CN113707941A - Electrolyte for improving gas production of lithium ion battery and manufacturing method thereof - Google Patents

Electrolyte for improving gas production of lithium ion battery and manufacturing method thereof Download PDF

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Publication number
CN113707941A
CN113707941A CN202111019472.8A CN202111019472A CN113707941A CN 113707941 A CN113707941 A CN 113707941A CN 202111019472 A CN202111019472 A CN 202111019472A CN 113707941 A CN113707941 A CN 113707941A
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electrolyte
additive
lithium ion
carbonate
percent
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余志文
陈水彬
付诗清
陈鑫
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Heyuan Lianmao New Material Co ltd
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Heyuan Lianmao New Material 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
    • H01M10/058—Construction or manufacture
    • 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
    • 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
    • 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
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

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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)
  • Materials Engineering (AREA)
  • Physics & Mathematics (AREA)
  • Condensed Matter Physics & Semiconductors (AREA)
  • General Physics & Mathematics (AREA)
  • Inorganic Chemistry (AREA)
  • Secondary Cells (AREA)

Abstract

The invention discloses an electrolyte for improving gas production of a lithium ion battery, which comprises a positive electrode, a negative electrode and the electrolyte, and is characterized in that: the composition ratio of the positive electrode material is LiCo, 2: acetylene black: PVDF, 90:5:5 (mass ratio); the negative electrode material comprises artificial graphite, conductive carbon black, sodium carboxymethylcellulose and styrene butadiene rubber in a ratio of 94.7:1.5:1.5: 2.3; 0.1 to 0.5 percent of triphenyl phosphite (TPPI) is added into the electrolyte; the electrolyte is added with triphenyl phosphite (TPPI) stabilizer to generate slow hydrolysis reaction in the electrolyte, and the alkaline hydrolysis product can effectively capture trace HF in the electrolyte, thereby effectively reducing the water content of the electrolyte and inhibiting the acidity rise.

Description

Electrolyte for improving gas production of lithium ion battery and manufacturing method thereof
The technical field is as follows:
the invention relates to the technical field of battery manufacturing and processing, in particular to an electrolyte for improving gas production of a lithium ion battery and a manufacturing method thereof.
Background art:
against the background of energy crisis and environmental problems, fuel-powered vehicles are being prohibited from use in all countries of the world, and it has become an urgent task to develop new energy vehicles, such as Electric Vehicles (EV) or Hybrid Electric Vehicles (HEV).
As is well known, the formation at normal temperature in the production process of the lithium battery consumes long time, the interface of the negative electrode is poor, and particularly, the gas production is greatly increased when the moisture and the air are not strictly controlled in the manufacturing process. Therefore, how to reduce gas generation in the pre-charging process by regulating and controlling the composition of the electrolyte is the key for improving the production efficiency of the battery and the performance of the battery.
In addition, the sealing performance of the battery on an outer packaging material is poor, or some impurities are introduced into the battery in the production process, so that the battery can be inflated in the storage stage, and the problems are always one of the puzzlement factors of the industrialization process of the lithium ion battery for a long time;
at present, the mechanism of an SEI layer is relatively researched more, various factors influencing the property of the SEI layer are researched less, particularly, the gas generation mechanism of a lithium ion battery is researched less, generally, people mainly consider the influence of the solvent on the formation and stability of the SEI layer and the influence of the gas generated in a formation stage and the gas generated in a storage stage of the battery on the electric conductivity of a formed electrolyte solvent system and the temperature performance of the battery from the aspects of the viscosity, the dielectric constant, the freezing point, the boiling point and the like of the solvent, in the actual work, the research on the influence of the solvent on the formation and the stability of the SEI layer and the gas generated in the storage stage of the battery is not much, and through research and discussion on a unit electrolyte and the gas generated in the formation process of a multi-element electrolyte battery, the research and discussion on the unit electrolyte solvent are found to be the defects of the unit electrolyte solvent, whether the formation process of the SEI layer in the formation or the self-repairing of the SEI layer in the storage stage, reductive decomposition of the solvent easily causes generation of a large amount of gas, which is not favorable for sealing the battery.
For example, Chinese patent publication No. 103872396A discloses an electrolyte for inhibiting gas production of lithium titanate batteryAiming at the gas generation of the lithium titanate battery, a specific amount of potassium salt is added into the electrolyte, and the electrolyte is kept stable on the surface of the lithium titanate negative electrode through the electrochemical stabilization effect on the lithium titanate negative electrode, so that the gas generation of the lithium titanate battery is inhibited2And the chemical and gas generation caused by O and HF.
The electrolyte of the ultrahigh-temperature high-voltage lithium ion battery and the lithium ion battery using the electrolyte have the Chinese patent publication No. 105261791A, adopt a sultone sulfonate compound to inhibit gas generation in the high-temperature storage process of the lithium ion battery, but do not aim at the formed gas generation and do not consider the influence of the sultone sulfonate compound on the low-temperature performance.
The invention content is as follows:
the invention aims to overcome the defects of the prior art and provide an electrolyte for improving the gas production of a lithium ion battery and a manufacturing method thereof.
The scheme for solving the technical problems is as follows:
the utility model provides an improve lithium ion battery and produce gas electrolyte which characterized in that: the paint comprises the following components in percentage by mass: 80.5 to 85.5 percent of nonaqueous organic solvent; 12.5 to 15 percent of electrolyte lithium salt; 0.5 to 1.5 percent of negative film forming additive; 0.5-1% of additive for inhibiting gas production and eliminating H 20 and 0.5-1% of HF additive.
The electrolyte lithium salt is lithium hexafluorophosphate (LiPF)6)。
The non-aqueous organic solvent includes cyclic carbonates and linear carbonates.
The cyclic carbonate includes at least one of Ethylene Carbonate (EC) and Propylene Carbonate (PC); the linear carbonate includes diethyl carbonate (DEC) and Ethyl Methyl Carbonate (EMC); the mass ratio of the cyclic carbonate, diethyl carbonate (DEC) and Ethyl Methyl Carbonate (EMC) is 30:20: 50.
The negative film forming additive is vinylene carbonate (vc).
The additive for inhibiting gas production is a functional additive of sulfite alkene ester, and comprises one or more than two of ES, DTD, BS, PS and the like.
The elimination of H2An additive of 0 and HF is triphenyl phosphite (TPPi).
A manufacturing method for improving gas production electrolyte of a lithium ion battery is characterized by comprising the following steps: the method comprises the following steps:
(1) firstly, respectively weighing the following components in percentage by mass: 80.5 to 85.5 percent of nonaqueous organic solvent; 12.5 to 15 percent of electrolyte lithium salt; 0.5 to 1.5 percent of negative film forming additive; additive for inhibiting gas production 0.5-1%; elimination of H20.5-1% of additive of HF and 0;
(2) then dissolving electrolyte lithium salt in a non-aqueous organic solvent, and stirring to form a uniform solution A;
(3) then, the negative electrode film forming additive, the additive for inhibiting gas generation and the additive for eliminating H are added2And (3) adding additives of 0 and HF into the solution A obtained in the step (2) one by one to obtain the electrolyte.
The invention has the following outstanding effects:
compared with the prior art, after the electrolyte containing the functional additive of the alkene sulfite is used, the gas production of the battery is effectively controlled, a small amount of alkene sulfite is added, the formation and the stability of SEI on the surface of negative electrode particles are facilitated, the gas production of the dissolution and the regeneration of the SEI is reduced, and meanwhile, the compatibility of a lithium cobaltate positive electrode and the electrolyte is greatly improved.
Description of the drawings:
FIG. 1 is a schematic view of gas production between a comparative example and an example;
FIG. 2 is a graph of the relationship between the gas production volume of electrolyte and the pre-charge voltage and pre-charge time with different gas production inhibiting additive amounts.
The specific implementation mode is as follows:
the present invention is described in detail below with reference to specific preferred embodiments so that the advantages and features of the present invention can be more easily understood by those skilled in the art, and these embodiments are for illustrative purposes only and are not intended to limit the scope of the present invention.
Example (b): the utility model provides an improve lithium ion battery and produce gas electrolyte which characterized in that: the paint comprises the following components in percentage by mass: 80.5 to 85.5 percent of nonaqueous organic solvent; 12.5 to 15 percent of electrolyte lithium salt; 0.5 to 1.5 percent of negative film forming additive; 0.5-1% of additive for inhibiting gas production and eliminating H 20 and 0.5-1% of HF additive.
The electrolyte lithium salt is lithium hexafluorophosphate (LiPF for short)6)。
The non-aqueous organic solvent includes cyclic carbonates and linear carbonates.
The cyclic carbonate comprises at least one of Ethylene Carbonate (EC) and Propylene Carbonate (PC); the linear carbonic ester comprises diethyl carbonate (DEC) and Ethyl Methyl Carbonate (EMC); the mass ratio of the cyclic carbonate, diethyl carbonate (DEC) and Ethyl Methyl Carbonate (EMC) is 30:20: 50.
The negative film-forming additive is vinylene carbonate (vc for short).
The additive for inhibiting the gas production is a functional additive of sulfite alkene ester, and comprises one or more of Ethylene Sulfite (ES), ethylene sulfate (DTD), Butylene Sulfite (BS), Propylene Sulfite (PS) and the like.
The elimination of H2The additive of 0 and HF is triphenyl phosphite (abbreviated as TPPi).
A manufacturing method for improving gas production electrolyte of a lithium ion battery comprises the following steps:
(1) firstly, respectively weighing the following components in percentage by mass: 80.5 to 85.5 percent of nonaqueous organic solvent; 12.5 to 15 percent of electrolyte lithium salt; 0.5 to 1.5 percent of negative film forming additive; additive for inhibiting gas production 0.5-1%; elimination of H20.5-1% of additive of HF and 0;
(2) then dissolving electrolyte lithium salt in a non-aqueous organic solvent, and stirring to form a uniform solution A;
(3) then the negative electrode is made intoFilm additive, additive for inhibiting gas generation, and H elimination2And (3) adding additives of 0 and HF into the solution A obtained in the step (2) one by one to obtain the electrolyte. Denoted BEF.
Wherein the additive for inhibiting gas generation comprises one or more than two of ES, DTD, BS, PS and the like.
Experimental comparisons were made between the examples and the existing electrolyte:
the existing electrolyte was prepared as a comparative example:
the electrolyte contains a negative electrode film-forming additive VC and a nonaqueous organic solvent, wherein the mass percent of the nonaqueous organic solvent in the electrolyte is 83.5%, the nonaqueous organic solvent is a mixture of EC, EMC and DEC, the mass ratio of the nonaqueous organic solvent to the EMC and DEC is 30:20:50, and the electrolyte is 1mol/L of LiPF6，LiPF6The mass percentage of the electrolyte is 12.5 percent.
The preparation method comprises the following steps:
(1) weighing the raw material components according to the mass percentage and the mass ratio respectively;
(2) then lithium salt LiPF is used as electrolyte6Dissolving in a mixture of non-aqueous organic solvents EC, EMC and DEC, and stirring to form a uniform solution; a sample of electrolyte was prepared and is designated 3272.
The gas production between the comparative example and the example is shown in fig. 1;
as can be seen from the figure, the electrolyte has a particularly obvious influence on the gas production rate of the battery pre-charging, and after the BEF electrolyte containing the additive is used, the gas production rate of the battery is effectively controlled and is only about half of that of the 3272 electrolyte. The reason is that the addition of a small amount of the allyl sulfite is beneficial to the formation and the stability of SEI on the surface of negative electrode particles, reduces the gas production rate of SEI dissolution and regeneration, and simultaneously improves the compatibility of the lithium cobaltate positive electrode and the electrolyte.
FIG. 2 is a graph showing the relationship between the gas generation volume of the electrolyte and the precharge voltage and precharge time for different gas generation inhibiting additives.
As can be seen from FIG. 2, in the case of different additives for suppressing gas evolution from the electrolyte, one, two, three or more additives for suppressing gas evolution and H elimination are added to the different additives2Addition of 0 and HFThe charging voltages corresponding to the maximum volume of the generated gas of the electrolyte of the agent are respectively ps<，ps、es<，ps、es、bs<ps、es、bs、dtd<ps, es, bs, dtd and TPPi, wherein one additive for inhibiting gas generation is added to generate gas about 100min after the pre-charging is started, most of two or three additives for inhibiting gas generation are added to generate gas within 200min of pre-charging, the electrolyte added with more than four additives for inhibiting gas generation reaches the maximum value about 250min, and the four additives for inhibiting gas generation and the additive for eliminating H are added2The electrolyte of additives 0 and HF reaches a maximum around 280 min.
A large number of documents show that the lithium ion battery anode material can have a film forming process in the charging and discharging processes, manganese can be dissolved in an electrolyte in the charging and discharging processes under the condition that an anode system is the same, and due to the fact that Mn4+ ions have high oxidizability in a high delithiation state and oxidize the electrolyte to generate gas, the additive disclosed by the invention can enable the surface of an electrode of a lithium ion battery to form an excellent CEI/SEI film in the pre-charging process, can well prevent the direct contact between the electrode of the lithium ion battery and an electrolyte solvent, and reduces the generation of gas, so that the additive disclosed by the invention can well inhibit the gas generation of the lithium ion battery in the pre-charging process. The inhibition of pre-charging gas generation can be developed from the reliability design of the electrolyte additive, so that the influence of the pre-charging gas generation on the performance of the battery is eliminated. Aiming at a battery system with more gas production, a certain amount of functional additives such as sulfite and phosphate are added into the electrolyte, so that the stability of the electrolyte is improved, the formation and the stability of SEI are promoted, and some side reactions participated by the electrolyte are inhibited.
The above embodiments are only for illustrating the invention and are not to be construed as limiting the invention, and those skilled in the art can make various changes and modifications without departing from the spirit and scope of the invention, therefore, all equivalent technical solutions also belong to the scope of the invention, and the scope of the invention is defined by the claims.

Claims (8)

1. An electrolyte for improving gas production of lithium ion battery, which is characterized in thatIn the following steps: the paint comprises the following components in percentage by mass: 80.5 to 85.5 percent of nonaqueous organic solvent; 12.5 to 15 percent of electrolyte lithium salt; 0.5 to 1.5 percent of negative film forming additive; 0.5-1% of additive for inhibiting gas production and eliminating H20 and 0.5-1% of HF additive.
2. The improved gas generation electrolyte for lithium ion batteries according to claim 1, wherein: the electrolyte lithium salt is lithium hexafluorophosphate.
3. The improved gas generation electrolyte for lithium ion batteries according to claim 1, wherein: the non-aqueous organic solvent includes cyclic carbonates and linear carbonates.
4. The improved gas generation electrolyte for lithium ion batteries according to claim 3, wherein: the cyclic carbonate comprises at least one of ethylene carbonate and propylene carbonate; the linear carbonate comprises diethyl carbonate and ethyl methyl carbonate; the mass ratio of the cyclic carbonate, the diethyl carbonate and the ethyl methyl carbonate is 30:20: 50.
5. The improved gas generation electrolyte for lithium ion batteries according to claim 1, wherein: the negative film-forming additive is vinylene carbonate.
6. The improved gas generation electrolyte for lithium ion batteries according to claim 1, wherein: the additive for inhibiting gas production is a functional additive of sulfite alkene ester, and comprises one or more than two of ES, DTD, BS, PS and the like.
7. The improved gas generation electrolyte for lithium ion batteries according to claim 1, wherein: the elimination of H2An additive of 0 and HF is triphenyl phosphite.
8. A method for manufacturing an improved gas-producing electrolyte for a lithium ion battery according to any one of claims 1 to 7, wherein: the method comprises the following steps:
(1) firstly, respectively weighing the following components in percentage by mass: 80.5 to 85.5 percent of nonaqueous organic solvent; 12.5 to 15 percent of electrolyte lithium salt; 0.5 to 1.5 percent of negative film forming additive; additive for inhibiting gas production 0.5-1%; elimination of H20.5-1% of additive of HF and 0;
(2) then dissolving electrolyte lithium salt in a non-aqueous organic solvent, and stirring to form a uniform solution A;
(3) then, the negative electrode film forming additive, the additive for inhibiting gas generation and the additive for eliminating H are added2And (3) adding additives of 0 and HF into the solution A obtained in the step (2) one by one to obtain the electrolyte.
CN202111019472.8A 2021-09-01 2021-09-01 Electrolyte for improving gas production of lithium ion battery and manufacturing method thereof Pending CN113707941A (en)

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Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN103985904A (en) * 2014-05-21 2014-08-13 珠海市赛纬电子材料有限公司 Non-aqueous electrolyte capable of improving high-temperature performance for lithium ion battery
CN108242566A (en) * 2016-12-26 2018-07-03 宁德时代新能源科技股份有限公司 Electrolyte solution and secondary battery
CN108878977A (en) * 2018-06-29 2018-11-23 桑顿新能源科技有限公司 Inhibit the chemical conversion of lithium battery high temperature to produce gas and improves the electrolyte and preparation method of cryogenic property

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN103985904A (en) * 2014-05-21 2014-08-13 珠海市赛纬电子材料有限公司 Non-aqueous electrolyte capable of improving high-temperature performance for lithium ion battery
CN108242566A (en) * 2016-12-26 2018-07-03 宁德时代新能源科技股份有限公司 Electrolyte solution and secondary battery
CN108878977A (en) * 2018-06-29 2018-11-23 桑顿新能源科技有限公司 Inhibit the chemical conversion of lithium battery high temperature to produce gas and improves the electrolyte and preparation method of cryogenic property

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Application publication date: 20211126