CN114373991A - Non-aqueous electrolyte for lithium battery and lithium ion battery - Google Patents
Non-aqueous electrolyte for lithium battery and lithium ion battery Download PDFInfo
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- CN114373991A CN114373991A CN202111663904.9A CN202111663904A CN114373991A CN 114373991 A CN114373991 A CN 114373991A CN 202111663904 A CN202111663904 A CN 202111663904A CN 114373991 A CN114373991 A CN 114373991A
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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
- H01M10/0566—Liquid materials
- H01M10/0567—Liquid materials characterised by the additives
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
- H01M10/4235—Safety or regulating additives or arrangements in electrodes, separators or electrolyte
-
- 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
Abstract
The invention discloses a non-aqueous electrolyte for a lithium battery and the lithium battery. The non-aqueous electrolyte for the lithium battery comprises an electrolyte salt, a non-aqueous solvent and an additive, wherein the additive comprises an olefinic acid ester additive. The non-aqueous electrolyte for the lithium battery is added with a small amount of the olefine acid ester additive, so that the non-aqueous electrolyte has high film forming sensitivity, improves the lithium conducting capacity of the battery, and reduces the impedance of the battery.
Description
Technical Field
The invention relates to the technical field of electrolyte, in particular to a non-aqueous electrolyte for a lithium battery and the lithium battery.
Background
A lithium ion battery is a type of secondary battery that mainly operates by movement of lithium ions between a positive electrode and a negative electrode. The lithium ion battery has the important advantages of high voltage and high capacity, long cycle life and good safety performance, so that the lithium ion battery has wide application prospects in various aspects such as portable electronic equipment, electric automobiles, space technology, national defense industry and the like. The lithium ion battery mainly comprises an anode, a cathode, a diaphragm and electrolyte.
In the electrolyte, the commonly used film forming additives mainly comprise Vinylene Carbonate (VC) and Fluorinated Ethylene Carbonate (FEC), and although the film forming additives can improve the high-temperature cycle stability of the battery and reduce high-temperature storage gas generation, the thicker film forming also brings larger initial direct current impedance and direct current impedance (DCR) increase. In the application of the ternary battery and the lithium iron battery, when the addition amount of VC is insufficient, the improvement effect of high-temperature cycle stability is not obvious, and when the addition amount of VC exceeds a certain mass percentage, the initial DCR and DCR are increased greatly; in addition, VC prices are high in the background of increased demand for energy storage batteries. The FEC is thin relative to VC film forming and low in impedance, the action principle is that the FEC is used for slowly removing HF to generate VC under electrocatalysis, and the application is more in a silicon-carbon system, but the problems of acidity increase and high-temperature cycle gas generation of electrolyte with high FEC content are caused due to the fact that the FEC is high in price, and the cycle performance and the high-temperature stability of a battery are threatened.
Disclosure of Invention
Aiming at the defects of the prior art, the invention aims to provide a non-aqueous electrolyte for a lithium battery and the lithium ion battery.
One of the objectives of the present invention is to provide a nonaqueous electrolyte for a lithium battery, and to achieve the objective, the present invention adopts the following technical scheme:
a non-aqueous electrolyte for a lithium battery includes an electrolyte salt, a non-aqueous solvent, and an additive including an olefinic acid ester additive.
According to the non-aqueous electrolyte for the lithium battery, the olefine acid ester additive is introduced, and the characteristic that the conjugated double bond of the olefine acid ester starts polymerization under electrocatalysis is utilized, so that the non-aqueous electrolyte has strong film forming sensitivity, and the addition amount of the additive can be reduced; meanwhile, by introducing asymmetric alkenyl side groups, the density of the formed SEI film can be regulated, the lithium conduction capability is improved, and the battery impedance is reduced; the fluoride-free structure of the olefinic acid ester additive can prevent the acidity of the electrolyte from rising due to HF removal, and further influences the cycle performance and high-temperature stability of the battery.
In the invention, the olefine acid ester additive is a compound shown as a formula (I):
wherein, in the formula (I), R1、R3And R4The groups are independently selected from hydrogen, alkyl with unsaturation degree of 0 to 6 and skeleton carbon atom number of 1 to 6, and carbon oxygen group;
R2selected from hydrocarbon groups or carbon oxygen groups with the unsaturation degree of 0 to 6 and the skeleton carbon atom number of 1 to 6.
The above-mentioned carboxy group may be a group containing a single carbon-oxygen bond, such as an alkoxy group or an ether, or a group containing a double carbon-oxygen bond, such as a C ═ O-containing aldehyde, ketone, carboxylic acid, or a derivative thereof.
Further, the hydrocarbyl or carboxy groups independently comprise-CN, halogen substituents.
In a preferred embodiment of the present invention, the olefinic acid ester additive is
And/or
In the invention, the nonaqueous electrolyte for the lithium battery comprises the following components in percentage by weight:
specifically, the nonaqueous electrolyte for the lithium battery comprises the following components in percentage by weight:
the weight percentage of the additional electrolyte salt is 0.01-20%, for example, 0.01%, 1%, 2%, 3%, 4%, 5%, 6%, 7%, 8%, 9%, 10%, 11%, 12%, 13%, 14%, 15%, 16%, 17%, 18%, 19%, 20%, or the like.
The lithium salt additive is 0.01 to 10% by weight, for example, 0.01%, 0.02%, 0.03%, 0.04%, 0.05%, 0.06%, 0.07%, 0.08%, 0.09%, 1%, 2%, 3%, 4%, 5%, 6%, 7%, 8%, 9%, or 10%, etc.
The nonaqueous solvent is 0.01 to 85% by weight, for example, 0.01%, 0.02%, 0.03%, 0.04%, 0.05%, 0.06%, 0.07%, 0.08%, 0.09%, 1%, 2%, 3%, 4%, 5%, 6%, 7%, 8%, 9%, 10%, 15%, 20%, 25%, 30%, 35%, 40%, 45%, 50%, 55%, 60%, 65%, 70%, 75%, 76%, 77%, 78%, 79%, 80%, 81%, 82%, 83%, 84%, or 85%.
The weight percentage of the olefinic acid ester-based additive is 0.01 to 40%, for example, 0.01%, 0.02%, 0.03%, 0.04%, 0.05%, 0.06%, 0.07%, 0.08%, 0.09%, 1%, 2%, 3%, 4%, 5%, 6%, 7%, 8%, 9%, 10%, 11%, 12%, 13%, 14%, 15%, 16%, 17%, 18%, 19%, 20%, 21%, 22%, 23%, 24%, 25%, 26%, 27%, 28%, 29%, 30%, 31%, 32%, 33%, 34%, 35%, 36%, 37%, 38%, 39%, or 40%.
The carbonate-based additive may be 0.01 to 40% by weight, for example, 0.01%, 0.02%, 0.03%, 0.04%, 0.05%, 0.06%, 0.07%, 0.08%, 0.09%, 1%, 2%, 3%, 4%, 5%, 6%, 7%, 8%, 9%, 10%, 15%, 20%, 25%, 30%, 35%, or 40%.
The sulfonate-based additive is 0.01 to 10% by weight, for example, 0.01%, 0.02%, 0.03%, 0.04%, 0.05%, 0.06%, 0.07%, 0.08%, 0.09%, 1%, 2%, 3%, 4%, 5%, 6%, 7%, 8%, 9%, or 10%.
In the present invention, the additional electrolyte, the lithium salt additive, the nonaqueous solvent, and the sulfonate-based additive satisfy at least one of the following conditions (1) to (4):
(1) the additional electrolyte is lithium hexafluorophosphate (LiPF)6)；
(2) The lithium salt additive is lithium difluorophosphate (LiPO)2F2) Any one or a mixture of at least two of lithium difluorobis (oxalato) phosphate, lithium tetrafluoroborate, lithium difluorooxalato borate, lithium bis (trifluoromethanesulfonyl) imide, and lithium bis (fluorosulfonyl) imide (LiFSI);
(3) the non-aqueous solvent is any one or a mixture of at least two of carbonate, carboxylate, ether or amine solvents;
(4) the sulfonate additive is any one or a mixture of at least two of 1, 3-Propane Sultone (PS), 1, 3-Propene Sultone (PST) and vinyl sulfate (DTD).
The carbonate additive is any one or a mixture of at least two of a linear carbonate additive, a cyclic carbonate additive and a fluorinated carbonate additive, and the carbonate additive satisfies at least one of the following conditions (5) to (7):
(5) the straight-chain carbonate additive is any one or a mixture of at least two of methyl ethyl carbonate, dimethyl carbonate and diethyl carbonate;
(6) the cyclic carbonate additive is any one or a mixture of at least two of Ethylene Carbonate (EC), propylene carbonate, Vinylene Carbonate (VC) and ethylene carbonate (VEC);
(7) the fluorinated carbonate additive is one or a mixture of at least two of Fluorinated Ethylene Carbonate (FEC), 1, 2-difluoroethylene carbonate, methyl trifluoroethyl carbonate and bis trifluoroethyl carbonate.
It is a second object of the present invention to provide a lithium ion battery comprising a positive electrode, a negative electrode, a separator interposed between the positive electrode and the negative electrode, and the nonaqueous electrolytic solution for a lithium battery according to the first object.
The positive electrode includes a positive active material.
The positive electrode active material is selected from any one of lithium iron phosphate (LFP), lithium nickel cobalt composite oxide, and lithium nickel manganese composite oxide having a spinel structure, or a mixture of at least two thereof.
The general formula of the lithium nickel cobalt composite oxide is LixNiyCozMe(1-y-z)OaWherein x in the general formula satisfies the condition of 1 ≦ x ≦ 1.2, y and z are positive numbers satisfying the relationship of y + z < 1, the value of y is 0.5 or less, Me is any one or at least two metals selected from Al, Mn, Na, Fe, Cr, Cu, Zn, Ca, K, Mg and Pb, and a satisfies the condition of 1.5 ≦ a ≦ 2.5.
The negative electrode contains a carbon material containing carbon as a constituent element, a silicon material containing silicon as a constituent element, or a carbon-silicon composite material.
The carbon material is any one or a mixture of at least two of acetylene black, conductive carbon black, carbon fiber, carbon nanotube and Ketjen black.
The silicon material is any one or a mixture of at least two of silicon, silicon oxygen compound and silicon-based alloy.
The membrane is a membrane material commonly used in the field, for example, the membrane comprises a base membrane and a nano aluminum oxide coating coated on the base membrane.
Compared with the prior art, the invention has the beneficial effects that:
the non-aqueous electrolyte for the lithium battery is added with a small amount of the olefine acid ester additive, so that the non-aqueous electrolyte has high film forming sensitivity, improves the lithium conducting capacity of the battery, and reduces the impedance of the battery. Specifically, the initial DCR of the lithium ion battery prepared by the invention is 90-118 mOhm, the volume expansion rate of 60d at 60 ℃ is 11-38%, the DCR growth rate of 60d at 60 ℃ is 12-55%, and the number of SOH cycles of 80% at 45 ℃ is 993-2113.
Detailed Description
The technical solution of the present invention is further explained by the following embodiments.
The non-aqueous electrolyte for the lithium battery comprises electrolyte salt, a non-aqueous solvent and an additive, wherein the additive comprises an olefinic acid ester additive.
In the present invention, the lithium ion battery is a primary lithium battery or a secondary lithium battery, and includes: the battery comprises a positive electrode, a negative electrode, a separator between the positive electrode and the negative electrode, and an electrolyte.
The preparation method of the secondary lithium battery comprises the following steps:
(1) preparation of nonaqueous electrolyte for lithium battery
And preparing a non-aqueous solvent in a dry argon atmosphere, adding fully dried electrolyte salt, lithium salt additive, the non-aqueous solvent and additive, and uniformly mixing to obtain the non-aqueous electrolyte for the lithium battery.
(2) Preparation of secondary lithium battery
And (2) preparing a secondary lithium battery by taking the electrolyte obtained in the step 1) as a non-aqueous electrolyte for the lithium battery.
The anode material comprises the following components:
811 (abbreviated as 8 series) represents Li2Ni0.8Co0.1Mn0.1O2；
LFP(LiFePO4Abbreviation) represents lithium iron phosphate.
The negative electrode material adopts graphite or carbon silicon.
Example 1
The nonaqueous electrolyte for the lithium battery of the embodiment comprises the following components in percentage by weight:
wherein the non-aqueous solvent is a mixture of Ethylene Carbonate (EC), Ethyl Methyl Carbonate (EMC) and diethyl carbonate (DEC) in a mass ratio of 3:5:2, and the structural formula of the olefinic acid ester additive is shown in the specification
Is denoted as A.
The structural formula of another olefine acid ester additive is shown in the specification
Is denoted as B.
In addition, the nonaqueous solvents in examples 2 to 11 and comparative examples 1 to 6 were each a mixture of EC, EMC and DEC at a mass ratio of 3:5: 2.
In other examples and comparative examples, parameters were changed in addition to those in example 1, and specific changed parameters are shown in table 1.
TABLE 1
The lithium batteries prepared in examples 1 to 11 and comparative examples 1 to 6 were subjected to performance tests, and the test results are shown in table 2.
Among them, the secondary battery of the present invention was tested by the following method:
(1) secondary battery cycle test
And carrying out cyclic charge and discharge in a specified potential interval by using the current of 1C, recording the capacity of each circle, and finishing the test when the capacity of the battery reaches 80 percent of the capacity of the first circle.
(2) Direct Current Resistance (DCR) test of secondary battery
When the battery is discharged to 50% SOC (state of charge, reflecting the residual capacity of the battery) at a specified temperature by 1C current, the current is increased to 4C and kept for 30s, the difference between the updated stable voltage and the original platform voltage is detected, and the ratio of the value to the 3C current value is the direct current resistance of the battery. And comparing the DCR after the cycle is ended with the DCR at the beginning of the cycle to obtain the increase rate of the DCR.
(3) Volume change test of gas generated by secondary battery
Fixing the secondary battery with a string, completely soaking the secondary battery in water at 60 ℃, recording the weight difference before and after soaking, and converting according to the density of the water at 60 ℃ to obtain the volume difference.
TABLE 2
As can be seen from the data in Table 2, the comparison between examples 1 and 2 and comparative examples 1 and 2 shows that in the ternary system of the positive electrode, compared with the conventional VC and FEC, the adoption of the olefinic acid ester additive of the invention can lead the prepared battery to have lower battery impedance and more excellent cycle performance on the premise of less additive dosage.
Comparison between comparative example 3 and examples 6 and 9 shows that the olefine acid ester additive provided by the invention is adopted in a negative silicon-carbon system, and the prepared battery has lower battery impedance and more excellent cycle performance on the premise of less additive dosage.
Comparison between comparative example 4 and examples 10 and 11 shows that the adoption of the olefinic acid ester additive of the invention in a positive lithium iron phosphate system leads the prepared battery to have lower battery impedance and more excellent cycle performance under the premise of less additive dosage.
Examples 4-8 show that as the amount of the enoate additive increases, the initial DCR decreases and increases, the battery impedance decreases and the cycle performance improves.
In example 6, comparison of comparative example 5 shows that too small amount of the enoate additive increases initial DCR, increases battery resistance, and deteriorates cycle performance.
In comparison between example 6 and comparative example 6, it can be seen that the use of the olefinic acid ester additive in a large amount also increases the initial DCR, increases the battery resistance, and deteriorates the cycle performance.
The present invention is illustrated in detail by the examples described above, but the present invention is not limited to the details described above, i.e., it is not intended that the present invention be implemented by relying on the details described above. It should be understood by those skilled in the art that any modification of the present invention, equivalent substitutions of the raw materials of the product of the present invention, addition of auxiliary components, selection of specific modes, etc., are within the scope and disclosure of the present invention.
Claims (10)
1. The nonaqueous electrolyte for the lithium battery is characterized by comprising the following components in percentage by weight:
2. the nonaqueous electrolytic solution for a lithium battery according to claim 1, wherein the olefinic acid ester additive is a compound represented by formula (I):
wherein, in the formula (I), R1、R3And R4The groups are independently selected from hydrogen, alkyl with unsaturation degree of 0 to 6 and skeleton carbon atom number of 1 to 6, and carbon oxygen group;
R2selected from hydrocarbon groups or carbon oxygen groups with the unsaturation degree of 0 to 6 and the skeleton carbon atom number of 1 to 6.
3. The nonaqueous electrolytic solution for a lithium battery according to claim 2, wherein the hydrocarbon group or the carboxy group independently comprises-CN, a halogen substituent.
4. The nonaqueous electrolytic solution for a lithium battery according to claim 1 or 2, wherein the olefinic acid ester additive is
And/or
5. The nonaqueous electrolytic solution for a lithium battery according to claim 1, wherein the additional electrolyte, the lithium salt additive, the nonaqueous solvent, and the sulfonate additive satisfy at least one of the following conditions (1) to (4):
(1) the additional electrolyte is lithium hexafluorophosphate;
(2) the lithium salt additive is any one or a mixture of at least two of lithium difluorophosphate, lithium difluorobis (oxalato) phosphate, lithium tetrafluoroborate, lithium difluorooxalato borate, lithium bis (oxalato) borate, lithium bis (trifluoromethylsulfonyl) imide and lithium bis (fluorosulfonato) imide;
(3) the non-aqueous solvent is any one or a mixture of at least two of carbonate, carboxylate, ether or amine solvents;
(4) the sulfonate additive is any one or a mixture of at least two of 1, 3-propane sultone, 1, 3-propene sultone and vinyl sulfate.
6. The nonaqueous electrolyte for a lithium battery according to claim 1, wherein the carbonate additive is any one of a linear carbonate additive, a cyclic carbonate additive, and a fluorinated carbonate additive, or a mixture of at least two thereof, and the carbonate additive satisfies at least one of the following conditions (5) to (7):
(5) the straight-chain carbonate additive is any one or a mixture of at least two of methyl ethyl carbonate, dimethyl carbonate and diethyl carbonate;
(6) the cyclic carbonate additive is any one or a mixture of at least two of ethylene carbonate, propylene carbonate, vinylene carbonate and ethylene carbonate;
(7) the fluorinated carbonate additive is one or a mixture of at least two of fluorinated ethylene carbonate, 1, 2-difluoroethylene carbonate, methyl trifluoroethyl carbonate and bis trifluoroethyl carbonate.
7. A lithium ion battery comprising a positive electrode, a negative electrode, a separator between the positive electrode and the negative electrode, and the nonaqueous electrolytic solution for a lithium battery according to any one of claims 1 to 6.
8. The lithium ion battery of claim 7, wherein the positive electrode comprises a positive electrode active material,
the positive electrode active material is selected from any one of lithium iron phosphate, lithium nickel cobalt composite oxide and lithium nickel manganese composite oxide with a spinel structure or a mixture of at least two of the lithium iron phosphate, the lithium nickel cobalt composite oxide and the lithium nickel manganese composite oxide.
9. The lithium ion battery of claim 8, wherein the lithium nickel cobalt complex oxide has a general formula of LixNiyCozMe(1-y-z)OaWherein x in the formula satisfies the condition that x is 1. ltoreq. x.ltoreq.1.2, y and z are positive numbers satisfying the relationship of y + z < 1, the value of y is 0.5 or less, Me is any one or at least two metals selected from Al, Mn, Na, Fe, Cr, Cu, Zn, Ca, K, Mg and Pb, and a satisfies the condition that a is 1.5. ltoreq. a.ltoreq.2.5.
10. The lithium ion battery according to claim 9, wherein the negative electrode comprises a carbon material containing carbon as an element, a silicon material containing silicon as an element, or a carbon-silicon composite material,
the carbon material is any one or a mixture of at least two of acetylene black, conductive carbon black, carbon fiber, carbon nanotube and Ketjen black;
the silicon material is any one or a mixture of at least two of silicon, silicon oxygen compound and silicon-based alloy.
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN114784380A (en) * | 2021-05-28 | 2022-07-22 | 远景动力技术(江苏)有限公司 | Electrolyte, electrochemical device and electronic device thereof |
| CN115020809A (en) * | 2022-06-17 | 2022-09-06 | 远景动力技术(江苏)有限公司 | Electrolyte, electrochemical device and electronic device thereof |
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| CN101981749A (en) * | 2008-04-02 | 2011-02-23 | 宇部兴产株式会社 | Nonaqueous electrolyte for lithium battery and lithium battery using same |
| CN107863558A (en) * | 2017-10-26 | 2018-03-30 | 中国科学院青海盐湖研究所 | Electrolyte and its application for lithium ion battery |
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| CN1961452A (en) * | 2004-05-28 | 2007-05-09 | 宇部兴产株式会社 | Nonaqueous electrolyte solution and lithium secondary battery using same |
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| CN114784380A (en) * | 2021-05-28 | 2022-07-22 | 远景动力技术(江苏)有限公司 | Electrolyte, electrochemical device and electronic device thereof |
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| WO2022247929A1 (en) * | 2021-05-28 | 2022-12-01 | 远景动力技术(江苏)有限公司 | Electrolyte, electrochemical device thereof, and electronic device |
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