CN103413970A - Low-temperature type carbonic ester lithium battery electrolyte - Google Patents
Low-temperature type carbonic ester lithium battery electrolyte Download PDFInfo
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- Y02E60/10—Energy storage using batteries
Abstract
The invention discloses a low-temperature type carbonic ester lithium battery electrolyte. The electrolyte mainly comprises the following components: ethylene carbonate, dimethyl carbonate, ethyl methyl carbonate and propylene carbonate as solvents, lithium hexafluorophosphate and a low temperature additive. The four carbonic ester solvents are in the following weight ratio: EC: DMC: EMC: PC=2:3:5:1; the components are prepared into an 1 mol / L electrolyte containing LiPF6, four carbonic ester solvents, the low temperature additive; and the low temperature additive is one selected from polydimethylsiloxane, 1,3- propane sultone, and vinylene carbonate, or a combination thereof. According to the invention, optimization of composition of the carbonic ester solvents and addition of the low temperature additive are employed to increase solubility, degree of dissociation and conductivity of the electrolyte, improve structure of a solid phase interfacial film (SEI membrane) of the lithium ion battery cathode, the integral stability of the battery and battery cycling and prolong usage life. Especially, the invention provides a mainstream electrolyte for lithium ion power batteries used in a lowest temperature of -50 DEG C in most regions in northern China.
Description
Technical field
The invention belongs to the lithium battery electrolytes in the electrochemical material technical field, particularly relate to take the carbonates organic substance as solvent, improve the low form carbonic ester lithium battery electrolytes 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.Commercial lithium-ion batteries has been difficult to meet the needs of key areas such as electric motor car, space technology and military affairs at present, one of the main reasons is that the performance of battery 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 using person pays close attention to.By electrolyte, start with to improve temperature performance and be proved to be feasible technological approaches, this is because as in battery, playing the ion conductor of conduction, the performance of electrolyte and affect to a great extent the battery temperature performance with the state of interface that both positive and negative polarity forms.
Have result of study to show: ferric phosphate lithium cell, can be because the lower ionic conductivity of LiFePO 4 material affects the charge-discharge performance of battery under cryogenic conditions; The limiting value of climate change in recent years constantly refreshes historical record, and particularly northern winter temperature is low, in the battery use procedure, electric weight all can not be discharged under low temperature, affects the service efficiency of battery; For this shortcoming, some material producers and research institution attempt by preparing nano-scale particle, increase specific area, and the means such as surface coating modification are improved, but fail to solve fully eventually the cryogenic property problem of ferric phosphate lithium ion battery.Therefore, the electrolyte that exploitation has the wide temperature scope of application, the electrolyte that especially is applicable to northern low temperature season use is significant for cycle life, the raising of storage life of lithium battery.
Summary of the invention
The objective of the invention is to overcome the problem that prior art exists, a kind of good low form carbonic ester lithium battery electrolytes of electrical property be applicable under northern area and cryogenic conditions is provided.
The present invention forms and adds the special additives such as type siloxane, sulfone class and carbonates organic substance and realize the excellent electrical properties under low temperature by the multicomponent solvent of the organic solvent low by freezing point, that conductance is high.Preferably four kinds of carbonates are as solvent composition in the present invention, and its carbonic ester is linear carbonate or the cyclic carbonate directly be connected by 1 or two alkyl and carbon; Four kinds of carbonic esters are: dimethyl carbonate (DMC), methyl ethyl carbonate (EMC), ethylene carbonate (EC), add therein the additive that improves the electrolyte cryogenic property: dimethyl silicone polymer (PDMS), 1,3-N-morpholinopropanesulfonic acid lactone (PS) and vinylene carbonate (VC), the best of experiment definite low temperature additive adds proportioning, make between these several low temperature additives and the synergy between solvent and additive reaches maximum, to improve the electrical property of electrolyte under cryogenic conditions, keeping high discharge capacity and high rate performance.The present invention proposes following technical scheme:
A kind of low form carbonic ester lithium battery electrolytes, this electrolyte are mainly by the ethylene carbonate as solvent composition (EC), dimethyl carbonate (DMC), methyl ethyl carbonate (EMC) and propene carbonate (PC), lithium hexafluoro phosphate LiPF
6With the low temperature additive, form, it is characterized in that: the weight ratio of four kinds of carbonate solvents is EC: DMC: EMC: PC=2: 3: 5: 1, be made into 1mol/L LiPF
6+ tetra-kinds of carbonate solvents (2: 3: 5: the electrolyte that 1)+low temperature additive forms; Described low temperature additive comprises wherein a kind of or its combination in dimethyl silicone polymer (PDMS), PS (PS), vinylene carbonate (VC).
The percentage by weight of described low temperature additive in electrolyte is: dimethyl silicone polymer (PDMS) or PS (PS) 0.8%～2.5%, vinylene carbonate (VC) 0.6%～2.0%.
The preferred weight percent of described low temperature additive in electrolyte is: dimethyl silicone polymer (PDMS) 1.3%, vinylene carbonate (VC) 0.8%.
The preferred weight percent of described low temperature additive in electrolyte is: dimethyl silicone polymer (PDMS) 1.0%, vinylene carbonate (VC) 1.0%.
The preferred weight percent of described low temperature additive in electrolyte is: PS (PS) 1.5%, vinylene carbonate (VC) 0.6%.
The preferred weight percent of described low temperature additive in electrolyte is: PS (PS) 1.5%, vinylene carbonate (VC) 1.5%.
The present invention has at first preferably determined polynary combination and the best proportioning of solvent.Ethylene carbonate in solvent composition (EC) fusing point is higher, although in use can form stable SEI film, but limited its battery application under cryogenic conditions as electrolyte, in order to improve the cryogenic property of battery, the present invention is mixed to form the low-melting organic solvent of it and other blend solution of quaternary system.The methyl ethyl carbonate of ring-type and carboxylic acid esters fusing point are low, as cosolvent, can improve the cryogenic property of battery; Propene carbonate (PC) suppresses ethylene carbonate (EC) crystallization when low temperature effectively, make the low-temperature resistance of SEI film under cryogenic conditions, have higher ionic conductivity, effectively widened the temperature range that battery is used, minimum can arriving under-50 ℃ of low temperature used.
Another characteristics of the present invention are by adding additive to improve the Organic Electrolyte Solutions for Li-Ion Batteries cryogenic property.Because additive amount is little, the characteristics of instant effect, select type siloxane, sulfone class and carbonates organic substance such as dimethyl silicone polymer (PDMS), 1,3-N-morpholinopropanesulfonic acid lactone (PS), vinylene carbonate (VC) are as the low temperature additive, after interpolation, can effectively improve the decomposition voltage of electrolyte, can on graphite cathode surface, form passivating film, to positive pole, oxidation stability preferably also be arranged, improve effectively that electrolyte is minimum reaches-50 ℃ of service behaviours under low temperature.
The present invention is by optimizing carbonate solvent and form and selecting solubility, degree of dissociation and the conductivity that adds the low temperature additive and improve electrolyte, improve the structure of lithium ion battery negative solid-phase interfacial film (SEI film), reduce the SEI low-temperature resistance, improve cell integrated stability, improve cell integrated time lifetime (namely improving the storage service life of battery); Improve circulating battery and improve useful life.
Due to the technological break-through of low temperature aspect, not only for domestic traditional lithium ion battery provides high-performance, low-cost product, and provide security performance and serviceability electrolyte preferably for the dynamic lithium battery of electric automobile.Be in particular the northern China most areas, minimum serviceability temperature provides main flow electrolyte for the lithium-ion-power cell under-50 ℃ of conditions.The applicant has successfully produced the good lithium battery electrolytes of cryogenic property, and product detects through battery relevant departments, and indices reaches the electrokinetic cell instructions for use fully.
Embodiment
Below by the specific embodiment Data Comparison, the cryogenic property under low-temperature flame retardant type electrolyte-50 ℃ is described.Electrolyte solvent of the present invention is the carbonic ester of chain and the carboxylate of ring-type, electrolyte solvent is the quaternary solvent: the weight ratio of ethylene carbonate (EC), dimethyl carbonate (DMC), methyl ethyl carbonate (EMC) and four kinds of carbonate solvents of propene carbonate (PC) is EC: DMC: EMC: PC=2: 3: 5: 1, be made into 1mol/L lithium hexafluoro phosphate LiPF
6+ tetra-kinds of electrolyte that carbonate solvent+low temperature additive forms; By experiment and detect, find out the best proportioning of solvent composition proportioning and low temperature additive, make between additive and solvent and additive between synergy reach maximum.
Embodiment 1:
After in ethylene carbonate (EC), dimethyl carbonate (DMC), methyl ethyl carbonate (EMC) and propene carbonate (PC), adding the additive of 1.3% dimethyl silicone polymer (PDMS) and 0.8% vinylene carbonate (VC), synergy is maximum, discharge capacity and conductivity variations are very large, effectively improve lithium battery electrolytes the cryogenic property of-50 ℃, can keep higher conductivity and discharge capacity.Table 1 is the discharge capacity of these two kinds of electrolyte and the situation of change of conductivity.
Table 11mol/L LiPF
6Discharge capacity and the conductivity of electrolyte under different temperatures with the different solvents composition
Embodiment 2:
In ethylene carbonate (EC), dimethyl carbonate (DMC), methyl ethyl carbonate (EMC) and propene carbonate (PC), add cryogenic property after 1.3% dimethyl silicone polymer (PDMS) additive also to obtain the improvement of part, discharge capacity and Conductivity Ratio are additive-free is to make moderate progress, but effect is good not as two kinds of additive synergistic action effects.Table 2 is the discharge capacity of these two kinds of electrolyte and the situation of change of conductivity.
Table 21mol/L LiPF
6Discharge capacity and the conductivity of electrolyte under different additive amount and different temperatures with the same solvent composition
Embodiment 3:
After in ethylene carbonate (EC), dimethyl carbonate (DMC), methyl ethyl carbonate (EMC) and propene carbonate (PC), adding the additive of 0.8% vinylene carbonate (VC), cycle performance improves, but cryogenic property has no change.Table 3 is to add two kinds of additives and the discharge capacity of two kinds of electrolyte that add a kind of additive and the comparable situation of conductivity.
Table 31mol/L LiPF
6Discharge capacity and the conductivity of electrolyte under different additive amount and different temperatures with the same solvent composition
Embodiment 4:
At ethylene carbonate (EC), in dimethyl carbonate (DMC) and methyl ethyl carbonate (EMC) and propene carbonate (PC), add discharge capacity and the conductivity after 1% dimethyl silicone polymer (PDMS) and 1% vinylene carbonate (VC) additive and add 1.3% dimethyl siloxane (PDMS) and the additive of 0.8% vinylene carbonate (VC) relatively, discharge capacity and conductivity are all on the low side, the cryogenic property of lithium battery electrolytes makes moderate progress, and synergy decreases.Table 4 is to add the discharge capacity of two kinds of electrolyte of additive of different proportionings and the comparable situation of conductivity.
Table 41mol/L LiPF
6Discharge capacity and the conductivity of electrolyte under different additive amount and different temperatures with the same solvent composition
Embodiment 5:
In ethylene carbonate (EC), dimethyl carbonate (DMC), methyl ethyl carbonate (EMC) and propene carbonate (PC), add 1.5% 1, after the additive of 3-N-morpholinopropanesulfonic acid lactone (PS) and 1.5% vinylene carbonate (VC), discharge capacity and 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 descends.Table 5 is to add the discharge capacity of additive electrolyte of different proportionings and the situation of change of conductivity.
Table 51mol/L LiPF
6Discharge capacity and the conductivity of electrolyte under different additive amount and different temperatures with the same solvent composition
Embodiment 6:
In ethylene carbonate (EC), dimethyl carbonate (DMC), methyl ethyl carbonate (EMC) and propene carbonate (PC), add discharge capacity and conductivity after the additive of 2.5% dimethyl silicone polymer (PDMS) and 2% vinylene carbonate (VC) to make moderate progress under low temperature condition, but, along with the increase of additive addition, the electrical property of electrolyte is had to further impact.Table 6 is to add the discharge capacity of additive electrolyte of different proportionings and the situation of change of conductivity.
Table 61mol/L LiPF
6Discharge capacity and the conductivity of electrolyte under different additive amount and different temperatures with the same solvent composition
Embodiment 7:
In ethylene carbonate (EC), dimethyl carbonate (DMC), methyl ethyl carbonate (EMC) and propene carbonate (PC), add 1.5% 1, it is poor 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% dimethyl silicone polymer (PDMS) and 0.8% vinylene carbonate (VC), affected two kinds of materials in the cooperative effect of improving the lithium battery electrolytes electrical property, but the cryogenic property of lithium battery electrolytes also improves.Table 7 is to add the discharge capacity of additive electrolyte of different proportionings and the situation of change of conductivity.
Table 71mol/L LiPF
6Discharge capacity and the conductivity of electrolyte under different additive amount and different temperatures with the same solvent composition
Embodiment 8:
In ethylene carbonate (EC), dimethyl carbonate (DMC), methyl ethyl carbonate (EMC) and propene carbonate (PC), add 0.8% 1, after the additive of 3-N-morpholinopropanesulfonic acid lactone (PS) and 1% vinylene carbonate (VC), discharge capacity and conductivity make moderate progress, the cryogenic property of lithium battery electrolytes also increases, maximum but the synergy of two kinds of additives does not reach.Table 8 is to add the discharge capacity of additive electrolyte of different proportionings and the situation of change of conductivity.
Table 81mol/L LiPF
6Discharge capacity and the conductivity of electrolyte under different additive amount and different temperatures with the same solvent composition
Claims (6)
1. low form carbonic ester lithium battery electrolytes, this electrolyte is mainly by the ethylene carbonate as solvent composition (EC), dimethyl carbonate (DMC), methyl ethyl carbonate (EMC) and propene carbonate (PC), lithium hexafluoro phosphate LiPF
6With the low temperature additive, form, it is characterized in that: the weight ratio of four kinds of carbonate solvents is EC: DMC: EMC: PC=2: 3: 5: 1, be made into 1mol/L LiPF
6+ tetra-kinds of carbonate solvents (2: 3: 5: the electrolyte that 1)+low temperature additive forms; Described low temperature additive comprises wherein a kind of or its combination in dimethyl silicone polymer (PDMS), PS (PS), vinylene carbonate (VC).
2. low form carbonic ester lithium battery electrolytes as claimed in claim 1, it is characterized in that: the percentage by weight of described low temperature additive in electrolyte is: dimethyl silicone polymer (PDMS) or 1,3-N-morpholinopropanesulfonic acid lactone (PS) 0.8%～2.5%, vinylene carbonate (VC) 0.6%～2.0%.
3. low form carbonic ester lithium battery electrolytes as claimed in claim 1 or 2, it is characterized in that: the preferred weight percent of described low temperature additive in electrolyte is: dimethyl silicone polymer (PDMS) 1.3%, vinylene carbonate (VC) 0.8%.
4. low form carbonic ester lithium battery electrolytes as claimed in claim 1 or 2, it is characterized in that: the preferred weight percent of described low temperature additive in electrolyte is: dimethyl silicone polymer (PDMS) 1.0%, vinylene carbonate (VC) 1.0%.
5. low form carbonic ester lithium battery electrolytes as claimed in claim 1 or 2, it is characterized in that: the preferred weight percent of described low temperature additive in electrolyte is: 1,3-N-morpholinopropanesulfonic acid lactone (PS) 1.5%, vinylene carbonate (VC) 0.6%.
6. low form carbonic ester lithium battery electrolytes as claimed in claim 1 or 2, it is characterized in that: the preferred weight percent of described low temperature additive in electrolyte is: 1,3-N-morpholinopropanesulfonic acid lactone (PS) 1.5%, vinylene carbonate (VC) 1.5%.
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| 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 |
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| 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 |
| CN111224161A (en) * | 2018-11-26 | 2020-06-02 | 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 |
| CN112018446A (en) * | 2020-09-27 | 2020-12-01 | 珠海冠宇电池股份有限公司 | Electrolyte suitable for silicon-carbon system lithium ion battery |
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| 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 |
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| 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 |
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