CN101540419A - Electrolyte for lithium manganate power battery - Google Patents
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Abstract
The invention discloses an electrolyte for a lithium manganate power battery. The electrolyte comprises lithium salt and nonaqueous organic solvent and also comprises 0.5-5 of filming additive, 2-10 of anti-overcharge additive, 0.01-0.5 of additive capable of controlling acidity and water content and 0.1-5 of lithium salt stabilizer according to the weight percentage. The electrolyte selects the nonaqueous organic solvent with a high boiling point and adds functional additives such as the filming additive, the anti-overcharge additive, the additive capable of controlling the acidity and the water content, the lithium salt stabilizer, and the like so that the lithium manganate power battery adopting the electrolyte has excellent safety performance, high-temperature performance and recycle service life.
Description
Technical field
The present invention relates to a kind of lithium-ion battery electrolytes, relate in particular to a kind of LiMn2O4 electrokinetic cell electrolyte.
Background technology
Closely during the last ten years, lithium ion battery has been widely used in portable electronics such as mobile communication, video camera, camera, language repeater, MP3 player, and annual all with 20% speed increase.The electrokinetic cell that generally uses has four kinds at present: lead-acid battery, nickel-cadmium cell, Ni-MH battery and lithium ion battery.Lithium ion battery is generally believed to have following advantage: specific energy is big; The specific power height; Self discharge is little; Memory-less effect; Cycle characteristics is good; But repid discharge, and efficient height; Operating temperature range is wide; Therefore non-environmental-pollutions etc. are expected to enter best electrical source of power ranks of 21 century.
The electric motor car market, particularly electric bicycle (EB) in the whole world are in the stage of saving up strength to start out at present, according to scholarly forecast, will ignite the whole world and prevail greatly in nearly 2 years.According to the investigation of market researchy corporation, about 5,000,000 of the market demand of global EB in 2004 was about 1,000 ten thousand in 2005, estimated that annual speed with 30% increases progressively.Wherein the China's Mainland is maximum potential market, and annual requirement reaches more than 3,000,000.And the power supply of these electric motor cars main plumbic acid, NI-G and Ni-MH battery of using before 2005,2005 later on will be progressively by lithium ion battery generation, 2010~the year two thousand fifty is mainly adopted lithium ion battery.USDOE reaches a conclusion by inquiry: HEV will become the main product of recent market, estimate that the year two thousand twenty HEV will account for 50% of world car sum.
The performance of lithium ion battery depends primarily on the structure and the performance of used inside battery material.These inside battery materials comprise positive electrode, negative material, electrolyte and barrier film etc.Negative material is generally selected material with carbon element for use, present development comparative maturity, and the selection of positive electrode has become the key factor that restriction lithium ion battery performance further improves, price further reduces.In the present lithium ion battery of commercially producing, the cost of positive electrode accounts for about 40% of entire cell cost, and the reduction of positive electrode price is directly determining the reduction of lithium ion battery price.Compare with the current cobalt acid lithium that generally uses, the spinel lithium manganate aboundresources, cheap, and Heat stability is good, the overcharging resisting electricity, high rate during charging-discharging is superior, and environmentally safe is safe, becomes one of the most promising positive electrode.In the world, the dynamic lithium battery technical research of Japan the earliest, technical merit is the highest, is that the lithium battery producer of representative all selects LiMn2O4 as the power type lithium-ion battery anode material with Sanyo, Hitachi, and is widely used on electric bicycle and the electric automobile.LiMn2O4 is the positive electrode of present main flow.
The requirement of electrokinetic cell has: the energy density height; The specific power height can heavy-current discharge; Can charge rapidly; Can be in operate as normal under the higher temperature conditions, and the situation that safety problem and capacity, cycle performance are decayed does not significantly appear; Low price.LiMn2O4 becomes the most promising positive electrode of lithium ion battery with its aboundresources, advantage such as cheap, nontoxic, but the manganese dissolving takes place the LiMn2O4 structural instability easily, cause malformation, reduce cycle performance, especially under high temperature (55 ℃) condition, capacity attenuation is more serious.Except improving the cycle performance that improves LiMn2O4 by positive electrode modification and battery process, the excellent electrolyte of exploitation also is the important means of improving the LiMn2O4 capacity attenuation.
Summary of the invention
Technical problem to be solved by this invention is, a kind of LiMn2O4 electrokinetic cell electrolyte is provided, this electrolyte is by control non-aqueous organic solvent ratio, and the functional additives such as additive, lithium salts stabilizer that add film for additive, anti-overcharge additive, controlling acidity and water content, make and adopt the lithium ion battery of this electrolyte to have excellent security energy, cycle life and high-temperature behavior.
The present invention solves the technical scheme that its technical problem adopts:
A kind of LiMn2O4 electrokinetic cell electrolyte, this electrolyte comprises: lithium salts, non-aqueous organic solvent, also contain 0.5%~5% the film for additive that accounts for the electrolyte total weight, 2%~10% anti-overcharge additive, 0.01%~0.5% controlling acidity and the additive of water content and 0.1~5% lithium salts stabilizer.
Above-mentioned lithium salts is selected from LiPF
6, LiBF
4, any or several combinations among LiBOB or the LiODFB, content is 0.7M~1.5M.
Above-mentioned non-aqueous organic solvent is selected from any or several in carbonic ester and halo derivatives, carboxylate, sulphonic acid ester or the phosphate.
Above-mentioned 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.
Above-mentioned carboxylate is selected from any or several in methyl formate, Ethyl formate, methyl acetate, ethyl acetate, propyl acetate, ethyl propionate, methyl butyrate or the ethyl butyrate; Described sulphonic acid ester is selected from ethylene sulfite, propylene sulfite; Described phosphate is selected from any or several in trimethyl phosphate, triethyl phosphate or the tributyl phosphate.
Above-mentioned 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.
Above-mentioned anti-overcharge additive is selected from any or several combinations in phenylate and halo derivatives, phenyl compound, alkyl benzene ring derivatives, halogeno-benzene ring derivatives, thiophene, furans or the metallocenes.
The above-mentioned controlling acidity and the additive of water content are selected from any or several combinations in amine, the alkyl silazane class.
Above-mentioned lithium salts stabilizer is selected from any or several combinations in trifluoroethyl phosphorous acid (TTFP), pyrimidine, the isocyanic acid salt.
Advantage of the present invention is: choosing of higher boiling point non-aqueous organic solvent, can improve the stability under the high temperature resistant of electrolyte and the abuse state; Adding film for additive can form diaphragm on the both positive and negative polarity surface of battery, and the prevention positive and negative pole material contacts with electrolyte, suppresses the decomposition of electrolyte on the both positive and negative polarity surface; Add the additive of controlling acidity and water content and lithium salts stabilizer can the act synergistically decomposition that stops lithium salts and the rising of acidity, and then improve the storage time of electrolyte and the cycle performance of battery; Add anti-overcharge additive and can solve the safety problem of battery under the abuse state.The adding of multiple functional additive, synergy improves security performance, high-temperature behavior and the cycle life of LiMn2O4 electrokinetic cell.
Description of drawings
Fig. 1 is the electrolyte of embodiment 1, the LiMn2O4 electrokinetic cell normal temperature cycle life curve for preparing.
Fig. 2 is the electrolyte of embodiment 1,60 ℃ of cycle life curves of the LiMn2O4 electrokinetic cell for preparing.
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.
Embodiment 1
Will be as the LiPF of lithium salts
6Be dissolved 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) and obtain solution, wherein LiPF
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 monoethanolamine, press 3% of electrolyte total weight and add biphenyl, press 0.2% of electrolyte total weight and add trifluoroethyl phosphorous acid (TTFP), promptly make the electrolyte of hope.
Injecting the electrolyte into the monomer capacity is the LiMn2O4 soft-package battery of 10Ah, change into partial volume after, the normal-temperature circulating performance of test battery, 60 ℃ of cycle performances of high temperature and security performance.
The LiMn2O4 electrokinetic cell normal temperature cycle life curve that curve prepares for the electrolyte of embodiment 1 among Fig. 1.
60 ℃ of cycle life curves of LiMn2O4 electrokinetic cell that curve prepares for the electrolyte of embodiment 1 among Fig. 2.
By Fig. 1 and Fig. 2 as can be seen, prescription of the present invention has good normal temperature circulation and high temperature cyclic performance, and normal temperature circulated for 100 weeks, and capacity keeps 95.76%; In 60 ℃ of 100 weeks of circulation of high temperature, capacity keeps 85.45%.
Embodiment 2
Will be as the LiPF of lithium salts
6Be dissolved 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) and obtain solution, wherein LiPF
6Concentration be 1M.In this solution, press 1% of electrolyte total weight then and add vinylene carbonate (VC), press 2% of electrolyte total weight and add 1,3-sulfonic acid propiolactone (1,3-PS), press 0.05% of electrolyte total weight and add hexamethyldisiloxane, press 5% of electrolyte total weight and add biphenyl, press 0.2% of electrolyte total weight and add pyrimidine, promptly make the electrolyte of hope.
Embodiment 3
Will be as the LiPF of lithium salts
6Be dissolved 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) and obtain solution, wherein LiPF
6Concentration be 1M.In this solution, press 1% of electrolyte total weight then and add vinylene carbonate (VC), press 2% of electrolyte total weight and add 1,4-sulfonic acid butyrolactone (1,4-BS), press 0.01% of electrolyte total weight and add heptamethyldisilazane, press 7% of electrolyte total weight and add the 3-chloroanisole, press 2% of electrolyte total weight and add phenyl isocyanate, 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 in the mixed solvent of methyl ethyl carbonate (EMC)/ethyl butyrate (EB)/propene carbonate (PC) (mass ratio is 20/10/20/40/10), LiPF wherein
6Concentration be 1.2M.In this solution, press 3% of electrolyte total weight then and add 1,3-sulfonic acid propiolactone (1,3-PS), press 0.2% of electrolyte total weight and add TMSDEA, press 5% of electrolyte total weight and add 3 toluene fluorides, press 5% of electrolyte total weight and add ethyl isocyanate, 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 in the mixed solvent of methyl ethyl carbonate (EMC)/ethyl propionate (EP)/propene carbonate (PC) (mass ratio is 20/10/30/30/10), LiPF wherein
6Concentration be 1.5M.In this solution, press 1% of electrolyte total weight then and add vinylethylene carbonate (VEC), press 3% of electrolyte total weight and add 1,3-sulfonic acid propiolactone (1,3-PS), press 0.05% of electrolyte total weight and add monoethanolamine, press 5% of electrolyte total weight and add the 3-fluoroanisole, press 1% of electrolyte total weight and add pyrimidine, promptly make the electrolyte of hope.
Embodiment 6
Will be as the LiPF of lithium salts
6Be dissolved 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) and obtain solution, wherein LiPF
6Concentration be 1M.In this solution, press 3% of electrolyte total weight then and add vinylethylene carbonate (VEC), press 0.1% of electrolyte total weight and add monoethanolamine, press 2% of electrolyte total weight and add diphenyl ether, press 0.1% of electrolyte total weight and add trifluoroethyl phosphorous acid (TTFP), promptly make the electrolyte of hope.
Embodiment 7
Will be as the LiPF of lithium salts
6Be dissolved 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) and obtain solution, wherein LiPF
6Concentration be 1M.In this solution, press 2% of electrolyte total weight then and add vinylene carbonate (VC), press 2% of electrolyte total weight and add 1,3-sulfonic acid propiolactone (1,3-PS), press 0.05% of electrolyte total weight and add hexamethyldisiloxane, press 5% of electrolyte total weight and add 3-methylbenzene methyl ether, press 0.2% of electrolyte total weight and add pyrimidine, promptly make the electrolyte of hope.
Embodiment 8
Will be as the LiPF of lithium salts
6Be dissolved in the mixed solvent of ethylene carbonate (EC)/diethyl carbonate (DEC)/propene carbonate (PC) (mass ratio is 30/60/10) with LiBOB and obtain solution, wherein LiPF
6Concentration be 0.8M, the concentration of LiBOB is 0.2M.In this solution, press 1% of electrolyte total weight then and add vinylethylene carbonate (VEC), press 3% of electrolyte total weight and add 1,3-sulfonic acid propiolactone (1,3-PS), press 0.5% of electrolyte total weight and add monoethanolamine, add dimethylbenzene and cyclohexyl benzene respectively by 3%, 3% of electrolyte total weight, press 2% of electrolyte total weight and add trifluoroethyl phosphorous acid (TTFP), promptly make the electrolyte of hope.
Embodiment 9
Will be as the LiPF of lithium salts
6Be dissolved in the mixed solvent of ethylene carbonate (EC)/diethyl carbonate (DEC)/propene carbonate (PC) (mass ratio is 30/60/10) with LiODFB and obtain solution, wherein LiPF
6Concentration be 0.8M, the concentration of LiODFB is 0.2M.In this solution, press 1% of electrolyte total weight then and add vinylethylene carbonate (VEC), press 3% of electrolyte total weight and add 1,3-sulfonic acid propiolactone (1,3-PS), press 0.5% of electrolyte total weight and add monoethanolamine, press 5% of electrolyte total weight and add the 4-chloroanisole, press 0.1% of electrolyte total weight and add trifluoroethyl phosphorous acid (TTFP), promptly make the electrolyte of hope.
Will be as the LiPF of lithium salts
6, LiBF
4, LiBOB is dissolved in the mixed solvent of ethylene carbonate (EC)/diethyl carbonate (DEC)/propene carbonate (PC) (mass ratio is 30/60/10) and obtains solution, LiPF wherein
6Concentration be 0.8M, LiBF
4Concentration be 0.2M, the concentration of LiBOB is 0.1M.In this solution, press 1% of electrolyte total weight then and add vinylethylene carbonate (VEC), press 3% of electrolyte total weight and add 1,3-sulfonic acid propiolactone (1,3-PS), press 0.2% of electrolyte total weight and add monoethanolamine, press 5% of electrolyte total weight and add 4-methylbenzene methyl ether, press 0.1% of electrolyte total weight and add trifluoroethyl phosphorous acid (TTFP), promptly make the electrolyte of hope.
Embodiment 11
To be dissolved in as the LiODFB of lithium salts 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) and obtain solution, wherein the concentration of LiODFB is 1M.In this solution, press 1% of electrolyte total weight then and add vinylene carbonate (VC), press 2% of electrolyte total weight and add 1,3-sulfonic acid propiolactone (1,3-PS), press 0.2% of electrolyte total weight and add ethylenediamine, press 5% of electrolyte total weight and add the 4-fluoroanisole, press 0.2% of electrolyte total weight and add pyrimidine, promptly make the electrolyte of hope.
Embodiment 12
To be dissolved in as the LiBOB of lithium salts in the mixed solvent of ethylene carbonate (EC)/methyl ethyl carbonate (EMC)/diethyl carbonate (DEC)/propene carbonate (PC) (mass ratio is 30/20/40/10) and obtain solution, wherein the concentration of LiBOB is 0.7M.In this solution, press 2% of electrolyte total weight then and add vinylene carbonate (VC), press 2% of electrolyte total weight and add 1,3-sulfonic acid propiolactone (1,3-PS), press 0.1% of electrolyte total weight and add carbinolamine, press 10% of electrolyte total weight and add dimethylbenzene, promptly make the electrolyte of hope.
Embodiment 13
To be dissolved in as the LiBF4 of lithium salts 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) and obtain solution, wherein LiBF
4Concentration be 0.9M.In this solution, press 1% of electrolyte total weight then and add vinylene carbonate (VC), press 3% of electrolyte total weight and add 1,3-sulfonic acid propiolactone (1,3-PS), press 0.05% of electrolyte total weight and add monoethanolamine, press 6% of electrolyte total weight and add the 2-chloroanisole, press 0.1% of electrolyte total weight and add pyrimidine, promptly make the electrolyte of hope.
Embodiment 14
To be dissolved in as the LiPF6 of lithium salts in the mixed solvent of chlorocarbonic acid vinyl acetate (Cl-EC)/methyl ethyl carbonate (EMC)/ethyl acetate (EA)/propene carbonate (PC) (mass ratio is 30/40/20/10) and obtain solution, wherein LiPF
6Concentration be 1.1M.In this solution, press 2% of electrolyte total weight then and add vinylene carbonate (VC), press 3% of electrolyte total weight and add 1,3-sulfonic acid propiolactone (1,3-PS), press 0.05% of electrolyte total weight and add heptamethyldisilazane, press 4% of electrolyte total weight and add 2-methylbenzene methyl ether, press 1% of electrolyte total weight and add pyrimidine, promptly make the electrolyte of hope.
Embodiment 15
Will be as the LiBF of lithium salts
4, LiBOB is dissolved in the mixed solvent of ethylene carbonate (EC)/methyl butyrate (MB)/propylene sulfite (PS)/propene carbonate (PC) (mass ratio is 30/30/30/10) and obtains solution, LiBF wherein
4Concentration be 1M, the concentration of LiBOB is 0.3M.In this solution, press 0.5% of electrolyte total weight then and add vinylethylene carbonate (VEC), press 3% of electrolyte total weight and add 1,3-sulfonic acid propiolactone (1,3-PS), add monoethanolamine and heptamethyldisilazane respectively by 0.1% and 0.05% of electrolyte total weight, press 5% of electrolyte total weight and add ferrocene, press 0.02% of electrolyte total weight and add trifluoroethyl phosphorous acid (TTFP), promptly make the electrolyte of hope.
Embodiment 16
Will be as the LiPF of lithium salts
6Be dissolved in the mixed solvent of ethylene carbonate (EC)/methyl ethyl carbonate (EMC)/propyl acetate (PA)/propene carbonate (PC) (mass ratio is 30/40/20/10) and obtain solution, wherein LiPF
6Concentration be 1M.In this solution, press 3% of electrolyte total weight then and add 1,3-sulfonic acid propiolactone (1,3-PS), press 0.1% of electrolyte total weight and add hexamethyldisiloxane, press 5% of electrolyte total weight and add dibenzothiophenes, press 0.02% of electrolyte total weight and add trifluoroethyl phosphorous acid (TTFP), promptly make the electrolyte of hope.
Embodiment 17
To be dissolved in as the LiPF6 of lithium salts in the mixed solvent of ethylene carbonate (EC)/methyl ethyl carbonate (EMC)/tributyl phosphate (TBP)/propene carbonate (PC) (mass ratio is 30/40/20/10) and obtain solution, wherein LiPF
6Concentration be 1.2M.In this solution, press 3% of electrolyte total weight then and add 1,4-sulfonic acid butyrolactone (1,4-BS), press 0.05% of electrolyte total weight and add hexamethyldisiloxane, press 3% of electrolyte total weight and add benzofuran, press 0.03% of electrolyte total weight and add trifluoroethyl phosphorous acid (TTFP), promptly make the electrolyte of hope.
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 (9)
1, a kind of LiMn2O4 electrokinetic cell electrolyte, this electrolyte comprises: lithium salts, non-aqueous organic solvent is characterized in that: also contain 0.5%~5% the film for additive that accounts for the electrolyte total weight, 2%~10% anti-overcharge additive, 0.01%~0.5% controlling acidity and the additive of water content and 0.1~5% lithium salts stabilizer.
2, LiMn2O4 electrokinetic cell electrolyte according to claim 1, it is characterized in that: described lithium salts is selected from LiPF
6, LiBF
4, any or several combinations among LiBOB or the LiODFB, content is 0.7M~1.5M.
3, LiMn2O4 electrokinetic cell electrolyte 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, carboxylate, sulphonic acid ester or the phosphate.
4, LiMn2O4 electrokinetic cell electrolyte according to claim 3, 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.
5, LiMn2O4 electrokinetic cell electrolyte according to claim 3 is characterized in that: described carboxylate is selected from any or several in methyl formate, Ethyl formate, methyl acetate, ethyl acetate, propyl acetate, ethyl propionate, methyl butyrate or the ethyl butyrate; Described sulphonic acid ester is selected from ethylene sulfite, propylene sulfite; Described phosphate is selected from any or several in trimethyl phosphate, triethyl phosphate or the tributyl phosphate.
6, LiMn2O4 electrokinetic cell electrolyte according to claim 1, it is characterized in that: described 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.
7, LiMn2O4 electrokinetic cell electrolyte according to claim 1 is characterized in that: described anti-overcharge additive is selected from any or several combinations in phenylate and halo derivatives, phenyl compound, alkyl benzene ring derivatives, halogeno-benzene ring derivatives, thiophene, furans or the metallocenes.
8, LiMn2O4 electrokinetic cell electrolyte according to claim 1 is characterized in that: the additive of described controlling acidity and water content is selected from any or several combinations in amine, the alkyl silazane class.
9, LiMn2O4 electrokinetic cell electrolyte according to claim 1 is characterized in that: described lithium salts stabilizer is selected from any or several combinations in trifluoroethyl phosphorous acid (TTFP), pyrimidine, the isocyanic acid salt.
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