CN111883845A - Electrolyte for lithium battery, lithium battery and application of bisborate solvent - Google Patents

Electrolyte for lithium battery, lithium battery and application of bisborate solvent Download PDF

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Publication number
CN111883845A
CN111883845A CN202010881154.1A CN202010881154A CN111883845A CN 111883845 A CN111883845 A CN 111883845A CN 202010881154 A CN202010881154 A CN 202010881154A CN 111883845 A CN111883845 A CN 111883845A
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electrolyte
lithium
lithium battery
solvent
carbonate
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赵生荣
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Hubei Eve Power Co Ltd
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Hubei Eve Power Co Ltd
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    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00Secondary cells; Manufacture thereof
    • H01M10/05Accumulators with non-aqueous electrolyte
    • H01M10/056Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0564Accumulators 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
    • H01M10/0566Liquid materials
    • H01M10/0569Liquid materials characterised by the solvents
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00Secondary cells; Manufacture thereof
    • H01M10/05Accumulators with non-aqueous electrolyte
    • H01M10/052Li-accumulators
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00Secondary cells; Manufacture thereof
    • H01M10/05Accumulators with non-aqueous electrolyte
    • H01M10/056Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0564Accumulators 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
    • H01M10/0566Liquid materials
    • H01M10/0567Liquid materials characterised by the additives
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00Electrolytes
    • H01M2300/0017Non-aqueous electrolytes
    • H01M2300/0025Organic electrolyte
    • H01M2300/0028Organic electrolyte characterised by the solvent
    • H01M2300/0037Mixture of solvents
    • YGENERAL 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
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02EREDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10Energy storage using batteries

Abstract

The invention relates to an electrolyte for a lithium battery, the lithium battery and application of a bisborate solvent. The electrolyte has a wider liquid range, simultaneously considers the high-low temperature performance and the safety performance of the battery, and the prepared lithium battery has excellent cycle life, improves the high-temperature gas production of the battery and the increase of direct-current internal resistance in the cycle process, and improves the safety and the reliability of the battery.

Description

Electrolyte for lithium battery, lithium battery and application of bisborate solvent
Technical Field
The invention relates to the technical field of lithium batteries, in particular to an electrolyte for a lithium battery and application of the lithium battery and a bisborate solvent.
Background
The modern society has increasingly urgent need for high-energy power sources due to the development of mobile communication, digital products, electric tools and electric vehicles. Lithium ion batteries are widely researched as a chemical energy storage system with high energy density, excellent cycle performance and environmental friendliness, and the electrolyte plays a significant role in exerting the application range, safety performance and capacity of the batteries as a bridge for connecting the positive electrode and the negative electrode of the lithium batteries.
The ideal electrolyte should have several characteristics: high ionic conductivity, stability in a wide temperature range, low electronic conductivity, good chemical stability, low cost, nonflammability, good safety, no toxicity, no pollution and the like. The currently commonly used carbonate electrolyte can be oxidized and decomposed when the charge cut-off voltage exceeds 4.2V, so that the battery expands and the internal resistance rises, and the comprehensive performance of the whole battery is reduced. In addition, most of conventional electrolyte solvents are alkyl carbonate compounds, and the flash point of the electrolyte solvents is low, so that the safety and reliability of the electrolyte solvents cannot completely meet the use conditions.
CN111261924A provides an electrolyte for a lithium battery, including lithium salt, organic solvent and functional additive, the functional additive includes a first additive accounting for 0.1% -10% of the total mass of the lithium battery electrolyte, a second additive accounting for 0.1% -2% of the total mass of the lithium battery electrolyte and a third additive accounting for 0.1% -3% of the total mass of the lithium battery electrolyte, the first additive is fluorinated cyclic carbonate and/or fluorinated ether, the second additive is a silane compound, and the third additive is a nitrile compound. In the lithium ion battery with the high-nickel anode material matched with the silicon cathode, the coordination of the fluorinated cyclic carbonate, the fluoroether, the silane and the nitrile in the non-aqueous electrolyte improves the initial capacity, inhibits the increase of internal resistance, and improves the normal-temperature cycle performance and the high-temperature gas expansion. However, the electrolyte of the present invention has a relatively low battery capacity percentage at 25 ℃.
CN103943883A discloses an application of a borate compound as an additive of a high-voltage lithium ion battery electrolyte, and the invention discloses a high-voltage lithium ion battery electrolyte which is obtained by adding a functional additive with the mass equivalent to 0.1-5% of that of a common electrolyte into the common electrolyte. The common electrolyte consists of a cyclic carbonate solvent, a linear carbonate solvent and a conductive lithium salt, and the functional additive is the borate compound. The addition of the additive optimizes the interface of the positive electrode/electrolyte, reduces the surface activity of the positive electrode and inhibits the oxidative decomposition of the electrolyte; on the other hand, the safety of the electrolyte is also improved due to the introduction of boron. The high-voltage lithium ion battery electrolyte can improve the safety performance and the cycle performance of a high-voltage (3-4.9 Vvs. Li/Li +) lithium battery. However, boron element is present as an additive in the electrolyte, and there is a limit to improvement of safety.
In conclusion, it is necessary to develop an electrolyte which has both high and low temperature performance and safety performance.
Disclosure of Invention
The invention provides an electrolyte for a lithium battery, the lithium battery and an application of a bisborate solvent, wherein the electrolyte has a wider liquid range and simultaneously gives consideration to the high-low temperature performance and the safety performance of the battery.
In order to achieve the purpose, the invention adopts the following technical scheme:
an object of the present invention is to provide an electrolyte for a lithium battery, which contains a lithium salt and a solvent, the solvent including a compound represented by formula a:
Figure BDA0002654157560000021
in the formula A, R is1、R2And R3Each independently selected from C1-C10 (e.g., C1, C2, C3, C4, C5, C6, C7, C8, C9, etc.) alkylene or C2-C10 (e.g., C2, C3, C4, C5, C6, C7, C8, C9, etc.) alkenylene.
The solvent shown in formula A is added into the electrolyte, and the solvent is a borate compound with a bicyclic structure. The boric acid ester compound with a bicyclic structure has a higher boiling point than that of the conventional carbonic ester>160 ℃ and lower melting point: (<-40 ℃) and exhibits good chemical stability to the decomposition of the positive electrode and, at room temperature, a strong electrical conductivity (10 ℃)-3~10-2S/cm). Oxidation potential of the electrolyte when mixed with a portion of the carbonate (e.g., ethylene carbonate)>5.8V(vsLi/Li+). Therefore, the liquid process of the solvent A is wider, and the high-temperature and low-temperature performance of the lithium battery is promoted; secondly, the solvent has better stability in a high-voltage system, and the safety and reliability of the lithium battery are improved; meanwhile, compared with other solvents, the solvent is low in viscosity and good in fluidity, pole pieces and diaphragms are easy to infiltrate, the alternating current internal resistance and the direct current internal resistance of the lithium battery are reduced, and the power performance and the cycle performance of the battery are improved.
Preferably, said R is1、R2And R3Each independently selected from-CH2-、-CH=CH-、-CH2CH2-、-CH(CH3)-、-CH2CH2CH2-、-C(CH3)2-or-C (═ CH)2) Any one of the above-mentioned. The short straight lines at both ends of the aforementioned group represent the connecting bonds.
Preferably, the solvent comprises any one or a combination of at least two of the compounds represented by formula a1 to formula A3:
Figure BDA0002654157560000031
the three compounds with specific structures are preferably used as solvents, and the compounds are all boric acid ester compounds with bicyclic structures, so that the high-low temperature performance, the stability and the cycle life of the lithium battery can be further improved.
Preferably, the solvent further includes any one or at least two combinations of Ethylene Carbonate (EC), diethyl carbonate (DEC), Ethyl Methyl Carbonate (EMC), dimethyl carbonate (DMC), Propylene Carbonate (PC), dipropyl carbonate (DPC), γ -butyrolactone (GBL), 1, 3-Dioxolane (DOL), dimethyl ether (DME), methyl hexanoate (MA), Methyl Propionate (MP), dimethyl sulfone, diethyl sulfone, and Tetrahydrofuran (THF).
Preferably, the solvent accounts for 60 wt% to 92 wt% of the total mass of the electrolyte, such as 62 wt%, 64 wt%, 66 wt%, 68 wt%, 70 wt%, 72 wt%, 74 wt%, 76 wt%, 78 wt%, 80 wt%, 82 wt%, 84 wt%, 86 wt%, 88 wt%, 90 wt%, etc.
Preferably, the compound represented by formula A accounts for 2 wt% to 65 wt%, such as 5 wt%, 10 wt%, 15 wt%, 20 wt%, 25 wt%, 30 wt%, 35 wt%, 40 wt%, 45 wt%, 50 wt%, 55 wt%, 60 wt%, etc., of the total mass of the electrolyte.
The addition amount of the solvent of formula A is preferably 2-65 wt%, and in the range, the optimal high and low temperature performance, stability and cycle life can be obtained. The addition amount is too low, so that the liquid process of an electrolyte system can not meet the use condition, and the advantage of the solvent can not be exerted; when the amount of the additive is too high, the lithium salt concentration is insufficient, and the ionic conductivity and conductivity of the electrolyte are reduced, which deteriorates the performance of the lithium battery.
Preferably, the first and second electrodes are formed of a metal,the lithium salt includes lithium hexafluorophosphate (LiPF)6) Lithium hexafluoroarsenate (LiAsF)6) Lithium perchlorate (LiClO)4) Lithium bis (trifluoromethanesulfonate imide) (LiN (SO)2CF3)2) Lithium trifluoromethanesulfonate (LiCF)3SO3) Lithium tetrafluoroborate (LiBF)4) Lithium bis (fluorooxalato) borate (LiBF)2C2O4) Lithium bis (oxalato) borate (LiB (C)2O4)2) Or lithium bis (fluorosulfonylimide) (LiN (SO)2F)2Any one or a combination of at least two of them.
Preferably, the lithium salt accounts for 5 wt% to 30 wt%, such as 10 wt%, 15 wt%, 20 wt%, 25 wt%, etc., of the total mass of the electrolyte.
Preferably, the electrolyte further comprises an additive.
Preferably, the additive includes lithium fluoride (LiF), Fluorinated Ethylene Carbonate (FEC), Vinylene Carbonate (VC), Propylene Sulfite (PS), 1, 4-Butanesultone (BS), 1,3- (1-Propene) Sultone (PST), vinyl sulfite (ES), ethylene sulfate (DTD), ethylene sulfite, Biphenyl (BP), Cyclohexylbenzene (CHP), tetracyanoethylene, sulfur dioxide (SO)2) Carbon disulfide (CS)2) Boron trioxide (B)2O3) Any one or at least two of trimethyl phosphate (TMP) and triethyl phosphate (TEP).
Preferably, the additive comprises 0.5 wt% to 10 wt% of the total mass of the electrolyte, such as 1 wt%, 1.5 wt%, 2 wt%, 2.5 wt%, 3 wt%, 3.5 wt%, 4 wt%, 4.5 wt%, 5 wt%, 5.5 wt%, 6 wt%, 6.5 wt%, 6 wt%, 7.5 wt%, 8 wt%, 8.5 wt%, 9 wt%, 9.5 wt%, etc.
The second object of the present invention is to provide a lithium battery comprising a positive electrode, a negative electrode, a separator, a structural member and the electrolyte for a lithium battery according to the first object.
The lithium battery provided by the invention has excellent cycle life, improves the high-temperature gas production of the battery and the increase of direct-current internal resistance in the cycle process, and improves the safety and reliability of the battery.
The invention also aims to provide an application of a bisborate solvent in a battery electrolyte, wherein the bisborate solvent comprises a compound shown as a formula A;
Figure BDA0002654157560000051
in the formula A, R is1、R2And R3Each independently selected from C1 to C10 alkylene or C2 to C10 alkenylene. That is, the compound represented by a provided by the present application is not limited to be used in lithium battery electrolytes, but may also have potential to be used in non-lithium battery electrolytes. It should be noted that the solvent of the bisborate ester is only a transitional word, and the nature thereof is also the compound shown in the formula A. The specific form of the compound shown in the formula a is suitable for the content described in one of the purposes, and is not described herein again.
Compared with the prior art, the invention has the following beneficial effects:
according to the invention, a new solvent A is added into the lithium battery electrolyte, and the solvent A has a wider liquid process, so that the high-temperature and low-temperature performance of the lithium battery can be improved; secondly, the solvent has better stability in a high-voltage system, and the safety and reliability of the lithium battery are improved; meanwhile, compared with other solvents, the solvent is low in viscosity and good in fluidity, pole pieces and diaphragms are easy to infiltrate, the alternating current internal resistance and the direct current internal resistance of the lithium battery are reduced, and the power performance and the cycle performance of the battery are improved.
The lithium battery prepared by the electrolyte has high-low temperature capacity retention rate and overcharge failure voltage, excellent thermal shock resistance and high safety, wherein the high-temperature (45 ℃) capacity retention rate is 97-104%, most of the capacity retention rate is more than 100%, the low-temperature (-20 ℃) capacity retention rate is 86-93%, most of the capacity retention rate is more than 90%, the overshoot failure voltage is 5.0-5.9V, most of the overshoot failure voltage is more than 5.5V, and the lithium battery does not open a valve, does not ignite and does not explode under the condition of 30min at 130 ℃.
Detailed Description
The technical solution of the present invention is further explained by the following embodiments. It should be understood by those skilled in the art that the examples are only for the understanding of the present invention and should not be construed as the specific limitations of the present invention.
The following examples and comparative examples each provide a lithium battery whose electrolyte composition is specified in table 1, and information on the compositions of the positive electrode, the negative electrode, and the separator is specified in table 2.
TABLE 1
Figure BDA0002654157560000061
Figure BDA0002654157560000071
In table 1, the percentages represent the percentages of the respective components in the total mass of the electrolyte;
in table 1, the structure of D1 is as follows:
Figure BDA0002654157560000072
TABLE 2
Figure BDA0002654157560000073
Figure BDA0002654157560000081
In the anode formula, the numbers represent the mass ratio of different anode materials, and the anode formula is the same.
The materials and sources for the english abbreviations referred to in table 2 are shown in table 3:
TABLE 3
Figure BDA0002654157560000082
Figure BDA0002654157560000091
Performance testing
For the lithium batteries of the above examples and comparative examples, the following performance tests were performed:
(1) high and low temperature capacity retention rate test: the test is carried out according to GB/T31486-2015, and the low-temperature capacity retention rate is not lower than 70% of the initial capacity; the high-temperature capacity retention ratio is not less than 90% of the initial capacity.
(2) And (3) testing the overshoot failure voltage: the test was carried out with reference to GB 38031-2020.
(3) And (3) thermal shock test: the test was carried out with reference to GB 38031-2020.
The above test results are shown in table 4:
TABLE 4
Figure BDA0002654157560000092
As can be seen from Table 1, the lithium battery prepared by the electrolyte has high and low temperature retention rate and overshoot failure voltage, and has excellent thermal shock performance and high safety, wherein the high temperature (45 ℃) capacity retention rate is 97-104%, most of the capacity retention rate is more than 100%, the low temperature (-20 ℃) capacity retention rate is 86-93%, most of the capacity retention rate is more than 90%, the overshoot failure voltage is 5.0-5.9V, most of the capacity retention rate is more than 5.5V, and the lithium battery does not open a valve, does not ignite and does not explode under the condition of 30min at 130 ℃.
It is understood from comparative examples 1 and 6 to 9 that when the ratio of the solvent of the formula A is in the range of 2 wt% to 65 wt% (examples 1 and 6 to 7), the high/low temperature capacity retention ratio and the overshoot failure voltage can be further improved, and that the effect is deteriorated when the ratio is too low or too high.
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. An electrolyte for a lithium battery, comprising a lithium salt and a solvent, wherein the solvent comprises a compound represented by formula a:
Figure FDA0002654157550000011
in the formula A, R is1、R2And R3Each independently selected from C1 to C10 alkylene or C2 to C10 alkenylene.
2. The electrolyte for lithium battery according to claim 1, wherein R is1、R2And R3Each independently selected from-CH2-、-CH=CH-、-CH2CH2-、-CH(CH3)-、-CH2CH2CH2-、-C(CH3)2-or-C (═ CH)2) Any one of the above-mentioned.
3. The electrolyte for a lithium battery according to claim 1 or 2, wherein the solvent comprises any one or at least two combinations of compounds represented by formula a1 to formula A3:
Figure FDA0002654157550000012
4. the electrolyte for a lithium battery according to any one of claims 1 to 3, wherein the solvent further comprises any one or a combination of at least two of ethylene carbonate, diethyl carbonate, ethyl methyl carbonate, dimethyl carbonate, propylene carbonate, dipropyl carbonate, γ -butyrolactone, 1, 3-dioxolane, dimethyl ether, methyl hexanoate, methyl propionate, dimethyl sulfone, diethyl sulfone, or tetrahydrofuran.
5. The electrolyte for a lithium battery according to any one of claims 1 to 4, wherein the solvent accounts for 60 to 92 wt% of the total mass of the electrolyte;
preferably, the compound shown in the formula A accounts for 2-65 wt% of the total mass of the electrolyte.
6. The electrolyte for a lithium battery according to any one of claims 1 to 5, wherein the lithium salt comprises any one or a combination of at least two of lithium hexafluorophosphate, lithium hexafluoroarsenate, lithium perchlorate, lithium bis (trifluoromethylsulfonyl) imide, lithium trifluoromethylsulfonate, lithium tetrafluoroborate, lithium difluorooxalato borate, lithium dioxaoxalato borate, or lithium difluorosulfonylimide.
7. The electrolyte for a lithium battery according to any one of claims 1 to 6, wherein the lithium salt accounts for 5 to 30 wt% of the total mass of the electrolyte.
8. The electrolyte for a lithium battery according to any one of claims 1 to 7, further comprising an additive;
preferably, the additive comprises any one or at least two of lithium fluoride, fluorinated ethylene carbonate, vinylene carbonate, propylene sulfite, 1, 4-butanesultone, 1,3- (1-propylene) sultone, ethylene sulfite, ethylene sulfate, ethylene sulfite, biphenyl, cyclohexylbenzene, tetracyanoethylene, sulfur dioxide, carbon disulfide, diboron trioxide, trimethyl phosphate or triethyl phosphate;
preferably, the additive accounts for 0.5 wt% -10 wt% of the total mass of the electrolyte.
9. A lithium battery comprising a positive electrode, a negative electrode, a separator, a structural member, and the electrolyte for a lithium battery as claimed in any one of claims 1 to 8.
10. The application of the dicarboxylic acid ester solvent in the battery electrolyte is characterized in that the dicarboxylic acid ester solvent comprises a compound shown as a formula A;
Figure FDA0002654157550000021
in the formula A, R is1、R2And R3Each independently selected from C1 to C10 alkylene or C2 to C10 alkenylene.
CN202010881154.1A 2020-08-27 2020-08-27 Electrolyte for lithium battery, lithium battery and application of bisborate solvent Pending CN111883845A (en)

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Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO1997016862A1 (en) * 1995-11-03 1997-05-09 Arizona Board Of Regents Wide electrochemical window solvents for use in electrochemical devices and electrolyte solutions incorporating such solvents
JPH113728A (en) * 1997-04-17 1999-01-06 Fuji Photo Film Co Ltd Nonaqueous electrolyte secondary battery
JP2001229730A (en) * 2000-02-21 2001-08-24 Showa Denko Kk Electrolyte material and its use
JP2005222830A (en) * 2004-02-06 2005-08-18 Sony Corp Liquid electrolyte and battery
CN103346351A (en) * 2013-06-28 2013-10-09 国家电网公司 Novel borate solvent for lithium-ion secondary battery
CN108112276A (en) * 2015-06-22 2018-06-01 野猫技术开发公司 For the electrolyte preparations of lithium ion battery

Patent Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO1997016862A1 (en) * 1995-11-03 1997-05-09 Arizona Board Of Regents Wide electrochemical window solvents for use in electrochemical devices and electrolyte solutions incorporating such solvents
JPH113728A (en) * 1997-04-17 1999-01-06 Fuji Photo Film Co Ltd Nonaqueous electrolyte secondary battery
JP2001229730A (en) * 2000-02-21 2001-08-24 Showa Denko Kk Electrolyte material and its use
JP2005222830A (en) * 2004-02-06 2005-08-18 Sony Corp Liquid electrolyte and battery
CN103346351A (en) * 2013-06-28 2013-10-09 国家电网公司 Novel borate solvent for lithium-ion secondary battery
CN108112276A (en) * 2015-06-22 2018-06-01 野猫技术开发公司 For the electrolyte preparations of lithium ion battery

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