CN103413970B - Low-temperature type carbonic ester lithium battery electrolyte - Google Patents
Low-temperature type carbonic ester lithium battery electrolyte Download PDFInfo
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Abstract
Disclosure one low-temperature type carbonic ester lithium battery electrolyte, this electrolyte is mainly constituted by as the ethylene carbonate of solvent composition, dimethyl carbonate, Ethyl methyl carbonate and Allyl carbonate, lithium hexafluoro phosphate and low temperature additive, the weight ratio of four kinds of carbonate solvents is EC: DMC: EMC: PC=2: 3: 5: 1, is made into 1mol/L LiPF6The electrolyte of+four kinds of carbonate solvent+low temperature additive compositions；Low temperature additive is the one in polydimethylsiloxane, PS, vinylene carbonate or its combination。The present invention forms and selects and add low temperature additive by optimizing carbonate solvent and improve the dissolubility of electrolyte, degree of dissociation and electrical conductivity, improve the structure of lithium ion battery negative solid-phase interfacial film (SEI film), reduce SEI low-temperature resistance, improve battery stability in the large, improve circulating battery and improve service life。Being in particular northern China most area, minimum use temperature is that the lithium-ion-power cell under-50 DEG C of conditions provides main flow electrolyte。
Description
Technical field
The invention belongs to the lithium battery electrolytes in electrochemical material technical field, particularly relate to be solvent with carbonates Organic substance, improve the low-temperature type carbonic ester lithium battery electrolyte of electrolyte cryogenic property。
Background technology
Along with the lithium ion battery marketization deepens continuously, people are more and more higher to the expectation of battery performance。Current commercial lithium-ion batteries is difficult to meet the needs of the such as key areas such as electric motor car, space technology and military affairs, one of the main reasons is that battery performance under high and low temperature is not good, and therefore widening operating temperature range has become the Important Problems that Study on Li-ion batteries person pays close attention to。Being started with by electrolyte and improve temperature performance and have proven to feasible technological approaches, this is because as the ion conductor playing conduction in battery, the performance of electrolyte and the state of interface formed with both positive and negative polarity thereof largely affect battery temperature performance。
There is result of study to show: ferric phosphate lithium cell, because the relatively low ionic conductivity of LiFePO 4 material, battery charge-discharge performance under cryogenic can be affected；The ultimate value of climate change in recent years constantly refreshes historical record, and particularly north winter temperature is low, can not all be discharged by electricity, affect the service efficiency of battery under low temperature in battery use procedure；The means such as this shortcoming, some material producers and research institution attempt by preparing nano-scale particle, increase specific surface area, surface coating modification improve, but fail to be fully solved the cryogenic property problem of ferric phosphate lithium ion battery eventually。Therefore, exploitation has wide temperature and uses the electrolyte of scope, and the electrolyte being especially adapted for use in north low temperature season use is significant for the raising of the cycle life of lithium battery, storage life。
Summary of the invention
It is an object of the invention to overcome prior art Problems existing, it is provided that a kind of low-temperature type carbonic ester lithium battery electrolyte excellent suitable in the electrical property under northern area and cryogenic conditions。
By the present invention in that the multicomponent solvent of organic solvent low by freezing point, that conductivity is high forms and adds the special additives such as type siloxane, sulfone class and carbonates Organic substance and realizes the excellent electrical properties under low temperature。The present invention preferably four kinds of carbonates are as solvent composition, and its carbonic ester is the linear carbonate or cyclic carbonate that are joined directly together by 1 or two alkyl and carbon；Four kinds of carbonic esters are: dimethyl carbonate (DMC), Ethyl methyl carbonate (EMC), ethylene carbonate (EC), add wherein and improve the additive of electrolyte cryogenic property: polydimethylsiloxane (PDMS), 1,3-N-morpholinopropanesulfonic acid lactone (PS) and vinylene carbonate (VC), test and determine that the best of low temperature additive adds proportioning, the synergism between these several low temperature additives and between solvent and additive is made to reach maximum, to improve electrolyte electrical property under cryogenic, remain high discharge capacity and high rate performance。The present invention proposes following technical scheme:
A kind of low-temperature type carbonic ester lithium battery electrolyte, this electrolyte is mainly by as the ethylene carbonate (EC) of solvent composition, dimethyl carbonate (DMC), Ethyl methyl carbonate (EMC) and Allyl carbonate (PC), lithium hexafluoro phosphate LiPF6Constitute with low temperature additive, it is characterised in that: the weight ratio of four kinds of carbonate solvents is EC: DMC: EMC: PC=2: 3: 5: 1, is made into 1mol/LLiPF6The electrolyte of+four kinds of carbonate solvent (2: 3: 5: 1)+low temperature additive compositions；Described low temperature additive includes the one of which in polydimethylsiloxane (PDMS), PS (PS), vinylene carbonate (VC) or its combination。
Described low temperature additive percentage by weight in the electrolytic solution is: polydimethylsiloxane (PDMS) or PS (PS) 0.8%～2.5%, vinylene carbonate (VC) 0.6%～2.0%。
Described low temperature additive preferred weight percent in the electrolytic solution is: polydimethylsiloxane (PDMS) 1.3%, vinylene carbonate (VC) 0.8%。
Described low temperature additive preferred weight percent in the electrolytic solution is: polydimethylsiloxane (PDMS) 1.0%, vinylene carbonate (VC) 1.0%。
Described low temperature additive preferred weight percent in the electrolytic solution is: PS (PS) 1.5%, vinylene carbonate (VC) 0.6%。
Described low temperature additive preferred weight percent in the electrolytic solution is: PS (PS) 1.5%, vinylene carbonate (VC) 1.5%。
The present invention first preferably determines multiplexed combination and the optimum proportioning of solvent。Ethylene carbonate (EC) fusing point in solvent composition is higher, although stable SEI film in use can be formed, but limit it as the application under cryogenic of the battery of electrolyte, in order to improve the cryogenic property of battery, low-melting to it and other organic solvent is mixed to form the blend solution of quaternary system by the present invention。Ethyl methyl carbonate and the carboxylic acid esters fusing point of ring-type are low, can improve the cryogenic property of battery as cosolvent；Allyl carbonate (PC) suppresses ethylene carbonate (EC) to precipitate out at crystallization at low temperatures effectively, make the low-temperature resistance of SEI film under cryogenic, having higher ionic conductivity, effectively widened the temperature range that battery uses, minimum can arriving uses under-50 DEG C of low temperature。
Another of the present invention is characterized as being and improves Organic Electrolyte Solutions for Li-Ion Batteries cryogenic property by adding additive。Because additive amount is little, the feature of instant effect, select type siloxane, sulfone class and carbonates Organic substance such as polydimethylsiloxane (PDMS), 1,3-N-morpholinopropanesulfonic acid lactone (PS), vinylene carbonate (VC) are as low temperature additive, the decomposition voltage of electrolyte can be effectively improved after interpolation, passivating film can be formed on graphite cathode surface, positive pole is also had good oxidation stability, the effective raising minimum service behaviour reached under-50 DEG C of low temperature of electrolyte。
The present invention forms and selects and add low temperature additive by optimizing carbonate solvent and improve the dissolubility of electrolyte, degree of dissociation and electrical conductivity, improve the structure of lithium ion battery negative solid-phase interfacial film (SEI film), reduce SEI low-temperature resistance, improve battery stability in the large, improve the time lifetime (namely improving the storage service life of battery) that battery is overall；Improve circulating battery and improve service life。
Due to the technological break-through of low temperature aspect, it is not only domestic conventional lithium ion battery and provides high-performance, low cost product, and the dynamic lithium battery for electric automobile provides security performance and the good electrolyte of serviceability。Being in particular northern China most area, minimum use temperature is that the lithium-ion-power cell under-50 DEG C of conditions provides main flow electrolyte。Applicant has successfully produced the lithium battery electrolytes that cryogenic property is excellent, and product detects through battery relevant departments, and indices has been fully achieved electrokinetic cell instructions for use。
Detailed description of the invention
Below by way of specific embodiment Data Comparison, the cryogenic property at low-temperature flame retardant type electrolyte-50 DEG C is described。The electrolyte solvent of the present invention is the carboxylate of the carbonic ester of chain and ring-type, electrolyte solvent is quaternary solvent: the weight ratio of ethylene carbonate (EC), dimethyl carbonate (DMC), Ethyl methyl carbonate (EMC) and Allyl carbonate (PC) four kinds of carbonate solvents is EC: DMC: EMC: PC=2: 3: 5: 1, is made into 1mol/L lithium hexafluoro phosphate LiPF6The electrolyte of+four kinds of carbonate solvent+low temperature additive compositions；By experiment and detection, find out solvent composition and ratio and the optimum proportioning of low temperature additive, make the synergy between additive and between solvent and additive reach maximum。
Embodiment 1:
After ethylene carbonate (EC), dimethyl carbonate (DMC), Ethyl methyl carbonate (EMC) and Allyl carbonate (PC) add the additive of 1.3% polydimethylsiloxane (PDMS) and 0.8% vinylene carbonate (VC), synergism is maximum, discharge capacity and conductivity variations are very big, it is effectively improved the cryogenic property that lithium battery electrolytes is at-50 DEG C, higher electrical conductivity and discharge capacity can be kept。Table 1 is the situation of change of the discharge capacity of both electrolyte and electrical conductivity。
Table 11mol/LLiPF6With the electrolyte discharge capacity at different temperatures of different solvents composition and electrical conductivity
Embodiment 2:
After adding polydimethylsiloxane (PDMS) additive of 1.3% in ethylene carbonate (EC), dimethyl carbonate (DMC), Ethyl methyl carbonate (EMC) and Allyl carbonate (PC), cryogenic property have also been obtained the improvement of part, discharge capacity and Conductivity Ratio additive-free be make moderate progress, but effect not as two kinds of additive synergistic action effects good。Table 2 is the situation of change of the discharge capacity of both electrolyte and electrical conductivity。
Table 21mol/LLiPF6With the electrolyte discharge capacity under different additive amount and different temperatures of same solvent composition and electrical conductivity
Embodiment 3:
The additive Posterior circle performance adding 0.8% vinylene carbonate (VC) in ethylene carbonate (EC), dimethyl carbonate (DMC), Ethyl methyl carbonate (EMC) and Allyl carbonate (PC) improves, but cryogenic property has no change。Table 3 is the comparable situation adding two kinds of additives discharge capacity with two kinds of electrolyte of a kind of additive of addition and electrical conductivity。
Table 31mol/LLiPF6With the electrolyte discharge capacity under different additive amount and different temperatures of same solvent composition and electrical conductivity
Embodiment 4:
At ethylene carbonate (EC), discharge capacity and electrical conductivity after adding 1% polydimethylsiloxane (PDMS) and 1% vinylene carbonate (VC) additive in dimethyl carbonate (DMC) and Ethyl methyl carbonate (EMC) and Allyl carbonate (PC) compare with the additive of addition 1.3% dimethyl siloxane (PDMS) and 0.8% vinylene carbonate (VC), discharge capacity and electrical conductivity are all on the low side, the cryogenic property of lithium battery electrolytes makes moderate progress, and synergism decreases。Table 4 is the comparable situation of the discharge capacity of two kinds of electrolyte of additive and the electrical conductivity adding different ratio。
Table 41mol/LLiPF6With the electrolyte discharge capacity under different additive amount and different temperatures of same solvent composition and electrical conductivity
Embodiment 5:
Ethylene carbonate (EC), dimethyl carbonate (DMC), Ethyl methyl carbonate (EMC) and Allyl carbonate (PC) add the 1 of 1.5%, after the additive of 3-N-morpholinopropanesulfonic acid lactone (PS) and 1.5% vinylene carbonate (VC), discharge capacity and electrical conductivity also make moderate progress, and the cryogenic property of lithium battery electrolytes gets a promotion；Because the amount of additive increases, so the electrical property of lithium battery electrolytes declines。Table 5 is the situation of change of the discharge capacity of additive electrolyte and the electrical conductivity adding different ratio。
Table 51mol/LLiPF6With the electrolyte discharge capacity under different additive amount and different temperatures of same solvent composition and electrical conductivity
Embodiment 6:
After adding the additive of 2.5% polydimethylsiloxane (PDMS) and 2% vinylene carbonate (VC) in ethylene carbonate (EC), dimethyl carbonate (DMC), Ethyl methyl carbonate (EMC) and Allyl carbonate (PC), discharge capacity and electrical conductivity make moderate progress at low temperatures, but, along with the increase of additive addition, the electrical property of electrolyte there is further impact。Table 6 is the situation of change of the discharge capacity of additive electrolyte and the electrical conductivity adding different ratio。
Table 61mol/LLiPF6With the electrolyte discharge capacity under different additive amount and different temperatures of same solvent composition and electrical conductivity
Embodiment 7:
Ethylene carbonate (EC), dimethyl carbonate (DMC), Ethyl methyl carbonate (EMC) and Allyl carbonate (PC) add the 1 of 1.5%, polydimethylsiloxane (PDMS) and 0.8% vinylene carbonate (VC) that after the additive of 3-N-morpholinopropanesulfonic acid lactone (PS) and 0.6% vinylene carbonate (VC), discharge capacity and Conductivity Ratio add 1.3% are poor, have impact on two kinds of materials in the cooperative effect improving lithium battery electrolytes electrical property, but the cryogenic property of lithium battery electrolytes also improves。Table 7 is the situation of change of the discharge capacity of additive electrolyte and the electrical conductivity adding different ratio。
Table 71mol/LLiPF6With the electrolyte discharge capacity under different additive amount and different temperatures of same solvent composition and electrical conductivity
Embodiment 8:
Ethylene carbonate (EC), dimethyl carbonate (DMC), Ethyl methyl carbonate (EMC) and Allyl carbonate (PC) add the 1 of 0.8%, after the additive of 3-N-morpholinopropanesulfonic acid lactone (PS) and 1% vinylene carbonate (VC), discharge capacity and electrical conductivity make moderate progress, the cryogenic property of lithium battery electrolytes also increases, but the synergy of two kinds of additives is not reaching to maximum。Table 8 is the situation of change of the discharge capacity of additive electrolyte and the electrical conductivity adding different ratio。
Table 81mol/LLiPF6With the electrolyte discharge capacity under different additive amount and different temperatures of same solvent composition and electrical conductivity
Claims (5)
1. a low-temperature type carbonic ester lithium battery electrolyte, this electrolyte is mainly by as the ethylene carbonate EC of solvent composition, dimethyl carbonate DMC, Ethyl methyl carbonate EMC and Allyl carbonate PC, lithium hexafluoro phosphate LiPF6Constitute with low temperature additive, it is characterised in that: the weight ratio of four kinds of carbonate solvents is EC: DMC: EMC: PC=2: 3: 5: 1, is made into 1mol/LLiPF6The electrolyte of+four kinds of carbonate solvent+low temperature additive compositions；
Described low temperature additive includes the combination of polydimethylsiloxane and vinylene carbonate VC or the combination of PS PS and vinylene carbonate VC；
Described low temperature additive percentage by weight in the electrolytic solution is: polydimethylsiloxane or PS PS0.8%～2.5%, vinylene carbonate VC0.6%～2.0%。
2. low-temperature type carbonic ester lithium battery electrolyte as claimed in claim 1, it is characterised in that: described low temperature additive percentage by weight in the electrolytic solution is: polydimethylsiloxane 1.3% and vinylene carbonate VC0.8%。
3. low-temperature type carbonic ester lithium battery electrolyte as claimed in claim 1, it is characterised in that: described low temperature additive percentage by weight in the electrolytic solution is: polydimethylsiloxane 1.0% and vinylene carbonate VC1.0%。
4. low-temperature type carbonic ester lithium battery electrolyte as claimed in claim 1, it is characterised in that: described low temperature additive percentage by weight in the electrolytic solution is: PS PS1.5% and vinylene carbonate VC0.6%。
5. low-temperature type carbonic ester lithium battery electrolyte as claimed in claim 1, it is characterised in that: described low temperature additive percentage by weight in the electrolytic solution is: PS PS1.5% and vinylene carbonate VC1.5%。
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| CN105140561A (en) * | 2015-07-08 | 2015-12-09 | 深圳新宙邦科技股份有限公司 | Non-aqueous electrolyte of lithium ion battery and lithium ion battery |
| CN107611462A (en) * | 2017-08-27 | 2018-01-19 | 长沙小新新能源科技有限公司 | A kind of anolyte and preparation method thereof, the biobattery containing anolyte |
| WO2019183351A1 (en) * | 2018-03-23 | 2019-09-26 | Maxwell Technologies, Inc. | Electrolyte additives and formulations for energy storage devices |
| CN111224161B (en) * | 2018-11-26 | 2021-06-15 | 中国科学院大连化学物理研究所 | Method for improving low-temperature service performance of lithium ion battery by electrolyte containing additive |
| CN110556582A (en) * | 2019-09-16 | 2019-12-10 | 营口路航新能源科技有限公司 | Lithium iron phosphate battery, electrolyte and preparation method of lithium iron phosphate battery |
| EP3913721B1 (en) * | 2019-12-03 | 2022-11-23 | Contemporary Amperex Technology Co., Limited | Secondary battery, electrolyte, and device containing said secondary battery |
| CN112018446B (en) * | 2020-09-27 | 2022-07-01 | 珠海冠宇电池股份有限公司 | Electrolyte suitable for silicon-carbon system lithium ion battery |
| CN114006041A (en) * | 2021-10-12 | 2022-02-01 | 合肥国轩高科动力能源有限公司 | Low-temperature electrolyte for improving low-temperature performance of lithium iron phosphate-graphite battery |
| CN114566706A (en) * | 2022-01-19 | 2022-05-31 | 湖北亿纬动力有限公司 | Lithium battery electrolyte and lithium battery |
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