CN104466245A - Lithium ion battery electrolyte solution composition - Google Patents

Lithium ion battery electrolyte solution composition Download PDF

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Publication number
CN104466245A
CN104466245A CN201310416954.6A CN201310416954A CN104466245A CN 104466245 A CN104466245 A CN 104466245A CN 201310416954 A CN201310416954 A CN 201310416954A CN 104466245 A CN104466245 A CN 104466245A
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China
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ch
electrolyte solution
carbonate
lithium ion
ion battery
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CN201310416954.6A
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Chinese (zh)
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吴晓东
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苏州纳新新能源科技有限公司
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Priority to CN201310416954.6A priority Critical patent/CN104466245A/en
Publication of CN104466245A publication Critical patent/CN104466245A/en

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    • HELECTRICITY
    • H01BASIC ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00Secondary cells; Manufacture thereof
    • H01M10/05Accumulators with non-aqueous electrolyte
    • H01M10/052Li-accumulators
    • H01M10/0525Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • HELECTRICITY
    • H01BASIC ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00Secondary cells; Manufacture thereof
    • H01M10/05Accumulators with non-aqueous electrolyte
    • H01M10/056Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0564Accumulators 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
    • H01M10/0566Liquid materials
    • H01M10/0567Liquid materials characterised by the additives

Abstract

The invention relates to a lithium ion battery electrolyte solution composition, which comprises an electrolyte solution and an additive. The additive is selected from one or more of formula (I) compound: RaM(-X1R1) (-X2R2)...... (-XZRZ) (I), wherein Ra optionally can be C1-C10, preferably C1-C6 alkyl, C3-C6 cycloalkyl, and C6-C10 aryl substituted C1-C10, preferably C1-C6 alkyl, C3-C6 cycloalkyl, or C2-C6 alkenyl or does not exist; R1, R2,... RZ independently and optionally can be C1-C10, preferably C1-C6 alkyl, C3-C6 cycloalkyl, and C6-C10 aryl substituted C1-C10, preferably C1-C6 alkyl, C3-C6 cycloalkyl, or C2-C6 alkenyl; X1, X2,....XZ can independently be O, S, N or P or does not exist; Z is an integer keeping the formula (I) compound electroneutral; and M is Al, B, Be, Mg, Si, Ca, Sr, Ba, Ra or Zr. The invention also relates to a lithium ion battery containing the electrolyte solution composition.

Description

Lithium ion battery electrolyte liquid composite

Technical field

The present invention relates to lithium ion battery, be specifically related to a kind of electrolyte solution composition of lithium ion battery.

Background technology

Since nineteen ninety, Sony corporation of Japan successfully developed lithium ion battery, energy density is high owing to having for lithium ion battery, specific power is large, good cycle, memory-less effect, the feature such as pollution-free, many electronic installations such as such as mobile phone, notebook computer, digital camera are applied widely.Recently, a series of progress that electric automobile power battery research and development obtains, make the application of lithium ion battery further be expanded, have higher requirement to the various aspects such as cycle performance of lithium ion battery, security performance.

Lithium ion battery is made up of positive pole, negative pole, electrolyte and barrier film usually, and wherein positive pole adopts LiCoO usually 2, Li 2mnO 3, LiFePO 4, Li 2fePO 4the positive electrodes such as F are made; Negative material adopts graphite material usually, and the material had been found that at present comprises following several:

The first is carbon negative pole material: the negative material being actually used in lithium ion battery is all carbon materials substantially, as electrographite, native graphite, carbonaceous mesophase spherules, petroleum coke, carbon fiber, thermal decomposed resins carbon etc.[5]

The second is tin base cathode material: tin base cathode material can be divided into oxide and the Sn-polymetallic orefield two kinds of tin.Oxide refers to the oxide of various valence state metallic tin.

The third is lithium-containing transition metal nitride negative material.

4th kind is alloy type negative material: comprise kamash alloy, silicon-base alloy, germanium-base alloy, acieral, antimony-containing alloy, magnesium base alloy and other alloy.

5th kind is nanoscale negative material: CNT (carbon nano-tube), Nanoalloy material.

6th kind of nano material is nanometer oxide material

The lithium ion battery of prior art is very strict to the conditional request of discharge and recharge, and particularly charge-discharge performance is under high pressure poor.It is generally acknowledged, when positive electrode used at present under high pressure charges, positive electrode and electrolyte interact, and easily cause cathode performance to worsen, even battery failure.Therefore this area still needs the technology improving performance of lithium ion battery.

Summary of the invention

The present inventor, through studying widely, finds the performance obviously can improving lithium ion battery by adding special additive in the electrolytic solution unexpectedly.Therefore, the invention provides a kind of electrolyte solution composition of lithium ion battery, it comprises electrolyte solution and additive.Described electrolyte solution can be any electrolyte solution of lithium ion battery, and it comprises electrolyte solute and solvent, and wherein said electrolyte can be any electrolyte for lithium ion battery known in the art, such as lithium perchlorate (LiClO 4), lithium hexafluoro phosphate (LiPF 6), LiBF4 (LiBF 4) etc. or its mixture.Any electrolyte solvent for lithium ion battery that described solvent is known in the art, such as ether, ethylene carbonate, propylene carbonate, diethyl carbonate, methyl ethyl carbonate, dimethyl carbonate etc. or its mixture.Described additive is for being selected from one or more of formula (I) compound:

R aM(-X 1R 1)(-X 2R 2)……(-X ZR Z) (I)

Wherein: R afor optionally can by C 1– C 10preferred C 1– C 6alkyl, C 3– C 6cycloalkyl, C 6-C 10the C that aryl replaces 1– C 10preferred C 1– C 6alkyl, C 3– C 6cycloalkyl or C 2– C 6thiazolinyl or do not exist;

R 1, R 2... R zbe optionally can by C independently of one another 1– C 10preferred C 1– C 6alkyl, C 3– C 6cycloalkyl, C 6-C 10the C that aryl replaces 1– C 10preferred C 1– C 6alkyl, C 3– C 6cycloalkyl or C 2– C 6thiazolinyl;

X 1, X 2... .X zbe O, S, N or P or do not exist independently of one another;

Z is freeze mode (I) compound is electroneutral integer;

M is Al, B, Be, Mg, Si, Ca, Sr, Ba, Ra or Zr.

In a preferred embodiment, the additive of described formula (I) is for being selected from CH 3-Al (-O-CH 3) (-O-CH 3), C 2h 5-B (-O-CH 3) (-O-C 3h 7), CH 3-Si (-O-C 2h 5) (-O-C 2h 5) (-O-C 2h 5), C 2h 5-Si (-O-CH 3) (-O-CH 3) (-O-CH 2-C 6h 5), CH 3-S-Al-(OCH 3) 2, C 2h 5-NH-Al-(OCH 3) 2, CH 3-S-Zr-(OC 3h 7) 3, C 6h 5-CH 2-S-Al-(OCH 3) 2in one or more.

The content of additive of the present invention in electrolyte solution composition is the 0.2-5% of electrolyte solution composition total weight, is preferably 1.0-3.5%.

Any method preparation that electrolyte solution composition of the present invention can adopt prior art known.Such as first can prepare electrolyte solution, then add additive of the present invention and make it dissolve; Or electrolyte solute to be added together with additive in solvent and to make it dissolve.

In one embodiment, first prepare the homogeneous mixture of electrolyte solvent or electrolyte solvent, then electrolyte solute is joined in electrolyte solvent and form electrolyte solution, finally additive of the present invention to be joined in described electrolyte solution and to make it fully dissolve, being formed according to electrolyte solution composition of the present invention.

In electrolyte solution composition of the present invention, described electrolyte is selected from lithium perchlorate (LiClO 4), lithium hexafluoro phosphate (LiPF 6), LiBF4 (LiBF 4) in one or more, its content based on described electrolyte solution from as 0.7mol/l ~ 1.3mol/l.

In electrolyte solution of the present invention, described solvent be selected from ether, ethylene carbonate, propylene carbonate, diethyl carbonate, methyl ethyl carbonate and dimethyl carbonate one or more, be preferably in diethyl carbonate, ethylene carbonate, propylene carbonate, methyl ethyl carbonate and dimethyl carbonate one or more, be particularly preferably in ethylene carbonate and propylene carbonate one or both.When using mixed solvent, the combination solvent of arbitrary proportion can be used, as long as it can dissolution solvent and additive of the present invention fully, such as, can adopt the mixed solvent of following volume ratio in the present invention, ethylene carbonate: diethyl carbonate=1:1; Ethylene carbonate: methyl ethyl carbonate=1:1; Ethylene carbonate: diethyl carbonate: methyl ethyl carbonate=1:1:1; Ethylene carbonate: diethyl carbonate: methyl ethyl carbonate=2:1:2; Ethylene carbonate: diethyl carbonate: methyl ethyl carbonate: propylene carbonate=6:6:7:1 etc.

Electrolyte solution in the present invention can also comprise additive well known in the prior art, such as LiBOB and VC(vinylene carbonate) etc., its content can be such as the 0.2-5% of described electrolyte solution total weight.

In order to make additive of the present invention fully dissolve, the method for this area routine can be used as stirring, heating etc.Equally, in order to make electrolyte solute fully dissolve in a solvent, this area conventional method also can be used as stirring and heating etc.

In one embodiment, the invention provides a kind of lithium ion battery, it comprises positive pole, negative pole, barrier film and according to electrolyte solution composition of the present invention.

In the present invention, positive pole can adopt itself known material in prior art to make, such as spinel lithium manganate, rich lithium phase manganese-based anode material, ternary material etc.Described positive pole can be mixed by one or both.Negative pole can be made up of self known material in prior art, such as, in Delanium, native graphite, hard carbon, lithium titanate one or both.Barrier film can adopt any barrier film of the prior art, such as PE single layer microporous film, PE/PP composite double layer microporous barrier, PP/PE/PP three-layer composite microporous membrane etc.Lithium ion battery of the present invention can also comprise plus plate current-collecting body, such as 15 trifling ~ aluminium foil of 22 microns; And negative current collector, the such as Copper Foil of 7-15 micron.

The present inventor finds, when electrolyte solution composition of the present invention is used for lithium ion battery, in the charge and discharge process of lithium ion battery, the positive pole of lithium ion battery can form uniform film.In a specific embodiment, the thickness of described film is 0.5nm to 10nm, is preferably 1nm to 8nm, is more preferably 2nm to 6nm.

In another embodiment, the invention provides a kind of positive pole of lithium ion battery.Described positive pole comprises conventional lithium ion cell positive matrix and owing to have employed electrolyte solution composition of the present invention and at the film that positive electrode substrate surface is formed after discharge and recharge in this lithium ion battery.

Be not limited to any theory, the present inventor thinks, owing to defining uniform film on the positive pole of lithium ion battery, thus protection lithium ion cell positive, make positive electrode be not easy to react with solute, thus improve the battery performance of lithium ion battery.Be not limited to any theory, the present inventor thinks, additive of the present invention, in positive pole generation oxidation reaction, causes the key between M atom and X atom or the bond fission between M atom and each group, thus form film on positive electrode surface, stop the reaction of positive electrode and electrolyte solution.Meanwhile, this film is excellent ion conductor, electronic body, can suppress the further decomposition of electrolyte, does not harm the transmission of lithium ion between electrolyte and negative pole simultaneously, substantially increases the efficiency for charge-discharge of lithium ion battery.And it is little on internal resistance of cell impact, also improves the cycle performance of battery.Further, what use this this compound has good high and low temperature performance and good anti-overcharge ability and anti-flammability.

Embodiment

Object of the present invention, advantage and disadvantage, make an explanation the non-limitative illustration by preferred embodiment below.These embodiments are only the exemplary embodiments of application technical solution of the present invention, allly take equivalent replacement or equivalent transformation and the technical scheme that formed, all drop within the scope of protection of present invention.

Embodiment 1

The preparation of electrolyte solution composition:

By the CH of 0.2g 3-Al (-O-CH 3) (-O-CH 3) be dissolved in the lithium hexafluoro phosphate of 0.8mol/l at ethylene carbonate: in the solution (99.8g) in dimethyl carbonate=50:50, obtain the electrolyte solution composition of embodiment 1.

Embodiment 2 to 10

The material that employing goes out as shown in Table 1 below and consumption repeat the experiment in embodiment 1, obtain corresponding electrolyte solution composition respectively.

Comparative example 1 to 2

As shown in the table, prepare lithium hexafluoro phosphate respectively at ethylene carbonate: diethyl carbonate=1:1 and ethylene carbonate: the electrolyte solution composition of the solution that the concentration in carbonic acid methylene ester=1:1 is respectively 0.9mol/L and 1.0mol/L as a comparison case in 1 to 2, adds the conventional additives LiBOB of 1.5 % by weight in the electrolyte solution composition wherein in comparative example 2.

Testing example

By the electrolyte solution composition of embodiment 1-10 and comparative example 1-2 as electrolyte, adopt spinel lithium manganate as positive pole; Artificial graphite electrode is as negative pole, and PE single layer microporous film is as barrier film, and the aluminium foil of 18 microns is as plus plate current-collecting body, and the Copper Foil of 10 microns, as negative current collector, prepares lithium ion battery respectively.

LiMn2O4, conductive agent SuperP, binding agent PVDF are configured in the ratio of 93:3:4, slurry solid content is 50%, obtained anode pole piece after aluminium foil slurry being coated in 18 microns being dried roll-in.After the two-sided roll-in of positive plate, thickness is 150 microns (containing aluminium foils).Delanium, conductive electrode SuperP, binding agent PVDF are configured in the ratio of 94:2:4, slurry solid content 45%, obtained cathode pole piece after the electrolytic copper foil being coated in 10 microns being dried roll-in.The capacity ratio of positive/negative plate is 1.0:1.1.Barrier film adopts PE single layer microporous film, thickness 40 microns, porosity 40%.By positive plate, barrier film and negative plate by automatic direction battery winder winding and dry, inject corresponding electrolyte after obtain the corresponding test battery of Soft Roll that design capacity is 5Ah.Prepared by 3 identical batteries for often kind of electrolyte solution composition.

For the battery as above prepared, under the charge-discharge velocity of 0.5C, carry out cycle charge-discharge experiment according to IEC62133 standard, measure the cycle life under different condition respectively.After circulation experiment terminates, take each battery apart, and utilize each positive pole of microexamination.For the battery utilizing the electrolyte solution composition of embodiment 1 to 10 to prepare, positive pole all finds the formation of film.And utilize transmission electron microscope to measure the thickness of its film.Three batteries prepared for utilizing the electrolyte solution composition of each embodiment, get the thickness of its mean value as the film formed in this embodiment.Its thickness is listed in the following table.Do not find in the battery utilizing the electrolyte solution composition of comparative example 1 and 2 to prepare to form film on positive pole.Corresponding experimental data is summarized in following table:

Above data show, electrolyte solution composition of the present invention can form film in charge and discharge process on positive pole, and significantly improve the cycle performance of battery relative to control cell.By comparison, utilizing in the battery do not prepared containing the electrolyte solution composition of special additive of the present invention, film is not formed at positive pole.The cycle performance of the battery utilizing the electrolyte solution composition of comparative example to prepare significantly is inferior to the cycle performance of the battery utilizing electrolyte solution composition of the present invention to prepare, especially compared with the cycle performance under critical conditions, such as, about high-temperature cycle life and high voltage cycle life etc.

The foregoing is only preferred embodiment of the present invention, be not intended to limit protection scope of the present invention.All any amendments done within the spirit and principles in the present invention, equivalent replacement, improvement etc., be all included in protection scope of the present invention.

Claims (10)

1. for an electrolyte solution composition for lithium ion battery, it comprises electrolyte solution and additive, and described additive is for being selected from one or more of formula (I) compound:
R aM(-X 1R 1)(-X 2R 2)……(-X ZR Z) (I)
Wherein: R afor optionally can by C 1– C 10preferred C 1– C 6alkyl, C 3– C 6cycloalkyl, C 6-C 10the C that aryl replaces 1– C 10preferred C 1– C 6alkyl, C 3– C 6cycloalkyl or C 2– C 6thiazolinyl or do not exist;
R 1, R 2... R zbe optionally can by C independently of one another 1– C 10preferred C 1– C 6alkyl, C 3– C 6cycloalkyl, C 6-C 10the C that aryl replaces 1– C 10preferred C 1– C 6alkyl, C 3– C 6cycloalkyl or C 2– C 6thiazolinyl;
X 1, X 2... .X zbe O, S, N or P or do not exist independently of one another;
Z is freeze mode (I) compound is electroneutral integer;
M is Al, B, Be, Mg, Si, Ca, Sr, Ba, Ra or Zr;
The content of described additive is the 0.2-5% of electrolyte solution composition total weight, is preferably 1.0-3.5%.
2. electrolyte solution composition according to claim 1, wherein said electrolyte solution comprises solute and solvent, and described solute is for being selected from lithium perchlorate (LiClO 4), lithium hexafluoro phosphate (LiPF 6), LiBF4 (LiBF 4) in one or more, described solvent be selected from ether, ethylene carbonate, propylene carbonate, diethyl carbonate, methyl ethyl carbonate and dimethyl carbonate one or more, be preferably in diethyl carbonate, ethylene carbonate, propylene carbonate, methyl ethyl carbonate and dimethyl carbonate one or more, be particularly preferably in ethylene carbonate and propylene carbonate one or both.
3. electrolyte solution composition according to claim 2, the content of wherein said solute based on electrolyte solution from as 0.8M ~ 1.3M.
4., according to the electrolyte solution composition of claim 1 – 3, wherein said additive is for being selected from CH 3-Al (-O-CH 3) (-O-CH 3), C 2h 5-B (-O-CH 3) (-O-C 3h 7), C 2h 5-Al (-O-CH 3) (-O-C 10h 21), CH 3-Si (-O-C 2h 5) (-O-C 2h 5) (-O-C 2h 5), C 2h 5-Si (-O-CH 3) (-O-CH 3) (-O-CH 2-C 6h 5), CH 3-S-Al-(OCH 3) 2, C 2h 5-NH-Al-(OCH 3) 2, CH 3-S-Zr-(OC 3h 7) 3, C 6h 5-CH 2-S-Al-(OCH 3) 2in one or more, be preferably selected from CH 3-Si (-O-C 2h 5) (-O-C 2h 5) (-O-C 2h 5), C 2h 5-Si (-O-CH 3) (-O-CH 3) (-O-CH 2-C 6h 5), CH 3-S-Al-(OCH 3) 2in one or more.
5. a lithium ion battery, electrolyte solution composition wherein used comprises electrolyte solution and additive, and described additive is for being selected from one or more of formula (I) compound:
R aM(-X 1R 1)(-X 2R 2)……(-X ZR Z) (I)
Wherein: R afor optionally can by C 1– C 10preferred C 1– C 6alkyl, C 3– C 6cycloalkyl, C 6-C 10the C that aryl replaces 1– C 10preferred C 1– C 6alkyl, C 3– C 6cycloalkyl or C 2– C 6thiazolinyl or do not exist;
R 1, R 2... R zbe optionally can by C independently of one another 1– C 10preferred C 1– C 6alkyl, C 3– C 6cycloalkyl, C 6-C 10the C that aryl replaces 1– C 10preferred C 1– C 6alkyl, C 3– C 6cycloalkyl or C 2– C 6thiazolinyl;
X 1, X 2... .X zbe O, S, N or P or do not exist independently of one another;
Z is freeze mode (I) compound is electroneutral integer;
M is Al, B, Be, Mg, Si, Ca, Sr, Ba, Ra or Zr;
The content of described additive is the 0.2-5% of electrolyte solution composition total weight, is preferably 1.0-3.5%.
6. lithium ion battery according to claim 5, wherein said electrolyte solution comprises solute and solvent, and described solute is for being selected from lithium perchlorate (LiClO 4), lithium hexafluoro phosphate (LiPF 6), LiBF4 (LiBF 4) in one or more, described solvent be selected from ether, ethylene carbonate, propylene carbonate, diethyl carbonate, methyl ethyl carbonate and dimethyl carbonate one or more, be preferably in diethyl carbonate, ethylene carbonate, propylene carbonate, methyl ethyl carbonate and dimethyl carbonate one or more, be particularly preferably in ethylene carbonate, propylene carbonate, methyl ethyl carbonate and dimethyl carbonate one or both.
7. lithium ion battery according to claim 6, the content of wherein said solute relative to described electrolyte solution from as 0.7M ~ 1.3M.
8., according to the lithium ion battery of claim 5 – 7, wherein said additive is for being selected from CH 3-Al (-O-CH 3) (-O-CH 3), C 2h 5-B (-O-CH 3) (-O-C 3h 7), CH 3-Si (-O-C 2h 5) (-O-C 2h 5) (-O-C 2h 5), C 2h 5-Si (-O-CH 3) (-O-CH 3) (-O-CH 2-C 6h 5), CH 3-S-Al-(OCH 3) 2, C 2h 5-NH-Al-(OCH 3) 2, CH 3-S-Zr-(OC 3h 7) 3, C 6h 5-CH 2-S-Al-(OCH 3) 2in one or more, be preferably selected from CH 3-Si (-O-C 2h 5) (-O-C 2h 5) (-O-C 2h 5), C 2h 5-Si (-O-CH 3) (-O-CH 3) (-O-CH 2-C 6h 5), CH 3-S-Al-(OCH 3) 2in one or more.
9. a positive pole for lithium ion battery, described positive pole comprises by LiCoO 2, Li 2mnO 3, LiFePO 4, Li 2fePO 4the positive electrode substrate that one or more materials in F are made, and the film formed in described positive electrode substrate after making electrolyte solution composition according to claim 1 experience charge and discharge process, preferably described film is excellent ion conductor and electronic body, more preferably the thickness of described film is 0.5nm to 10nm, be preferably 1nm to 8nm, be more preferably 2nm to 6nm.
10. a lithium ion battery, comprises positive pole as claimed in claim 9.
CN201310416954.6A 2013-09-13 2013-09-13 Lithium ion battery electrolyte solution composition CN104466245A (en)

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN105119013A (en) * 2015-07-28 2015-12-02 珠海市赛纬电子材料有限公司 Flame retardation-type lithium ion battery electrolyte and lithium ion battery

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Publication number Priority date Publication date Assignee Title
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CN101836312A (en) * 2007-11-21 2010-09-15 株式会社Lg化学 Secondary battery with improved storage characteristics and method for manufacturing the same
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Application publication date: 20150325