WO2017020431A1 - Électrolyte non aqueux de batterie au lithium-ion et batterie au lithium-ion - Google Patents

Électrolyte non aqueux de batterie au lithium-ion et batterie au lithium-ion Download PDF

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Publication number
WO2017020431A1
WO2017020431A1 PCT/CN2015/091507 CN2015091507W WO2017020431A1 WO 2017020431 A1 WO2017020431 A1 WO 2017020431A1 CN 2015091507 W CN2015091507 W CN 2015091507W WO 2017020431 A1 WO2017020431 A1 WO 2017020431A1
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Prior art keywords
ion battery
carbonate
lithium ion
electrolyte
compound
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PCT/CN2015/091507
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English (en)
Chinese (zh)
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石桥
林木崇
谌谷春
胡时光
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深圳新宙邦科技股份有限公司
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Publication of WO2017020431A1 publication Critical patent/WO2017020431A1/fr

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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
    • 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 invention relates to the technical field of lithium ion battery electrolytes, in particular to a lithium ion battery non-aqueous electrolyte and a lithium ion battery.
  • non-aqueous electrolyte lithium-ion batteries have been increasingly used in the 3C consumer electronics market, and with the development of new energy vehicles, non-aqueous electrolyte lithium-ion batteries are increasingly becoming the power supply system for automobiles. popular. Although these non-aqueous electrolyte batteries have been put to practical use, they have not been satisfactory in durability, especially at a high temperature of 45 ° C for a short service life. Especially for power vehicles and energy storage systems, non-aqueous electrolyte lithium-ion batteries require normal operation in cold regions, and high temperature performance.
  • the non-aqueous electrolyte is a key factor affecting the high and low temperature performance of the battery.
  • the additive in the non-aqueous electrolyte is particularly important for the performance of the high-low temperature performance of the battery.
  • the currently practical non-aqueous electrolyte uses a conventional film-forming additive such as vinylene carbonate (VC) to ensure excellent cycle performance of the battery.
  • VC vinylene carbonate
  • VC vinylene carbonate
  • Patent document US6919141B2 discloses a phosphate non-aqueous electrolyte additive containing an unsaturated bond, which can reduce the irreversible capacity of a lithium ion battery and improve the cycle performance of the lithium battery.
  • the patent document 201410534841.0 also discloses a novel film-forming additive for a phosphate compound containing a triple bond, which not only improves high temperature cycle performance, but also significantly improves storage performance.
  • the scientific and technological workers in the field found that the passivation film formed by the three-bond phosphate ester additive at the electrode interface is poor in conductivity, resulting in large interfacial impedance, significantly degrading low temperature performance, and inhibiting nonaqueous lithium ions. The application of the battery under low temperature conditions.
  • the present invention provides a lithium ion battery nonaqueous electrolyte having high temperature characteristics and low impedance, and further provides a lithium ion battery including the above lithium ion battery nonaqueous electrolyte.
  • a lithium ion battery nonaqueous electrolyte comprising Aqueous organic solvent, lithium salt and additives, the above additives include substances containing the following compounds (A) and (B):
  • R 1 , R 2 and R 3 are each independently selected from a hydrocarbon group having 1 to 4 carbon atoms, and at least one of R 1 , R 2 and R 3 is an unsaturated hydrocarbon group having a hydrazone bond;
  • the above compound (A) accounts for 0.1% to 2%, preferably 0.2% to 1% by weight based on the total weight of the above electrolyte; and the above compound (B) accounts for 0.1% to 5% of the total weight of the above electrolyte. %, preferably 0.2% to 1%.
  • the ratio of the weight of the above compound (B) to the above electrolyte solution to the weight of the above compound (A) to the above electrolyte solution is equal to or more than 0.2.
  • the above compound (A) is selected from one or more of the following compounds 1 to 6,
  • the nonaqueous organic solvent is a mixture of a cyclic carbonate and a chain carbonate
  • the cyclic carbonate is selected from the group consisting of ethylene carbonate, propylene carbonate and butylene carbonate.
  • the above chain carbonate is selected from the group consisting of dimethyl carbonate, diethyl carbonate, and carbonic acid One or more of ethyl ester and methyl propyl carbonate.
  • the above lithium salt is selected from the group consisting of LiPF 6 , LiBF 4 , LiSbF 6 , LiAsF 6 , LiN(SO 2 CF 3 ) 2 , LiN(SO 2 C 2 F 5 ) 2 , LiC (SO 2 ) One or more of CF 3 ) 3 and LiN(SO 2 F) 2 .
  • the above additive further includes one or more of vinylene carbonate, 1,3-propane sultone, fluoroethylene carbonate, and vinyl ethylene carbonate.
  • a lithium ion battery comprising a positive electrode, a negative electrode and a separator interposed between the positive electrode and the negative electrode, and further comprising the lithium ion battery nonaqueous electrolyte of the first aspect.
  • the above positive electrode is selected from the group consisting of LiCoO 2 , LiNiO 2 , LiMn 2 O 4 , LiCo 1-y M y O 2 , LiNi 1-y M y O 2 , LiMn 2-y M y O 4 and one of 2 LiNi x Co y Mn z M 1-xyz O , or two or more thereof, wherein, M is selected Fe, Co, Ni, Mn, Mg, Cu, Zn, Al, Sn, B, Ga, Cr One or more of Sr, V and Ti, and 0 ⁇ y ⁇ 1, 0 ⁇ x ⁇ 1, 0 ⁇ z ⁇ 1, x + y + z ⁇ 1.
  • the above-described lithium ion battery has a charge cutoff voltage greater than or equal to 4.35V.
  • the lithium ion battery non-aqueous electrolyte of the present invention contains the compound (A), can form a film in the positive and negative electrodes, effectively protects the positive and negative electrodes, and improves the high-temperature performance of the lithium ion battery, particularly the high-temperature cycle performance; Trimethylsilane) phosphate is mainly used to reduce the battery impedance and improve the low temperature performance of the battery.
  • the lithium ion battery nonaqueous electrolyte of the present invention achieves lower impedance, better low temperature performance and high temperature performance of the lithium ion battery by the combination of the compound (A) and tris(trimethylsilane) phosphate.
  • One embodiment of the present invention provides a lithium ion battery nonaqueous electrolyte comprising a nonaqueous organic solvent, a lithium salt and an additive, the above additive comprising a substance containing the following compounds (A) and (B):
  • R 1 , R 2 and R 3 are each independently selected from a hydrocarbon group having 1 to 4 carbon atoms, and at least one of R 1 , R 2 and R 3 is an unsaturated hydrocarbon group having a hydrazone bond;
  • the compound (A) accounts for 0.1% to 2% by weight of the total electrolyte solution, preferably 0.2% to 1%; and the compound (B) accounts for 0.1% by weight of the total electrolyte solution. 5%, preferably 0.2% to 1%.
  • 0.1% to 2% of the compound (A) is added, which can form a film on the positive and negative electrodes, effectively protect the positive and negative electrodes, and improve the high-temperature performance of the lithium ion battery, particularly the high-temperature cycle performance.
  • the content of the compound (A) is less than 0.1%, the film forming effect of the positive and negative electrodes is poor, and the performance is not improved as expected; when the content is more than 2%, the film formation at the electrode interface is performed. Thicker, it will seriously increase the battery impedance and degrade the battery performance.
  • TMSP tris(trimethylsilane) phosphate
  • the lithium ion battery achieves lower impedance, better low temperature performance, and high temperature performance by the combination of the compound (A) and TMSP.
  • the ratio of the weight of the above compound (B) to the above electrolyte solution to the weight of the above compound (A) to the above electrolyte solution is equal to or more than 0.2.
  • the ratio is less than 0.2, the effect of reducing the impedance is limited, and the low temperature performance of the battery cannot be effectively improved.
  • the above compound (A) is selected from one or more of the following compounds 1 to 6,
  • the nonaqueous organic solvent is a mixture of a cyclic carbonate and a chain carbonate
  • the cyclic carbonate is selected from the group consisting of ethylene carbonate, propylene carbonate and butylene carbonate.
  • the above chain carbonate is one or more selected from the group consisting of dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate and methyl propyl carbonate.
  • a mixture of a high dielectric constant cyclic carbonate organic solvent and a low viscosity chain carbonate organic solvent is used as a solvent for a lithium ion battery electrolyte, so that the organic solvent mixture has high ionic conductivity and high at the same time. Dielectric constant and low viscosity.
  • the above lithium salt is selected from the group consisting of LiPF 6 , LiBF 4 , LiSbF 6 , LiAsF 6 , LiN(SO 2 CF 3 ) 2 , LiN(SO 2 C 2 F 5 ) 2 , LiC (SO) One or two or more of 2 CF 3 ) 3 and LiN(SO 2 F) 2 , and the lithium salt is preferably a mixture of LiPF 6 or LiPF 6 and other lithium salts.
  • the above additives further include vinylene carbonate (VC), 1,3-propane sultone (1,3-PS), fluoroethylene carbonate (FEC), and vinyl carbonate.
  • VC vinylene carbonate
  • 1,3-propane sultone (1,3-PS) 1,3-propane sultone
  • FEC fluoroethylene carbonate
  • VEC vinyl esters
  • the above film-forming additive can form a more stable SEI film on the surface of the graphite negative electrode, thereby significantly improving the cycle performance of the lithium ion battery.
  • One embodiment of the present invention provides a lithium ion battery comprising a positive electrode, a negative electrode, and a separator interposed between the positive electrode and the negative electrode, and further includes the lithium ion battery nonaqueous electrolyte of the first aspect.
  • the above positive electrode is selected from the group consisting of LiCoO 2 , LiNiO 2 , LiMn 2 O 4 , LiCo 1-y M y O 2 , LiNi 1-y M y O 2 , LiMn 2-y M y O 4 and LiNi x Co y Mn z M 1 -xyz O 2 in one or two or more, wherein, M is selected Fe, Co, Ni, Mn, Mg, Cu, Zn, Al, Sn, B, Ga, One or more of Cr, Sr, V, and Ti, and 0 ⁇ y ⁇ 1, 0 ⁇ x ⁇ 1, 0 ⁇ z ⁇ 1, x + y + z ⁇ 1.
  • the lithium ion battery has a charge cutoff voltage greater than or equal to 4.35V.
  • the positive electrode material is LiNi 0.5 Co 0.2 Mn 0.3 O 2
  • the negative electrode material is artificial graphite
  • the charge cutoff voltage of the lithium ion battery is equal to 4.35V.
  • the concentration is 1 mol/L, and then 0.5% of the compound 1 based on the total mass of the electrolyte is added (the compound 1, the compound 2 in the specific examples refers to the corresponding numbered compound listed above, the following examples)
  • the phosphate compound shown, and 0.5% of TMSP based on the total mass of the electrolyte are examples of the phosphate compound shown, and 0.5% of TMSP based on the total mass of the electrolyte.
  • the positive active material lithium nickel cobalt manganese oxide LiNi 0.5 Co 0.2 Mn 0.3 O 2 , conductive carbon black Super-P and binder polyvinylidene fluoride (PVDF) were mixed at a mass ratio of 93:4:3, and then they were mixed.
  • Dispersion in N-methyl-2-pyrrolidone (NMP) gave a positive electrode slurry. The slurry was uniformly coated on both sides of the aluminum foil, dried, calendered and vacuum dried, and the aluminum lead wire was welded by an ultrasonic welder to obtain a positive electrode plate having a thickness of 120-150 ⁇ m.
  • the negative active material artificial graphite, conductive carbon black Super-P, binder styrene butadiene rubber (SBR) and carboxymethyl cellulose (CMC) were mixed at a mass ratio of 94:1:2.5:2.5, and then dispersed.
  • SBR binder styrene butadiene rubber
  • CMC carboxymethyl cellulose
  • a polyethylene microporous film having a thickness of 20 ⁇ m is placed as a separator between the positive electrode plate and the negative electrode plate, and then a sandwich structure composed of a positive electrode plate, a negative electrode plate and a separator is wound, and the wound body is flattened and placed in a square aluminum.
  • the lead wires of the positive and negative electrodes are respectively welded to the corresponding positions of the cover plate, and the cover plate and the metal shell are welded together by a laser welding machine to obtain a battery core to be injected.
  • the electrolyte prepared above is injected into the cell through the injection hole, and the amount of the electrolyte is required to fill the gap in the cell. Then proceed according to the following steps: 0.05C constant current charging for 3min, 0.2C constant current charging for 5min, 0.5C constant current charging for 25min, after 1hr of rest, shaping and sealing, then further charging with constant current of 0.2C to 4.35V, leaving at room temperature After 24 hr, it was discharged at a constant current of 0.2 C to 3.0 V.
  • the battery was placed in an oven at a constant temperature of 45 ° C, charged at a constant current of 1 C to 4.35 V and then charged at a constant voltage until the current dropped to 0.1 C, and then discharged at a constant current of 1 C to 3.0 V, thus circulating for 500 weeks, recording
  • the discharge capacity of the first week and the discharge capacity of the 500th week are calculated by the following formula. Hold rate:
  • Capacity retention rate discharge capacity at week 500 / discharge capacity at week 1 * 100%
  • the formed battery was charged to 4.35 V at a normal temperature with a constant current of 1 C, and the initial discharge capacity of the battery was measured. Then, after storage at 60 ° C for 30 days, the battery was discharged to 3 V at 1 C, and the holding capacity and recovery capacity of the battery were measured. Calculated as follows:
  • Battery capacity retention rate (%) retention capacity / initial capacity ⁇ 100%;
  • Battery capacity recovery rate (%) recovery capacity / initial capacity ⁇ 100%.
  • the formed battery was charged to 4.35 V with a constant current of 1 C at 25 ° C, and then discharged to 3.0 V with a constant current of 1 C, and the discharge capacity was recorded. Then, 1C constant current and constant voltage were charged to 4.35V, and after being placed in an environment of -20 ° C for 12 hours, a constant current of 0.3 C was discharged to 3.0 V, and the discharge capacity was recorded.
  • Table 1 shows the high temperature cycle performance, high temperature storage performance and low temperature performance of the test except that 0.5% of Compound 1 was replaced with 0.5% of Compound 2 in the preparation of the electrolyte.
  • Table 1 shows the high temperature cycle performance, high temperature storage performance and low temperature performance of the test except that 0.5% of Compound 1 was replaced with 0.5% of Compound 4 in the preparation of the electrolyte.
  • Table 1 shows the high temperature cycle performance, high temperature storage performance and low temperature performance of the test except that 0.5% of compound 1 was replaced with 0.5% of compound 5 in the preparation of the electrolyte.
  • Example 4 The same as in Example 1, except that 1% of vinylene carbonate (VC) was additionally added to the preparation of the positive electrode material LiNi 0.5 Co 0.2 Mn 0.3 O 2 to LiNi 0.8 Co 0.15 Al 0.05 O 2 and the electrolytic solution.
  • VC vinylene carbonate
  • the high temperature cycle performance was tested in the same manner as in Example 1 except that 1% of vinylene carbonate (VC) was additionally added to the preparation of the positive electrode material LiNi 0.5 Co 0.2 Mn 0.3 O 2 for LiCoO 2 and the electrolytic solution.
  • VC vinylene carbonate
  • the high temperature tested was the same as in Example 1 except that 1% of vinylene carbonate (VC) was additionally added to the preparation of the positive electrode material LiNi 0.5 Co 0.2 Mn 0.3 O 2 for LiMn 2 O 4 and the electrolytic solution.
  • VC vinylene carbonate
  • Example 1 In addition to replacing the positive electrode material LiNi 0.5 Co 0.2 Mn 0.3 O 2 with LiNi 1/3 Co 1/3 Mn 1/3 O 2 and the electrolyte, 0.5% of compound 1 and 0.5% of TMSP were replaced by 1%. Other than Example 1, the data of the high temperature cycle performance, high temperature storage performance and low temperature performance of the test were as shown in Table 4 except for the vinylene carbonate (VC).
  • VC vinylene carbonate
  • the addition of tris(trimethylsilane) phosphate to the nonaqueous electrolyte of the lithium ion battery of the present invention enables the lithium ion battery to obtain lower impedance, better low temperature performance and high temperature performance.

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Abstract

L'invention concerne un électrolyte non aqueux d'une batterie au lithium-ion et une batterie au lithium-ion. L'électrolyte comprend un solvant organique non aqueux, un sel de lithium et un additif. L'additif comprend des substances contenant les composés suivants (A) et (B) : (A), où R1, R2, R3 sont indépendamment choisis parmi des groupes hydrocarbonés ayant 1 à 4 atomes de carbone respectivement, et au moins l'un des éléments parmi R1, R2, R3 est un groupe hydrocarboné insaturé contenant une liaison triple ; (B) tris (triméthylsilyl) phosphate. L'électrolyte non aqueux de la batterie au lithium-ion permet à la batterie au lithium-ion d'avoir une impédance inférieure et de meilleures performances à basse température et à haute température.
PCT/CN2015/091507 2015-08-03 2015-10-09 Électrolyte non aqueux de batterie au lithium-ion et batterie au lithium-ion WO2017020431A1 (fr)

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CN201510481660.0A CN105161763A (zh) 2015-08-03 2015-08-03 一种锂离子电池非水电解液及锂离子电池
CN201510481660.0 2015-08-03

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CN113948768A (zh) * 2020-07-15 2022-01-18 浙江中蓝新能源材料有限公司 一种硅烷类添加剂及含该添加剂的电解液和锂离子电池
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CN111384442A (zh) * 2018-12-29 2020-07-07 浙江省化工研究院有限公司 一种电池电解液正极成膜添加剂及使用该添加剂的电解液和锂离子电池
CN111384442B (zh) * 2018-12-29 2023-09-12 浙江省化工研究院有限公司 一种电池电解液正极成膜添加剂及使用该添加剂的电解液和锂离子电池
CN113948768A (zh) * 2020-07-15 2022-01-18 浙江中蓝新能源材料有限公司 一种硅烷类添加剂及含该添加剂的电解液和锂离子电池
CN114122491A (zh) * 2020-08-31 2022-03-01 深圳新宙邦科技股份有限公司 锂离子电池
CN114583243A (zh) * 2020-11-30 2022-06-03 深圳新宙邦科技股份有限公司 锂离子电池
CN114695956A (zh) * 2020-12-28 2022-07-01 深圳新宙邦科技股份有限公司 一种非水电解液及电池

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