having infiltrated electrolyte and cathode and corresponding collector
Tabletting assembling is carried out in sequence.After being completed, battery is placed in the test cabinet that can automatically control circulation and data record
In, constant current cycle is carried out according to the electric current of 7mA/g, to obtain character voltage-capacity curve of battery.
The present invention further will be illustrated by specific example below.
Embodiment 1
The characteristics such as operating voltage and the capacity for making a single ion lithium embedded sample battery to show existing lithium ion battery
Parameter.Anode constituents include: 28%(diameter 20-60nm) V2O5, 6% conductive carbon black, 15%PVDF binder, 23%DBP plasticizer with
And 28% acetone.One layer of stabilizing films are formd after anode constituents are 0.5 hour dry at 22 DEG C, face is then cut from film
Long-pending 1cm2Round anode pole piece, then the plasticizer in anode pole piece is extracted with ether.One typical positive pole
V containing 5-20mg in piece2O5Active material.
The production process of cathode pole piece is similar with anode pole piece, only with silicon powder instead of V2O5Powder, by dry purification
Silicon powder film afterwards, which is covered in metallic lithium foil, just forms Li-Si alloy LixSi cathode pole piece, finally cuts cathode pole piece
At the disk of size corresponding with anode pole piece, wherein LixThe specific surface area of Si is 0.5m2/ g or more.
Positive/negative plate was infiltrated to the borosilicate fiberglass film of electrolyte in -80 DEG C of dew point of glove box and in advance
It is assembled, electrolyte prescription therein is 1M LiPF6, EC(ethylene carbonate): DMC(dimethyl carbonate)=2: 1.Later will
Assembled battery carries out charge-discharge test: the Li in electrolyte+It is embedded in positive active material, charging process during discharge
In be then reduced in cathode.Such as the Li in Fig. 2+For the first time shown in discharge characteristic curve, the discharge capacity for the first time of battery is
150mAh/g。
Embodiment 2
Using production process in the same manner as in Example 1, makes another money Dual-ion cell and organize test as a comparison: positive and negative anodes
Active material is respectively V2O5And MoS x , the formula of electrolyte is 0.5M Y (ClO4)3, EC(ethylene carbonate): DMC(carbonic acid two
Methyl esters)=2: 1.Assembled battery according to identical condition test in example 1 and is recorded into data: such as the Y in Fig. 23+It discharges for the first time
Shown in indicatrix, the discharge capacity for the first time of battery is promoted to 200mAh/g.
Embodiment 3
Using the production process and active material similar with embodiment 2, make in specific embodiments of the present invention it is double from
Sub- battery: at least a kind of ion is Al in double ion3+.Specifically, although the active material of positive and negative anodes is identical with example 1,
But the active cation in electrolyte is different: the formula for solving liquid is 0.5M Al (ClO4)3, EC(ethylene carbonate): DMC(carbon
Dimethyl phthalate)=2: 1.Such as the Al in Fig. 23+For the first time shown in discharge characteristic curve, the discharge capacity for the first time of battery is promoted significantly, is reached
300mAh/g is arrived.
Embodiment 4
Another group of contrast test battery is made using production process identical with above-mentioned example, by corresponding electrolyte component and work
Property substance is changed to trifluoromethyl sulfonic acid (CF3SO3-) and the partial size more greatly V of (60-90nm)2O5.By assembled battery according to
With condition test identical in above-mentioned example and record data: such as the single ion Li in Fig. 3-5+With double ion Y3+、Al3+It puts for the first time
Shown in electrical feature curve, not only the discharge capacity for the first time of battery is promoted, and operating voltage range is also improved.
Embodiment 5
Another specific embodiment of the invention uses production process identical with above-mentioned example, by corresponding positive electrode active material
Matter is changed to by thermally decomposing four thio ammonium molybdate [ (NH4)2MoS4Obtained MoSx；1.0M has been used in electrolyte respectively
Li(CF3SO3) and 0.5M Al (CF3SO3)3, while charge and discharge cycles test is carried out using the electric current of 7mA/h.Fig. 6 is to put for the first time
The indicatrix of capacitance, it can be seen that double ion (Al3+) discharge capacity of battery is apparently higher than existing single ion (Li+) electricity
Pond.Fig. 7 is cycle specificity curve, it can be seen that double ion (Al after cycling3+) discharge capacity of battery is still able to maintain
In 525mAh/g or so.
It discloses one kind in the present invention to have excellent performance, economic and practical double ion secondary cell；Its used electrolyte
Middle polyvalent metal ion does not include the alkaline-earth metal ions referred in background technique completely, can be more effectively carried out charge and discharge,
Migration mechanism of the multivalent ion between positive/negative plate is changed, the energy density of battery is effectively improved.In addition in cathode
High active substance ion is added, such as alkali metal ion Li+；Abjection polyvalent metal ion can be reversibly embedded in by containing in anode
Transistion metal compound balances reversible abjection insertion reaction of the alkali metal ion in cathode with this.
The basic principles, main features and advantages of the present invention have been shown and described above.The technology of the industry
Personnel are it should be appreciated that the present invention is not limited to the above embodiments, and what is described in the above embodiment and the description is only the present invention
Principle, various changes and improvements may be made to the invention without departing from the spirit and scope of the present invention, these variation and
Improvement is both fallen in the range of claimed invention.The present invention claims protection scope by appended claims and its
Equivalent defines.
Claims (9)
1. a kind of lithium aluminium double ion rechargeable battery, including anode pole piece, cathode pole piece, be located at anode pole piece and cathode pole piece it
Diaphragm and the electrolyte in diaphragm, be characterized in that:
Electrolyte solution is made of multivalence aluminium ion solute and non-aqueous solvent, and anode pole piece is by can reversibly deviate from and be embedded in
The active material of polyvalent cation forms, and cathode pole piece reversibly from above-mentioned solvent by that can be embedded in and deviate from second of ion
Active material composition.
2. a kind of lithium aluminium double ion rechargeable battery according to claim 1, which is characterized in that second of ion be
Alkali metal ion.
3. a kind of lithium aluminium double ion rechargeable battery according to claim 2, which is characterized in that the work of the anode pole piece
Property substance be one of transition metal oxide, sulfide, fluoride, carbon fluoride or a variety of.
4. a kind of lithium aluminium double ion rechargeable battery according to claim 3, which is characterized in that the active matter of anode pole piece
Matter is one of the oxide of vanadium, sulfide, the oxide of molybdenum, sulfide or a variety of.
5. a kind of lithium aluminium double ion rechargeable battery according to claim 4, which is characterized in that the active matter of anode pole piece
Matter is V2O5Or MoS x 。
6. a kind of lithium aluminium double ion rechargeable battery according to claim 2, which is characterized in that the cathode pole piece activity
Substance is that can be embedded in one of alkali metal, alkali metal alloy, carbonaceous material of alkali metal ion or a variety of.
7. a kind of lithium aluminium double ion rechargeable battery according to claim 6, which is characterized in that the work of the cathode pole piece
Property substance be one of lithium metal, metallic sodium, lithium alloy, sodium alloy or a variety of.
8. a kind of lithium aluminium double ion rechargeable battery according to claim 2, which is characterized in that the multivalence sun of anode pole piece
Ion is Al3+, second of ion is Li+、Na+、K+、Rb+、Cs+One of or it is a variety of.
9. a kind of lithium aluminium double ion rechargeable battery according to claim 1, which is characterized in that the multivalence aluminium ion is molten
Matter is aluminum fluoride [ AlF3, lithium perchlorate [ Al (ClO4)3, tetrafluoro boric acid aluminium [ Al (BF4)3, hexafluorophosphoric acid aluminium [ Al (PF6)3?
One of or it is a variety of.
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN110817962A (en) * | 2019-11-18 | 2020-02-21 | 福建师范大学 | A kind of preparation method of high rate performance sulfur-like cathode material molybdenum polysulfide nanosheets |
| CN111313086A (en) * | 2019-12-24 | 2020-06-19 | 安徽圣格能源科技有限公司 | Electrolyte and lithium ion battery |
| CN114784272A (en) * | 2022-06-07 | 2022-07-22 | 江西安驰新能源科技有限公司 | Environment-friendly lithium iron phosphate battery and preparation method thereof |
| CN115939375A (en) * | 2022-01-11 | 2023-04-07 | 中国科学院宁波材料技术与工程研究所 | High-capacity molybdenum polysulfide positive electrode material, preparation method and application thereof in all-solid-state battery |
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| CN110817962A (en) * | 2019-11-18 | 2020-02-21 | 福建师范大学 | A kind of preparation method of high rate performance sulfur-like cathode material molybdenum polysulfide nanosheets |
| CN111313086A (en) * | 2019-12-24 | 2020-06-19 | 安徽圣格能源科技有限公司 | Electrolyte and lithium ion battery |
| CN115939375A (en) * | 2022-01-11 | 2023-04-07 | 中国科学院宁波材料技术与工程研究所 | High-capacity molybdenum polysulfide positive electrode material, preparation method and application thereof in all-solid-state battery |
| CN114784272A (en) * | 2022-06-07 | 2022-07-22 | 江西安驰新能源科技有限公司 | Environment-friendly lithium iron phosphate battery and preparation method thereof |
| CN114784272B (en) * | 2022-06-07 | 2024-04-12 | 江西安驰新能源科技有限公司 | Environment-friendly lithium iron phosphate battery and preparation method thereof |
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