CN102324568A - Electrolyte solution for improving swelling of lithium ion battery - Google Patents
Electrolyte solution for improving swelling of lithium ion battery Download PDFInfo
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- CN102324568A CN102324568A CN201110273215A CN201110273215A CN102324568A CN 102324568 A CN102324568 A CN 102324568A CN 201110273215 A CN201110273215 A CN 201110273215A CN 201110273215 A CN201110273215 A CN 201110273215A CN 102324568 A CN102324568 A CN 102324568A
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- carbonate
- ester
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Abstract
The invention relates to electrolyte solution which can improve the swelling of a lithium ion battery; the electrolyte solution for improving the swelling of the lithium ion battery comprises three types of components: (1) lithium salt; (2) composite organic solvent of carbonate ester and cyclic lactone compounds; and (3) composite additive; the molar concentration of lithium salt in the electrolyte solution is 0.01 to 2 mol/L; the mass percentage of the composite additive in the electrolyte solution is 0.01 percent to 5 percents; in the lithium salt, one or more of the following substances coexist: LiBF4, LiN (CF3SO2) 2, LiC4F9SO3, LiN (CxF2x+1SO2) (CyF2y+1SO2) (x and y are natural numbers), LiB (C2O4) 2 or LiBF2C2O4. According to the invention, through the composition design of the electrolyte solution and the comprehensive application of composite organic solvent of carbonate ester and cyclic lactone compounds and the composite additive, the reactivity with a high nickel positive pole material is reduced, the swelling problem of a secondary lithium ion battery based on the high nickel positive pole material when in high-temperature storage is greatly solved, and the electrochemical properties of the lithium ion battery can be well displayed.
Description
Technical field
The present invention relates to a kind of electrolyte solution, a kind of specifically electrolyte solution that improves the lithium ion battery air-blowing.
Background technology
Lithium ion battery be at present ideal in the world also be the highest chargeable chemical cell of technology, compare with other batteries, lithium ion battery each item performance is more outstanding.The chemical property of lithium ion battery depends primarily on used electrode material structure and performance, and electrolyte material be guarantee electrode material play superiority can bridge.Positive electrode always is the emphasis that people research and develop as the critical material of lithium ion battery electrode material, and the performance that improves positive electrode is to improve the key of lithium ion battery performance.The performance that improves positive electrode specifically can show as two aspects: the one, and the every raising 50% of the capacity of positive electrode, the power density of battery will improve 28%; Another is the shared cost difference of each several part material in the battery, and positive electrode occupies the cost greater than 40%.Ternary or polynary positive pole material comprehensive three kinds or multiple positive electrode are avoided defective to reach optimum serviceability through synergy.Ternary or polynary positive pole material are the new type lithium ion battery positive electrodes that grows up recent years; Have excellent specific properties such as high power capacity, cost is low, fail safe is good; In small-scale lithium ion cell, progressively occupied certain market share, and bright development prospect has also been arranged in the power lithium-ion battery field.But tertiary cathode material is applied in the problem that there is air-blowing in lithium ion battery; Especially in the nickelic tertiary cathode material system; More active owing to nickel element in the charged storing process of high temperature; Be prone to cause this lithium ion battery air-blowing, cause the internal resistance of cell sharply to increase simultaneously and make the charge-discharge performance of battery descend with the electrolyte generated reactive gas.
Summary of the invention
Technical problem to be solved by this invention is; Shortcoming to above prior art existence; A kind of electrolyte solution that improves the lithium ion battery air-blowing is proposed; Can reduce the reactivity of electrolyte solution and nickelic positive electrode, thereby suppress the air-blowing of nickelic positive electrode lithium ion battery, guarantee the superior performance of chemical property of this lithium ion battery.
The technical scheme that the present invention solves above technical problem is:
A kind of electrolyte solution that improves the lithium ion battery air-blowing is made up of three types of compositions: ⑴ lithium salts, the compounded organic solvent of ⑵ carbonats compound and annular lactone compound, ⑶ compound additive; The molar concentration of lithium salts in this electrolyte solution is 0.01～2 mol; Compound additive shared mass percent in this electrolyte solution is 0.01%～5%; Lithium salts is one or more coexistences in the following material: LiBF
4, LiN (CF
3SO
2)
2, LiC
4F
9SO
3,, LiN (C
xF
2x+1SO
2) (CyF
2y+1SO2) (x and y are natural number in the formula), LiB (C
2O
4)
2Or LiBF
2C
2O
4
The present invention selects the compounded organic solvent system for use, and carbonats compound wherein can guarantee that electrolyte has enough conductivity and suitable viscosity; And the annular lactone compound can form diaphragm on the positive pole surface, thereby stops nickel and the air-blowing of electrolyte reaction inhibition battery in the positive electrode; Carbonats compound and annular lactone compound are used the oxidation resistance that can improve electrolyte system.
The technical scheme that the present invention further limits is:
The aforesaid electrolyte solution that improves the lithium ion battery air-blowing, in the compounded organic solvent, the percentage by weight that carbonats compound accounts for compounded organic solvent is 30～70%, the percentage by weight that the annular lactone compound accounts for compounded organic solvent is 30～70%.
The aforesaid electrolyte solution that improves the lithium ion battery air-blowing, carbonats compound are that the cyclic carbonate compounds is or/and the linear carbonate compounds; The cyclic carbonate compounds is selected from one or more coexistences in ethylene carbonate, propene carbonate, the butylene; The linear carbonate compounds is selected from one or more coexistences in ethyl butyl carbonate, carbonic acid first butyl ester, dibutyl carbonate, diethyl carbonate, dimethyl carbonate, trifluoromethyl ethylene carbonate, carbonic acid di-n-propyl ester, carbonic acid diisopropyl ester, methyl ethyl carbonate, ethyl propyl carbonic acid ester, the carbonic acid first propyl ester.
The aforesaid electrolyte solution that improves the lithium ion battery air-blowing, the structural formula of annular lactone compound is:
Wherein n is the integer of 0-5.
The aforesaid electrolyte solution that improves the lithium ion battery air-blowing; Compound additive is by at least two kinds of coexistences in the following compounds: vinylene carbonate, ethylene thiazolinyl vinyl acetate, single fluorine ethylene carbonate, two fluorine ethylene carbonate, methylene vinyl carbonic ester 1; 3-propane sultone, 1; 4-butyl sulfonic acid lactone, ethylene sulfite, sulfonic acid vinyl acetate, sulfuric acid vinyl ester, two-(trifluoromethyl sulfonyl) imines lithium, phthalic anhydride, propylene sulfite, 1,3-propene sulfonic acid lactone, 4-methyl ethylene sulfite, methane-disulfonic acid methylene ester, succinonitrile.The selection of compound additive of the present invention is the high-temperature behavior that can improve negative material.
The aforesaid electrolyte solution that improves the lithium ion battery air-blowing is used for nickelic positive electrode lithium ion battery, and the chemical formula of nickelic positive electrode is Li
aNi
bCo
cM
dO
2, wherein M is selected from a kind of among Al, Mn, the Mg, 0.2≤a≤1.2,0.5≤b≤0.9,0.1≤c≤0.4,0≤d≤0.2, b+c+d=1.
The invention has the beneficial effects as follows: the present invention is through the composition design of electrolyte; Adopt the integrated use of carbonates and annular lactone compound compounded organic solvent and compound additive; Reduce the reactivity of itself and nickelic positive electrode; Air-blowing problem in the time of can significantly reducing the high temperature storage of nickelic positive electrode lithium rechargeable battery is with the superior performance of the chemical property that guarantees this lithium ion battery.
Embodiment
Embodiment 1
The 503048 square aluminum housing batteries of preparation 750mAh, wherein anode is Li
1.05Ni
0.8Co
0.17Al
0.03O
2, negative pole is a Delanium, barrier film is polypropylene (PP)/polyethylene (PE)/polypropylene (PP); Pour into different electrolyte respectively, after it is stored 85 degree 4 hours respectively and spends 30 days with 60, test its varied in thickness.Varied in thickness requires to be no more than 5% after high temperature storage.
Present embodiment specifically sees the following form:
| ? | Test electrolyte | 4 hours varied in thickness of 85 degree storages | 30 days varied in thickness of 60 degree storages |
| Embodiment 1-1 | 1M LiBF 4? EC-EMC（30/70,v/v），VC（1wt%）+PS（2wt%）+SN（1wt%） | 13.1% | 14.7% |
| Embodiment 1-2 | 1M LiBF 4? EC-EMC-GBL（30/40/30, v/v），VC（1wt%）+PS（2wt%）+SN（1wt%） | 4.3% | 4.5% |
| Embodiment 1-3 | 1M LiBF 4? EC-EMC-GBL（30/30/40, v/v），VC（1wt%）+PS（2wt%）+SN（1wt%） | 3.8% | 4.1% |
| Embodiment 1-4 | 1M LiBF 4? EC-EMC-GBL（30/20/50, v/v），VC（1wt%）+PS（2wt%）+SN（1wt%） | 2.5% | 2.6% |
| Embodiment 1-5 | 1M LiBF 4? EC-PC-GBL（30/5/65, v/v），VC（1wt%）+PS（2wt%）+SN（1wt%） | 2.7% | 3.1% |
Wherein EC represents ethylene carbonate, and PC represents propene carbonate, and EMC represents methyl ethyl carbonate, and GBL represents butyrolactone, and VC represents vinylene carbonate, and PS represents 1,3 propane sultone, and SN represents succinonitrile;
1M represents the molar concentration of salt, and unit is every liter of a mole.
From experimental data, through introducing butyrolactone (GBL) solvent and VC, PS and SN compound additive, battery respectively stored under the 85 degree conditions spent 30 days with 60 in 4 hours after, the battery bulging is effectively suppressed, varied in thickness is all in 5%.And discovery is along with the effect of the increase inhibition battery bulging of GBL consumption is more obvious.
Embodiment 2
The 523550 Soft Roll lithium ion batteries of preparation 1000mAh, wherein anode is Li
1.05Ni
0.8Co
0.17Al
0.03O
2, negative pole is a Delanium, barrier film is polypropylene (PP)/polyethylene (PE)/polypropylene (PP); Pour into different electrolyte respectively, after it is stored 85 degree 4 hours respectively and spends 30 days with 60, test its varied in thickness.Varied in thickness requires to be no more than 10% after high temperature storage.
Present embodiment specifically sees the following form:
| ? | Electrolyte | 4 hours varied in thickness of 85 degree storages | 30 days varied in thickness of 60 degree storages |
| Embodiment 2-1 | 1M LiBF4? EC-EMC-GBL（30/20/50,v/v），VC（1.5wt%） | 23.1% | 24.7% |
| Embodiment 2-2 | 1M LiBF4? EC-EMC-GBL（30/20/50,v/v），VC（1.5wt%）+PS（1.5wt%） | 8.3% | 8.5% |
| Embodiment 2-3 | 1M LiBF4? EC-EMC-GBL（30/20/50,v/v），VC（1.5wt%）+SN（1wt%） | 6.8% | 7.1% |
| Embodiment 2-4 | 1M LiBF4? EC-EMC-GBL（30/20/50,v/v），VC（1wt%）+PS（1wt%）+SN（1wt%） | 5.5% | 5.7% |
| Embodiment 2-5 | 1M LiBF4? EC-EMC-GBL（30/20/50,v/v），VC（1wt%）+PS（2wt%）+SN（1wt%） | 4.6% | 5.1% |
Wherein EC represents ethylene carbonate, and PC represents propene carbonate, and EMC represents methyl ethyl carbonate, and GBL represents butyrolactone, and VC represents vinylene carbonate, and PS represents 1,3 propane sultone, and SN represents succinonitrile; 1M represents the molar concentration of salt, and unit is every liter of a mole.
Can find out from above-mentioned experimental data, VC, the use of PS and SN compound additive can significantly suppress the bulging of battery high-temperature storage.
Embodiment 3
The 523550 Soft Roll lithium ion batteries of preparation 1000mAh, wherein anode is Li
1.05Ni
0.8Co
0.17Al
0.03O
2, negative pole is a Delanium, barrier film is polypropylene (PP)/polyethylene (PE)/polypropylene (PP); Experimental result according to embodiment 2; Selected ethylene carbonate (EC)-methyl ethyl carbonate (EMC)-butyrolactone (GBL) (30/20/50 for use; V/v) dicyandiamide solution and vinylene carbonate (VC) are (1wt%)+1; 3 propane sultones (PS) (2wt%)+succinonitrile (SN) is a compound additive (1wt%), selects LiB (C for use
2O
4)
2Salt injects mesuring battary with its electrolyte, has tested the varied in thickness after the battery high-temperature storage (85 degree 4 hours).
Present embodiment specifically sees the following form:
| ? | Electrolyte | 4 hours varied in thickness of 85 degree storages |
| Embodiment 3-1 | 0.7M LiB(C 2O 4) 2? EC-EMC-GBL（30/20/50,v/v），VC（1.5wt%） | 5.3% |
Wherein EC represents ethylene carbonate, and EMC represents methyl ethyl carbonate, and GBL represents butyrolactone, and VC represents vinylene carbonate, and 0.7M represents the molar concentration of salt, and unit is every liter of a mole.
Experimental result shows that its varied in thickness is 5.3%, satisfies 4 hours varied in thickness of actual instructions for use 85 degree of client and is lower than 10%.
Embodiment 4
The 523550 Soft Roll lithium ion batteries of preparation 1000mAh, wherein anode is Li
1.05Ni
0.8Co
0.17Al
0.03O
2, negative pole is a Delanium, barrier film is polypropylene (PP)/polyethylene (PE)/polypropylene (PP); Pour into different electrolyte respectively, it is stored 85 degree 4 hours respectively, test its varied in thickness.Varied in thickness requires to be no more than 10% after high temperature storage.
Present embodiment specifically sees the following form:
| ? | Electrolyte | 4 hours varied in thickness of 85 degree storages | The battery capacity retention rate that the normal temperature circulation is 100 times |
| Embodiment 4-1 | 1M LiBF4? EC-EMC-GBL（30/20/50,v/v），VC（1wt%）+PS（2wt%）+SN（1wt%） | 4.6% | 98.1% |
| Embodiment 4-2 | 1M LiBF4? EC-EMC-VL（30/20/50,v/v），VC（1.5wt%）+PS（1.5wt%） | 4.2% | 94.2% |
| Embodiment 4-3 | 1M LiBF4? EC-EMC-HL（30/20/50,v/v），VC（1.5wt%）+PS（1.5wt%） | 4.1% | 93.4% |
Wherein EC represents ethylene carbonate, and EMC represents methyl ethyl carbonate, and GBL represents butyrolactone, and VC represents vinylene carbonate, and PS represents 1,3 propane sultone, and 1M represents the molar concentration of salt, and unit is every liter of a mole.
From above-mentioned experimental data; Bulging when solvent valerolactone (VL), caprolactone (HL) equally can suppress the battery high-temperature storage significantly with solvent butyrolactone (GBL); But because along with the increase viscosity of carbon atom in the lactonic ring increases thereupon, the cycle performance of battery there is slight negative effect.
Except that the foregoing description, the present invention can also have other execution modes.All employings are equal to the technical scheme of replacement or equivalent transformation formation, all drop on the protection range of requirement of the present invention.
Claims (6)
1. electrolyte solution that improves the lithium ion battery air-blowing, it is characterized in that: said electrolyte solution is made up of three types of compositions: ⑴ lithium salts, the compounded organic solvent of ⑵ carbonats compound and annular lactone compound, ⑶ compound additive; The molar concentration of said lithium salts in this electrolyte solution is 0.01～2 mol; Said compound additive shared mass percent in this electrolyte solution is 0.01%～5%; Said lithium salts is one or more coexistences in the following material: LiBF
4, LiN (CF
3SO
2)
2, LiC
4F
9SO
3,, LiN (C
xF
2x+1SO
2) (CyF
2y+1SO2) (x and y are natural number in the formula), LiB (C
2O
4)
2Or LiBF
2C
2O
4
2. the electrolyte solution that improves the lithium ion battery air-blowing as claimed in claim 1; It is characterized in that: in the said compounded organic solvent; The percentage by weight that said carbonats compound accounts for said compounded organic solvent is 30～70%, and the percentage by weight that said annular lactone compound accounts for said compounded organic solvent is 30～70%.
3. according to claim 1 or claim 2 the electrolyte solution that improves the lithium ion battery air-blowing, it is characterized in that: said carbonats compound is that the cyclic carbonate compounds is or/and the linear carbonate compounds; Said cyclic carbonate compounds is selected from one or more coexistences in ethylene carbonate, propene carbonate, the butylene; Said linear carbonate compounds is selected from one or more coexistences in ethyl butyl carbonate, carbonic acid first butyl ester, dibutyl carbonate, diethyl carbonate, dimethyl carbonate, trifluoromethyl ethylene carbonate, carbonic acid di-n-propyl ester, carbonic acid diisopropyl ester, methyl ethyl carbonate, ethyl propyl carbonic acid ester, the carbonic acid first propyl ester.
4. according to claim 1 or claim 2 the electrolyte solution that improves the lithium ion battery air-blowing, it is characterized in that: the structural formula of said annular lactone compound is:
Wherein n is the integer of 0-5.
5. according to claim 1 or claim 2 the electrolyte solution that improves the lithium ion battery air-blowing; It is characterized in that: said compound additive is by at least two kinds of coexistences in the following compounds: vinylene carbonate, ethylene thiazolinyl vinyl acetate, single fluorine ethylene carbonate, two fluorine ethylene carbonate, methylene vinyl carbonic ester 1; 3-propane sultone, 1; 4-butyl sulfonic acid lactone, ethylene sulfite, sulfonic acid vinyl acetate, sulfuric acid vinyl ester, two-(trifluoromethyl sulfonyl) imines lithium, phthalic anhydride, propylene sulfite, 1,3-propene sulfonic acid lactone, 4-methyl ethylene sulfite, methane-disulfonic acid methylene ester, succinonitrile.
6. according to claim 1 or claim 2 the electrolyte solution that improves the lithium ion battery air-blowing, it is characterized in that: be used for nickelic positive electrode lithium ion battery, the chemical formula of said nickelic positive electrode is Li
aNi
bCo
cM
dO
2, wherein M is selected from a kind of among Al, Mn, the Mg, 0.2≤a≤1.2,0.5≤b≤0.9,0.1≤c≤0.4,0≤d≤0.2, b+c+d=1.
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|---|---|---|---|
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| CN102637894A (en) * | 2012-04-06 | 2012-08-15 | 宁德新能源科技有限公司 | Secondary battery with non-aqueous electrolyte |
| CN103000944A (en) * | 2012-12-03 | 2013-03-27 | 湖州创亚动力电池材料有限公司 | Lithium ion battery electrolyte with high-temperature and low-temperature properties |
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| CN103985905A (en) * | 2014-05-30 | 2014-08-13 | 厦门大学 | Electrolyte adopting propylene carbonate as main solvent |
| CN104112869A (en) * | 2013-04-19 | 2014-10-22 | 南通力合新能源有限公司 | Nonaqueous electrolyte additive capable of improving high-temperature impedance performance of manganese-contained lithium ion battery |
| CN105186032A (en) * | 2015-10-19 | 2015-12-23 | 东莞市凯欣电池材料有限公司 | High-voltage lithium-ion battery electrolyte and lithium-ion battery using high-voltage lithium-ion battery electrolyte |
| WO2016095116A1 (en) * | 2014-12-17 | 2016-06-23 | Basf Corporation | Electrolyte compositions for rechargeable lithium ion batteries |
| CN106340674A (en) * | 2016-11-29 | 2017-01-18 | 河南省法恩莱特新能源科技有限公司 | Electrolyte for ternary overcharge battery |
| CN106410276A (en) * | 2016-09-21 | 2017-02-15 | 珠海光宇电池有限公司 | Non-aqueous electrolyte and lithium ion battery comprising non-aqueous electrolyte |
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| CN104112869A (en) * | 2013-04-19 | 2014-10-22 | 南通力合新能源有限公司 | Nonaqueous electrolyte additive capable of improving high-temperature impedance performance of manganese-contained lithium ion battery |
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| WO2016095116A1 (en) * | 2014-12-17 | 2016-06-23 | Basf Corporation | Electrolyte compositions for rechargeable lithium ion batteries |
| CN105186032A (en) * | 2015-10-19 | 2015-12-23 | 东莞市凯欣电池材料有限公司 | High-voltage lithium-ion battery electrolyte and lithium-ion battery using high-voltage lithium-ion battery electrolyte |
| US11637322B2 (en) | 2016-02-12 | 2023-04-25 | Samsung Sdi Co., Ltd. | Lithium battery |
| US11335952B2 (en) | 2016-02-12 | 2022-05-17 | Samsung Sdi Co., Ltd. | Lithium battery |
| US11264644B2 (en) | 2016-02-12 | 2022-03-01 | Samsung Sdi Co., Ltd. | Lithium battery |
| US11251432B2 (en) | 2016-02-12 | 2022-02-15 | Samsung Sdi Co., Ltd. | Lithium battery |
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| CN113540570B (en) * | 2021-09-16 | 2021-12-10 | 北京壹金新能源科技有限公司 | Electrolyte, preparation method and lithium ion battery comprising electrolyte |
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