CN103985904A - Non-aqueous electrolyte capable of improving high-temperature performance for lithium ion battery - Google Patents
Non-aqueous electrolyte capable of improving high-temperature performance for lithium ion battery Download PDFInfo
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- CN103985904A CN103985904A CN201410215791.XA CN201410215791A CN103985904A CN 103985904 A CN103985904 A CN 103985904A CN 201410215791 A CN201410215791 A CN 201410215791A CN 103985904 A CN103985904 A CN 103985904A
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators 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
- H01M10/0566—Liquid materials
- H01M10/0567—Liquid materials characterised by the additives
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators 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
- H01M10/0566—Liquid materials
- H01M10/0569—Liquid materials characterised by the solvents
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0025—Organic electrolyte
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0025—Organic electrolyte
- H01M2300/0028—Organic electrolyte characterised by the solvent
- H01M2300/0037—Mixture of solvents
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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
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
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Abstract
The invention discloses a non-aqueous electrolyte capable of improving high-temperature performance for a lithium ion battery. By adopting the non-aqueous electrolyte, the moisture and the HF (Hydrogen Fluoride) content in electrolyte can be reduced, and the charge-discharge cycle performance of the battery can be improved. The non-aqueous electrolyte is prepared from the components in parts by weight: 100 parts of organic solvent, lithium salts and an additive, wherein the solvent is at least one of cyclic carbonate or chainlike carbonate, the additive comprises the components in parts by weight: 1-5 parts of 1,3-propanesultone, 0.01-1 part of silazane and 1-5 parts of an ether nitrile additive. With the adoption of the non-aqueous electrolyte, by virtue of combination use of silazane, 1,3-propanesultone and the ether nitrile additive, the moisture and the HF content in the electrolyte are remarkably reduced, and the high-temperature storage and high-temperature cycle performances are obviously improved.
Description
[technical field]
The present invention relates to a kind of lithium-ion battery electrolytes, relate in particular to a kind of non-aqueous electrolyte for lithium ion cell that improves battery high-temperature behavior.
[background technology]
Lithium ion battery has the advantages such as operating voltage is high, energy density is high, environmental friendliness, stable circulation, safety because of it, be widely used in the various electronic equipments of notebook computer, mobile phone, MP4 etc.But along with the raising of battery capacity in electronic equipment, people also have higher requirement to the operating voltage of lithium ion battery and energy density.But, along with operational environment improves moisture temperature requirement, in electrolyte, water content is too high causes it to accelerate with reacting also of electrolyte thereupon, and generation HF finally causes under normal temperature and high temperature inflatable serious, cycle performance reduces, and has seriously restricted the performance of battery performance performance.
[summary of the invention]
The technical problem to be solved in the present invention is to provide a kind ofly can reduce moisture and HF content in electrolyte, improve the good non-aqueous electrolyte for lithium ion cell that improves battery high-temperature behavior of battery charging and discharging cycle performance.
In order to solve the problems of the technologies described above, the technical solution used in the present invention is: the present invention includes organic solvent, lithium salts and additive, described solvent is at least one in cyclic carbonate or linear carbonate, described additive comprises 1,3-N-morpholinopropanesulfonic acid lactone, silazane and ether nitrile additive, wherein, by weight, described organic solvent is that 100 weight portions, described PS are that 1～5 weight portion, described silazane are that 0.01～1 weight portion, described ether nitrile additive are 1～5 weight portion.
Optimize, described additive also comprises conventional additives, and described conventional additives is 0.1～5 weight portion, described typical additives is the sub-ethene of carbonic acid, vinyl ethylene carbonate vinegar, 1, at least one in 3-propane sultone, Isosorbide-5-Nitrae-butyl sultone and propenyl-1,3-sulfonic acid lactone.
Optimize, described cyclic carbonate is at least one in ethylene carbonate, propene carbonate and fluorinated ethylene carbonate or gamma-butyrolacton.
Optimize, described linear carbonate is at least one in dimethyl carbonate, diethyl carbonate, methyl ethyl carbonate, methyl propyl carbonate and ethyl propyl carbonic acid ester.
Optimize, described silazane is at least one in hexamethyldisiloxane, heptamethyldisilazane or fluoro silazane.
Optimize, described ether nitrile is added to ethylene glycol monobutyl ether, ethylene glycol bis (propionitrile) ether, 1,2, at least one of 3-tri-(2-cyanato-) propane.
Optimize, the molar concentration of described lithium salts in described organic solvent is 0.8～1.5mol/L, and described lithium salts is LiPF
6, LiBF
4, LiC10
4, LiAsF
6, LiCF
3sO
2, LiN (CF
3s0
2)
2, LiBOB, LiDFOB, LiPF
4c
20
4or LiN (C
2f
5s0
2)
2in at least one.
The invention has the beneficial effects as follows: by by silazane, 1, 3～propane sultone, ether nitrile additive combine use, ether nitriles substance can absorb a small amount of water and HF, form amide substance, reduction is due to the catalysis of HF and POF3 etc., the high temperature flatulence that electrolyte solvent decomposition is caused is eliminated, nitriles substance can form stabilising membrane on anodal surface in first charge-discharge process, effectively suppress anodal oxidation electrolyte, thereby suppress high temperature flatulence, under high temperature storage condition, the decomposition of described lithium salts, HF, PF6 etc. can make nonaqueous electrolytic solution be acid, in acid solution, oxidation reaction in the anodal surface of nonaqueous electrolytic solution can be accelerated, yet, have oxygen (0-) in the ether of dinitrile compound of ehter bond can with nonaqueous electrolytic solution in HF, PF6 etc. form key, thus, can prevent the formation of acid solution, with the restriction oxidation of nonaqueous electrolytic solution and the acceleration of decomposition reaction, silazane can suppress hydrolysis and the pyrolysis of electrolyte LiPF6 in storage process, the content of H2O and HF in minimizing electrolyte, obviously improve storage stability and the thermal stability of lithium-ion electrolyte, can improve chemical property and the cycle performance of lithium ion battery simultaneously, 1, 3 propane sultones (PS) can form fine and close SEI film at negative pole, can effectively improve the high-temperature storage characteristics of lithium rechargeable battery, the use of combining of above three kinds of additives significantly improves moisture and HF content in electrolyte, obviously improve high-temperature storage and high temperature cyclic performance
[embodiment]
The present invention includes organic solvent, lithium salts and additive, described organic solvent is at least one in cyclic carbonate or linear carbonate, described cyclic carbonate is at least one in ethylene carbonate, propene carbonate and fluorinated ethylene carbonate or gamma-butyrolacton, and described linear carbonate is at least one in dimethyl carbonate, diethyl carbonate, methyl ethyl carbonate, methyl propyl carbonate and ethyl propyl carbonic acid ester.Described additive comprises 1,3-N-morpholinopropanesulfonic acid lactone, silazane class additive, ether nitrile additive and conventional additives, wherein, by weight, described organic solvent is 100 weight portions, described 1,3-N-morpholinopropanesulfonic acid lactone is that 1～5 weight portion, described silazane class additive are that 0.01～1 weight portion, described ether nitrile additive are that 1～5 weight portion, described conventional additives are 0.1～5 weight portion, described typical additives is the sub-ethene of carbonic acid, vinyl ethylene carbonate vinegar, 1, at least one in 4-butyl sultone and propenyl-1,3-sulfonic acid lactone.Wherein, described silazane class additive is at least one in hexamethyldisiloxane, heptamethyldisilazane or fluoro silazane, described ether nitrile additive is ethylene glycol bis (propionitrile) ether, 1,2, at least one in 3-tri-(2-cyanato-) propane, the molar concentration of described lithium salts in described organic solvent is 0.8～1.5mol/L, and described lithium salts is LiPF
6, LiBF
4, LiC10
4, LiAsF
6, LiCF
3sO
2, LiN (CF
3s0
2)
2, LiBOB, LiDFOB, LiPF
4c
20
4or LiN (C
2f
5s0
2)
2in at least one,
By by silazane, 1, 3～propane sultone, ether nitrile additive combine use, ether nitriles substance can absorb a small amount of water and HF, form amide substance, reduction is due to the catalysis of HF and POF3 etc., the high temperature flatulence that electrolyte solvent decomposition is caused is eliminated, nitriles substance can form stabilising membrane on anodal surface in first charge-discharge process, effectively suppress anodal oxidation electrolyte, thereby suppress high temperature flatulence, under high temperature storage condition, the decomposition of described lithium salts, HF, PF6 etc. can make nonaqueous electrolytic solution be acid, in acid solution, oxidation reaction in the anodal surface of nonaqueous electrolytic solution can be accelerated, yet, have oxygen (0-) in the ether of dinitrile compound of ehter bond can with nonaqueous electrolytic solution in HF, PF6 etc. form key, thus, can prevent the formation of acid solution, with the restriction oxidation of nonaqueous electrolytic solution and the acceleration of decomposition reaction, silazane can suppress hydrolysis and the pyrolysis of electrolyte LiPF6 in storage process, the content of H2O and HF in minimizing electrolyte, obviously improve storage stability and the thermal stability of lithium-ion electrolyte, can improve chemical property and the cycle performance of lithium ion battery simultaneously.PS (PS) can form fine and close SEI film at negative pole, can effectively improve the high-temperature storage characteristics of lithium rechargeable battery.The use of combining of above three kinds of additives significantly improves moisture and HF content in electrolyte, obviously improves high-temperature storage and high temperature cyclic performance.
Below in conjunction with specific embodiment, the present invention is described in detail:
Embodiment mono-:
The present embodiment is to prepare electrolyte in BRAUN glove box, in glove box, be full of purity and be 99.999% nitrogen, be controlled at≤5ppm of moisture in glove box, temperature is at room temperature, 30 grams of ethylene carbonates and 70 grams of methyl ethyl carbonates are mixed to rear sealing, put into refrigerator and be cooled to after 8 ℃ until it, be transferred in glove box, then add in two batches LiPF
6fully mix, forming lithium salts molar concentration is the nonaqueous electrolytic solution of the lithium ion battery of 1 mol/L, in above nonaqueous electrolytic solution, add described organic solvent gross mass 0.01% hexamethyldisiloxane, 3% 1, after 3-N-morpholinopropanesulfonic acid lactone, 1% ethylene glycol monobutyl ether and 1% vinylene carbonate evenly mix, obtain the lithium ion nonaqueous electrolytic solution of the present embodiment.
Wherein, FEC(CAS:114435-02-8), SN (CAS:110-61-2), AND (111-69-3), PS(CAS:1120-71-4) etc. material purchased from lark prestige Science and Technology Ltd..
Embodiment bis-:
The present embodiment and embodiment mono-are roughly the same, different, and what in the present embodiment, adopt is that 40 grams of ethylene carbonates and 60 grams of diethyl carbonates mix rear sealing, puts into refrigerator and is cooled to after 8 ℃ until it, is transferred in glove box, then adds in two batches LiPF
6fully mix, forming lithium salts molar concentration is the nonaqueous electrolytic solution of the lithium ion battery of 1.2 mol/L, in described nonaqueous electrolytic solution, add described organic solvent gross mass 0.1% hexamethyldisiloxane, 2% 1,3-N-morpholinopropanesulfonic acid lactone, 2% 1,2, after 3-tri-(2-cyanato-) propane and 2% vinylene carbonate evenly mix, obtain the lithium ion nonaqueous electrolytic solution of the present embodiment.
Embodiment tri-:
The present embodiment and embodiment mono-are roughly the same, different, what in the present embodiment, adopt is that 20 grams of ethylene carbonates, 50 grams of methyl ethyl carbonates and 30 grams of diethyl carbonates mix rear sealing, puts into refrigerator and is cooled to after 8 ℃ until it, be transferred in glove box, then add in two batches LiPF
6fully mix, form the nonaqueous electrolytic solution of the lithium ion battery that lithium salts molar concentration is 1.2mol/L, in described nonaqueous electrolytic solution, add described organic solvent gross mass 0.2% heptamethyldisilazane, 5% 1, after 3-N-morpholinopropanesulfonic acid lactone, 1.5% ethylene glycol bis (propionitrile) ether and 3% vinylene carbonate evenly mix, obtain the lithium ion nonaqueous electrolytic solution of the present embodiment.
Embodiment tetra-:
The present embodiment and embodiment mono-are roughly the same, different, what in the present embodiment, adopt is that 30 grams of ethylene carbonates, 30 grams of methyl ethyl carbonates and 40 grams of diethyl carbonates mix rear sealing, puts into refrigerator and is cooled to after 8 ℃ until it, be transferred in glove box, then add in two batches LiPF
6fully mix, form the nonaqueous electrolytic solution of the lithium ion battery that lithium salts molar concentration is 0.8mol/L, in described nonaqueous electrolytic solution, add described organic solvent gross mass 0.5% hexamethyldisiloxane, 3% 1,3-N-morpholinopropanesulfonic acid lactone, 1% 1,2, after 3-tri-(2-cyanato-) propane and 2% vinylene carbonate evenly mix, obtain the lithium ion nonaqueous electrolytic solution of the present embodiment.
Embodiment five:
The present embodiment and embodiment mono-are roughly the same, different, what in the present embodiment, adopt is that 40 grams of ethylene carbonates, 30 grams of methyl ethyl carbonates and 30 grams of diethyl carbonates mix rear sealing, puts into refrigerator and is cooled to after 8 ℃ until it, be transferred in glove box, then add in two batches LiPF
6fully mix, form the nonaqueous electrolytic solution of the lithium ion battery that lithium salts molar concentration is 1.5mol/L, in described nonaqueous electrolytic solution, add described organic solvent gross mass 0.1% heptamethyldisilazane, 1% 1, after 3-N-morpholinopropanesulfonic acid lactone, 5% ethylene glycol bis (propionitrile) ether and 5% vinylene carbonate evenly mix, obtain the lithium ion nonaqueous electrolytic solution of the present embodiment.
Comparative example:
Applicant has according to circumstances selected the original formulation system of 5 kinds of different proportions to carry out comparative illustration, does not comprise the disclosed 3 kinds of additives of the application in these 5 kinds of formula systems.
Table 1: the constituent content table of embodiment 1-5
The constituent content table of table 2: comparative example 1-5
Electrolyte of the present invention has carried out cycle performance test after assembled battery, and method is as follows:
The cobalt acid lithium of take is positive electrode, and negative pole adopts carbonaceous mesophase spherules, and both positive and negative polarity collector is distributed as aluminium foil and Copper Foil, and barrier film adopts ceramic diaphragm to form soft-package battery, injects after electrolyte, is assembled into soft-package battery in glove box, after standing 8 hours, tests.Under 25 ℃ of constant temperature of room temperature, discharge and recharge battery is activated respectively with 1/10C 3.0V to 4.2V, the circulation under 45 ℃ of conditions subsequently all discharges and recharges with 1C.
From table 3 cycle performance test data, adopt the higher capability retention that has after 300 circulations of embodiment battery of nonaqueous electrolytic solution of the present invention; The capability retention of the comparative example battery of employing prior art electrolyte is low very low.
Table 3: embodiment and comparative example loop test result
60 ℃/7D memory property test, lower list 4 is to deposit 7D at battery stands after standard charging 60 ℃ again, measures subsequently the capability retention of battery.
Table 4: embodiment and comparative example high-temperature storage performance test result
The additive 1 using in the electrolyte of the above embodiment of the present invention, 3-N-morpholinopropanesulfonic acid lactone, silazane class additive, ether nitrile additive can be worked in coordination with normal temperature and the high-temperature storage performance of improving battery under voltage, therefore, electrolyte of the present invention ties up under hot and humid condition, has good normal-temperature circulating performance and high-temperature storage performance.
The present invention has following advantage and effect with respect to prior art:
(1) lithium battery that uses the above-described anti-hot and humid storage inflatable electrolyte nonaqueous electrolytic solution of the present invention to prepare has better normal temperature circulation and high-temperature storage performance.
(2) use the nonaqueous electrolytic solution additive therefor cost of the above-described lithium ion battery of the present invention low, there is larger cost advantage.
Claims (7)
1. a non-aqueous electrolyte for lithium ion cell that improves battery high-temperature behavior, it comprises organic solvent, lithium salts and additive, it is characterized in that: described solvent is at least one in cyclic carbonate or linear carbonate, described additive comprises 1,3-N-morpholinopropanesulfonic acid lactone, silazane class additive and ether nitrile additive, wherein, by weight, described organic solvent is that 100 weight portions, described PS are that 1～5 weight portion, described silazane class additive are that 0.01～1 weight portion, described ether nitrile additive are 1～5 weight portion.
2. the non-aqueous electrolyte for lithium ion cell that improves battery high-temperature behavior according to claim 1: it is characterized in that: described additive also comprises conventional additives, described conventional additives is 0.1～5 weight portion, described typical additives is vinylene carbonate, vinyl ethylene carbonate, 1, at least one in 4-butyl sultone and propenyl-1,3-sulfonic acid lactone.
3. the non-aqueous electrolyte for lithium ion cell that improves battery high-temperature behavior according to claim 1, is characterized in that: described cyclic carbonate is at least one in ethylene carbonate, propene carbonate and fluorinated ethylene carbonate or gamma-butyrolacton.
4. the non-aqueous electrolyte for lithium ion cell that improves battery high-temperature behavior according to claim 1, is characterized in that: described linear carbonate is at least one in dimethyl carbonate, diethyl carbonate, methyl ethyl carbonate, methyl propyl carbonate and ethyl propyl carbonic acid ester.
5. the non-aqueous electrolyte for lithium ion cell that improves battery high-temperature behavior according to claim 1, is characterized in that: described silazane class additive is at least one in hexamethyldisiloxane, heptamethyldisilazane or fluoro silazane.
6. the non-aqueous electrolyte for lithium ion cell that improves battery high-temperature behavior according to claim 1, it is characterized in that: described ether nitrile additive is ethylene glycol monobutyl ether, ethylene glycol bis (propionitrile) ether, 1, at least one in 2,3-tri-(2-cyanato-) propane.
7. the non-aqueous electrolyte for lithium ion cell that improves battery high-temperature behavior according to claim 1, is characterized in that: the molar concentration of described lithium salts in described nonaqueous electrolytic solution is 0.8～1.5mol/L, and described lithium salts is LiPF
6, LiBF
4, LiC10
4, LiAsF
6, LiCF
3sO
2, LiN (CF
3s0
2)
2, LiBOB, LiDFOB, LiPF
4c
20
4or LiN (C
2f
5s0
2)
2in at least one.
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| CN105470563A (en) * | 2015-01-28 | 2016-04-06 | 万向A一二三系统有限公司 | Lithium ion battery electrolyte suitably used for silicon-carbon negative electrode |
| CN105789699A (en) * | 2016-03-22 | 2016-07-20 | 芜湖天弋能源科技有限公司 | Lithium secondary battery and preparation method thereof as well as lithium secondary battery electrolyte |
| CN107055574A (en) * | 2017-04-10 | 2017-08-18 | 多氟多化工股份有限公司 | A kind of method of purification of lithium hexafluoro phosphate |
| CN107611479A (en) * | 2017-09-08 | 2018-01-19 | 广东天劲新能源科技股份有限公司 | Lithium ion power battery electrolyte and lithium rechargeable battery |
| CN109256586A (en) * | 2017-07-14 | 2019-01-22 | 宁德时代新能源科技股份有限公司 | Electrolyte and electrochemical device |
| CN111244542A (en) * | 2020-03-21 | 2020-06-05 | 湖州安和材料科技有限公司 | Low-temperature-resistant lithium battery electrolyte and preparation process thereof |
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| CN107611479A (en) * | 2017-09-08 | 2018-01-19 | 广东天劲新能源科技股份有限公司 | Lithium ion power battery electrolyte and lithium rechargeable battery |
| CN107611479B (en) * | 2017-09-08 | 2022-10-11 | 广东天劲新能源科技股份有限公司 | Lithium ion power battery electrolyte and lithium ion secondary battery |
| CN112290088A (en) * | 2019-07-23 | 2021-01-29 | 张家港市国泰华荣化工新材料有限公司 | Non-aqueous electrolyte and lithium ion battery |
| CN111244542A (en) * | 2020-03-21 | 2020-06-05 | 湖州安和材料科技有限公司 | Low-temperature-resistant lithium battery electrolyte and preparation process thereof |
| CN111682264B (en) * | 2020-06-05 | 2022-04-01 | 惠州锂威新能源科技有限公司 | Electrolyte additive, electrolyte and lithium ion battery |
| CN111682264A (en) * | 2020-06-05 | 2020-09-18 | 惠州锂威新能源科技有限公司 | Electrolyte additive, electrolyte and lithium ion battery |
| CN112234253A (en) * | 2020-10-26 | 2021-01-15 | 珠海冠宇电池股份有限公司 | Electrolyte for lithium secondary battery and lithium secondary battery comprising same |
| CN112151867A (en) * | 2020-10-26 | 2020-12-29 | 珠海冠宇电池股份有限公司 | Electrolyte for lithium secondary battery and lithium secondary battery comprising same |
| CN113707941A (en) * | 2021-09-01 | 2021-11-26 | 河源市联懋新材料有限公司 | Electrolyte for improving gas production of lithium ion battery and manufacturing method thereof |
| WO2023123353A1 (en) * | 2021-12-31 | 2023-07-06 | 东莞新能源科技有限公司 | Electrochemical device and electronic device |
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