CN104934637A - High voltage lithium ion battery nonaqueous electrolytic solution - Google Patents

High voltage lithium ion battery nonaqueous electrolytic solution Download PDF

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Publication number
CN104934637A
CN104934637A CN201410107830.4A CN201410107830A CN104934637A CN 104934637 A CN104934637 A CN 104934637A CN 201410107830 A CN201410107830 A CN 201410107830A CN 104934637 A CN104934637 A CN 104934637A
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China
Prior art keywords
fluoro
carbonate
formula
electrolytic solution
linear carbonate
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CN201410107830.4A
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Chinese (zh)
Inventor
晨晖
王格日勒图
李卫
其鲁
廖细英
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Scarlett Inagh Chemical Technology (beijing) Co Ltd
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Scarlett Inagh Chemical Technology (beijing) Co Ltd
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Priority to CN201410107830.4A priority Critical patent/CN104934637A/en
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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
    • H01M10/0569—Liquid materials characterised by the solvents
    • 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
    • H01M10/0568—Liquid materials characterised by the solutes
    • 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

Abstract

The present invention provides a high voltage lithium ion secondary battery nonaqueous solution electrolytic solution, and the nonaqueous solution electrolytic solution comprises 10 to 30% by volume of a cyclic carbonate, 40 to 60% by volume of a chain carbonate, 20-30% by volume of a fluorinated chain ether or a fluorinated chain carbonate nonaqueous electrolytic solution solvent and an electrolyte lithium salt with the concentration of 0.8M-1.5M. The nonaqueous solution electrolytic solution can improve the compatibility of a positive electrode material of the a high voltage lithium ion secondary battery in the voltage range of 3.5-5.0V so as to effectively improve the charge discharge capacity and cycle stability of the high voltage lithium ion secondary battery, and the process is simple and easy to implement.

Description

A kind of high-voltage lithium ion batteries nonaqueous electrolytic solution
Technical field
The present invention relates to electrolyte of lithium-ion secondary battery field, a kind of nonaqueous electrolytic solution solvent and the nonaqueous electrolytic solution comprising this solvent of high-voltage lithium ion secondary battery.
Technical background
Energy crisis and serious problem of environmental pollution force the mankind to find the life style of more energy-conserving and environment-protective.Under energy historical background, lithium rechargeable battery is as the superior secondary power supply of current combination property, it is high that it has operating voltage, specific capacity is large, have extended cycle life, low and the environment amenable advantage of self-discharge rate, its range of application is from small-sized portable type electronic product (smart mobile phone, bluetooth earphone etc.) be extended to energy traffic aspect (large-scale energy storage device, hybrid vehicle, pure electric automobile etc.), this namely to lithium rechargeable battery in energy density, have higher requirement in the aspect such as cycle life and security performance, also be the emphasis of research at present.
But lithium ion anode material is the characteristic such as energy density and specific power directly affecting lithium rechargeable battery.High-voltage anode material is as LiNi xmn (2-x)o 4, LiMnPO 4, LiCoPO 4etc. having higher voltage platform (4.0 ~ 5.0V), but encounter lot of challenges in actual applications, except improving except the chemical property of material by doping, the method such as coated, developing the high voltage type electrolyte system matched with it is also another kind ofly need one of difficult point of solution.As the organic electrolyte such as conventional organic electrolyte 1.0M EC:EMC:DMC=1:1:1wt, 1.0M EC:EMC=3:7wt, EC:DMC=1:1wt, under high voltage condition, oxidation Decomposition can be produced with high-voltage anode surface, the oxidative decomposition of organic electrolyte self also can impel the deteriorative reaction of positive electrode simultaneously, cannot obtain stable charge and discharge platform and higher cycle efficieny.
Summary of the invention
The present invention is to provide a kind of nonaqueous electrolytic solution solvent of high-voltage lithium ion secondary battery and comprises the nonaqueous electrolytic solution of this solvent, under voltage range (3.5 ~ 5.0V), has stable charging/discharging voltage platform, higher cycle efficieny.
The present invention relates to a kind of high-voltage lithium ion secondary battery nonaqueous solution electrolysis liquid, this nonaqueous solution electrolysis liquid includes nonaqueous electrolytic solution solvent and (IV) electrolyte lithium salt of (I) cyclic carbonate, (II) linear carbonate, (III) fluoro chain ether or fluoro linear carbonate.
Described (I) cyclic carbonate is the cyclic carbonate solvents of at least one be selected from the cyclic carbonate shown in formula shown in Fig. 1 (X).
M in formula 1 ~ 6for :-H(M 1) ,-F(M 2) ,-CF 3(M 3) ,-CF 2cF 3(M 4) ,-CH 2cF 3(M 5) ,-CH 2cF (CF 3) 2(M 6) at least one, it can improve effect and the high voltage performance of dielectric constant and affect high temperature performance.
Described (II) linear carbonate is selected from least one carbonic ester in dimethyl carbonate (DMC) or methyl ethyl carbonate (EMC), and its boiling point is high, viscosity is low, and cryogenic property is better.
Described (III) fluoro chain ether or fluoro linear carbonate are selected from least one in the fluoro chain ether shown in formula (Y1) or the fluoro linear carbonate shown in formula (Y2);
Formula (Y1): Rf 1oRf 2
In formula (Y1), Rf 1and Rf 2identical or different, Rf 1carbon number be the fluoro-alkyl of 1 ~ 4, Rf 2carbon number be the fluoro-alkyl of 2 ~ 4, its carbon atom more than 4 (or too much), too much can not increase the viscosity of solvent on the contrary, reduces, thus affect charge/discharge capacity and cycle performance to electrolyte lithium salt dissolubility.
Described Rf 1such as :-CF 3,-CF 2cF 3,-CH 2cF 3,-CHFCF 3,-CF 2cF 2cF 3,-CF 2cF 2cF 2cF 3deng; Rf 2such as :-CF 2cF 3,-CH 2cF 3,-CF 2cF 2cF 3,-CF 2cF 2cF 2cF 3deng.
Described (Y1) exemplifies: CF 3cF 2oCF 2cF 3, (Y1a), CF 3cF 2oCHFCF 3(Y1b) etc.
Formula (Y2): Rf 3oCOORf 4
In formula (Y2), Rf 3and Rf 4identical or different, Rf 3and Rf 4carbon number be 1 ~ 4 alkyl or fluoro-alkyl, Rf 3and Rf 4in at least one be fluoro-alkyl, it improves speed characteristic, improves dissolubility and have good compatibility with (I) cyclic carbonate.
Described Rf 3such as :-CH 3,-CH 2cH 3,-CH 2cH 2cH 3,-CH 2cH 2cH 2cH 3,-CF 3,-CF 2cF 3,-CH 2cF 3,-CF 2cF 2cF 3,-CF 2cF 2cF 2cF 3deng.Rf 4such as :-CF 3,-CF 2cF 3,-CH 2cF 3,-CF 2cF 2cF 3,-CF 2cF 2cF 2cF 3deng.
Described (Y2) exemplifies: CF 3cH 2oCOOCF 2cF 2cF 3(Y2a), CF 3oCOOCH 2cH 3(Y2b) etc.
The described nonaqueous electrolytic solution solvent containing (I) cyclic carbonate, (II) linear carbonate, (III) fluoro chain ether or fluoro linear carbonate, when its (I) cyclic carbonate, (II) linear carbonate are set to 100 volume % with (III) fluoro chain ether or fluoro linear carbonate three kinds of nonaqueous electrolytic solution solvents totals, (I) cyclic carbonate contains 10 ~ 30 volume %, its this kind solvent very few (lower than 10%), then electrolyte lithium salt dissolubility is reduced, desired design concentration can not be reached.And on the other hand, this kind solvent too much (higher than 30%), when lower temperature (-40 DEG C ~-20 DEG C), easily can solidify, the cryogenic property of nonaqueous electrolytic solution directly can be affected.(II) linear carbonate contains 40 ~ 60 volume %, although this kind solvent effectively improves with the compatibility of (I) cyclic carbonate, improves electrolyte lithium salt solvent borne, while content is too much, oxidative resistance reduction, burning-point also decline.(III) fluoro chain ether or fluoro linear carbonate contain 20 ~ 30 volume %, this kind solvent too much can increase electrolyte viscosity, reduce electrolyte lithium salt dissolubility and with (I) cyclic carbonate, (II) linear carbonate solvent compatibility, lamination may be produced, if this kind solvent is very few can reduce cryogenic property and anti-flammability.
Described (IV) electrolyte lithium salt is selected from lithium hexafluoro phosphate (LiPF 6) and trifluoromethyl sulfonic acid lithium (LiN (SO 2cF 3) 2) at least one or mixed, its lithium salt is 0.8M ~ 1.5M, because electrolyte combination property is considered preferentially to elect lithium hexafluoro phosphate (LiPF as 6) be 1.0M.
Advantage of the present invention is: the compatibility that can improve electrolyte and high-voltage anode, reduces the decomposition of electrolyte on high-voltage anode material surface in charging process, makes positive electrode have stable charging/discharging voltage platform, higher cycle efficieny; And technique is simple, easy to implement, be suitable for suitability for industrialized production, has a extensive future.
Accompanying drawing explanation
Fig. 1 is the structural formula of formula (X).
Fig. 2 is LiNi prepared by embodiment 1 electrolyte 0.5mn 1.5o 4battery charging and discharging curve chart.
Fig. 3 is LiNi prepared by embodiment 1 and comparative example electrolyte 0.5mn 1.5o 4the charge-discharge performance figure of battery.
Fig. 4 is embodiment 1 ~ 6 and comparative example different component proportioning and electrochemical property test result.
Embodiment
Exemplify embodiment to be described further the present invention, but the present invention is not limited in these embodiments.
Embodiment 1
By electrolyte lithium salt (IV) LiPF 6be dissolved in solvent (I) XM 1/ solvent (II) DMC/ solvent (III) Y1a(volume % is 30/40/30) mixed solvent in obtain solution, its LiPF 6concentration be 1.0M, fully stir, prepare high-voltage lithium ion secondary battery nonaqueous solution electrolysis liquid of the present invention.
Embodiment 2
By electrolyte lithium salt (IV) LiPF 6be dissolved in solvent (I) XM 2/ solvent (II) DMC/ solvent (III) Y1b(volume % is 25/50/25) mixed solvent in obtain solution, its LiPF 6concentration 1.0M, fully stir, prepare high-voltage lithium ion secondary battery nonaqueous solution electrolysis liquid of the present invention.
Embodiment 3
By electrolyte lithium salt (IV) LiPF 6be dissolved in solvent (I) XM 3/ solvent (II) EMC/ solvent (III) Y2a(volume % is 20/55/25) mixed solvent in obtain solution, its LiPF 6concentration 1.0M, fully stir, prepare high-voltage lithium ion secondary battery nonaqueous solution electrolysis liquid of the present invention.
Embodiment 4
By electrolyte lithium salt (IV) LiPF 6be dissolved in solvent (I) XM 4/ solvent (II) EMC/ solvent (III) Y2a(volume % is 10/60/30) mixed solvent in obtain solution, its LiPF 6concentration 1.0M, fully stir, prepare high-voltage lithium ion secondary battery nonaqueous solution electrolysis liquid of the present invention.
Embodiment 5
By electrolyte lithium salt (IV) LiPF 6be dissolved in solvent (I) XM 5/ solvent (II) DMC/ solvent (III) Y1a+Y2a(volume % is 27/53/10+10) mixed solvent in obtain solution, its LiPF 6concentration 1.0M, fully stir, prepare high-voltage lithium ion secondary battery nonaqueous solution electrolysis liquid of the present invention.
Embodiment 6
By electrolyte lithium salt (IV) LiPF 6be dissolved in solvent (I) XM 6/ solvent (II) EMC/ solvent (III) Y1a(volume % is 25/47/28) mixed solvent in obtain solution, its LiPF 6concentration 1.0M, fully stir, prepare high-voltage lithium ion secondary battery nonaqueous solution electrolysis liquid of the present invention.
Comparative example
By electrolyte lithium salt (IV) LiPF 6be dissolved in solvent (I) XM 1/ solvent (II) EMC(volume % is 30/70) mixed solvent in obtain solution, its LiPF 6concentration 1.0M, fully stir, prepare high-voltage lithium ion secondary battery nonaqueous solution electrolysis liquid of the present invention.
Electrochemical property test
By high-voltage anode material LiNi0.5Mn1.5O4(with reference to capacity 130 ~ 132mAh/g) be uniformly mixed form slurry with acetylene black conductor and PVDF by the mass ratio of 88:6:6, carry out applying on aluminium foil with scraper, coated pole piece carries out 70 DEG C of dryings, continuous 120 DEG C of vacuumize 2h, again blunderbuss become diameter be the pole piece of 14mm, weighing, dry after stand-by, the active material quality of each pole piece is about 6.0 ~ 8.0mg.Subsequently, proceeded to by dried pole piece in the glove box being full of argon gas atmosphere and carry out being assembled into 2032 button batteries, negative pole is metal lithium sheet, the electrolyte of electrolyte prepared by embodiment 1 ~ 6 and comparative example, its charging/discharging voltage interval is under 3.5 ~ 5.0V, 0.3C multiplying power.
Result is as shown in Figure 3 known, charging/discharging voltage interval is 3.5 ~ 5.0V, under 0.3C multiplying power, embodiment 1 ~ 6 and comparative example 1 nonaqueous solution electrolysis liquid are assembled into battery, its specific discharge capacity is respectively: 132.7mAh/g, 131.2mAh/g, 130.2mAh/g, 129.8mAh/g, 132.1mAh/g, 131.6mAh/g, 130.3mAh/g, and after 100 circulations, conservation rate is respectively: 93.8%, 91.6%, 90.7%, 88.5%, 92.6%, 91.3%, 77.6%.

Claims (10)

1. a high-voltage lithium ion secondary battery nonaqueous solution electrolysis liquid, is characterized in that: the nonaqueous electrolytic solution solvent containing (I) cyclic carbonate, (II) linear carbonate, (III) fluoro chain ether or fluoro linear carbonate and (IV) electrolyte lithium salt.
2. (I) cyclic carbonate according to claim 1, is characterized in that: be selected from one or more cyclic carbonate solvents in the cyclic carbonate shown in formula (X),
Formula (X)
In formula, M is :-H ,-F ,-CF 3,-CF 2cF 3,-CH 2cF 3,-CH 2cF (CF 3) 2in one or more.
3. according to (II) linear carbonate described in claim 1 ~ 2, it is characterized in that: be selected from one or more carbonic esters in dimethyl carbonate (DMC) or methyl ethyl carbonate (EMC).
4. according to (III) fluoro chain ether described in claim 1 ~ 3 or fluoro linear carbonate, it is characterized in that: be selected from one or more in the fluoro chain ether shown in formula (Y1) or the fluoro linear carbonate shown in formula (Y2);
Formula (Y1): Rf 1oRf 2
In formula (Y1), Rf 1and Rf 2identical or different, Rf 1carbon number be the fluoro-alkyl of 1 ~ 4, Rf 2carbon number be the fluoro-alkyl of 2 ~ 4;
Formula (Y2): Rf 3oCOORf 4
In formula (Y2), Rf 3and Rf 4identical or different, Rf 3and Rf 4carbon number be 1 ~ 4 alkyl or fluoro-alkyl, Rf 3and Rf 4in one or more are fluoro-alkyls.
5. according to the nonaqueous electrolytic solution solvent containing (I) cyclic carbonate, (II) linear carbonate, (III) fluoro chain ether or fluoro linear carbonate described in claim 1 ~ 4, it is characterized in that: when (I) cyclic carbonate, (II) linear carbonate are set to 100 volume % with (III) fluoro chain ether or fluoro linear carbonate three kinds of nonaqueous electrolytic solution solvents totals, (I) cyclic carbonate contains 10 ~ 30 volume %, (II) linear carbonate contains 40 ~ 60 volume %, and (III) fluoro chain ether or fluoro linear carbonate contain 20 ~ 30 volume %.
6. according to (IV) electrolyte lithium salt described in claim 1 ~ 5, it is characterized in that: (IV) electrolyte lithium salt is selected from lithium hexafluoro phosphate (LiPF 6) and trifluoromethyl sulfonic acid lithium (LiN (SO 2cF 3) 2) in one or more.
7. according to (IV) electrolyte lithium salt described in claim 1 ~ 6, it is characterized in that: the concentration of (IV) electrolyte lithium salt is 0.8M ~ 1.5M.
8. a high-voltage lithium ion secondary battery nonaqueous solution electrolysis liquid, it comprises nonaqueous electrolytic solution solvent described in claim 1 ~ 7 and electrolyte lithium salt.
9. a high-voltage lithium ion secondary battery, it uses nonaqueous solution electrolysis liquid according to claim 8.
10. according to the high-voltage lithium ion secondary battery described in claim 1 ~ 9, it is characterized in that: high-voltage anode material is selected from LiNi 0.5mn 1.5o 4, LiCoPO 4there are one or more in high voltage platform (4.0 ~ 5.0V).
CN201410107830.4A 2014-03-21 2014-03-21 High voltage lithium ion battery nonaqueous electrolytic solution Pending CN104934637A (en)

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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN109546221A (en) * 2018-11-30 2019-03-29 福建省劲德电源科技有限公司 A kind of lithium-ion battery electrolytes of wide temperature electric discharge
CN114024036A (en) * 2021-11-05 2022-02-08 中南大学 Low-concentration lithium ion battery electrolyte and lithium ion battery prepared from same

Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN101584075A (en) * 2006-12-22 2009-11-18 大金工业株式会社 Nonaqueous electrolyte solution
CN102479977A (en) * 2010-11-29 2012-05-30 张家港市国泰华荣化工新材料有限公司 Non-aqueous electrolyte solution and application thereof
CN103460491A (en) * 2011-03-28 2013-12-18 日本电气株式会社 Secondary battery and electrolyte

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN101584075A (en) * 2006-12-22 2009-11-18 大金工业株式会社 Nonaqueous electrolyte solution
CN102479977A (en) * 2010-11-29 2012-05-30 张家港市国泰华荣化工新材料有限公司 Non-aqueous electrolyte solution and application thereof
CN103460491A (en) * 2011-03-28 2013-12-18 日本电气株式会社 Secondary battery and electrolyte

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN109546221A (en) * 2018-11-30 2019-03-29 福建省劲德电源科技有限公司 A kind of lithium-ion battery electrolytes of wide temperature electric discharge
CN114024036A (en) * 2021-11-05 2022-02-08 中南大学 Low-concentration lithium ion battery electrolyte and lithium ion battery prepared from same

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