CN110265722A - A kind of Dual-ion cell electrolyte and application - Google Patents
A kind of Dual-ion cell electrolyte and application Download PDFInfo
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- CN110265722A CN110265722A CN201910514714.7A CN201910514714A CN110265722A CN 110265722 A CN110265722 A CN 110265722A CN 201910514714 A CN201910514714 A CN 201910514714A CN 110265722 A CN110265722 A CN 110265722A
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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
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
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- H01M10/0569—Liquid materials characterised by the solvents
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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
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0025—Organic electrolyte
- H01M2300/0028—Organic electrolyte characterised by the solvent
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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
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0025—Organic electrolyte
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Abstract
The present invention provides a kind of Dual-ion cell electrolyte and application, is related to electrochemical technology field.The electrolyte includes electrolyte and organic solvent；The organic solvent is the mixture of dimethyl carbonate and diethyl carbonate；Or the mixture of dimethyl carbonate, diethyl carbonate and methyl ethyl carbonate；Or the mixture of dimethyl carbonate, diethyl carbonate and sulfolane；Or the mixture of dimethyl carbonate, diethyl carbonate and fluorinated ethylene carbonate.The present invention also provides application of the above-mentioned Dual-ion cell electrolyte in lithium/graphite half-cell or double graphite full batteries.The experimental results showed that for commercial graphite anode, output can be stablized up to~100mAh g using Dual-ion cell electrolyte of the invention‑1Specific capacity；For commercial graphite cathode, output can be stablized up to~345mAh g‑1Specific capacity, applied to can stablize in double graphite full batteries output 95mAh g‑1Positive electrode specific capacity.
Description
Technical field
The present invention relates to electrochemical technology fields, and in particular to a kind of Dual-ion cell electrolyte and application.
Background technique
Chemical cell chief component has anode, cathode and electrolyte.As a kind of new type of energy storage device, double ion electricity
Pond is positive with graphite, negative electrode material, has both the advantage of high-performance (higher operating voltage and energy density) and low cost.Its work
Make principle substantially anions and canons to move between anode/electrolyte, cathode/electrolyte respectively, respectively in anode and cathode storage
It deposits/discharges.Have the following using graphite as positive and negative electrode material main advantage: (1) it is high to insert embedding operating voltage for positive anion
Embedding lithium theoretical capacity height (the 374mAh g of (to lithium 5V or more) (2) cathode-1), and the structure that works long hours still is stablized, and it will not
It is abundant to generate Li dendrite (3) material storage, it is cheap.Currently, the electrolyte of Dual-ion cell mainly has ionic liquid, solid-state
Electrolyte and three kinds of organic solvent electrolyte.Wherein, the high viscosity of ionic liquid makes multiplying power, cryogenic property are poor, complicated
The purifying technique for preparing keep its with high costs, at present can not large-scale application；And the low conductivity of solid electrolyte and undesirable
Electrode/electrolyte interface compatibility can not also overcome at present.Therefore, the electrolyte of organic solvent system is still current commercial electrolyte
The main body of liquid.
There is also a major issues for organic solvent electrolyte: the solvation behavior of anion.Different anion-solvents
Combine graphite anode insert embedding difficulty and stability difference is very big, have tremendous influence to the performance of battery entirety.Quotient at present
It is 1mol/L lithium hexafluoro phosphate (LiPF with battery electrolyte6) to be dissolved in the mixing of ethylene carbonate (EC)/methyl ethyl carbonate (EMC) molten
In agent (V (EC)/V (EMC)=3/7), wherein EC can form solid electrolyte membrane (SEI) in graphite cathode to guarantee Li+'s
Interface transmission and negative pole structure are stablized, and EMC energy and PF6 -Solvation inserts/deintercalation behavior to improve it in graphite anode.In addition,
Fan Hui's et al. studies have shown that PF can be improved by adding a small amount of EMC6 -Solvation knot in poor solvent (such as sulfolane)
Structure effectively facilitates anion and inserts embedding in graphite anode, and operating voltage is up to 5.4V.However, the price of EMC is almost several times as much as it
His organic solvent, this makes the electrolyte of EMC base hold at high price.Although the concentration for improving electrolytic salt can be effectively improved
Electrolyte property, but the production cost of electrolyte also increases considerably.Therefore, a kind of low-cost high-efficiency Dual-ion cell electrolyte
Huge practical value it is self-evident.
Summary of the invention
The object of the present invention is to provide a kind of Dual-ion cell electrolyte, which may be used on lithium/graphite half-cell
And in the full battery of double graphite.With above-mentioned Dual-ion cell electrolyte replace methyl ethyl carbonate ester group electrolyte be applied to it is double from
The use to methyl ethyl carbonate ester solvent can be greatly reduced in sub- battery under the premise of guaranteeing battery performance.
To achieve the goals above, technical solution of the present invention is specific as follows:
Present invention firstly provides a kind of Dual-ion cell electrolyte, which includes electrolyte and organic solvent；
The organic solvent is the mixture of dimethyl carbonate (DMC) and diethyl carbonate (DEC)；Or dimethyl carbonate,
The mixture of diethyl carbonate and methyl ethyl carbonate (EMC)；Or the mixing of dimethyl carbonate, diethyl carbonate and sulfolane (SL)
Object；Or the mixture of dimethyl carbonate, diethyl carbonate and fluorinated ethylene carbonate (FEC).
Preferably, in the mixture of the dimethyl carbonate (DMC) and diethyl carbonate (DEC), DMC, which is accounted for, described to be had
The percent by volume of solvent is 10%~40%, to account for the percent by volume of the organic solvent be 60%~90% to DEC.
Preferably, in the mixture of the dimethyl carbonate, diethyl carbonate and methyl ethyl carbonate (EMC), EMC is accounted for
The volume ratio that the percent by volume of the organic solvent is 0.1%~99.9%, DMC and DEC is 2:8.
Preferably, in the mixture of the dimethyl carbonate, diethyl carbonate and sulfolane (SL), SL, which is accounted for, described to be had
The volume ratio that the percent by volume of solvent is 0.1%~99.9%, DMC and DEC is 2:8.
Preferably, in the mixture of the dimethyl carbonate, diethyl carbonate and fluorinated ethylene carbonate (FEC),
It is 2:8 that FEC, which accounts for the volume ratio that the percent by volume of the organic solvent is 0.1%~99.9%, DMC and DEC,.
Preferably, the electrolyte is lithium salts.
Preferably, molar concentration of the lithium salts in the organic solvent is 1mol/L~3mol/L.
Preferably, the lithium salts is lithium hexafluoro phosphate.
The present invention also provides above-mentioned Dual-ion cell electrolyte to apply the application in lithium/graphite half-cell.
The present invention also provides above-mentioned Dual-ion cell electrolyte to apply the application in double graphite full batteries.
The beneficial effects of the invention are as follows
The present invention provides a kind of Dual-ion cell electrolyte, and the Dual-ion cell electrolyte includes electrolyte and organic
Solvent；The organic solvent is the mixture of DMC and DEC.Compared with prior art, Dual-ion cell electrolysis provided by the invention
The Solvation State of hexafluorophosphoricacid acid ions in the solution in wherein solution occurs by physical mixed DMC and DEC in liquid
Change, hexafluorophosphoricacid acid ions electrolyte/graphite can also be made efficiently reversibly to transmit without methyl ethyl carbonate (EMC),
Final the height ratio capacity (~100mAh g for realizing graphite anode-1) and stable circulation；Make the half-cell of cathode, this hair for graphite
The electrolyte of bright offer can be realized efficient reversible storage graphite cathode of the lithium ion in non-EC electrolyte, effectively avoid EC base
The use of electrolyte is limited to, and provides high output capacity (~345mAh g-1) and stable circulation；Electrolyte energy provided by the invention
The ingredient of enough effectively substitution EMC base electrolyte, mixes equal energy with EMC base electrolyte arbitrary proportion for electrolyte provided by the invention
Enough in the just extremely stable output~100mAh g of graphite-1Specific capacity；Electrolyte provided by the invention can effectively replace sulfolane
(SL) in base electrolyte EMC ingredient function, with electrolyte provided by the invention substitution SL base electrolyte in 100%EMC at
Point, output~110mAh g can be stablized under the high voltage of 5.4V using the battery of the electrolyte-1Specific capacity, reach with text
Offer the consistent battery performance of report；Electrolyte provided by the invention can effectively replace fluorinated ethylene carbonate (FEC) base to be electrolysed
The function of EMC ingredient in liquid uses this with the 100%EMC ingredient in electrolyte provided by the invention substitution FEC base electrolyte
The battery of electrolyte can stablize output~100mAh g-1Specific capacity, reach consistent with the battery performance of reported in literature；DMC
Cheap with DEC, electrolyte provided by the invention substitutes EMC using the two mixture as electrolyte solvent and can be greatly reduced
The production cost of Dual-ion cell electrolyte.
Detailed description of the invention
Fig. 1 is the first circle capacity of the battery of comparative example 1,2 of the present invention preparation and the relation curve of cell voltage；
Fig. 2 is the first circle capacity of battery prepared by the embodiment of the present invention 1~4 and the relation curve of cell voltage；
Fig. 3 is the specific discharge capacity of battery prepared by the embodiment of the present invention 1~4 and the relational graph of cycle-index；
Fig. 4 is the relational graph of battery discharge specific capacity prepared by the embodiment of the present invention 5,6 and cycle-index；
Fig. 5 is the relation curve of preceding two the circles specific capacity and cell voltage of battery prepared by the embodiment of the present invention 7；
Fig. 6 is the charge specific capacity of battery prepared by the embodiment of the present invention 7 and the relational graph of cycle-index；
Fig. 7 is the relation curve of preceding two the circles positive electrode specific capacity and cell voltage of battery prepared by the embodiment of the present invention 8；
Fig. 8 is the positive discharge specific capacity of battery prepared by the embodiment of the present invention 8 and the relational graph of cycle-index；
Fig. 9 is the relation curve of preceding two the circles specific capacity and cell voltage of battery prepared by the embodiment of the present invention 9；
Figure 10 is the relation curve of preceding two the circles specific capacity and cell voltage of battery prepared by the embodiment of the present invention 10；
Figure 11 is the relation curve of preceding two the circles specific capacity and cell voltage of battery prepared by the embodiment of the present invention 11；
Figure 12 is the relation curve of preceding two the circles specific capacity and cell voltage of battery prepared by the embodiment of the present invention 12；
Figure 13 is the relation curve of preceding two the circles specific capacity and cell voltage of battery prepared by the embodiment of the present invention 13；
Figure 14 is the relation curve of preceding two the circles specific capacity and cell voltage of battery prepared by the embodiment of the present invention 14；
Figure 15 is the relation curve of preceding two the circles specific capacity and cell voltage of battery prepared by the embodiment of the present invention 15；
Figure 16 is the relation curve of preceding two the circles specific capacity and cell voltage of battery prepared by the embodiment of the present invention 16；
Figure 17 is the relation curve of preceding two the circles specific capacity and cell voltage of battery prepared by the embodiment of the present invention 17；
Figure 18 is the relation curve of preceding two the circles specific capacity and cell voltage of battery prepared by the embodiment of the present invention 18；
Figure 19 is the relation curve of preceding two the circles specific capacity and cell voltage of battery prepared by the embodiment of the present invention 19.
Specific embodiment
Below in conjunction with inventive embodiments, technical solution of the present invention is clearly and completely described, it is clear that retouched
The embodiment stated is only a part of the embodiment of the present invention, instead of all the embodiments.Based on the embodiments of the present invention, originally
Field those of ordinary skill other all embodiments obtained without making creative work, belong to the present invention
The range of protection.
All raw materials of the present invention, are not particularly limited its source, buying on the market or according to those skilled in the art
The preparation of conventional method known to member.
All raw materials of the present invention, are not particularly limited its purity, and the present invention is preferentially pure using analyzing.
The present invention provides a kind of Dual-ion cell electrolyte, the electrolyte includes electrolyte and organic solvent；
The organic solvent preferably includes the mixture of dimethyl carbonate (DMC) and diethyl carbonate (DEC)；Or carbonic acid two
The mixture of methyl esters, diethyl carbonate and methyl ethyl carbonate (EMC)；Or dimethyl carbonate, diethyl carbonate and sulfolane (SL)
Mixture；Or the mixture of dimethyl carbonate, diethyl carbonate and fluorinated ethylene carbonate (FEC).
In organic solvent of the present invention, the ratio of the DMC and DEC are not particularly limited, and those skilled in the art can
With according to the actual situation, properties of product and quality requirement be adjusted, the dimethyl carbonate (DMC) and diethyl carbonate
(DEC) in mixture, the percent by volume that the DMC occupies solvent is preferably 10%~40%, more preferably 10%~
30%, most preferably 10%~20%；The percent by volume that DEC accounts for the organic solvent is 60%~90%, more preferably
30%~70%, most preferably 20%~80%；
In the mixture of the dimethyl carbonate, diethyl carbonate and methyl ethyl carbonate (EMC), the ratio of the EMC
Be not particularly limited, those skilled in the art can according to the actual situation, properties of product and quality requirement be adjusted, this hair
The percent by volume of organic solvent shared by the bright EMC is preferably 0.1%~99.9%, and more preferably 10~90%%；DMC with
The volume ratio of DEC is 2:8；
In the mixture of the dimethyl carbonate, diethyl carbonate and sulfolane (SL), the ratio of the SL is without spy
Do not limit, those skilled in the art can according to the actual situation, properties of product and quality requirement be adjusted, it is of the present invention
The percent by volume of organic solvent shared by SL is preferably the volume ratio of 0.1%~99.9%, more preferably 80%, DMC and DEC
For 2:8；
In the mixture of the dimethyl carbonate, diethyl carbonate and fluorinated ethylene carbonate (FEC), the FEC's
Ratio is not particularly limited, those skilled in the art can according to the actual situation, properties of product and quality requirement be adjusted,
FEC account for the organic solvent percent by volume be preferably 0.1%~99.9%, more preferably 42%, DMC and DEC volume
Ratio is 2:8.
The electrolyte is not particularly limited in the present invention, can be used in such battery with well known to those skilled in the art
With the electrolyte in organic solvent, the present invention is preferably lithium salts, and the lithium salts is more specifically preferably lithium hexafluoro phosphate.
The present invention is not particularly limited lithium salt, those skilled in the art can according to the actual situation, properties of product
And quality requirement is adjusted, the molar concentration of lithium salt of the present invention in organic solvent be preferably 1mol/L~
3mol/L, more preferably 1mol/L~2mol/L, most preferably 1mol/L.
The present invention using lithium salts be used as electrolyte, especially lithium hexafluoro phosphate, in above-mentioned organic solution solubility height,
Degree of dissociation is high, anion inoxidizability is strong, solvation structure is advantageous, it is ensured that anion is stored in the high reversible of graphite anode
And stabilization of the electrolyte under high working voltage.
The present invention also provides above-mentioned Dual-ion cell electrolyte to apply the application in lithium/graphite half-cell.
The present invention also provides above-mentioned Dual-ion cell electrolyte to apply the application in double graphite full batteries.
In the above-mentioned technical solutions, graphite and lithium piece, electrolyte, diaphragm are formed into lithium/graphite half-cell；By graphite and stone
Ink, electrolyte, diaphragm group graphite full battery in pairs.The electrolyte is Dual-ion cell electrolyte of the present invention, described
The material of diaphragm is glass fibre.
The graphite is not particularly limited in the present invention, with graphite well known to those skilled in the art.The present invention couple
The anode and positive electrode that other are not specifically limited, this field can according to the actual situation, properties of product and quality want
It asks and is selected and adjusted, the present invention is preferably natural graphite material.The present invention is not particularly limited the material of the diaphragm,
This field can according to the actual situation, properties of product and quality requirement selected and adjusted, the present invention is preferably glass fibers
Dimension.
The present invention is not particularly limited the preparation method of the battery, using preparation electricity well known to those skilled in the art
The method in pond.Specific steps are preferred are as follows: above-mentioned Dual-ion cell electrolyte are prepared in glove box, by lithium piece and graphite
Anode or lithium piece and graphite cathode, diaphragm and the Dual-ion cell electrolyte are assembled into lithium/graphite half-cell；Just by graphite
Pole, graphite cathode, diaphragm and the Dual-ion cell electrolyte assemble graphite full battery in pairs.
To battery provided by the invention carry out charge-discharge test, come characterize lithium/graphite half-cell graphite shop pole capacity and
The positive electrode specific capacity and cycle performance of cycle performance and double graphite full batteries, 25 DEG C of test temperature, current density: 50mA g-1.Experiment shows using cost-efficiently Dual-ion cell electrolyte provided by the invention, in lithium/graphite half-cell, stone
Black anode can stablize output up to~100mAh g-1Specific capacity, graphite cathode can stablize output up to~345mAh g-1's
Specific capacity；In double graphite full batteries, output can be stablized up to~95mAh g-1Positive electrode specific capacity.
In order to further illustrate the present invention, below with reference to embodiment to a kind of low-cost high-efficiency double ion provided by the invention
Battery electrolyte and its application in lithium/graphite half-cell and double graphite full batteries be described in detail, it is of the invention
Protection scope is not limited by the following examples.
Reagent used in following embodiment is market sale.
Comparative example 1
1mol/L lithium hexafluorophosphate solution is configured in glove box, wherein the solvent of the solution is dimethyl carbonate, will
Above-mentioned configured solution left standstill 12 hours.Using above-mentioned solution as electrolyte, battery is made in glove box, wherein cathode is
Lithium piece, just extremely graphite, diaphragm are glass fibre.
Comparative example 2
1mol/L lithium hexafluorophosphate solution is configured in glove box, wherein the solvent of the solution is diethyl carbonate, will
Above-mentioned configured solution left standstill 12 hours.Using above-mentioned solution as electrolyte, battery is made in glove box, wherein cathode is
Lithium piece, just extremely graphite, diaphragm are glass fibre.
Fig. 1 is the first circle capacity of the battery of comparative example 1,2 of the present invention preparation and the relation curve of cell voltage；It can by Fig. 1
Know, 1mol/L lithium hexafluoro phosphate is dissolved in dimethyl carbonate or diethyl carbonate solvent as in the battery of electrolyte, and graphite exports
Capacity only close to 20mAh g-1, and first circle irreversible capacity accounts for 70% or more, illustrates electrolyte decomposition, not with graphite anode
It is compatible.
Embodiment 1
In glove box configure 1mol/L lithium hexafluorophosphate solution, wherein the solvent of the solution be dimethyl carbonate and
With the mixed solvent of diethyl carbonate, the volume content of dimethyl carbonate is 40%, and above-mentioned configured solution left standstill 12 is small
When.Using above-mentioned solution as electrolyte, battery is made in glove box, wherein cathode is lithium piece, and just extremely graphite, diaphragm are glass
Glass fiber.
Embodiment 2
In glove box configure 1mol/L lithium hexafluorophosphate solution, wherein the solvent of the solution be dimethyl carbonate and
With the mixed solvent of diethyl carbonate, the volume content of dimethyl carbonate is 30%, and above-mentioned configured solution left standstill 12 is small
When.Using above-mentioned solution as electrolyte, battery is made in glove box, wherein cathode is lithium piece, and just extremely graphite, diaphragm are glass
Glass fiber.
Embodiment 3
In glove box configure 1mol/L lithium hexafluorophosphate solution, wherein the solvent of the solution be dimethyl carbonate and
With the mixed solvent of diethyl carbonate, the volume content of dimethyl carbonate is 20%, and above-mentioned configured solution left standstill 12 is small
When.Using above-mentioned solution as electrolyte, battery is made in glove box, wherein cathode is lithium piece, and just extremely graphite, diaphragm are glass
Glass fiber.
Embodiment 4
In glove box configure 1mol/L lithium hexafluorophosphate solution, wherein the solvent of the solution be dimethyl carbonate and
With the mixed solvent of diethyl carbonate, the volume content of dimethyl carbonate is 10%, and above-mentioned configured solution left standstill 12 is small
When.Using above-mentioned solution as electrolyte, battery is made in glove box, wherein cathode is lithium piece, and just extremely graphite, diaphragm are glass
Glass fiber.
Fig. 2 is the first circle capacity of battery prepared by the embodiment of the present invention 1~4 and the relation curve of cell voltage；It can by Fig. 2
To know, 1mol/L lithium hexafluoro phosphate is dissolved in dimethyl carbonate and diethyl carbonate mixed organic solvents as in the battery of electrolyte,
The capacity of graphite output is obviously improved, and illustrates that these electrolyte are compatible with graphite anode.Wherein, dimethyl carbonate percentage by volume
For the 20% best (~95mAh g of electrolyte effect-1)。
Fig. 3 is the specific discharge capacity of battery prepared by the embodiment of the present invention 1~4 and the relational graph of cycle-index；It can by Fig. 3
To know, 1mol/L lithium hexafluoro phosphate is dissolved in dimethyl carbonate and diethyl carbonate mixed organic solvents as in the battery of electrolyte,
Battery can stablize 300 circle of circulation or more, and the capacity held stationary of graphite anode output illustrates these electrolyte and graphite anode
It is compatible.Wherein, dimethyl carbonate percentage by volume be 20% electrolyte it is best, can make graphite just it is extremely stable output~
100mAh g-1Specific capacity.
Embodiment 5
In glove box configure 2mol/L lithium hexafluorophosphate solution, wherein the solvent of the solution be dimethyl carbonate and
With the mixed solvent of diethyl carbonate, the volume content of dimethyl carbonate is 20%, and above-mentioned configured solution left standstill 12 is small
When.Using above-mentioned solution as electrolyte, battery is made in glove box, wherein cathode is lithium piece, and just extremely graphite, diaphragm are glass
Glass fiber.
Embodiment 6
In glove box configure 3mol/L lithium hexafluorophosphate solution, wherein the solvent of the solution be dimethyl carbonate and
With the mixed solvent of diethyl carbonate, the volume content of dimethyl carbonate is 20%, and above-mentioned configured solution left standstill 12 is small
When.Using above-mentioned solution as electrolyte, battery is made in glove box, wherein cathode is lithium piece, and just extremely graphite, diaphragm are glass
Glass fiber.
Fig. 4 is the relational graph of battery discharge specific capacity prepared by the embodiment of the present invention 5,6 and cycle-index；As shown in Figure 4,
2mol/L and 3mol/L lithium hexafluoro phosphate is dissolved in electricity of the mixed organic solvents of 20% (volume) dimethyl carbonate as electrolyte
Chi Zhong, graphite anode can stablize output~95mAh g-1Specific capacity be more than 200 circle, illustrate these electrolyte and graphite anode
It is compatible.
Embodiment 7
In glove box configure 1mol/L lithium hexafluorophosphate solution, wherein the solvent of the solution be dimethyl carbonate and
With the mixed solvent of diethyl carbonate, the volume content of dimethyl carbonate is 20%, and above-mentioned configured solution left standstill 12 is small
When.Using above-mentioned solution as electrolyte, battery is made in glove box, wherein cathode is graphite, and just extremely lithium piece, diaphragm are glass
Glass fiber.
Fig. 5 is the relation curve of preceding two the circles specific capacity and cell voltage of battery prepared by the embodiment of the present invention 7；By Fig. 5
It is found that 1mol/L lithium hexafluoro phosphate is dissolved in battery of the mixed organic solvents of 20% (volume) dimethyl carbonate as electrolyte
In, capacity~345mAh g of graphite cathode output-1, second circle coulombic efficiency up to 90% or more, illustrate this electrolyte and stone
Black cathode is compatible.
Fig. 6 is the charge specific capacity of battery prepared by the embodiment of the present invention 7 and the relational graph of cycle-index；It will be appreciated from fig. 6 that
1mol/L lithium hexafluoro phosphate is dissolved in the mixed organic solvents of 20% (volume) dimethyl carbonate as in the battery of electrolyte, graphite
Cathode can export~345mAh g-1Specific capacity up to 25 circle more than, illustrate that this electrolyte is compatible with graphite cathode.
Embodiment 8
In glove box configure 1mol/L lithium hexafluorophosphate solution, wherein the solvent of the solution be dimethyl carbonate and
With the mixed solvent of diethyl carbonate, the volume content of dimethyl carbonate is 20%, and above-mentioned configured solution left standstill 12 is small
When.Using above-mentioned solution as electrolyte, battery is made in glove box, wherein cathode is graphite, and just extremely graphite, diaphragm are glass
Glass fiber.
Fig. 7 is the relation curve of preceding two the circles positive electrode specific capacity and cell voltage of battery prepared by the embodiment of the present invention 8；By
Fig. 7 is it is found that 1mol/L lithium hexafluoro phosphate is dissolved in electricity of the mixed organic solvents of 20% (volume) dimethyl carbonate as electrolyte
Chi Zhong, positive electrode specific capacity~95mAh g of battery output-1, second circle coulombic efficiency up to 90% or more, illustrate this electrolyte with
Double graphite full batteries are compatible.
Fig. 8 is the positive discharge specific capacity of battery prepared by the embodiment of the present invention 8 and the relational graph of cycle-index；By Fig. 8
It is found that 1mol/L lithium hexafluoro phosphate is dissolved in battery of the mixed organic solvents of 20% (volume) dimethyl carbonate as electrolyte
In, double graphite full batteries can stablize output~90mAh g-1Positive electrode specific capacity up to more than 40 circles, this bright electrolyte and double stones
Black full battery is compatible.
Embodiment 9
1mol/L lithium hexafluorophosphate solution is configured in glove box, wherein the solvent of the solution is dimethyl carbonate, carbon
The mixed solvent of diethyl phthalate and methyl ethyl carbonate, the volume content of methyl ethyl carbonate are 90%, dimethyl carbonate and carbonic acid two
The volume ratio of ethyl ester was 2:8, by above-mentioned configured solution left standstill 12 hours.Using above-mentioned solution as electrolyte, in glove box
Make battery, wherein cathode is lithium piece, and just extremely graphite, diaphragm are glass fibre.
Fig. 9 is the relation curve of preceding two the circles specific capacity and cell voltage of battery prepared by the embodiment of the present invention 9；By Fig. 9
It is found that 1mol/L lithium hexafluoro phosphate is dissolved in mixed organic solvents (its of dimethyl carbonate, diethyl carbonate and methyl ethyl carbonate
In, methyl ethyl carbonate percentage by volume is 90%, and the volume ratio of dimethyl carbonate and diethyl carbonate is 2:8) it is used as electrolyte
Battery in, battery output positive electrode specific capacity~105mAh g-1, second circle coulombic efficiency up to 90% or more, illustrate carbonic acid
The mixture (percent by volume 2:8) of dimethyl ester and diethyl carbonate can be substituted effectively in methyl ethyl carbonate ester group electrolyte
The methyl ethyl carbonate ingredient of 10% (percentage by volume), this electrolyte are compatible with graphite anode.
Embodiment 10
1mol/L lithium hexafluorophosphate solution is configured in glove box, wherein the solvent of the solution is dimethyl carbonate, carbon
The mixed solvent of diethyl phthalate and methyl ethyl carbonate, the volume content of methyl ethyl carbonate are 80%, dimethyl carbonate and carbonic acid two
The volume ratio of ethyl ester was 2:8, by above-mentioned configured solution left standstill 12 hours.Using above-mentioned solution as electrolyte, in glove box
Make battery, wherein cathode is lithium piece, and just extremely graphite, diaphragm are glass fibre.
Figure 10 is the relation curve of preceding two the circles specific capacity and cell voltage of battery prepared by the embodiment of the present invention 10；By scheming
10 it is found that 1mol/L lithium hexafluoro phosphate is dissolved in mixed organic solvents (its of dimethyl carbonate, diethyl carbonate and methyl ethyl carbonate
In, methyl ethyl carbonate percentage by volume is 80%, and the volume ratio of dimethyl carbonate and diethyl carbonate is 2:8) it is used as electrolyte
Battery in, battery output positive electrode specific capacity~100mAh g-1, second circle coulombic efficiency up to 90% or more, illustrate carbonic acid
The mixture (percent by volume 2:8) of dimethyl ester and diethyl carbonate can be substituted effectively in methyl ethyl carbonate ester group electrolyte
The methyl ethyl carbonate ingredient of 20% (percentage by volume), this electrolyte are compatible with graphite anode.
Embodiment 11
1mol/L lithium hexafluorophosphate solution is configured in glove box, wherein the solvent of the solution is dimethyl carbonate, carbon
The mixed solvent of diethyl phthalate and methyl ethyl carbonate, the volume content of methyl ethyl carbonate are 70%, dimethyl carbonate and carbonic acid two
The volume ratio of ethyl ester was 2:8, by above-mentioned configured solution left standstill 12 hours.Using above-mentioned solution as electrolyte, in glove box
Make battery, wherein cathode is lithium piece, and just extremely graphite, diaphragm are glass fibre.
Figure 11 is the relation curve of preceding two the circles specific capacity and cell voltage of battery prepared by the embodiment of the present invention 11；By scheming
11 it is found that 1mol/L lithium hexafluoro phosphate is dissolved in mixed organic solvents (its of dimethyl carbonate, diethyl carbonate and methyl ethyl carbonate
In, methyl ethyl carbonate percentage by volume is 70%, and the volume ratio of dimethyl carbonate and diethyl carbonate is 2:8) it is used as electrolyte
Battery in, battery output positive electrode specific capacity~108mAh g-1, second circle coulombic efficiency up to 90% or more, illustrate carbonic acid
30% in the mixture (percent by volume 2:8) of dimethyl ester and diethyl carbonate effectively substitution methyl ethyl carbonate ester group electrolyte
The methyl ethyl carbonate ingredient of (percentage by volume), this electrolyte are compatible with graphite anode.
Embodiment 12
1mol/L lithium hexafluorophosphate solution is configured in glove box, wherein the solvent of the solution is dimethyl carbonate, carbon
The mixed solvent of diethyl phthalate and methyl ethyl carbonate, the volume content of methyl ethyl carbonate are 60%, dimethyl carbonate and carbonic acid two
The volume ratio of ethyl ester was 2:8, by above-mentioned configured solution left standstill 12 hours.Using above-mentioned solution as electrolyte, in glove box
Make battery, wherein cathode is lithium piece, and just extremely graphite, diaphragm are glass fibre.
Figure 12 is the relation curve of preceding two the circles specific capacity and cell voltage of battery prepared by the embodiment of the present invention 12；By scheming
12 it is found that 1mol/L lithium hexafluoro phosphate is dissolved in mixed organic solvents (its of dimethyl carbonate, diethyl carbonate and methyl ethyl carbonate
In, methyl ethyl carbonate percentage by volume is 60%, and the volume ratio of dimethyl carbonate and diethyl carbonate is 2:8) it is used as electrolyte
Battery in, battery output positive electrode specific capacity~100mAh g-1, second circle coulombic efficiency up to 90% or more, illustrate carbonic acid
The mixture (percent by volume 2:8) of dimethyl ester and diethyl carbonate can be substituted effectively in methyl ethyl carbonate ester group electrolyte
The methyl ethyl carbonate ingredient of 40% (percentage by volume), this electrolyte are compatible with graphite anode.
Embodiment 13
1mol/L lithium hexafluorophosphate solution is configured in glove box, wherein the solvent of the solution is dimethyl carbonate, carbon
The mixed solvent of diethyl phthalate and methyl ethyl carbonate, the volume content of methyl ethyl carbonate are 50%, dimethyl carbonate and carbonic acid two
The volume ratio of ethyl ester was 2:8, by above-mentioned configured solution left standstill 12 hours.Using above-mentioned solution as electrolyte, in glove box
Make battery, wherein cathode is lithium piece, and just extremely graphite, diaphragm are glass fibre.
Figure 13 is the relation curve of preceding two the circles specific capacity and cell voltage of battery prepared by the embodiment of the present invention 13；By scheming
13 it is found that 1mol/L lithium hexafluoro phosphate is dissolved in mixed organic solvents (its of dimethyl carbonate, diethyl carbonate and methyl ethyl carbonate
In, methyl ethyl carbonate percentage by volume is 50%, and the volume ratio of dimethyl carbonate and diethyl carbonate is 2:8) it is used as electrolyte
Battery in, battery output positive electrode specific capacity~100mAh g-1, second circle coulombic efficiency up to 90% or more, illustrate carbonic acid
The mixture (percent by volume 2:8) of dimethyl ester and diethyl carbonate can be substituted effectively in methyl ethyl carbonate ester group electrolyte
The methyl ethyl carbonate ingredient of 50% (percentage by volume), this electrolyte are compatible with graphite anode.
Embodiment 14
1mol/L lithium hexafluorophosphate solution is configured in glove box, wherein the solvent of the solution is dimethyl carbonate, carbon
The mixed solvent of diethyl phthalate and methyl ethyl carbonate, the volume content of methyl ethyl carbonate are 40%, dimethyl carbonate and carbonic acid two
The volume ratio of ethyl ester was 2:8, by above-mentioned configured solution left standstill 12 hours.Using above-mentioned solution as electrolyte, in glove box
Make battery, wherein cathode is lithium piece, and just extremely graphite, diaphragm are glass fibre.
Figure 14 is the relation curve of preceding two the circles specific capacity and cell voltage of battery prepared by the embodiment of the present invention 14；By scheming
14 it is found that 1mol/L lithium hexafluoro phosphate is dissolved in mixed organic solvents (its of dimethyl carbonate, diethyl carbonate and methyl ethyl carbonate
In, methyl ethyl carbonate percentage by volume is 40%, and the volume ratio of dimethyl carbonate and diethyl carbonate is 2:8) it is used as electrolyte
Battery in, battery output positive electrode specific capacity~100mAh g-1, second circle coulombic efficiency up to 90% or more, illustrate carbonic acid
The mixture (percent by volume 2:8) of dimethyl ester and diethyl carbonate can be substituted effectively in methyl ethyl carbonate ester group electrolyte
The methyl ethyl carbonate ingredient of 60% (percentage by volume), this electrolyte are compatible with graphite anode.
Embodiment 15
1mol/L lithium hexafluorophosphate solution is configured in glove box, wherein the solvent of the solution is dimethyl carbonate, carbon
The mixed solvent of diethyl phthalate and methyl ethyl carbonate, the volume content of methyl ethyl carbonate are 30%, dimethyl carbonate and carbonic acid two
The volume ratio of ethyl ester was 2:8, by above-mentioned configured solution left standstill 12 hours.Using above-mentioned solution as electrolyte, in glove box
Make battery, wherein cathode is lithium piece, and just extremely graphite, diaphragm are glass fibre.
Figure 15 is the relation curve of preceding two the circles specific capacity and cell voltage of battery prepared by the embodiment of the present invention 15；By scheming
15 it is found that 1mol/L lithium hexafluoro phosphate is dissolved in mixed organic solvents (its of dimethyl carbonate, diethyl carbonate and methyl ethyl carbonate
In, methyl ethyl carbonate percentage by volume is 30%, and the volume ratio of dimethyl carbonate and diethyl carbonate is 2:8) it is used as electrolyte
Battery in, battery output positive electrode specific capacity~110mAh g-1, second circle coulombic efficiency up to 90% or more, illustrate carbonic acid
The mixture (percent by volume 2:8) of dimethyl ester and diethyl carbonate can be substituted effectively in methyl ethyl carbonate ester group electrolyte
The methyl ethyl carbonate ingredient of 70% (percentage by volume), this electrolyte are compatible with graphite anode.
Embodiment 16
1mol/L lithium hexafluorophosphate solution is configured in glove box, wherein the solvent of the solution is dimethyl carbonate, carbon
The mixed solvent of diethyl phthalate and methyl ethyl carbonate, the volume content of methyl ethyl carbonate are 20%, dimethyl carbonate and carbonic acid two
The volume ratio of ethyl ester was 2:8, by above-mentioned configured solution left standstill 12 hours.Using above-mentioned solution as electrolyte, in glove box
Make battery, wherein cathode is lithium piece, and just extremely graphite, diaphragm are glass fibre.
Figure 16 is the relation curve of preceding two the circles specific capacity and cell voltage of battery prepared by the embodiment of the present invention 16；By scheming
16 it is found that 1mol/L lithium hexafluoro phosphate is dissolved in mixed organic solvents (its of dimethyl carbonate, diethyl carbonate and methyl ethyl carbonate
In, methyl ethyl carbonate percentage by volume is 20%, and the volume ratio of dimethyl carbonate and diethyl carbonate is 2:8) it is used as electrolyte
Battery in, battery output positive electrode specific capacity~105mAh g-1, second circle coulombic efficiency up to 90% or more, illustrate carbonic acid
The mixture (percent by volume 2:8) of dimethyl ester and diethyl carbonate can be substituted effectively in methyl ethyl carbonate ester group electrolyte
The methyl ethyl carbonate ingredient of 80% (percentage by volume), this electrolyte are compatible with graphite anode.
Embodiment 17
1mol/L lithium hexafluorophosphate solution is configured in glove box, wherein the solvent of the solution is dimethyl carbonate, carbon
The mixed solvent of diethyl phthalate and methyl ethyl carbonate, the volume content of methyl ethyl carbonate are 10%, dimethyl carbonate and carbonic acid two
The volume ratio of ethyl ester was 2:8, by above-mentioned configured solution left standstill 12 hours.Using above-mentioned solution as electrolyte, in glove box
Make battery, wherein cathode is lithium piece, and just extremely graphite, diaphragm are glass fibre.
Figure 17 is the relation curve of preceding two the circles specific capacity and cell voltage of battery prepared by the embodiment of the present invention 17；By scheming
17 it is found that 1mol/L lithium hexafluoro phosphate is dissolved in mixed organic solvents (its of dimethyl carbonate, diethyl carbonate and methyl ethyl carbonate
In, methyl ethyl carbonate percentage by volume is 10%, and the volume ratio of dimethyl carbonate and diethyl carbonate is 2:8) it is used as electrolyte
Battery in, battery output positive electrode specific capacity~100mAh g-1, second circle coulombic efficiency up to 90% or more, illustrate carbonic acid
The mixture (percent by volume 2:8) of dimethyl ester and diethyl carbonate can be substituted effectively in methyl ethyl carbonate ester group electrolyte
The methyl ethyl carbonate ingredient of 90% (percentage by volume), this electrolyte are compatible with graphite anode.
Embodiment 18
1mol/L lithium hexafluorophosphate solution is configured in glove box, wherein the solvent of the solution is dimethyl carbonate, carbon
The mixed solvent of diethyl phthalate and sulfolane, the volume content of sulfolane are 80%, the body of dimethyl carbonate and diethyl carbonate
Product was than being 2:8, by above-mentioned configured solution left standstill 12 hours.Using above-mentioned solution as electrolyte, battery is made in glove box,
Wherein, cathode is lithium piece, and just extremely graphite, diaphragm are glass fibre.
Figure 18 is the relation curve of preceding two the circles specific capacity and cell voltage of battery prepared by the embodiment of the present invention 18；By scheming
18 it is found that (wherein, 1mol/L lithium hexafluoro phosphate is dissolved in the mixed organic solvents of dimethyl carbonate, diethyl carbonate and sulfolane
Sulfolane percentage by volume is 80%, battery of the volume ratio of dimethyl carbonate and diethyl carbonate for 2:8) as electrolyte
In, battery can be in 5.4V steady operation, positive electrode specific capacity~110mAh g of output-1, the coulombic efficiency of the second circle is up to 90%
More than, illustrate that the mixture (percent by volume 2:8) of dimethyl carbonate and diethyl carbonate being capable of effective alternate collar fourth sulfuryl
The methyl ethyl carbonate ingredient of (percentage by volume), this electrolyte are compatible with graphite anode 100% in electrolyte.
Embodiment 19
1mol/L lithium hexafluorophosphate solution is configured in glove box, wherein the solvent of the solution is dimethyl carbonate, carbon
The mixed solvent of diethyl phthalate and fluorinated ethylene carbonate, the volume content of fluorinated ethylene carbonate are 42%, dimethyl carbonate
Volume ratio with diethyl carbonate was 2:8, by above-mentioned configured solution left standstill 12 hours.Using above-mentioned solution as electrolyte,
Battery is made in glove box, wherein cathode is lithium piece, and just extremely graphite, diaphragm are glass fibre.
Figure 19 is the relation curve of preceding two the circles specific capacity and cell voltage of battery prepared by the embodiment of the present invention 19.By scheming
19 it is found that the mixing that is dissolved in dimethyl carbonate, diethyl carbonate and fluorinated ethylene carbonate of 1mol/L lithium hexafluoro phosphate is organic molten
Agent (wherein, fluorinated ethylene carbonate percentage by volume is 42%, and the volume ratio of dimethyl carbonate and diethyl carbonate is 2:8) is made
For positive electrode specific capacity~110mAh g that in the battery of electrolyte, battery is exported-1, the coulombic efficiency of the second circle up to 90% or more,
Illustrate that the mixture (percent by volume 2:8) of dimethyl carbonate and diethyl carbonate can effectively substitute fluorinated ethylene carbonate
The methyl ethyl carbonate ingredient of (percentage by volume), this electrolyte are compatible with graphite anode 100% in base electrolyte.
The above description of the embodiment is only used to help understand the method for the present invention and its core ideas.It should be pointed out that pair
For those skilled in the art, the present invention can also be carried out under the premise of not departing from inventive principle several
Improvement and modification, these improvements and modifications also fall within the scope of protection of the claims of the present invention.
The foregoing description of the disclosed embodiments makes professional and technical personnel in the field can be realized and use the present invention.
Various modifications to these embodiments will be readily apparent to those skilled in the art, as defined herein
General Principle can be realized in other embodiments without departing from the spirit or scope of the present invention.Therefore, of the invention
It will not be limited and the embodiments shown herein, and it is consistent to be to fit to the principles and novel features disclosed herein
Widest scope.
Claims (10)
1. a kind of Dual-ion cell electrolyte, which is characterized in that the electrolyte includes electrolyte and organic solvent；
The organic solvent is the mixture of dimethyl carbonate and diethyl carbonate；Or dimethyl carbonate, diethyl carbonate and carbon
The mixture of sour methyl ethyl ester；Or the mixture of dimethyl carbonate, diethyl carbonate and sulfolane；Or dimethyl carbonate, carbonic acid two
The mixture of ethyl ester and fluorinated ethylene carbonate.
2. a kind of Dual-ion cell electrolyte according to claim 1, which is characterized in that the dimethyl carbonate and carbon
In the mixture of diethyl phthalate, the percent by volume that dimethyl carbonate accounts for the organic solvent is 10%~40%, carbonic acid diethyl
The percent by volume that ester accounts for the organic solvent is 60%~90%.
3. a kind of Dual-ion cell electrolyte according to claim 1, which is characterized in that the dimethyl carbonate, carbon
In the mixture of diethyl phthalate and methyl ethyl carbonate, methyl ethyl carbonate account for the organic solvent percent by volume be 0.1%~
99.9%, the volume ratio of dimethyl carbonate and diethyl carbonate is 2:8.
4. a kind of Dual-ion cell electrolyte according to claim 1, which is characterized in that the dimethyl carbonate, carbon
In the mixture of diethyl phthalate and sulfolane, the percent by volume that sulfolane accounts for the organic solvent is 0.1%~99.9%, carbon
The volume ratio of dimethyl phthalate and diethyl carbonate is 2:8.
5. a kind of Dual-ion cell electrolyte according to claim 1, which is characterized in that the dimethyl carbonate, carbon
In the mixture of diethyl phthalate and fluorinated ethylene carbonate, the percent by volume that fluorinated ethylene carbonate accounts for the organic solvent is
0.1%~99.9%, the volume ratio of dimethyl carbonate and diethyl carbonate is 2:8.
6. a kind of Dual-ion cell electrolyte according to claim 1, which is characterized in that the electrolyte is lithium salts.
7. a kind of Dual-ion cell electrolyte according to claim 1, which is characterized in that the lithium salts is described organic molten
Molar concentration in agent is 1mol/L~3mol/L.
8. a kind of Dual-ion cell electrolyte according to claim 6, which is characterized in that the lithium salts is hexafluorophosphoric acid
Lithium.
9. application of the Dual-ion cell electrolyte described in claim 1-8 any one in lithium/graphite half-cell.
10. application of the Dual-ion cell electrolyte described in claim 1-8 any one in double graphite full batteries.
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN114725509A (en) * | 2022-04-25 | 2022-07-08 | 西安交通大学 | Sulfone-based lithium battery electrolyte and lithium battery |
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