CN106058316A - High-nickel ternary lithium ion power battery electrolyte and high-nickel ternary lithium ion power battery - Google Patents

High-nickel ternary lithium ion power battery electrolyte and high-nickel ternary lithium ion power battery Download PDF

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Publication number
CN106058316A
CN106058316A CN201610653856.8A CN201610653856A CN106058316A CN 106058316 A CN106058316 A CN 106058316A CN 201610653856 A CN201610653856 A CN 201610653856A CN 106058316 A CN106058316 A CN 106058316A
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lithium ion
power battery
lithium
electrolyte
ion power
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吕家斌
仰永军
潘立宁
万华平
胡巍
曾庆鹏
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Guangzhou Tinci Materials Technology Co Ltd
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Dongguan City Kai Xin Battery 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
    • H01M2220/00—Batteries for particular applications
    • H01M2220/20—Batteries in motive systems, e.g. vehicle, ship, plane
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries

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

Abstract

The invention discloses a high-nickel ternary lithium ion power battery electrolyte and a high-nickel ternary lithium ion power battery. The electrolyte includes a non-aqueous organic solvent, a lithium salt, a conductive additive, a film forming additive and an infiltration additive, wherein the conductive additive is lithium difluorophosphate, the film forming additive is ethylene sulfate, and the infiltration additive is at least one of fluorophosphazene and fluoroethylene carbonate; and synergism and mutual promotion of the three additives makes an excellent SEI film be formed on the surface of an electrode and effectively promotes all dynamic processes in the lithium ion battery. The power battery electrolyte has the advantages of good lithium ion transmission characteristic, good oxidation resistance, guaranteeing of high power characteristic and good cycle performances of the power battery, and high safety.

Description

A kind of nickelic ternary lithium ion power battery electrolyte and nickelic ternary lithium ion power Battery
Technical field
The present invention relates to field of lithium ion battery, be specifically related to a kind of nickelic ternary lithium ion power battery electrolyte and height Nickel ternary lithium-ion-power cell.
Background technology
Lithium ion battery is owing to having high working voltage, high-energy-density, long-life and advantages of environment protection, by extensively It is applied to the fields such as 3C digital product, electric tool, electric automobile, Aero-Space.Particularly in electric automobile field, 2015 Since present explosive growth.According to country " energy-conservation and new-energy automobile industrial development planning ", it is desirable to electrokinetic cell energy is close Degree reaches more than 300Wh/Kg at the year two thousand twenty.
Electric automobile is as a kind of vehicles, and its distance travelled, acceleration, climbing capacity and security performance etc. are all Concerned emphasis, these aspects depend primarily on the performance of the electrokinetic cell as critical component.Lithium ion cell positive material Material aspect, ternary material (NCM, NCA) is owing to having higher gram volume and compacted density, and in terms of energy density, advantage shows Write, favored by more and more automobile production manufacturers.For reaching higher battery energy density requirement, ternary in above-mentioned planning Material is inevitable to be developed toward nickelic, high voltage direction, needs exploitation to adapt additive to solve electrokinetic cell in electrolyte field Electrolyte decomposition problem.
But, along with ternary material develops to nickelic direction, material water absorption strengthens, stability also decreases, especially Being under the high temperature conditions, the catalytic action of nickel element can accelerate the decomposition of conventional electrolysis liquid, thus causes whole battery system The decline of energy, particularly capacity is decayed rapidly.Add in electrode surface reactivity, interpolation both positive and negative polarity film forming to reduce electrolyte Adding agent is to improve electrode/electrolyte interface compatibility most efficient method.
Lithium-ion-power cell power out-put characteristic is as an important indicator, by the multiple kinetics of inside lithium ion cell Process determines, wherein relevant with electrolyte: the transmission in the electrolytic solution of a. lithium ion；B. lithium ion passes through active material The diffusion of grain surface SEI film；Above-mentioned two process and lithium ion transport properties, SEI membrane impedance and electrolyte in electrolyte are to electricity Pole material wellability is closely related.
The Chinese patent of application publication number CN 104332650 A disclose a kind of nickelic tertiary cathode material system lithium from The high-voltage electrolyte of sub-battery, it comprises methane-disulfonic acid methylene ester and fluorinated ethylene carbonate, wherein positive pole film former methane Disulfonic acid methylene ester impedance is relatively big, is unfavorable for lithium ion battery high-power output, and nickelic battery safety is the most to be improved.This Outward, in existing art solutions, infiltration additive is seldom used to promote that lithium ion is transmitted across in the kinetics of electrode interface Journey.In consideration of it, a kind of electrolyte of necessary offer is to ensure the high power of nickelic ternary electrokinetic cell, long circulating and high safety Property characteristic.
Summary of the invention
In view of problem present in background technology, it is an object of the invention to provide a kind of nickelic ternary lithium ion power electricity Pond electrolyte and nickelic ternary lithium-ion-power cell, power battery electrolyte has good lithium ion transport properties and oxytolerant Change characteristic, it is ensured that the high power characteristic of electrokinetic cell and good cycle performance, the most also there is higher safety.
To achieve these goals, the technical solution used in the present invention is:
A kind of nickelic ternary lithium ion power battery electrolyte, including: non-aqueous organic solvent, lithium salts, conductive additive-two Lithium fluophosphate, film for additive-sulfuric acid vinyl ester；And infiltration additive, described infiltration additive is fluoro phosphonitrile and fluoro In ethylene carbonate at least one.
In technique scheme, described fluoro phosphonitrile is for having the compound of structure shown in formula (1):
Wherein, R1And R2Represent fluorine atom, or alkyl, oxyl or the phenoxy group that carbon number is 1～6 respectively, or hydrogen is former Subdivision or the alkyl, oxyl or the phenoxy group that are all replaced by fluorine；M represents the integer of 3-6, R1And R2Can be independently of one another For different groups between cells, and formula (1) is chain or circulus.
Preferably, described conductive additive quality accounts for described electrolyte gross mass 0.1%～1.0%.
Preferably, described film for additive quality accounts for described electrolyte gross mass 0.3%～3.0%.
Preferably, described infiltration additive quality accounts for described electrolyte gross mass 0.1%～10.0%.
Preferably, described non-aqueous organic solvent is cyclic carbonate and the mixture of chain ester, and described cyclic carbonate selects One or more in ethylene carbonate, Allyl carbonate, described chain ester is selected from dimethyl carbonate, diethyl carbonate, carbon Acid methyl ethyl ester and methyl propyl carbonate, propyl propionate, ethyl propionate in one or more.
Preferably, described lithium salts be lithium hexafluoro phosphate, double fluorine sulfimide lithium and difluorine oxalic acid boracic acid lithium one or both And above mixing lithium salts, the mol ratio of three kinds of lithium salts is 1:0～0.2:0～0.2.
Preferably, described electrolyte also comprise vinylene carbonate, 1,3-propane sultone, succinonitrile, adiponitrile, second One or more in double (propionitrile) ether of glycol.
The present invention also provides for a kind of nickelic ternary lithium-ion-power cell, including anode pole piece, cathode pole piece and above-mentioned Lithium ion power battery electrolyte, described anode pole piece includes plus plate current-collecting body and positive pole diaphragm, and described cathode pole piece includes bearing Pole collector and cathode membrane, described positive pole diaphragm includes positive active material, conductive agent and binding agent, described cathode pole piece bag Including negative electrode active material, conductive agent and binding agent, described positive active material is LiNi1-x-y-zCoxMnyAlzO2, wherein: 0≤x ≤ 0.5,0≤y≤0.5,0≤z≤0.5 and 0≤x+y+z≤0.5；Described negative electrode active material be Delanium, native graphite, Lithium titanate or SiOwThe Si-C composite material being composited with graphite.
Preferably, at least one during described positive active material is nickle cobalt lithium manganate, nickel cobalt lithium aluminate；Described negative pole is lived Silicone content accounting 0.001%～20% in property material.
It is an advantage of the current invention that:
1, conductive additive difluorophosphate adds in electrolyte, can improve lithium ion transport properties in electrolyte, subtract Few lithium hexafluoro phosphate consumption, improves lithium ion battery dynamics, promotes electrokinetic cell capacity and exports with power, the most permissible Improve high-temperature lithium ion battery performance and low temperature output performance.
2, compare conventional additives, and film for additive sulfuric acid vinyl ester has higher reactivity, can preferentially decompose Film forming, in its catabolite, S-O component can effectively modify and improve SEI film component and structure, is formed and easily to pass lithium, high stable SEI film, protects tertiary cathode material structural stability, reduces the destruction of metallic element anticathode layer structure, promotes battery and follows Ring performance and high-temperature behavior；The SEI membrane impedance that sulfur-containing compound participates in being formed simultaneously is relatively low, is conducive to promoting electrokinetic cell output Power characteristic and cryogenic property.
3, the present invention creatively have employed fluorine-containing infiltration additive, adds fluoro phosphonitrile or fluoro ethylene in electrolyte Alkene ester, it is possible to decrease contact angle, strengthens electrode/electrolyte interface wellability, beneficially lithium ion and transmits in the kinetics of electrode interface Process, improves electrokinetic cell capacity and plays and long circulation life.
4, further, in invention, fluoro phosphonitrile also has good flame-retarding characteristic, is conducive to improving power safety performance, It is particularly well-suited to nickelic tertiary cathode material system electrokinetic cell；Fluorinated ethylene carbonate also has excellent negative terminal surface film forming Characteristic, can significantly improve cycle performance of battery, is particularly well-suited to part doping SiOwSi-C composite material system electrokinetic cell.
Accompanying drawing explanation
Fig. 1 be the lithium ion power battery electrolyte of embodiment 1 and comparative example 1 prepare 4.20V graphite/ LiNi0.5Co0.2Mn0.3O2Electrokinetic cell formation process capacitance-voltage differential curve comparison diagram.
Detailed description of the invention
Being described further the present invention below in conjunction with embodiment, the enforcement of the present invention includes but not limited to following embodiment party Formula.Any change without departing from present invention or replacement can be understood by the person skilled in the art, all should be in the present invention Protection domain within.
Embodiment 1
Electrolyte quota step: in the glove box of full argon, by ethylene carbonate, diethyl carbonate and methyl ethyl carbonate Ester mixes for EC:DEC:EMC=3:2:5 in mass ratio, and being then slowly added to concentration to mixed solution is 1.0mol/L's Lithium hexafluoro phosphate, is eventually adding difluorophosphate (LiPO based on electrolyte gross weight 0.3wt%2F2), 1wt% sulphuric acid ethylene Ester (DTD), 2wt% ethyoxyl five fluorine ring three phosphonitrile, 0.5wt% vinylene carbonate (VC), obtain embodiment 1 after stirring Lithium-ion battery electrolytes.
The 4.20V graphite that the lithium ion power battery electrolyte injection process prepared fully is dried/ LiNi0.5Co0.2Mn0.3O2Electrokinetic cell (energy density > 200Wh/kg) or 4.20V silicon-carbon composite graphite/ LiNi0.8Co0.15Al0.05O2In electrokinetic cell (energy density > 250Wh/kg), battery through 45 DEG C shelve, high-temperature clamp chemical conversion After secondary sealing, carry out conventional partial volume.
1) normal-temperature circulating performance test: at 25 DEG C, the battery after partial volume is charged to 4.20V by 1C constant current constant voltage, cut-off Electric current 0.02C, then presses 1C constant-current discharge to 3.0V, circulates according to this, calculates the 3000th cycle and follow after 3000 circulations of charge/discharge Ring capability retention.Computing formula is as follows:
3000th circulation volume conservation rate (%)=(the 3000th cyclic discharge capacity/first cyclic discharge capacity) × 100%；
2)-10 DEG C/1C low temperature discharge: at 25 DEG C, battery is pressed 1.0C discharge and recharge once, cut-off current 0.02C, record 1C discharge capacity at 25 DEG C.Then press 1.0C constant current constant voltage to be full of, full electricity battery is placed in the calorstat of-10 DEG C that to shelve 16 little Shi Hou, is discharged to 3.0V by 1.0C, 1C discharge capacity at record-10 DEG C, and calculates-10 DEG C/1C electric discharge ratio.Computing formula is such as Under:
-10 DEG C/1C electric discharge ratio (%)=-10 DEG C of discharge capacity/25 DEG C discharge capacity × 100%.
3) battery 5C multiplying power discharging test: the battery after partial volume is charged to 4.20V, cut-off current by 1C constant current constant voltage 0.02C, then presses 1C constant-current discharge to 3.0V, record 1C discharge capacity；It is charged to 4.20V the most again, cut-off by 1C constant current constant voltage Electric current 0.02C, presses 5C constant-current discharge to 3.0V, record 5C discharge capacity after battery is fully charged.Calculate electrokinetic cell 5C/1C times Rate electric discharge ratio, computing formula is as follows:
5C/1C multiplying power discharging ratio (%)=(battery 5C discharge capacity/battery 1C discharge capacity) × 100%.
Embodiment 2～10 and comparative example 1～6
In embodiment 2～10 and comparative example 1～6, except battery plus-negative plate system is pressed with electrolyte functional additive composition Outside adding shown in table 1, other is the most same as in Example 1.Table 1 is the battery plus-negative plate body of embodiment 1～10 and comparative example 1～6 System, electrolyte functional additive composition and battery performance test result:
Table 1
In above-mentioned table 1, it is as follows that corresponding title write a Chinese character in simplified form in each chemical substance letter:
LiPO2F2(difluorophosphate), DTD (sulfuric acid vinyl ester), FEC (fluorinated ethylene carbonate).
In Fig. 1, embodiment 1 understands with the battery forming process capacitance-voltage differential curve contrast in comparative example 1: embodiment After electrolyte adds DTD in 1, vinylene carbonate can be had precedence over and decompose film forming, and be obviously reduced the decomposition of VC under higher voltage Film strength；In conjunction with embodiment 1 in table 1 and comparative example 1 test result, show that the SEI film properties that DTD participates in being formed is more excellent, steady Qualitative higher, can effectively promote battery cryogenic property, cycle performance and multiplying power discharging property.
In table 1, test result shows: contrast simply uses each comparative example of two of which additive, makes in the present invention simultaneously With conductive additive, film for additive and each embodiment battery cryogenic property, cycle performance and the multiplying power discharging of infiltration additive Performance has and promotes in various degree.
In summary, by by conductive additive, film for additive and the synergism of three kinds of additives of infiltration additive, Mutually promote, excellent SEI film can be formed at electrode surface, and effectively facilitate each dynamic process of inside lithium ion cell, protect The high power characteristic of electrokinetic cell and good cycle performance are demonstrate,proved.
It is above illustrating of the section Example for the present invention, is not intended to limit the scope of the claims of the present invention, All changes without departing from present invention or replacement, all should be within protection scope of the present invention.

Claims (10)

1. a nickelic ternary lithium ion power battery electrolyte, including: non-aqueous organic solvent, lithium salts, conductive additive-difluoro Lithium phosphate, film for additive-sulfuric acid vinyl ester；And infiltration additive, described infiltration additive is fluoro phosphonitrile and fluoro carbon In vinyl acetate at least one.
2. according to the nickelic ternary lithium ion power battery electrolyte described in claim 1, it is characterised in that described fluoro phosphorus Nitrile is for having the compound of structure shown in formula (1):
Formula (1)
Wherein, R1And R2 Represent fluorine atom, or alkyl, oxyl or the phenoxy group that carbon number is 1 ~ 6, or hydrogen atom respectively Some or all of alkyl, oxyl or the phenoxy group replaced by fluorine；M represents the integer of 3-6, R1And R2Can be each independently Different groups between cells, and formula (1) is chain or circulus.
3. according to the nickelic ternary lithium ion power battery electrolyte described in claim 1, it is characterised in that described conduction adds Add agent quality and account for described electrolyte gross mass 0.1% ~ 1.0%.
4. according to the nickelic ternary lithium ion power battery electrolyte described in claim 1, it is characterised in that described film forming adds Add agent quality and account for described electrolyte gross mass 0.3% ~ 3.0%.
5. according to the nickelic ternary lithium ion power battery electrolyte described in claim 1, it is characterised in that described infiltration adds Add agent quality and account for described electrolyte gross mass 0.1% ~ 10.0%.
6. according to the nickelic ternary lithium ion power battery electrolyte described in claim 1, it is characterised in that described non-aqueous have Machine solvent is cyclic carbonate and the mixture of chain ester, and described cyclic carbonate is in ethylene carbonate, Allyl carbonate One or more, described chain ester is selected from dimethyl carbonate, diethyl carbonate, Ethyl methyl carbonate and methyl propyl carbonate, propanoic acid One or more in propyl ester, ethyl propionate.
7. according to the nickelic ternary lithium ion power battery electrolyte described in claim 1, it is characterised in that described lithium salts is Lithium hexafluoro phosphate, double fluorine sulfimide lithium and difluorine oxalic acid boracic acid lithium one or both and above mixing lithium salts, three kinds of lithium salts Mol ratio be 1:0 ~ 0.2:0 ~ 0.2.
8. according to the nickelic ternary lithium ion power battery electrolyte described in claim 1, it is characterised in that described electrolyte Also comprise the one in vinylene carbonate, 1,3-propane sultone, succinonitrile, adiponitrile, ethylene glycol bis (propionitrile) ether or Above.
9. a nickelic ternary lithium-ion-power cell, including anode pole piece, cathode pole piece and claim 1 to 8 any one Described lithium ion power battery electrolyte, described anode pole piece includes plus plate current-collecting body and positive pole diaphragm, described cathode pole piece Including negative current collector and cathode membrane, described positive pole diaphragm includes positive active material, conductive agent and binding agent, described negative pole Pole piece includes negative electrode active material, conductive agent and binding agent, it is characterised in that described positive active material is LiNi1-x-y- zCoxMnyAlzO2, wherein: 0≤x≤0.5,0≤y≤0.5,0≤z≤0.5 and 0≤x+y+z≤ 0.5；Described negative electrode active material is Delanium, native graphite, lithium titanate or SiOwThe silicon-carbon being composited with graphite is combined Material.
Nickelic ternary lithium-ion-power cell the most according to claim 9, it is characterised in that described positive active material For at least one in nickle cobalt lithium manganate, nickel cobalt lithium aluminate；Silicone content accounting 0.001% ~ 20% in described negative electrode active material.
CN201610653856.8A 2016-08-10 2016-08-10 High-nickel ternary lithium ion power battery electrolyte and high-nickel ternary lithium ion power battery Pending CN106058316A (en)

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