CN101394007A - Electrolysis liquid for lithium manganate battery - Google Patents
Electrolysis liquid for lithium manganate battery Download PDFInfo
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- CN101394007A CN101394007A CNA2008102188096A CN200810218809A CN101394007A CN 101394007 A CN101394007 A CN 101394007A CN A2008102188096 A CNA2008102188096 A CN A2008102188096A CN 200810218809 A CN200810218809 A CN 200810218809A CN 101394007 A CN101394007 A CN 101394007A
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- 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
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- Y02E60/10—Energy storage using batteries
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Abstract
The invention discloses electrolyte solution of a manganic acid lithium battery. The electrolyte solution comprises lithium salt, non-aqueous organic solvent, film-forming additive and stabilizing additive, namely seven-methyl two-silazane. Because the stabilizing additive, seven-methyl two-silazane is added into the electrolyte solution, the acidity of the electrolyte solution can be controlled. The cycle life and the high temperature storage performance of a lithium ion battery can be improved by using the electrolyte solution to prepare a battery.
Description
Technical field
The present invention relates to a kind of lithium-ion battery electrolytes, relate in particular to a kind of electrolyte of lithium manganate battery.
Background technology
The secondary cell that generally uses has four kinds at present: lead-acid battery, nickel-cadmium cell, Ni-MH battery and lithium ion battery.Characteristics such as lithium ion battery has that operating voltage height, volume are little, light weight, specific energy height, memory-less effect, self discharge are little, have extended cycle life, environmentally safe, now be widely used as the power supply of pocket valuable household electrical appliance such as mobile phone, portable computer, video camera etc., and in Aeronautics and Astronautics, navigation, artificial satellite, small medical and military domain of communication equipment, progressively substituted traditional battery, be the desirable energy of 21 century development.
Commercial lithium ion battery is at first released in the nineties in 20th century by Sony company.Lithium ion battery mainly is made up of positive electrode, negative material, electrolyte, barrier film four parts, and wherein, electrolyte is the ion conductor that plays conduction between the battery positive and negative electrode, and the performance of itself influences the performance of battery to a great extent.
Spinelle has the three-dimensional tunnel structure and takes off lithium character preferably, its aboundresources, cheap, fail safe good, easy synthetic, nontoxic, environmentally safe, is used as the positive electrode of lithium ion battery widely.There is serious capacity attenuation problem in spinel lithium manganate, especially under hot conditions, its capacity attenuation reason mainly contains: the dissolving of manganese, Jahn-Teller effect and electrolyte decomposition etc., wherein electrolyte is the immediate cause that causes capacity attenuation and cycle performance to worsen to the corrosion of LiMn2O4.
In containing the electrolyte of lithium salts, under the effect of trace water, lithium salts decomposes the generation hydrogen ion, and following reaction: LiMn takes place for hydrogen ion and LiMn2O4
2O
4+ 4H
+→ Li
++ λ-MnO
2+Mn
2++ 2H
2O, the Mn of generation
2+Be dissolved in the electrolyte, the dissolving of manganese not only makes LiMn
2O
4The absolute magnitude of active material reduces, and also can cause LiMn
2O
4The transformation of lattice structure makes LiMn
2O
4Die or the part lose electro-chemical activity, reduce its stability, influence the cycle life of battery.Under the hot conditions, LiMn
2O
4Electrode has the effect that catalytic electrolysis liquid decomposes, and the decomposition of electrolyte can produce hydrogen ion again, and then has promoted the dissolving of manganese.
Number of patent application is 200410062610.0, a kind of method that improves spinel lithium manganate cell volume and cycle performance is disclosed, in electrolyte, add earlier deacidification agent and remove free acid HF in the electrolyte, and then remove after the depickling excessive water in the electrolyte with dehydrating agent.Wherein deacidification agent is one or more mixture or aluminium or the magnesium in the oxide of zinc, aluminium, magnesium, calcium.The oxide of zinc, aluminium, magnesium, calcium, metallic aluminium, magnesium etc. join in the electrolyte as additive, and they will react with the HF of trace in the electrolyte, reduce the content of HF, stop it to the destruction of electrode with to LiPF
6The catalytic action of decomposing improves the stability of electrolyte, thereby improves battery performance.But it is slower that these materials are removed the speed of HF, therefore is difficult to accomplish to stop the destruction of HF to battery performance; And introduce metal impurities easily with metal oxide treated electrolyte.
U.S. Pat 6235431 adopts hexamethyldisiloxane, and (chemical formula is (CH
3)
3SiNHSi (CH
3)
3) as dewatering plumper, its mechanism of action is: (CH
3)
3SiNHSi (CH
3)
3+ H
2O → (CH
3)
3SiOSi (CH
3)
3+ NH
3, the NH of generation
3Can react with HF again, and then reduce the acidity of electrolyte, improve the cycle performance of lithium ion battery.But hexamethyldisiloxane itself is unstable, decomposes easily in air, is difficult for preserving; And itself and H
2The NH that the O reaction generates
3, be combined into NH with HF
4F is very unstable, especially decomposes easily under hot conditions, is difficult to play the purpose that improves the lithium manganate battery high-temperature behavior.
Summary of the invention
Technical problem to be solved by this invention is, a kind of electrolyte of lithium manganate battery is provided, owing to the adding of stabilization additives, can control the acidity of electrolyte in this electrolyte, use this electrolyte to prepare cycle life and high-temperature storage performance that battery can improve lithium ion battery.
The present invention solves the technical scheme that its technical problem adopts:
A kind of electrolyte of lithium manganate battery, this electrolyte comprises: lithium salts, non-aqueous organic solvent, film for additive and heptamethyldisilazane.
The addition of described heptamethyldisilazane is 0.1%~5% of an electrolyte total weight.
The addition of described heptamethyldisilazane is 0.1%~2% of an electrolyte total weight.
Described lithium salts is selected from LiPF
6, LiBF
4, LiClO
4Or any or several combinations among the LiBOB.
Described non-aqueous organic solvent is selected from any or several in carbonic ester and halo derivatives, ester, ether or the ketone.
Described electrolyte comprises cyclic carbonate and linear carbonate mixed solvent.
Described electrolyte comprises the mixed solvent of carbonic ester and ester.
Described electrolyte comprises the mixed solvent of carbonic ester and ether.
Described electrolyte comprises carbonic ester, ester and ether mixed solvent.
Described carbonic ester and halo derivatives thereof are selected from ethylene carbonate, propene carbonate, dimethyl carbonate, diethyl carbonate, any or several in methyl ethyl carbonate, carbonic acid first propyl ester, chlorocarbonic acid vinyl acetate, chlorocarbonic acid propylene ester, dichloro-propene carbonate, three chloro propene carbonates, fluorinated ethylene carbonate, fluoro propene carbonate, two fluoro propene carbonates or the three fluoro propene carbonates.
Described ester is selected from any or several in methyl formate, Ethyl formate, methyl acetate, ethyl acetate, propyl acetate, ethyl propionate, methyl butyrate, ethyl butyrate, ethylene sulfite, propylene sulfite, trimethyl phosphate, triethyl phosphate or the tributyl phosphate.
Described ether is selected from dimethoxymethane, 1,2-dimethoxy-ethane, 1,2-diethoxyethane, oxinane, dimethyl-tetrahydrofuran, diethylene glycol dimethyl ether or tetramethyl-1, any or several in the 3-dioxolane.
Described ketone is selected from N-methyl pyrrolidone or acetone.
Described film for additive is selected from vinylene carbonate, vinylethylene carbonate, 1,3-sulfonic acid propiolactone or 1, and any or several combinations in the 4-sulfonic acid butyrolactone, content is 2%~5% of electrolyte total weight.
Advantage of the present invention is: add heptamethyldisilazane in lithium-ion battery electrolytes after, heptamethyldisilazane can be met the product hydrogen ion reaction of water decomposition with lithium salts in the electrolyte, thereby the acidity of control electrolyte, the cycle life and the high-temperature storage performance of raising lithium ion battery.
Heptamethyldisilazane and hydrogen ion reaction principle are as shown in the formula described:
The salt compounds that reaction generates at high temperature has very strong stability, is difficult to decompose generate hydrogen ion again, therefore can well control the acidity in the electrolyte, and then improves the cycle performance and the high-temperature storage performance of lithium manganate battery.
Description of drawings
Fig. 1 is the electrolyte of Comparative Examples 1, embodiment 1, the lithium manganate battery cycle life correlation curve for preparing.
Fig. 2 is the electrolyte of Comparative Examples 1, embodiment 1, and the lithium manganate battery for preparing is placed 7 days high-temperature storage performance correlation curves for 60 ℃.
Embodiment
The present invention is described in further detail below in conjunction with embodiment and accompanying drawing, but embodiments of the present invention are not limited thereto.
Comparative Examples 1
Will be as the LiPF of lithium salts
6Be dissolved in and obtain solution, wherein LiPF in the mixed solvent of ethylene carbonate (EC)/methyl ethyl carbonate (EMC)/propene carbonate (PC) (mass ratio is 30/60/10)
6Concentration be 1M.In this solution, press 2% of electrolyte total weight then and add vinylene carbonate (VC), promptly make contrast electrolyte.Be designated as the A sample.
Embodiment 1
Will be as the LiPF of lithium salts
6Be dissolved in and obtain solution, wherein LiPF in the mixed solvent of ethylene carbonate (EC)/methyl ethyl carbonate (EMC)/propene carbonate (PC) (mass ratio is 30/60/10)
6Concentration be 1M.In this solution, press 2% of electrolyte total weight then and add vinylene carbonate (VC), press 0.1% of electrolyte total weight and add heptamethyldisilazane, promptly make the electrolyte of hope.Be designated as the B sample.
In A sample and B sample, add 1 distilled water respectively, with the moisture in coulomb cassette method test electrolyte, the acidity in the acid-base titration test electrolyte.
A sample and B sample normal temperature are placed the H before and after the week
2O and HF content results such as following table:
The concentration that has added free acid (HF) in the electrolyte of heptamethyldisilazane is obviously very low.
The lithium manganate battery cycle life correlation curve that curve among Fig. 1 (1) prepares for the electrolyte of Comparative Examples 1; The lithium manganate battery cycle life correlation curve that curve (2) prepares for the electrolyte of embodiment 1.As seen from the figure, in this solution, be significantly improved by its capacity behind the 0.1% adding heptamethyldisilazane of electrolyte total weight.
Curve among Fig. 2 (a) is placed 7 days high-temperature storage performance correlation curves for 60 ℃ for the lithium manganate battery that the electrolyte of Comparative Examples 1 prepares.Curve (b) is placed 7 days high-temperature storage performance correlation curves for 60 ℃ for the lithium manganate battery that the electrolyte of embodiment 1 prepares.As seen from the figure, in this solution, be significantly improved by its high-temperature storage performance behind the 0.1% adding heptamethyldisilazane of electrolyte total weight.
Embodiment 2
Will be as the LiPF of lithium salts
6Be dissolved in and obtain solution, wherein LiPF in the mixed solvent of ethylene carbonate (EC)/methyl ethyl carbonate (EMC)/diethyl carbonate (DEC)/propene carbonate (PC) (mass ratio is 30/10/50/10)
6Concentration be 1M.In this solution, press 2% of electrolyte total weight then and add vinylene carbonate (VC), press 0.5% of electrolyte total weight and add heptamethyldisilazane, promptly make the electrolyte of hope.
Embodiment 3
Will be as the LiPF of lithium salts
6Be dissolved in and obtain solution, wherein LiPF in the mixed solvent of ethylene carbonate (EC)/Ethyl formate (EF)/dimethyl carbonate (DMC) (mass ratio is 30/20/50)
6Concentration be 1.4M.In this solution, press 3% of electrolyte total weight then and add 1, and 3-sulfonic acid propiolactone (1,3-PS), press 1% of electrolyte total weight and add heptamethyldisilazane, promptly make the electrolyte of hope.
Embodiment 4
Will be as the LiPF of lithium salts
6Be dissolved in ethylene carbonate (EC)/three fluoro propene carbonate (CF
3-EC)/obtain solution, wherein LiPF in the mixed solvent of methyl ethyl carbonate (EMC)/ethyl acetate (EA)/propene carbonate (PC) (mass ratio is 20/10/20/40/10)
6Concentration be 1.2M.In this solution, add vinylene carbonate (VC), 1 respectively then by 2%, 3% of electrolyte total weight, and 3-sulfonic acid propiolactone (1,3-PS), press 1.5% of electrolyte total weight and add heptamethyldisilazane, promptly make the electrolyte of hope.
Embodiment 5
Will be as the LiPF of lithium salts
6Be dissolved in ethylene carbonate (EC)/three chloro propene carbonate (CCl
3-EC)/obtain solution, wherein LiPF in the mixed solvent of methyl ethyl carbonate (EMC)/ethyl propionate (EP)/propene carbonate (PC) (mass ratio is 20/10/10/50/10)
6Concentration be 1.2M.In this solution, add vinylene carbonate (VC), 1 respectively then by 1%, 2% of electrolyte total weight, and 3-sulfonic acid propiolactone (1,3-PS), press 2% of electrolyte total weight again and add heptamethyldisilazane, promptly make the electrolyte of hope.
Embodiment 6
Will be as the LiPF of lithium salts
6Be dissolved in ethylene carbonate (EC)/chlorocarbonic acid propylene ester (CH
2Cl-EC)/obtain solution, wherein LiPF in the mixed solvent of methyl ethyl carbonate (EMC)/ethyl butyrate (EB)/propene carbonate (PC) (mass ratio is 20/10/10/50/10)
6Concentration be 1.3M.In this solution, add vinylene carbonate (VC), 1 respectively then by 2%, 3% of electrolyte total weight, and 3-sulfonic acid propiolactone (1,3-PS), press 3% of electrolyte total weight again and add heptamethyldisilazane, promptly make the electrolyte of hope.
Embodiment 7
Will be as the LiPF of lithium salts
6Be dissolved in and obtain solution, wherein LiPF in the mixed solvent of fluorinated ethylene carbonate (F-EC)/methyl ethyl carbonate (EMC)/ethylene sulfite (ES)/propene carbonate (PC) (mass ratio is 30/20/40/10)
6Concentration be 1M.In this solution, add vinylene carbonate (VC), 1 respectively then by 2%, 3% of electrolyte total weight, and 3-sulfonic acid propiolactone (1,3-PS), press 3.5% of electrolyte total weight again and add heptamethyldisilazane, promptly make the electrolyte of hope.
Embodiment 8
Will be as the LiPF of lithium salts
6Be dissolved in and obtain solution, wherein LiPF in the mixed solvent of chlorocarbonic acid vinyl acetate (Cl-EC)/methyl ethyl carbonate (EMC)/trimethyl phosphate (TMP)/propene carbonate (PC) (mass ratio is 30/20/40/10)
6Concentration be 1M.In this solution, add vinylene carbonate (VC), 1 respectively then by 2%, 3% of electrolyte total weight, and 3-sulfonic acid propiolactone (1,3-PS), press 4% of electrolyte total weight again and add heptamethyldisilazane, promptly make the electrolyte of hope.
Embodiment 9
Will be as the LiPF of lithium salts
6Be dissolved in ethylene carbonate (EC)/carbonic acid first propyl ester (MPC)/1, obtain solution, wherein LiPF in the mixed solvent of 2-dimethoxy-ethane (DME)/propene carbonate (PC) (mass ratio is 30/20/40/10)
6Concentration be 1.2M.In this solution, add vinylene carbonate (VC), 1 respectively then by 2%, 3% of electrolyte total weight, and 3-sulfonic acid propiolactone (1,3-PS), press 4.5% of electrolyte total weight again and add heptamethyldisilazane, promptly make the electrolyte of hope.
Embodiment 10
Will be as the LiPF of lithium salts
6Be dissolved in ethylene carbonate (EC)/methyl butyrate (MB)/1, obtain solution, wherein LiPF in the mixed solvent of 2-diethoxyethane (DEE)/propene carbonate (PC) (mass ratio is 30/30/30/10)
6Concentration be 1M.In this solution, add vinylene carbonate (VC), 1 respectively then by 1%, 4% of electrolyte total weight, and 3-sulfonic acid propiolactone (1,3-PS), press 5% of electrolyte total weight again and add heptamethyldisilazane, promptly make the electrolyte of hope.
Embodiment 11
Will be as the LiPF of lithium salts
6Be dissolved in and obtain solution, wherein LiPF in the mixed solvent of ethylene carbonate (EC)/oxolane (THP)/tributyl phosphate (TBP)/propene carbonate (PC) (mass ratio is 30/30/30/10)
6Concentration be 1M.In this solution, add vinylene carbonate (VC), 1 respectively then by 2%, 3% of electrolyte total weight, and 3-sulfonic acid propiolactone (1,3-PS), press 2% of electrolyte total weight again and add heptamethyldisilazane, promptly make the electrolyte of hope.
Embodiment 12
Will be as the LiPF of lithium salts
6Be dissolved in ethylene carbonate (EC)/fluoro propene carbonate (CH
2F-EC)/obtain solution, wherein LiPF in the mixed solvent of diethylene glycol dimethyl ether (DG)/triethyl phosphate (TEP)/propene carbonate (PC) (mass ratio is 20/10/30/30/10)
6Concentration be 1M.In this solution, add vinylethylene carbonate (VEC), 1 respectively then by 2%, 3% of electrolyte total weight, and 3-sulfonic acid propiolactone (1,3-PS), press 2% of electrolyte total weight again and add heptamethyldisilazane, promptly make the electrolyte of hope.
Embodiment 13
Will be as the LiPF of lithium salts
6Be dissolved in LiBOB and obtain solution, wherein LiPF in the mixed solvent of ethylene carbonate (EC)/methyl formate (MF)/propylene sulfite (PS)/propene carbonate (PC) (mass ratio is 30/10/50/10)
6Concentration be 0.8M, the concentration of LiBOB is 0.2M.In this solution, add vinylene carbonate (VC), 1 respectively then by 2%, 3% of electrolyte total weight, and 4-sulfonic acid butyrolactone (1,4-BS), press 1% of electrolyte total weight again and add heptamethyldisilazane, promptly make the electrolyte of hope.
Embodiment 14
Will be as the LiClO of lithium salts
4Be dissolved in ethylene carbonate (EC)/methyl butyrate (MB)/1, obtain solution, wherein LiClO in the mixed solvent of 2-diethoxyethane (DEE)/acetone (mass ratio is 30/20/40/10)
4Concentration be 1.3M.In this solution, add vinylethylene carbonate (VEC), 1 respectively then by 1.5%, 3.5% of electrolyte total weight, and 4-sulfonic acid butyrolactone (1,4-BS), press 1% of electrolyte total weight again and add heptamethyldisilazane, promptly make the electrolyte of hope.
Embodiment 15
Will be as the LiPF of lithium salts
6And LiBF
4Be dissolved in ethylene carbonate (EC)/methyl acetate (MA)/tetramethyl-1, obtain solution, wherein LiPF in the mixed solvent of 3-dioxolane (4Me-DL)/propene carbonate (PC) (mass ratio is 30/30/30/10)
6Concentration be 0.8M, LiBF
4Concentration be 0.4M.In this solution, add vinylene carbonate (VC), 1 respectively then by 2%, 3% of electrolyte total weight, and 3-sulfonic acid propiolactone (1,3-PS), press 1% of electrolyte total weight again and add heptamethyldisilazane, promptly make the electrolyte of hope.
Comparative Examples 2
Will be as the LiBF of lithium salts
4Be dissolved in and obtain solution, wherein LiBF in the mixed solvent of ethylene carbonate (EC)/propyl acetate (PA)/dimethyl carbonate (DEC)/propene carbonate (PC) (mass ratio is 30/10/50/10)
4Concentration be 0.8M.In this solution, add vinylene carbonate (VC), 1 respectively then by 2%, 3% of electrolyte total weight, and 3-sulfonic acid propiolactone (1,3-PS), promptly make contrast electrolyte.Be designated as the C sample.
Embodiment 16
Will be as the LiBF of lithium salts
4Be dissolved in and obtain solution, wherein LiBF in the mixed solvent of ethylene carbonate (EC)/propyl acetate (PA)/dimethyl carbonate (DEC)/propene carbonate (PC) (mass ratio is 30/10/50/10)
4Concentration be 0.8M.In this solution, add vinylene carbonate (VC), 1 respectively then by 2%, 3% of electrolyte total weight, and 3-sulfonic acid propiolactone (1,3-PS), press 1% of electrolyte total weight again and add heptamethyldisilazane, promptly make the electrolyte of hope.Be designated as the D sample.
In C sample and D sample, add 1 distilled water respectively, with the moisture in coulomb cassette method test electrolyte, the acidity in the acid-base titration test electrolyte.
C sample and D sample normal temperature are placed the H before and after the week
2O and HF content results such as following table:
Above-mentioned embodiment is the preferred embodiments of the present invention; can not limit claim of the present invention; other any change or other equivalent substitute mode that does not deviate from technical scheme of the present invention and made is included within protection scope of the present invention.
Claims (10)
1, a kind of electrolyte of lithium manganate battery, this electrolyte comprises: lithium salts, non-aqueous organic solvent, film for additive is characterized in that: it also comprises heptamethyldisilazane.
2, the electrolyte of lithium manganate battery according to claim 1 is characterized in that: the addition of described heptamethyldisilazane is 0.1%~5% of an electrolyte total weight.
3, the electrolyte of lithium manganate battery according to claim 2 is characterized in that: the addition of described heptamethyldisilazane is 0.1%~2% of an electrolyte total weight.
4, the electrolyte of lithium manganate battery according to claim 1 is characterized in that: described lithium salts is selected from LiPF
6, LiBF
4, LiClO
4Or any or several combinations among the LiBOB.
5, the electrolyte of lithium manganate battery according to claim 1 is characterized in that: described non-aqueous organic solvent is selected from any or several in carbonic ester and halo derivatives, ester, ether or the ketone.
6, the electrolyte of lithium manganate battery according to claim 5, it is characterized in that: described carbonic ester and halo derivatives thereof are selected from ethylene carbonate, propene carbonate, dimethyl carbonate, diethyl carbonate, any or several in methyl ethyl carbonate, carbonic acid first propyl ester, chlorocarbonic acid vinyl acetate, chlorocarbonic acid propylene ester, dichloro-propene carbonate, three chloro propene carbonates, fluorinated ethylene carbonate, fluoro propene carbonate, two fluoro propene carbonates or the three fluoro propene carbonates.
7, the electrolyte of lithium manganate battery according to claim 5 is characterized in that: wherein said ester is selected from any or several in methyl formate, Ethyl formate, methyl acetate, ethyl acetate, propyl acetate, ethyl propionate, methyl butyrate, ethyl butyrate, ethylene sulfite, propylene sulfite, trimethyl phosphate, triethyl phosphate or the tributyl phosphate.
8, the electrolyte of lithium manganate battery according to claim 5, it is characterized in that: described ether is selected from dimethoxymethane, 1,2-dimethoxy-ethane, 1,2-diethoxyethane, oxinane, dimethyl-tetrahydrofuran, diethylene glycol dimethyl ether or tetramethyl-1, any or several in the 3-dioxolane.
9, according to the electrolyte of the lithium manganate battery described in the claim 5, it is characterized in that: described ketone is selected from N-methyl pyrrolidone or acetone.
10, electrolyte according to claim 5, wherein said film for additive is selected from vinylene carbonate, vinylethylene carbonate, 1,3-sulfonic acid propiolactone or 1, any or several combinations in the 4-sulfonic acid butyrolactone, content is 2%~5% of electrolyte total weight.
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2008
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