CN114665152A - Electrolyte containing fluoroalkyl borate compound and battery composed of electrolyte - Google Patents

Electrolyte containing fluoroalkyl borate compound and battery composed of electrolyte Download PDF

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CN114665152A
CN114665152A CN202210352711.XA CN202210352711A CN114665152A CN 114665152 A CN114665152 A CN 114665152A CN 202210352711 A CN202210352711 A CN 202210352711A CN 114665152 A CN114665152 A CN 114665152A
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electrolyte
carbonate
halogenated
battery
combination
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孙春胜
朱少华
申海鹏
郭营军
李新丽
顿温新
赖定坤
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Xianghe Kunlun New Energy Materials Co ltd
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Xianghe Kunlun New Energy 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
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
    • H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
    • H01G11/54—Electrolytes
    • H01G11/58—Liquid electrolytes
    • H01G11/64—Liquid electrolytes characterised by 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
    • H01M10/0567—Liquid materials characterised by the additives

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

Abstract

The invention discloses an electrolyte containing a fluoroalkyl borate compound and a battery consisting of the electrolyte. The electrolyte comprises an electrolyte, an organic solvent and a fluorinated alkyl borate compound shown as a formula I. The electrolyte is added with the compound shown in the formula I, so that when the electrolyte is used in a battery, the multi-aspect performance of the battery is improved, the 3C discharge rate at normal temperature in the battery is more than 79.5 percent at the 3C charge rate, the 1C discharge rate at-20 ℃ is more than 80.8 percent at the normal temperature, the capacity retention rate of 3C charge/1C discharge cycle at 800 times of normal temperature cycle is more than 82.6 percent, the capacity retention rate of 3C charge/1C discharge cycle at high temperature of 45 ℃ is more than 81.8 percent at 800 times of high temperature 3C charge/1C discharge cycle, and the comprehensive performance is excellent.

Description

Electrolyte containing fluoroalkyl borate compound and battery composed of electrolyte
Technical Field
The invention belongs to the technical field of electrochemical energy storage, and particularly relates to electrolyte containing fluoroalkyl borate compounds and a battery comprising the electrolyte.
Background
Currently, organic electrolyte materials used in the lithium battery industry are mainly alkyl carbonate compounds and LiPF6Lithium salt system, the performance of which is greatly reduced at high temperature (above 60 ℃), while the power battery for electric automobile requires a higher working temperature range (about-30 to 80 ℃); moreover, the alkyl carbonate organic electrolyte material has high flammability, so that the safety has great hidden trouble; especially in the field of hybrid and all-electric automotive applications, long-term cycling problems and safety are important factors that limit the practical application of these materials.
The electrolyte is an important component of the lithium ion battery, and plays a role in transmitting lithium ions between the positive electrode and the negative electrode. The safety, charge-discharge cycle, working temperature range and charge-discharge capacity of the battery are all important in relation to the electrochemical performance of the electrolyte. The traditional functional components in the electrolyte play a key role in prolonging the service life of the battery, but no long-term effective measure is provided for delaying or inhibiting the generation of lithium dendrites, so that the safety performance of the battery and the service life of charge-discharge cycles are greatly influenced.
CN106033824B discloses an electrolyte containing tris (trimethylsilyl) borate, and a high-voltage lithium ion battery containing the electrolyte has excellent normal-temperature cycle performance, high-temperature storage performance and low-temperature discharge performance. However, the oxidation potential of this substance is low, and it is difficult to satisfy the requirement of stable charge and discharge of the battery at a voltage of 4.3V or more.
The requirement of the battery on high energy density and high temperature and high voltage stability is higher and higher, so that it is important to develop an electrolyte for improving the stable circulation of the battery under the voltage of more than 4.3V.
Disclosure of Invention
The invention aims to provide an electrolyte containing a fluoroalkyl borate compound and a battery comprising the electrolyte.
An electrolyte containing a fluoroalkyl borate compound, the electrolyte comprising an electrolyte, an organic solvent, and a fluoroalkyl borate compound represented by formula I:
Figure BDA0003581415660000021
the electrolyte comprises XClO4、XPF6、XBF4、XTFSI、XFSI、XBOB、XODFB，XCF3SO3Or XAsF6Any one or a combination of at least two of them; wherein X is Li, Na or K.
The organic solvent includes any one of carbonate, carboxylate, fluorocarboxylate, propionate, fluoroether or aromatic hydrocarbon or a combination of at least two thereof.
The carbonate includes a halogenated carbonate and/or a non-halogenated carbonate; the non-halogenated carbonate comprises any one or the combination of at least two of ethylene carbonate, propylene carbonate, diethyl carbonate, dimethyl carbonate or ethyl methyl carbonate; the halogenated carbonate comprises any one or the combination of at least two of fluoroethylene carbonate, difluoroethylene carbonate, difluoropropylene carbonate, ethyl trifluoroacetate, trifluoroethyl methyl carbonate, trifluoromethyl ethylene carbonate, 4-trifluoromethyl ethylene carbonate, chloroethylene carbonate, bis (2,2, 2-trifluoroethyl) carbonate, methyl trifluoropropionate, 3,3, 3-trifluoro ethyl acetate, 2-trifluoromethyl methyl benzoate, 4,4, 4-trifluoro ethyl butyrate or 1,1,1,3,3, 3-hexafluoroisopropyl acrylate.
The carboxylic ester comprises halogenated carboxylic ester and/or non-halogenated carboxylic ester; the non-halogenated carboxylic acid ester comprises any one or a combination of at least two of propyl butyrate, propyl acetate, isopropyl acetate, butyl propionate, isopropyl propionate, ethyl butyrate, methyl propionate, ethyl propionate or propyl propionate; the halogenated carboxylic acid ester comprises any one or a combination of at least two of propyl fluorobutyrate, propyl fluoroacetate, isopropyl fluoroacetate, butyl fluoropropionate, isopropyl fluoropropionate, ethyl fluorobutyrate, methyl fluoropropionate, ethyl fluoropropionate and propyl fluoropropionate.
The fluorine ether is a fluorine ether having 7 or less carbon atoms.
The aromatic hydrocarbon comprises halogenated aromatic hydrocarbon and/or non-halogenated aromatic hydrocarbon; the halogenated aromatic hydrocarbon comprises any one or the combination of at least two of monofluorobenzene, difluorobenzene, 1,3, 5-trifluorobenzene, trifluorotoluene, 2-fluorotoluene or 2, 4-dichlorotrifluorotoluene.
The weight percentage of the electrolyte in the electrolyte is 8-49%; the weight percentage of the organic solvent in the electrolyte is 1-85%; the fluorine-containing alkyl borate compound shown in the formula I accounts for 0.01-50% of the electrolyte.
A battery comprises the electrolyte.
The battery comprises a lithium ion battery, a sodium ion battery, a potassium ion battery or a super capacitor; the negative electrode material of the lithium ion battery comprises any one or the combination of at least two of graphite, soft carbon, hard carbon, a composite material of monocrystalline silicon and graphite, a composite material of silicon oxide and graphite, and lithium titanate or niobium pentoxide.
The invention has the beneficial effects that: the electrolyte is added with the compound shown in the formula I, so that when the electrolyte is used in a battery, the multi-aspect performance of the battery is improved, the 3C discharge rate at normal temperature in the battery is more than 79.5 percent at the 3C charge rate, the 1C discharge rate at-20 ℃ is more than 80.8 percent at the normal temperature, the capacity retention rate of 3C charge/1C discharge cycle at 800 times of normal temperature cycle is more than 82.6 percent, the capacity retention rate of 3C charge/1C discharge cycle at high temperature of 45 ℃ is more than 81.8 percent at 800 times of high temperature 3C charge/1C discharge cycle, and the comprehensive performance is excellent.
Detailed Description
In order that the invention may be more fully understood, reference will now be made to the following description. This invention may, however, be embodied in many different forms and should not be construed as limited to the embodiments set forth herein. Rather, these embodiments are provided so that this disclosure will be thorough and complete.
The general test platform used in the examples is as follows: the anode of the experiment adopts a binder PVDF-S5130, a composite conductive agent Super-P/KS-6 (the mass ratio of Super-P: KS-6 is 2: 1), a 622 nickel cobalt manganese ternary anode material or a lithium cobaltate anode material and a solvent NMP (N-methyl-2-pyrrolidone), and the cathode adopts C-P15, a conductive agent Super-P solvent CMC, H2O and SBR (styrene butadiene rubber) are used as raw materials, slurry is prepared by adopting a wet pulping process respectively, the viscosity of a positive electrode is adjusted to 10000-13000 mPa & s, the viscosity of a negative electrode is adjusted to 1500-3000 mPa & s, the designed N/P ratio is 1.12, the capacity is 1671mAh, a lithium ion soft package battery is prepared by coating, slicing, rolling, slitting, drying at 140 ℃ for 8h, sticking an adhesive tape, rolling a battery core and drying at 80 ℃ for 48h, then the lithium ion soft package battery is prepared by injecting and sealing the lithium ion battery according to different electrolyte formulas, standing for 24h, forming, primary final sealing, aging and secondary final sealing, and then the battery is tested in cycle performance and safety performance.
The fluorochemical silane substituent compounds used in examples 1-7 were custom-made (99.5% purity) from Shijiazhuang Santa Clay chemical.
The electrolyte compositions of examples 1 to 11 and comparative examples 1 and 2 are shown in table 1.
The compositions of the electrolytes provided in examples 1 to 11 and comparative examples 1 and 2 were all in weight ratio and each contained 1% VC and 1% PS, as shown in table 1.
TABLE 1 (all in the table are weight ratios)
Figure BDA0003581415660000051
The electrolytes described in examples 1-10 and comparative example 1 were added to a 1.67Ah lithium ion battery containing a graphite negative electrode material (fir P15), NCM622 nickel cobalt manganese ternary material;
the following tests were performed:
(1) charge rate performance: the 1C current is 1.67A, and the 3C current is 5.01A; the charge and discharge potential range is 2.75V-4.35V. The charging rate of the 3C at the normal temperature is a ratio of a capacity C2 of the 3C constant current charging to a 1C constant current charging capacity C1.
(2) Cycle performance: the range of charging and discharging potential is 2.75V-4.35V, the charging current is 3C (5.01A) to 4.35V, the constant voltage charging of 4.35V is carried out until the cut-off current is less than or equal to 0.02C (0.0334A), after standing for 5 minutes, 1C (1.67A) is discharged to 2.75V, and the standing is carried out for 5 minutes; thus, the charge and discharge are cycled.
(3) Low-temperature discharge performance: the 1C (1.67A) discharge capacity at 25 ℃ was C1, and after full charge at 4.35V and freezing at-20 ℃ for 4 hours, the discharge was 1C (1.67A) to 2.75V, and the discharge capacity was C2. The discharge rate at-20 ℃ was C2/C1.
The electrolyte described in example 11 and comparative example 2 was added to a battery whose negative electrode material was a silicon-carbon negative electrode material (fibrate S420) and whose positive electrode material was 4.5V lithium cobalt oxide to prepare a 1.85Ah lithium ion battery;
the following tests were performed:
(1) charge rate performance: the 1C current is 1.85A, and the 3C current is 5.55A; the charge and discharge potential range is 2.75V-4.50V. The charging rate of the 3C at the normal temperature is a ratio of a capacity C2 of the 3C constant current charging to a 1C constant current charging capacity C1.
(2) Cycle performance: the range of charging and discharging potential is 2.75V-4.50V, the charging current is 3C (5.55A) to 4.50V, the charging is carried out at 4.50V with constant voltage until the cut-off current is less than or equal to 0.02C (0.037A), after standing for 5 minutes, 1C (1.85A) is discharged to 2.75V, and the standing is carried out for 5 minutes; thus, the charge and discharge are cycled.
(3) Low-temperature discharge performance: the 1C (1.85A) discharge capacity at 25 ℃ at room temperature was designated as C1, and after full charge at 4.5V and freezing at-20 ℃ for 4 hours, the discharge was 1C (1.85A) to 2.75V, and the discharge capacity was designated as C2. The discharge rate at-20 ℃ was C2/C1.
The test results are summarized in tables 2 to 4.
TABLE 2
Figure BDA0003581415660000061
Figure BDA0003581415660000071
TABLE 3
Figure BDA0003581415660000072
Figure BDA0003581415660000081
TABLE 4
Figure BDA0003581415660000082
As can be seen from the analysis of the data in tables 2 to 4, when the electrolyte disclosed by the invention is used in a battery, the multi-aspect performance of the battery is improved by adding the compound shown in the formula I, the 3C discharge rate of the battery obtained by the invention at normal temperature is more than 79.5%, the 1C discharge rate of the battery at 20 ℃ is more than 80.8%, the capacity retention rate of the 3C charge/1C discharge cycle of the battery subjected to 800 cycles at normal temperature is more than 82.6%, the capacity retention rate of the battery subjected to 800 cycles at high temperature of 45 ℃ is more than 81.8%, and the comprehensive performance is excellent.
As can be seen from the analysis of comparative example 1 and example 5, the performance of comparative example 1 is inferior to that of example 5, and the electrolyte added with the compound shown in formula I can improve the comprehensive performance of the battery. Analysis of comparative example 2 and example 11 revealed similar results. The electrolyte added with the compound shown in the formula I is proved to be beneficial to taking a silicon-containing material or graphite as a negative electrode and the charge-discharge cycle performance and the low-temperature discharge performance of a ternary material or a cobalt acid lithium battery.
The above-mentioned embodiments only express several embodiments of the present invention, and the description thereof is more specific and detailed, but not construed as limiting the scope of the invention. It should be noted that, for a person skilled in the art, several variations and modifications can be made without departing from the inventive concept, which falls within the scope of the present invention. Therefore, the protection scope of the present patent shall be subject to the appended claims.

Claims (10)

1. An electrolyte containing a fluoroalkyl borate compound, characterized by comprising an electrolyte, an organic solvent, and a fluoroalkyl borate compound represented by formula I:
Figure FDA0003581415650000011
2. the fluoroalkyl borate containing electrolyte of claim 1 wherein said electrolyte comprises XClO4、XPF6、XBF4、XTFSI、XFSI、XBOB、XODFB，XCF3SO3Or XAsF6Any one or a combination of at least two of them; wherein X is Li, Na or K.
3. The fluoroalkyl borate compound containing electrolyte of claim 1, wherein the organic solvent comprises any one of carbonate, carboxylate, fluorocarboxylate, propionate, fluoroether, or aromatic hydrocarbon or a combination of at least two thereof.
4. The fluoroalkyl borate containing compound electrolyte of claim 1 wherein said carbonate comprises a halogenated carbonate and/or a non-halogenated carbonate; the non-halogenated carbonate comprises any one or the combination of at least two of ethylene carbonate, propylene carbonate, diethyl carbonate, dimethyl carbonate or ethyl methyl carbonate; the halogenated carbonate comprises any one or the combination of at least two of fluoroethylene carbonate, difluoroethylene carbonate, difluoropropylene carbonate, ethyl trifluoroacetate, trifluoroethyl methyl carbonate, trifluoromethyl ethylene carbonate, 4-trifluoromethyl ethylene carbonate, chloroethylene carbonate, bis (2,2, 2-trifluoroethyl) carbonate, methyl trifluoropropionate, 3,3, 3-trifluoro ethyl acetate, 2-trifluoromethyl methyl benzoate, 4,4, 4-trifluoro ethyl butyrate or 1,1,1,3,3, 3-hexafluoroisopropyl acrylate.
5. The fluoroalkyl borate containing compound electrolyte of claim 1 wherein said carboxylate comprises halogenated carboxylate and/or non-halogenated carboxylate; the non-halogenated carboxylic acid ester comprises any one or a combination of at least two of propyl butyrate, propyl acetate, isopropyl acetate, butyl propionate, isopropyl propionate, ethyl butyrate, methyl propionate, ethyl propionate or propyl propionate; the halogenated carboxylic acid ester comprises any one or a combination of at least two of propyl fluorobutyrate, propyl fluoroacetate, isopropyl fluoroacetate, butyl fluoropropionate, isopropyl fluoropropionate, ethyl fluorobutyrate, methyl fluoropropionate, ethyl fluoropropionate and propyl fluoropropionate.
6. The electrolytic solution containing a fluoroalkyl borate compound according to claim 1, wherein the fluoroether is a fluoroether having 7 or less carbon atoms.
7. The fluoroalkyl borate containing compound electrolyte of claim 1 wherein said aromatic hydrocarbon comprises halogenated aromatic hydrocarbons and/or non-halogenated aromatic hydrocarbons; the halogenated aromatic hydrocarbon comprises any one or the combination of at least two of monofluorobenzene, difluorobenzene, 1,3, 5-trifluorobenzene, trifluorotoluene, 2-fluorotoluene or 2, 4-dichlorotrifluorotoluene.
8. The fluoroalkyl borate containing compound electrolyte of claim 1 wherein the weight percentage of said electrolyte in said electrolyte is 8-49%; the weight percentage of the organic solvent in the electrolyte is 1-85%; the fluorine-containing alkyl borate compound shown in the formula I accounts for 0.01-50% of the electrolyte.
9. A battery comprising the electrolyte of any one of claims 1-8.
10. The battery of claim 1, wherein the battery comprises a lithium ion battery, a sodium ion battery, a potassium ion battery, or a supercapacitor; the negative electrode material of the lithium ion battery comprises any one or the combination of at least two of graphite, soft carbon, hard carbon, a composite material of monocrystalline silicon and graphite, a composite material of silicon oxide and graphite, and lithium titanate or niobium pentoxide.
CN202210352711.XA 2022-04-06 2022-04-06 Electrolyte containing fluoroalkyl borate compound and battery composed of electrolyte Pending CN114665152A (en)

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Publication number Priority date Publication date Assignee Title
US20170365855A1 (en) * 2016-06-21 2017-12-21 Samsung Electronics Co., Ltd. Lithium battery
CN108123172A (en) * 2016-11-29 2018-06-05 宁德时代新能源科技股份有限公司 Electrolyte and secondary lithium battery
CN108242558A (en) * 2016-12-27 2018-07-03 丰田自动车株式会社 Lithium rechargeable battery
CN114188605A (en) * 2021-12-06 2022-03-15 湖南时代安能新能源科技有限公司 Lithium ion battery electrolyte for silicon-carbon cathode and lithium ion battery containing electrolyte

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20170365855A1 (en) * 2016-06-21 2017-12-21 Samsung Electronics Co., Ltd. Lithium battery
CN108123172A (en) * 2016-11-29 2018-06-05 宁德时代新能源科技股份有限公司 Electrolyte and secondary lithium battery
CN108242558A (en) * 2016-12-27 2018-07-03 丰田自动车株式会社 Lithium rechargeable battery
CN114188605A (en) * 2021-12-06 2022-03-15 湖南时代安能新能源科技有限公司 Lithium ion battery electrolyte for silicon-carbon cathode and lithium ion battery containing electrolyte

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Application publication date: 20220624