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WO2018120792A1 - Électrolyte et batterie secondaire - Google Patents

Électrolyte et batterie secondaire Download PDF

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Publication number
WO2018120792A1
WO2018120792A1 PCT/CN2017/093862 CN2017093862W WO2018120792A1 WO 2018120792 A1 WO2018120792 A1 WO 2018120792A1 CN 2017093862 W CN2017093862 W CN 2017093862W WO 2018120792 A1 WO2018120792 A1 WO 2018120792A1
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WO
WIPO (PCT)
Prior art keywords
sulfate
bis
electrolyte
group
secondary battery
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Ceased
Application number
PCT/CN2017/093862
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English (en)
Chinese (zh)
Inventor
王小梅
周晓崇
付成华
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Contemporary Amperex Technology Co Ltd
Original Assignee
Contemporary Amperex Technology Co Ltd
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Filing date
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Application filed by Contemporary Amperex Technology Co Ltd filed Critical Contemporary Amperex Technology Co Ltd
Publication of WO2018120792A1 publication Critical patent/WO2018120792A1/fr
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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Classifications

    • 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
    • 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
    • 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

Definitions

  • the present invention relates to the field of battery technologies, and in particular, to an electrolyte and a secondary battery.
  • the cycle performance and high temperature performance of lithium ion secondary batteries are affected by many factors.
  • electrolytes as an important component of lithium ion secondary batteries, have a significant impact on their performance.
  • the electrolyte can improve the kinetic performance of the lithium ion secondary battery, and can also improve the stability of the interface between the positive and negative electrodes in the cycle and high temperature storage process, thereby achieving the purpose of improving the cycle performance and storage performance of the lithium ion secondary battery.
  • an object of the present invention is to provide an electrolyte and a secondary battery which, when applied to a secondary battery, can provide a secondary battery with low internal resistance and good Low temperature discharge performance, as well as good high temperature storage performance and high temperature cycle performance.
  • the present invention provides an electrolyte comprising an electrolyte salt, an organic solvent, and an additive.
  • the additives include silyl sulfates as well as cyclic sulfates and/or cyclic sulfonates.
  • the invention provides a secondary battery comprising an electrolyte according to an aspect of the invention.
  • the electrolyte of the present invention includes both a silyl sulfate and a cyclic sulfate and/or a cyclic sulfonate.
  • the secondary battery When applied to a secondary battery, the secondary battery can be made more synergistically under the synergistic action of the above substances. Low internal resistance, good low temperature discharge performance, and good high temperature storage performance and high temperature cycle performance.
  • the electrolytic solution according to the first aspect of the invention includes an electrolyte salt, an organic solvent, and an additive.
  • the additives include silyl sulfates as well as cyclic sulfates and/or cyclic sulfonates.
  • the silane-based sulfate has a high reduction potential, which can reduce the interface resistance of the negative electrode, thereby improving the cycle performance of the secondary battery and reducing the internal resistance of the secondary battery. It improves the low-temperature discharge performance and the high-temperature cycle performance, but it cannot suppress the high-temperature storage gas generation of the secondary battery.
  • the cyclic sulfate and the cyclic sulfonate have a high reduction potential, and can preferentially form a film on the surface of the negative electrode at a high voltage, thereby effectively suppressing high-temperature storage gas generation of the secondary battery, but when the amount of addition is high, The internal resistance of the secondary battery is increased, and the low-temperature discharge performance and high-temperature cycle performance of the secondary battery are deteriorated.
  • the secondary battery can have a low internal resistance, a good low-temperature discharge performance, and good high-temperature storage performance and cycle performance under the synergistic action of the above substances.
  • the silyl sulfate is selected from one or more of the compounds represented by Formula 1.
  • R 1 , R 2 , R 3 , R 4 , R 5 and R 6 are each independently selected from an alkyl group having 1 to 5 carbon atoms, an alkenyl group having 2 to 5 carbon atoms, and a carbon number of One of an alkynyl group of 2 to 5 and an alkoxy group having 1 to 5 carbon atoms, and an H atom of an alkyl group, an alkenyl group, an alkynyl group or an alkoxy group may be further represented by F, Cl, Br, I, One or more substitutions of a cyano group, a carboxyl group, or a sulfonic acid group.
  • the silane-based sulfate is selected from the group consisting of Silicate, bis(triethylsilyl)sulfate, bis(tri-n-propylsilyl)sulfate, bis(triisopropylsilyl)sulfate, bis(tri-n-butylsilyl) Sulfate, bis(triisobutylsilyl)sulfate, bis(tri-tert-butylsilyl)sulfate, bis(trimethoxysilyl)sulfate, bis(triethoxysilyl)sulfate , bis(tri-n-propoxysilyl)sulfate, bis(triisopropoxysilyl)sulfate, bis(tri-n-butoxysilyl)sulfate, bis(tri-sec-butoxysilyl) Sulfate, bis(tri-tert-butoxysilyl) sulf
  • the cyclic sulfate is selected from one or more of the compounds represented by Formula 2.
  • n is an integer within 1 to 3; and R 21 , R 22 , R 23 and R 24 are each independently selected from H, F, Cl, Br, I, an alkyl group having 1 to 10 carbon atoms.
  • R 21 , R 22 , R 23 and R 24 are each independently selected from H, F, Cl, Br, I, an alkyl group having 1 to 10 carbon atoms.
  • an alkoxy group having 1 to 10 carbon atoms wherein the H atom on the alkyl group or the alkoxy group may be substituted with one or more of F, Cl, Br, and I.
  • the cyclic sulfate is selected from one or more of the following compounds:
  • the cyclic sulfonate is selected from one or more of the compounds represented by Formula 3.
  • n is an integer within 1 to 3
  • R 31 , R 32 , R 33 , R 34 , R 35 and R 36 are each independently selected from H, F, Cl, Br, I, and the number of carbon atoms is
  • an alkyl group having 1 to 10 carbon atoms and an alkoxy group having 1 to 10 carbon atoms may be substituted by one or more of F, Cl, Br, and I. .
  • the cyclic sulfonate is selected from one or more of the following compounds:
  • the content of the silyl sulfate is 0.5% to 10% by weight based on the total weight of the electrolytic solution, and preferably, the content of the silyl sulfate is 1% to 5% of the total weight of the electrolyte.
  • the total content of the cyclic sulfate and/or cyclic sulfonate is from 0.5% to 10% by weight based on the total weight of the electrolytic solution.
  • the total content of the cyclic sulfate and/or cyclic sulfonate is from 1% to 5% of the total weight of the electrolyte.
  • the electrolyte salt may be selected from a lithium salt, a sodium salt or a zinc salt, which varies depending on the secondary battery to which the electrolyte is applied.
  • the content of the electrolyte salt is 6.2% to 25% of the total weight of the electrolytic solution, and preferably, the content of the electrolyte salt is the electrolytic solution.
  • the total weight is from 6.25% to 18.8%, and further preferably, the content of the electrolyte salt is from 10% to 15% of the total weight of the electrolyte.
  • the specific kind of the organic solvent is not particularly limited and may be selected according to actual needs.
  • a non-aqueous organic solvent is used.
  • the non-aqueous organic solvent may include any kind of carbonate, carboxylate.
  • the carbonate may include a cyclic carbonate or a chain carbonate.
  • the non-aqueous organic solvent may also include a halogenated compound of a carbonate.
  • the organic solvent may be selected from the group consisting of ethylene carbonate (EC), propylene carbonate (PC), butylene carbonate, pentylene carbonate, fluoroethylene carbonate, dimethyl carbonate (DMC), Diethyl carbonate (DEC), dipropyl carbonate, ethyl methyl carbonate (EMC), methyl formate, ethyl formate, ethyl acetate, propyl propionate, ethyl propionate, ⁇ -butyrolactone (BL One or more of tetrahydrofuran (THF).
  • EC ethylene carbonate
  • PC propylene carbonate
  • PC butylene carbonate
  • pentylene carbonate fluoroethylene carbonate
  • DMC dimethyl carbonate
  • DEC Diethyl carbonate
  • EMC dipropyl carbonate
  • EMC ethyl methyl carbonate
  • BL tetrahydrofuran
  • a secondary battery according to a second aspect of the invention includes the electrolytic solution according to the first aspect of the invention.
  • the secondary battery in addition to the electrolytic solution, further includes: a positive electrode sheet, a negative electrode sheet, and a separator.
  • the positive electrode sheet includes a positive electrode current collector and a positive electrode film disposed on the positive electrode current collector, the positive electrode film including a positive electrode active material, a binder, and a conductive material Agent.
  • the negative electrode sheet includes a negative electrode current collector and an negative electrode film disposed on the negative electrode current collector, and the negative electrode film includes a negative electrode active material, a binder, and may also include a conductive agent.
  • the separator is spaced between the positive electrode tab and the negative electrode tab.
  • the separator may be any separator material used in the existing secondary battery, such as polyethylene, polypropylene, polyvinylidene fluoride, and multilayers thereof. Composite membranes, but are not limited to these.
  • the secondary battery may be a lithium ion secondary battery, a sodium ion secondary battery, or a zinc ion secondary battery.
  • the electrolyte salt may be selected from a lithium salt
  • the lithium salt is LiPF 6 .
  • the positive active material may be selected from one or more of lithium cobaltate (LiCoO 2 ), lithium nickel manganese cobalt ternary material, lithium iron phosphate, lithium manganese oxide. kind.
  • the anode active material may be selected from metallic lithium.
  • the negative active material may also be selected from materials capable of intercalating lithium at ⁇ 2 V (vs. Li/Li + ).
  • the negative active material may be selected from natural graphite, artificial graphite, mesophase micro carbon spheres (MCMB), hard carbon, soft carbon, silicon, silicon-carbon composite, Li-Sn alloy, Li-Sn-O alloy, Sn, SnO, SnO 2 , spinel structure lithiated TiO 2 -Li 4 Ti 5 One or more of O 12 and Li-Al alloys.
  • the secondary battery is a sodium ion secondary battery or a zinc ion secondary battery, it is only necessary to change the corresponding positive electrode active material, negative electrode active material, and electrolyte salt.
  • A1 bis(trifluoromethylsilyl) sulfate
  • the lithium ion secondary batteries of Examples 1-10 and Comparative Examples 1-3 were all prepared in the following manner.
  • the positive electrode active material lithium cobaltate (LiCoO 2 ), the binder polyvinylidene fluoride, and the conductive agent acetylene black are mixed at a weight ratio of 96:2:2, and N-methylpyrrolidone (NMP) is added under the action of a vacuum mixer.
  • NMP N-methylpyrrolidone
  • the negative electrode active material graphite, the conductive agent acetylene black, the binder styrene-butadiene rubber (SBR), and the thickener sodium carboxymethyl cellulose (CMC) are mixed at a weight ratio of 97:1:1:1, and deionized water is added.
  • the negative electrode sheet was obtained by slitting.
  • the content of LiPF 6 is 12.5% of the total weight of the electrolyte.
  • Table 1 The specific types and contents of the silyl sulfate, cyclic sulfate, and cyclic sulfonate used in the electrolytic solution are shown in Table 1.
  • Table 1 the content of the silyl sulfate, the cyclic sulfate, and the cyclic sulfonate is a weight percentage calculated based on the total weight of the electrolytic solution.
  • a 16 ⁇ m thick polypropylene separator (model C210, supplied by Celgard) was used.
  • the positive electrode sheet, the separator film and the negative electrode sheet are stacked in order, so that the separator is in a role of isolation between the positive and negative electrode sheets, and then wound to obtain a bare cell; the bare cell is placed in the outer package foil, and the electricity is placed in the outer package foil.
  • the prepared electrolyte is injected into the dried bare cell, and after vacuum encapsulation, standing, formation, shaping, etc., a lithium ion secondary battery is obtained. .
  • the lithium ion secondary battery was charged at a constant current of 1 C (nominal capacity) to a voltage of 4.45 V at 25 ° C. Further, the battery is charged at a constant voltage of 4.45 V until the current is ⁇ 0.05 C, left for 5 min, discharged at a constant current of 1 C to a voltage of 3 V, and the actual discharge capacity is recorded, and the lithium ion secondary battery is based on the discharge capacity (100% SOC). Adjust to 50% SOC.
  • the lithium ion secondary battery is allowed to stand at -25 ° C for more than 4 h, so that the temperature of the lithium ion secondary battery reaches -25 ° C, and the discharge is continued for 10 s at a current of 0.3 C, and the voltage before the discharge and the voltage at the end of the discharge are used. The difference is divided by the current to obtain the DCIR of the lithium ion secondary battery. 15 lithium ion secondary batteries were tested in each group and averaged.
  • the lithium ion secondary battery was charged at a constant current of 1 C (nominal capacity) to a voltage of 4.45 V at 25 ° C, and then charged at a constant voltage of 4.45 V until the current was less than or equal to 0.05 C. After leaving for 5 minutes, the constant current was 0.5 C.
  • the discharge to the cut-off voltage is 3V, at which time the actual discharge capacity is recorded as D0.
  • the lithium ion secondary battery was allowed to stand at -15 ° C for 1 h, charged at a constant current of 1 C to a voltage of 4.45 V, and then charged at a constant voltage of 4.45 V until the current was less than or equal to 0.05 C. After being left for 10 min, the constant current was 0.5 C. The discharge was discharged to a voltage of 3 V, and the discharge capacity at this time was recorded as D1.
  • Capacity retention rate (%) of low-temperature discharge of lithium ion secondary battery D1/D0 ⁇ 100%. 15 lithium ion secondary batteries were tested in each group and averaged.
  • the lithium ion secondary battery was charged at a constant current of 1 C to a voltage of 4.45 V at 45 ° C, further charged at a constant voltage of 4.45 V until the current was 0.05 C, and then discharged at a constant current of 1 C to a voltage of 3.0 V, which is a During the charge and discharge cycle, this discharge capacity is the discharge capacity of the first cycle.
  • the lithium ion secondary battery was subjected to 300 cycles of charge/discharge test in accordance with the above method, and the discharge capacity at the 300th cycle was detected.
  • the capacity retention ratio (%) of the lithium ion secondary battery after circulating at 45 ° C for 300 times (discharge capacity of 300 cycles of lithium ion secondary battery discharge / discharge capacity of the first cycle of lithium ion secondary battery) ⁇ 100%. 15 lithium ion secondary batteries were tested in each group and averaged.
  • the lithium ion secondary battery was charged at a constant current of 0.5 C to a voltage of 4.45 V at 25 ° C, and then charged at a constant voltage of 4.45 V to a current of 0.05 C to be fully charged at 4.45 V, at which time the lithium ion was tested.
  • the thickness of the secondary battery was recorded as h 0 ; thereafter, the lithium ion secondary battery was placed in an incubator at 60 ° C, and after 30 days of storage, it was taken out, and the thickness of the lithium ion secondary battery at this time was measured and recorded as h 1 .
  • the thickness expansion ratio of the lithium ion secondary battery after storage at 60 ° C for 30 days [(h 1 -h 0 ) / h 0 ] ⁇ 100%. Each group was tested for 15 lithium ion secondary batteries and averaged.
  • the lithium ion can be improved while reducing the internal resistance at the low temperature of the lithium ion secondary battery.
  • Two The capacity retention rate, high temperature cycle performance and high temperature storage performance of the secondary battery after low temperature discharge.

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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

L'invention porte sur un électrolyte et sur une batterie secondaire. L'électrolyte comprend un sel électrolytique, un solvant organique et un additif. L'additif comprend : du sulfate de silyle et du sulfate cyclique et/ou du sulfonate cyclique. Une fois que l'électrolyte est appliqué à la batterie secondaire, la batterie secondaire peut avoir une faible résistance interne, une bonne performance de décharge à basse température, une bonne performance de stockage à haute température et une performance de cycle à haute température sous l'action synergique des substances décrites.
PCT/CN2017/093862 2016-12-26 2017-07-21 Électrolyte et batterie secondaire Ceased WO2018120792A1 (fr)

Applications Claiming Priority (2)

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CN201611219501.4A CN108242557B (zh) 2016-12-26 2016-12-26 电解液及二次电池
CN201611219501.4 2016-12-26

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Cited By (5)

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WO2019050167A3 (fr) * 2017-09-06 2019-05-09 삼성에스디아이 주식회사 Électrolyte non aqueux pour batterie rechargeable au lithium et batterie rechargeable au lithium le comprenant
CN114245943A (zh) * 2019-12-24 2022-03-25 宁德时代新能源科技股份有限公司 二次电池及含有该二次电池的装置
US20220352552A1 (en) * 2021-04-21 2022-11-03 Prime Planet Energy & Solutions, Inc. Electrolyte solution for non-aqueous electrolyte secondary battery, and non-aqueous electrolyte secondary battery
US11721837B2 (en) 2017-09-06 2023-08-08 Samsung Sdi Co., Ltd. Lithium secondary battery including fluoroethylene carbonate in electrolyte
WO2025201436A1 (fr) * 2024-12-17 2025-10-02 惠州亿纬锂能股份有限公司 Électrolyte et batterie

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CN110808412B (zh) * 2018-08-06 2022-06-07 宁德时代新能源科技股份有限公司 电解液及锂离子电池
CN109755635B (zh) * 2019-01-18 2020-11-06 杉杉新材料（衢州）有限公司 一种兼顾高低温性能的电池电解液添加剂、电解液及高镍三元锂离子电池
WO2021128002A1 (fr) 2019-12-24 2021-07-01 宁德时代新能源科技股份有限公司 Batterie secondaire et dispositif comprenant ladite batterie secondaire
CN114284556A (zh) * 2020-09-18 2022-04-05 浙江蓝天环保高科技股份有限公司 一种锂离子电池电解液及锂离子快充电池
CN114695973A (zh) * 2022-03-21 2022-07-01 电子科技大学 一种低温锌离子电池的制备方法
CN116404251B (zh) * 2023-03-27 2025-08-19 广东省豪鹏新能源科技有限公司 一种电解液和锂离子电池
CN119301792A (zh) * 2023-03-31 2025-01-10 宁德时代新能源科技股份有限公司 二次电池及用电装置

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CN105914399A (zh) * 2016-05-04 2016-08-31 宁德新能源科技有限公司 一种电解液以及含有该电解液的锂离子电池

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Publication number Priority date Publication date Assignee Title
WO2019050167A3 (fr) * 2017-09-06 2019-05-09 삼성에스디아이 주식회사 Électrolyte non aqueux pour batterie rechargeable au lithium et batterie rechargeable au lithium le comprenant
US11557791B2 (en) 2017-09-06 2023-01-17 Samsung Sdi Co., Ltd. Non-aqueous electrolyte for lithium secondary battery and lithium secondary battery comprising same
US11721837B2 (en) 2017-09-06 2023-08-08 Samsung Sdi Co., Ltd. Lithium secondary battery including fluoroethylene carbonate in electrolyte
CN114245943A (zh) * 2019-12-24 2022-03-25 宁德时代新能源科技股份有限公司 二次电池及含有该二次电池的装置
US20220352552A1 (en) * 2021-04-21 2022-11-03 Prime Planet Energy & Solutions, Inc. Electrolyte solution for non-aqueous electrolyte secondary battery, and non-aqueous electrolyte secondary battery
WO2025201436A1 (fr) * 2024-12-17 2025-10-02 惠州亿纬锂能股份有限公司 Électrolyte et batterie

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