CN115036571A - Electrolyte and lithium ion battery - Google Patents

Electrolyte and lithium ion battery Download PDF

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Publication number
CN115036571A
CN115036571A CN202110252866.1A CN202110252866A CN115036571A CN 115036571 A CN115036571 A CN 115036571A CN 202110252866 A CN202110252866 A CN 202110252866A CN 115036571 A CN115036571 A CN 115036571A
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electrolyte
carbonate
substituted
additive
ion battery
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孙操
蔡伟
钱家辉
甘朝伦
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Zhangjiagang Guotai Huarong New Chemical Materials Co Ltd
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Zhangjiagang Guotai Huarong New Chemical Materials Co Ltd
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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
    • 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
    • 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
    • H01M10/0569—Liquid materials characterised by the solvents
    • 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
    • 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

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Physics & Mathematics (AREA)
  • Condensed Matter Physics & Semiconductors (AREA)
  • General Physics & Mathematics (AREA)
  • Inorganic Chemistry (AREA)
  • Materials Engineering (AREA)
  • Secondary Cells (AREA)

Abstract

The invention relates to an electrolyte and a lithium ion battery, and mainly solves the technical problem of poor wettability of the electrolyte in a high-energy density system. The invention better solves the problem through the synergistic action of the carboxylic ester solvent and various additives, improves the electrolyte wettability in the lithium ion battery of a high-energy density system, and has better rate discharge performance and quick charge cycle performance.

Description

Electrolyte and lithium ion battery
Technical Field
The invention relates to the technical field of batteries, in particular to an electrolyte and a lithium ion battery.
Background
Due to rapid development of modern socioeconomic and science and technology, the performance of the traditional lithium ion battery can not meet the current energy requirement. For example, in the fields of rapidly developing electric vehicles, intelligent consumer electronics, and the like, lithium ion batteries with higher energy density, long cycle, long service life, low cost, and high safety are urgently needed, and accordingly, the requirements for the positive and negative electrode materials and electrolyte performance of the batteries are increasingly high.
In terms of the electrical core layer, the rate performance of the lithium ion battery is restricted by the intrinsic transmission characteristics of a positive electrode/electrolyte/negative electrode material collocation system on one hand, and on the other hand, the pole piece process and the electrical core structure design also have great influence on the rate performance; in order to improve the volume energy density, the compaction density of the positive and negative pole pieces is gradually improved, and then higher requirements on the wettability of the electrolyte are provided. At present, the common electrolyte has poor wettability and cannot meet the requirement of a high-specific-energy system battery. In view of the above, it is desirable to provide a functional electrolyte solution to solve the above problems, so that the high specific energy system battery can be popularized and applied.
Disclosure of Invention
The invention aims to provide an electrolyte suitable for a lithium ion battery with a high specific energy system and a lithium ion battery with rate discharge performance and quick charge cycle performance.
In order to achieve the purpose, the technical scheme adopted by the invention is as follows:
one aspect of the invention provides an electrolyte comprising an electrolytic lithium salt, an organic solvent and additives, wherein the organic solvent comprises a carboxylate solvent, and the additives comprise a low impedance additive, a wetting agent and a film forming additive.
The structural formula of the carboxylic ester solvent is shown in the specification
Figure BDA0002966755020000011
R 1 、R 2 The halogen atoms are respectively and independently selected from hydrogen atoms, halogen atoms, substituted or unsubstituted alkyl groups, substituted or unsubstituted alkoxy groups, substituted or unsubstituted alkenyl groups and substituted or unsubstituted phenyl groups, the substituted substituent groups are one or more of phenyl groups, alkyl groups with 1-5 carbon atoms and halogen atoms, and the halogen atoms are selected from F, Cl or Br.
The low impedance additive is
Figure BDA0002966755020000021
Figure BDA0002966755020000022
One or more of (a).
The structural formula of the impregnating compound is shown as
Figure BDA0002966755020000023
The film-forming additive is
Figure BDA0002966755020000024
Figure BDA0002966755020000025
One or more of (a).
Preferably, said R is 1 、R 2 Each independently selected from substituted or unsubstituted alkyl, substituted or unsubstituted alkoxy, said substituted substituents being phenyl and/or halogen atoms selected from F, Cl or Br.
Further preferably, the carboxylate solvent is
Figure BDA0002966755020000026
Figure BDA0002966755020000031
Figure BDA0002966755020000032
One or more of (a).
Preferably, the mass of the carboxylate solvent accounts for 1% -30% of the total mass of the electrolyte, further 10% -30%, and further 15% -28%.
Preferably, the mass of the low-impedance additive accounts for 0.1-10%, further 0.5-5%, and further 1-2.5% of the total mass of the electrolyte.
Preferably, the weight of the impregnating compound accounts for 0.01-2%, further 0.01-1.5%, and further 0.05-1% of the total weight of the electrolyte.
Preferably, the mass of the film forming additive accounts for 0.1-5%, further 0.5-3%, and further 0.5-2% of the total mass of the electrolyte.
According to some specific and preferred embodiments, the organic solvent further comprises one or more of a carbonate, an ether, a sulfone.
Preferably, the carbonate is one or more of ethylene carbonate, propylene carbonate, butylene carbonate, dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate and propylene carbonate.
Further preferably, the carbonate is one or more of ethylene carbonate, dimethyl carbonate and ethyl methyl carbonate.
Preferably, the ether is one or more of dimethoxymethane, 1, 2-dimethoxyethane, tetrahydrofuran and 1, 3-dioxolane.
Preferably, the sulfone is one or more of dimethyl sulfoxide, sulfolane and dimethyl sulfone.
In the invention, when the organic solvents in the electrolyte comprise two or more types, the different types of organic solvents can be compounded in any weight ratio.
According to some specific and preferred embodiments, the electrolyte lithium salt is LiPF 6 、LiBF 4 、LiClO 4 、LiCH 3 SO 3 、LiSCN、LiNO 3 、LiO 3 SCF 2 CF 3 、LiAsF 6 、LiAlCl 4 And LiTFSI.
Preferably, the concentration of the electrolyte lithium salt in the electrolyte is 0.5 to 3mol/L, further 0.5 to 2mol/L, further 0.8 to 1.5mol/L, further 1 to 1.2 mol/L.
Further preferably, the electrolyte lithium salt is LiPF 6 。
Another aspect of the present invention provides a lithium ion battery, including an NCM positive plate and a graphite negative plate, wherein: the lithium ion battery also comprises the electrolyte.
Preferably, the compaction density of the NCM positive plate is more than or equal to 3.5g/cm 3 。
Preferably, the graphite negative electrode sheet is compacted in density≥1.65g/cm 3 。
Due to the application of the technical scheme, compared with the prior art, the invention has the following advantages: the invention can be applied to the lithium ion battery of a high energy density system while improving the wettability of the electrolyte through the synergistic action of various additives and the carboxylic ester solvent, and has better rate discharge performance and quick charge cycle performance.
Detailed Description
The present invention will be further described with reference to the following examples. However, the present invention is not limited to the following examples. The implementation conditions adopted in the embodiments can be further adjusted according to different requirements of specific use, and the implementation conditions not mentioned are conventional conditions in the industry. The technical features of the embodiments of the present invention may be combined with each other as long as they do not conflict with each other.
To more visually compare the electrolyte effects, the following comparative and example cells were unified with a 2650mAh model 18650 cylindrical cell of 4.2V NCM 523/artificial graphite system, in which the NCM523 positive electrode sheet had a compacted density of 3.55g/cm 3 The compacted density of the artificial graphite negative plate is 1.7g/cm 3 。
The electrolytes of the following comparative examples and examples were placed in an argon-filled glove box (H) 2 Content of O<10ppm) the configuration is complete.
1) The test method for the experimental results of the following comparative examples and examples is as follows:
multiplying power discharge: after the 1C constant current and constant voltage full charge, the discharge capacity of the discharge tube under the current density is obtained by constant current discharge of 3C and 5C respectively, and is compared with the 1C discharge capacity.
Quick charge cycle performance: and (3) testing the cycle performance of 3C constant-current constant-voltage charging and 1C discharging.
Contact angle test: and (3) carrying out contact angle test by using the positive pole piece, the negative pole piece and the diaphragm as matrixes.
2) The following comparative examples and examples were conducted using the following instruments for rate discharge, rapid charge cycle and contact angle testing:
a Shenzhen New power battery tester is adopted for multiplying power discharge and fast charge cycle tests;
contact angle testing was performed on a u.s.koro contact angle tester.
3) The following comparative examples and examples relate to a carboxylic ester solvent of
S-01
Figure BDA0002966755020000051
S-02
Figure BDA0002966755020000052
S-03
Figure BDA0002966755020000053
S-04
Figure BDA0002966755020000054
S-05
Figure BDA0002966755020000055
S-06
Figure BDA0002966755020000056
S-07
Figure BDA0002966755020000057
S-08
Figure BDA0002966755020000058
S-09
Figure BDA0002966755020000059
S-10
Figure BDA00029667550200000510
S-11
Figure BDA00029667550200000511
S-12
Figure BDA00029667550200000512
The low impedance additive is
Z-01
Figure BDA00029667550200000513
Z-02
Figure BDA00029667550200000514
Z-03
Figure BDA00029667550200000515
Z-04
Figure BDA00029667550200000516
Z-05
Figure BDA00029667550200000517
The impregnating compound is J-01
Figure BDA00029667550200000518
The film-forming additive is
M-01
Figure BDA0002966755020000061
M-02
Figure BDA0002966755020000062
M-03
Figure BDA0002966755020000063
M-04
Figure BDA0002966755020000064
M-05、
Figure BDA0002966755020000065
M-06
Figure BDA0002966755020000066
Comparative example 1
The organic solvent in the electrolyte is dimethyl carbonate, ethylene carbonate and methyl ethyl carbonate (the mass ratio of the dimethyl carbonate to the ethylene carbonate to the methyl ethyl carbonate is 5:3: 2); the electrolyte lithium salt is LiPF 6 The concentration of the electrolyte lithium salt in the electrolyte is 1 mol/L; no other functional additives are added.
Comparative example 2
The organic solvent in the electrolyte is dimethyl carbonate, ethylene carbonate and methyl ethyl carbonate (the mass ratio of the dimethyl carbonate to the ethylene carbonate to the ethyl methyl carbonate is 5:3: 2); the electrolyte lithium salt is LiPF 6 The concentration of the electrolyte lithium salt in the electrolyte is 1 mol/L; and a 5% carboxylate solvent S-01 by mass is also added into the electrolyte.
Comparative example 3
The organic solvent in the electrolyte is dimethyl carbonate, ethylene carbonate and methyl ethyl carbonate (the mass ratio of the dimethyl carbonate to the ethylene carbonate to the ethyl methyl carbonate is 5:3: 2); the electrolyte lithium salt is LiPF 6 The concentration of the electrolyte lithium salt in the electrolyte is 1 mol/L; and a low-impedance additive Z-01 with the mass ratio of 1% is also added into the electrolyte.
Comparative example 4
The organic solvent in the electrolyte is dimethyl carbonate, ethylene carbonate and methyl ethyl carbonate (the mass ratio of the dimethyl carbonate to the ethylene carbonate to the ethyl methyl carbonate is 5:3: 2); the electrolyte lithium salt is LiPF 6 The concentration of the electrolyte lithium salt in the electrolyte is 1 mol/L; 0.1 percent of impregnating compound J-01 by mass is also added into the electrolyte.
Comparative example 5
The organic solvent in the electrolyte is dimethyl carbonate, ethylene carbonate and methyl ethyl carbonate (the mass ratio of the dimethyl carbonate to the ethylene carbonate to the ethyl methyl carbonate is 5:3: 2); the electrolyte lithium salt is LiPF6, and the concentration of the electrolyte lithium salt in the electrolyte is 1 mol/L; and a film forming additive M-01 with the mass ratio of 1% is also added into the electrolyte.
Examples 1 to 10
The organic solvent in the electrolyte is dimethyl carbonate, ethylene carbonate and methyl ethyl carbonate (the mass ratio of the dimethyl carbonate to the ethylene carbonate to the ethyl methyl carbonate is 5:3: 2); the electrolyte lithium salt is LiPF 6 The concentration of the lithium salt in the electrolyte was 1mol/L, and the types and mass contents of the additives in the electrolyte are shown in table 1 below.
TABLE 1
Figure BDA0002966755020000071
Comparative and example rate discharge performance and fast charge cycle performance test results are shown in table 2 below.
TABLE 2
Figure BDA0002966755020000072
Figure BDA0002966755020000081
Comparative and example contact angle test results are shown in table 3 below.
TABLE 3
Figure BDA0002966755020000082
Figure BDA0002966755020000091
As can be seen from the performance test data of each example and comparative example in the tables 2 and 3, the contact angles of the electrolyte, the anode, the cathode and the diaphragm are reduced through the synergistic effect of the carboxylate solvent and the functional additive, so that the wettability of the electrolyte is greatly improved; and the lithium ion battery with the high energy density system can have better rate discharge performance and quick charge cycle performance.
The test result can intuitively find that the electrochemical performance of the 4.2V NCM523 lithium ion battery can be improved to a great extent by adopting the electrolyte formula, and particularly the formula in the embodiment 10 is particularly excellent in various performance performances.
The present invention has been described in detail for the purpose of illustration and description, and it will be apparent to those skilled in the art that the invention can be practiced without limitation to such detail, and all changes and modifications that come within the spirit of the invention are desired to be protected.

Claims (10)

1. An electrolytic solution comprising an electrolytic lithium salt, an organic solvent and an additive, characterized in that: the organic solvent comprises a carboxylic ester solvent, and the additives comprise a low-impedance additive, a sizing agent and a film-forming additive; wherein the carboxylic ester solvent has a structural formula
Figure FDA0002966755010000011
R 1 、R 2 Each independently selected from hydrogen atoms, halogen atoms, substituted or unsubstituted alkyl groups, substituted or unsubstituted alkoxy groups, substituted or unsubstituted alkenyl groups and substituted or unsubstituted phenyl groups, wherein the substituted substituent groups are one or more of phenyl groups, alkyl groups with 1-5 carbon atoms and halogen atoms, and the halogen atoms are selected from F, Cl or Br; the low impedance additive is
Figure FDA0002966755010000012
Figure FDA0002966755010000013
One or more of;
the structural formula of the impregnating compound is shown as
Figure FDA0002966755010000014
The film-forming additive is
Figure FDA0002966755010000015
Figure FDA0002966755010000016
One or more of (a).
2. The electrolyte of claim 1, wherein: the carboxylic ester solvent is
Figure FDA0002966755010000021
Figure FDA0002966755010000022
One or more of (a).
3. The electrolyte of claim 1 or 2, wherein: the mass of the carboxylate solvent accounts for 1-30% of the total mass of the electrolyte.
4. The electrolyte of claim 1, wherein: the mass of the low-impedance additive accounts for 0.1-10% of the total mass of the electrolyte.
5. The electrolyte of claim 1, wherein: the weight of the impregnating compound accounts for 0.01-2% of the total weight of the electrolyte.
6. The electrolyte of claim 1, wherein: the mass of the film forming additive accounts for 0.1-5% of the total mass of the electrolyte.
7. The electrolyte of claim 1, wherein: the organic solvent further comprises one or more of carbonate, ether and sulfone.
8. The electrolyte of claim 7, wherein: the carbonate is one or more of ethylene carbonate, propylene carbonate, butylene carbonate, dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate and propylene carbonate; the ether is one or more of dimethoxymethane, 1, 2-dimethoxyethane, tetrahydrofuran and 1, 3-dioxolane; the sulfone is one or more of dimethyl sulfoxide, sulfolane and dimethyl sulfone.
9. The electrolyte of claim 1, wherein: the electrolyte lithium salt is LiPF 6 、LiBF 4 、LiClO 4 、LiCH 3 SO 3 、LiSCN、LiNO 3 、LiO 3 SCF 2 CF 3 、LiAsF 6 、LiAlCl 4 And one or more of LiTFSI, wherein the concentration of electrolyte lithium salt in the electrolyte is 0.5-3 mol/L.
10. A lithium ion battery comprises an NCM positive plate and a graphite negative plate, and is characterized in that: the lithium ion battery further comprises the electrolyte of any of claims 1 to 9, wherein the NCM positive electrode sheet compacted density is not less than 3.5g/cm 3 The compacted density of the graphite negative plate is more than or equal to 1.65g/cm 3 。
CN202110252866.1A 2021-03-09 2021-03-09 Electrolyte and lithium ion battery Pending CN115036571A (en)

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Citations (10)

* Cited by examiner, † Cited by third party
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CN1527420A (en) * 2003-03-06 2004-09-08 三洋电机株式会社 Lithium battery
JP2011238373A (en) * 2010-05-06 2011-11-24 Sony Corp Secondary battery, electrolytic solution for secondary battery, electric tool, electric vehicle, and power storage system
CN106532117A (en) * 2016-11-17 2017-03-22 张家港市国泰华荣化工新材料有限公司 Lithium ion battery electrolyte and lithium ion battery
CN109119685A (en) * 2017-06-23 2019-01-01 宁德时代新能源科技股份有限公司 Electrolyte and lithium ion battery
CN109417200A (en) * 2016-07-01 2019-03-01 中央硝子株式会社 Non-aqueous electrolyte additive, non-aqueous electrolyte and nonaqueous electrolyte secondary battery using the additive
CN109417199A (en) * 2016-07-01 2019-03-01 中央硝子株式会社 Non-aqueous electrolyte and nonaqueous electrolyte secondary battery
CN109935783A (en) * 2019-02-21 2019-06-25 宁德新能源科技有限公司 Electrochemical appliance and electronic device
CN110911752A (en) * 2019-12-06 2020-03-24 广州天赐高新材料股份有限公司 Low-internal-resistance lithium secondary battery electrolyte and lithium secondary battery
CN111129598A (en) * 2019-12-30 2020-05-08 东莞市杉杉电池材料有限公司 High-voltage lithium ion battery non-aqueous electrolyte and lithium ion battery thereof
US20210043973A1 (en) * 2018-03-23 2021-02-11 Tomiyama Pure Chemical Industries, Ltd. Nonaqueous electrolyte solution for power storage devices

Patent Citations (10)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN1527420A (en) * 2003-03-06 2004-09-08 三洋电机株式会社 Lithium battery
JP2011238373A (en) * 2010-05-06 2011-11-24 Sony Corp Secondary battery, electrolytic solution for secondary battery, electric tool, electric vehicle, and power storage system
CN109417200A (en) * 2016-07-01 2019-03-01 中央硝子株式会社 Non-aqueous electrolyte additive, non-aqueous electrolyte and nonaqueous electrolyte secondary battery using the additive
CN109417199A (en) * 2016-07-01 2019-03-01 中央硝子株式会社 Non-aqueous electrolyte and nonaqueous electrolyte secondary battery
CN106532117A (en) * 2016-11-17 2017-03-22 张家港市国泰华荣化工新材料有限公司 Lithium ion battery electrolyte and lithium ion battery
CN109119685A (en) * 2017-06-23 2019-01-01 宁德时代新能源科技股份有限公司 Electrolyte and lithium ion battery
US20210043973A1 (en) * 2018-03-23 2021-02-11 Tomiyama Pure Chemical Industries, Ltd. Nonaqueous electrolyte solution for power storage devices
CN109935783A (en) * 2019-02-21 2019-06-25 宁德新能源科技有限公司 Electrochemical appliance and electronic device
CN110911752A (en) * 2019-12-06 2020-03-24 广州天赐高新材料股份有限公司 Low-internal-resistance lithium secondary battery electrolyte and lithium secondary battery
CN111129598A (en) * 2019-12-30 2020-05-08 东莞市杉杉电池材料有限公司 High-voltage lithium ion battery non-aqueous electrolyte and lithium ion battery thereof

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