CN115732755A - Electrolyte and secondary battery using same - Google Patents
Electrolyte and secondary battery using same Download PDFInfo
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- CN115732755A CN115732755A CN202111003281.2A CN202111003281A CN115732755A CN 115732755 A CN115732755 A CN 115732755A CN 202111003281 A CN202111003281 A CN 202111003281A CN 115732755 A CN115732755 A CN 115732755A
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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
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Abstract
The present invention relates to an electrolyte and a secondary battery using the same. In order to solve the problems that the conventional electrolyte can not simultaneously meet the requirements of improving the capacity retention rate of the battery at normal temperature and high temperature, inhibiting the swelling and the internal resistance increase of the battery at high temperature and reducing the phenomenon of lithium precipitation of a negative electrode of the battery at low temperature, the invention provides the electrolyte, which comprises a lithium salt, an organic solvent and an additive, wherein the additive comprises
Wherein R1 and R2 are independently C 1 ‑C 6 Alkyl or
Wherein G is 1 Is a bond, C 1 ‑C 5 Alkylene or heteroatom-containing substituent group, G 2 Is C 1 ‑C 5 Alkyl or a substituent group containing a hetero atom, and, G 1 、G 2 At least one of which is a substituent group containing a hetero atom, and at least one of R1 and R2 is
Description
Technical Field
The invention belongs to the technical field of lithium batteries, and particularly relates to an electrolyte and a secondary battery using the same.
Background
Lithium ion batteries have been receiving great attention from industries such as portable electronic devices, unmanned aerial vehicles, electric vehicles, and energy storage power stations because of their advantages such as relatively high energy density, high operating voltage, and excellent cycle performance. The electrolyte is an important component of a lithium ion battery, plays a role in conducting electrons between a positive electrode and a negative electrode of the lithium ion battery, and can be composed of a solvent, a lithium salt and an additive, the comprehensive performance of the lithium ion battery is improved by screening the additive in a common method at present, CN 109888393A discloses the electrolyte, and an SEI film formed by the synergistic effect of an alkyl silicon-based carboxylic ester compound and/or an alkyl silicon-based carbonate compound, 1, 3-propane sultone, succinonitrile and adiponitrile is compact and has high toughness and is not easy to break, so that the cycle performance of the battery is improved. CN 106415910B discloses an electrolyte containing an electrolyte and a non-aqueous solvent, and also containing a specific aromatic carboxylic ester, which can improve the initial capacity, efficiency, rate characteristics and initial gas production of a battery, as well as the capacity, efficiency, rate characteristics after high temperature storage and safety upon overcharge. CN 109802178B discloses an electrolyte containing a silicon solvent and a sulfonate additive, and a lithium ion battery using the electrolyte. The silicon solvent in the electrolyte can improve the oxidation resistance of the electrolyte, reduce the viscosity of the electrolyte and simultaneously improve the low-temperature performance and the rate capability of the lithium battery, and the sulfonic acid ester compound can cover the active site of the positive electrode, protect the positive electrode, inhibit the side reaction on the surface of the electrode and the dissolution of metal ions, and can obviously improve the high-temperature cycle performance and the high-temperature storage performance of the lithium ion battery on the premise of ensuring the low-temperature performance.
Although the performance of the lithium ion battery is improved to a certain extent by the above method, the method has certain limitations, and cannot simultaneously satisfy the improvement of the capacity retention rate of the battery at normal temperature and high temperature, inhibit the swelling and internal resistance increase of the battery at high temperature, and reduce the phenomenon of lithium precipitation of the negative electrode of the battery at low temperature.
Disclosure of Invention
The invention aims to provide an electrolyte capable of improving the thermal stability and the electrochemical stability of a positive electrode and a negative electrode of a lithium ion battery, further improving the charge-discharge characteristics of the lithium ion battery, improving the capacity retention rate of the battery at normal temperature and high temperature, simultaneously inhibiting the swelling and the increase of internal resistance of the battery at high temperature and slowing down the lithium precipitation phenomenon of the negative electrode of the battery at low temperature, and a secondary battery containing the electrolyte.
In order to achieve the purpose, the technical scheme adopted by the invention is as follows:
the invention provides an electrolyte, which comprises lithium salt, an organic solvent and an additive, wherein the additive comprises a carboxylic ester derivative, the carboxylic ester derivative is one or more of compounds shown in a structural formula (I), and the structure of the carboxylic ester derivative is shown in the specification
R1 and R2 are independently C 1 -C 6 Alkyl or
Wherein G is 1 Is a bond, C 1 -C 5 Alkylene or heteroatom-containing substituent group, G 2 Is C 1 -C 5 Alkyl orA substituent group containing a hetero atom, and, G 1 、G 2 At least one of which is a substituent group containing a hetero atom, and at least one of R1 and R2 is
Said bond is G 1 Is a single bond between two carbon atoms, not an atom, i.e. when G 1 In the case of a key, the key is,
is composed of
Preferably, the substituent group containing the heteroatom has a structural formula of R 5 OR 6 ，-OR 6 ，-R 5 SR 6 ，-SR 6 ，-S i R 6 R 7 R 8 or-R 5 S i R 6 R 7 R 8 Wherein R is 5 Is C 1 -C 5 Alkylene, R 6 、R 7 、R 8 Independently is C 1 -C 5 An alkyl group.
Further preferably, R is 5 Is C 1 -C 3 Alkylene radical, R 6 、R 7 、R 8 Independently is C 1 -C 4 An alkyl group.
Further preferably, one of R1 and R2 is C 1 -C 6 A straight chain alkyl radical, the other being
Said G 1 、G 2 One of which is a substituent group containing a heteroatom. According to some specific and preferred embodiments, the carboxylic ester derivative is selected from one or more of the following substances represented by the following structural formula:
preferably, the additive further comprises an aromatic compound, wherein the aromatic compound is one or more of compounds shown in a structural formula (II), and the structural formula (II) is
R3 and R4 are independently C 1 -C 6 Alkyl, unsubstituted or substituted phenyl, the substituents being halo, alkyl, haloalkyl, alkenyl, haloalkenyl, alkynyl, haloalkynyl, phenyl, halophenyl, carbonyl, nitro, amino, cyano, thio, at least one of R3 and R4 being unsubstituted or substituted phenyl.
According to some embodiments, the aromatic compound is selected from one or more of the following formulas:
preferably, the carboxylic ester derivative accounts for 0.01-5.0% of the total mass of the electrolyte.
More preferably, the carboxylic ester derivative accounts for 0.1-2% of the total mass of the electrolyte.
Preferably, the combination of the carboxylate derivative and the aromatic compound accounts for 0.01 to 5.0% of the total mass of the electrolyte.
More preferably, the carboxylic ester derivative accounts for 0.1-2% of the total mass of the electrolyte; the aromatic compound accounts for 0.1-1% of the total mass of the electrolyte.
Still more preferably, the carboxylic ester derivative accounts for 0.5-1.5% of the total mass of the electrolyte; the aromatic compound accounts for 0.1-0.8% of the total mass of the electrolyte.
More preferably, the mass ratio of the carboxylate derivative to the aromatic compound is 0.5 to 8.
Still more preferably, the mass ratio of the carboxylate derivative to the aromatic compound is 0.85 to 7.
Preferably, the organic solvent is one or more of carbonate, carboxylate, ether and sulfone.
Further preferably, the carbonate comprises a fluoro carbonate.
Further preferably, the carboxylic acid ester comprises a fluorocarboxylic acid ester.
Further preferably, the ether comprises a fluoroether.
Further preferably, the sulfone comprises one or more of sulfoxide, fluorosulfone and fluorosulfoxide.
Still more preferably, the organic solvent is a mixture of two or more selected from dimethyl carbonate, diethyl carbonate, ethylene carbonate, propylene carbonate, ethyl methyl carbonate, ethylene glycol dimethyl ether, r-butyrolactone, methyl acetate, ethyl acetate, propyl acetate, butyl acetate, methyl propionate, propyl propionate, butyl propionate, methyl butyrate, ethyl butyrate, sulfolane, methyl ethyl sulfone, dimethyl sulfoxide, fluoroethylene carbonate, difluoroethylene carbonate, trifluoroethyl carbonate, fluoroethylsulfone, and tetrafluoroethyl tetrafluoropropyl ether.
According to some embodiments, the organic solvent is a mixture of ethylene carbonate, propylene carbonate, diethyl carbonate, ethyl methyl carbonate.
More specifically, the mass ratio of the ethylene carbonate, the propylene carbonate, the diethyl carbonate and the ethyl methyl carbonate is (3-5) to (1), (2-4) to (7-9).
According to some embodiments, the organic solvent further comprises ethyl propionate and/or tetrafluoroethyl tetrafluoropropyl ether.
Preferably, the organic solvent accounts for 50-85% of the total amount of the electrolyte.
More preferably, the organic solvent accounts for 70-85% of the total amount of the electrolyte.
Preferably, the lithium salt is LiPF 6 、LiBF 4 、LiAsF 6 、LiClO 4 、LiCF 3 SO 3 、LiC 4 F 9 SO 3 、Li(CF 3 SO 2 ) 2 N、Li(SO 2 F) 2 N、Li(CF 3 SO 2 ) 3 C、Li(C 6 F 5 ) 4 B、Li(C 2 F 5 SO 2 ) 2 N、LiBF 3 C 2 F 5 、LiPF 3 (C2F 5 ) 3 One or more of them.
Preferably, the lithium salt accounts for 8% -25% of the total mass of the electrolyte.
More preferably, the lithium salt accounts for 8-15% of the total mass of the electrolyte.
Preferably, the electrolyte further comprises other additives, and the other additives are one or more of cyclic carbonate, sulfonate, sultone, sulfate, sulfite, a benzene-containing compound, a halogenated compound, a nitrile compound, a boron-containing compound, a cyclic ether compound, a phosphazene compound, phosphate, phosphite, an amine compound, an isocyanate compound, a silicon-containing compound, a lithium salt type compound, and a fluoroether compound.
<xnotran> , , , , , , ,1,3- ,1,3- , , , , , ,3,4- ,4- 2- , , ,1,2- -4- , N- , ,2,5- ,1,4- , , , , , , , N, N- , N, N- , , , , , , , , , , , , ( ) , , ( ) , ( ) , ( ) , (1,1,1,3,3,3- -2- ) ,1,1,2,2- -2,2,3,3- . </xnotran>
Still further preferably, the other additive is one or more of vinylene carbonate, lithium difluorophosphate, fluoroethylene carbonate and 1, 3-propane sultone.
According to some embodiments, the other additive is a combination of vinylene carbonate, lithium difluorophosphate, fluoroethylene carbonate and 1, 3-propane sultone in a mass ratio of (0.8-1.2) to (0.4-0.7) to (1.5-3) to 1.
Preferably, the other additives account for 0.5-15% of the total mass of the electrolyte.
More preferably, the other additives account for 1.0-10% of the total mass of the electrolyte.
More preferably, the other additives account for 3.0-6.0% of the total mass of the electrolyte.
The second aspect of the invention also provides a lithium ion battery, which comprises the electrolyte.
Specifically, the lithium ion battery comprises a shell, and a battery cell and the electrolyte which are accommodated in the shell.
More specifically, the battery cell comprises a positive electrode, a negative electrode, and a separator interposed between the positive electrode and the negative electrode.
More specifically, the positive electrode comprises a positive electrode current collector and a positive electrode material positioned on the surface of the positive electrode current collector, the positive electrode material comprises a positive electrode active substance, a positive electrode conductive agent and a positive electrode binder, and the positive electrode active substance can beIs LiCoO 2 、LiNi 0.5 Mn 1.5 O 4 、LiNiPO 4 、LiCoPO 4 、Li 3 V 2 (PO 4 ) 3 、LiNi 1-y-z Co y Mn z O 2 、LiNi 1-y-z Co y Al z O 2 Wherein x is more than or equal to 0 and less than or equal to 1, y is more than or equal to 0, z is more than or equal to 0, y + z is less than or equal to 1.
According to some embodiments, the positive active material is LiCoO 2 (LCO)/LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811)。
According to some embodiments, the positive electrode conductive agent is acetylene black or carbon nanotubes, and the positive electrode binder is polyvinylidene fluoride.
Specifically, the negative electrode comprises a negative electrode current collector and a negative electrode material positioned on the surface of the negative electrode current collector, wherein the negative electrode material comprises a negative electrode active material and a negative electrode binder, and the negative electrode material can also optionally comprise a negative electrode conductive agent.
More specifically, the negative electrode conductive agent and the positive electrode conductive agent may be the same or different and are conductive agents commonly used in the art.
More specifically, the negative electrode active material and the negative electrode binder may be those conventionally used in the art, for example, the negative electrode active material may be metallic lithium, metal oxide, lithium aluminum alloy, graphite, and modified carbon material, silicon and its silicon oxygen, silicon carbon.
According to some embodiments, the negative active material is graphite.
In particular, the separator layer is a separator layer conventionally used in the art.
Due to the application of the technical scheme, compared with the prior art, the invention has the following advantages:
according to the invention, by research, the carboxylate derivative additive shown in the structural general formula (I) is added, and the organic solvent and the lithium salt in the non-aqueous electrolyte are combined, so that the thermal stability and the electrochemical stability of the positive electrode and the negative electrode of the lithium ion battery can be improved, the charge-discharge characteristics of the lithium ion battery can be further improved, the capacity retention rate of the battery at normal temperature and high temperature can be improved, the battery swelling and internal resistance increase at high temperature can be inhibited, and the phenomenon of lithium precipitation of the negative electrode of the battery at low temperature can be relieved. Further, by adding a combination additive containing a carboxylic ester derivative represented by formula (I) and an aromatic compound represented by formula (II) in combination with other additives, the normal temperature and high temperature cycle performance of the battery can be further improved, the high temperature storage safety performance can be improved, and the low temperature charge and discharge performance can be improved at the same time. The electrolyte and the secondary battery have wide commercial prospect.
Detailed Description
The present invention will be further described with reference to the following examples. However, the present invention is not limited to the following examples. The implementation conditions adopted in the embodiments can be further adjusted according to different requirements of specific use, and the implementation conditions not noted are conventional conditions in the industry. The technical features of the embodiments of the present invention may be combined with each other as long as they do not conflict with each other.
In order to improve the comprehensive properties of the lithium secondary battery, including normal temperature and high temperature cycle performance, high temperature storage performance and safety performance, low temperature charge and discharge performance and the like, in the prior art, a plurality of additive combinations are generally used, the types of the additives are more, the use of different additive combinations generally cannot meet all the performance requirements at the same time, the more complex the additive components are, the greater the influence on the charge and discharge performance of the secondary battery is, the more the manufacturing cost of the battery is obviously improved, and the commercial development of the lithium secondary battery is not facilitated.
In view of the above problems, the present invention provides a novel carboxylate derivative additive, which can improve the capacity retention rate of a battery at normal temperature and high temperature, inhibit swelling and internal resistance increase of the battery at high temperature, and slow down lithium precipitation at the negative electrode of the battery at low temperature, and further combine it with a specific aromatic compound in a certain proportion to obtain a synergistic effect, thereby further improving the capacity retention rate of the battery at normal temperature and high temperature, reducing the swelling rate and internal resistance rate at high temperature, and improving the charge and discharge performance at low temperature. The commercial development of the lithium secondary battery is promoted while the comprehensive performance of the lithium secondary battery is ensured.
Preparing an electrolyte:
detailed description of the inventiona battery electrolyte was formulated in a glove box according to the formulation described in table 1. Among them, the names of substances referred to in the table are Ethylene Carbonate (EC), propylene Carbonate (PC), diethyl carbonate (DEC), ethyl Methyl Carbonate (EMC), ethyl Propionate (EP), vinylene Carbonate (VC), lithium bis-fluorosulfonylimide (LiFSI), lithium difluorophosphate (LiDFP), fluoroethylene carbonate (FEC), 1, 3-Propanesultone (PS), 4-fluorophenylmethyl acetate, trimethylsilyl ethyl acetate.
TABLE 1
The additives referred to in table 1 are as follows:
preparing a battery:
the electrolytes obtained in comparative examples 1 to 5 and examples 1 to 49 were injected into the same batch of LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM 811) in the 1Ah polymer soft package battery, the capacity retention ratio (discharge capacity after cycle/discharge capacity before cycle) after 500 cycles of 1C charge and discharge at 25 ℃ and 60 ℃ under the voltage of 4.3V was tested, and the test results are shown in the table2; the test results of the battery were shown in table 3, for the discharge capacity retention rate after being left at high temperature 60 ℃ for 7 days (discharge capacity after being left)/discharge capacity before being left) and the thickness change rate ((thickness after being left)/thickness before being left) at full charge of 4.3V. The test cells were charged at 0C at low temperature 0C for 4.3V and then 0.2C was discharged to 2.75V capacity after charging at 1C and 5C, respectively, and the test results are shown in table 4.
The experimental results are as follows:
TABLE 2
As can be seen from table 2, the electrolyte solution to which the carboxylate derivatives represented by S1 to S7 were added under normal temperature and high temperature conditions had an improved capacity retention rate after 25 ℃/500 weeks and an improved capacity retention rate after 60 ℃/500 weeks, and the electrolyte solution to which the carboxylate derivatives represented by S1 to S7 and the aromatic compounds represented by F1 to F8 were added at the same time had an improved capacity retention rate after 25 ℃/500 weeks and an improved capacity retention rate after 60 ℃/500 weeks.
TABLE 3
As can be seen from Table 3, the electrolyte solutions to which the carboxylate derivatives represented by S1 to S7 were added exhibited significantly higher capacity retention rates than the comparative examples after being left at 60 ℃ for 7 days, and significantly lower thickness growth rates and internal resistance growth rates than the comparative examples. And further simultaneously adding the carboxylate derivatives shown in S1-S7 and the electrolyte of the aromatic compounds shown in F1-F8, further improving the capacity retention rate after being placed for 7 days at 60 ℃, and further reducing the thickness growth rate and the internal resistance growth rate.
TABLE 4
It can be seen from table 4 that the electrolyte to which the carboxylate derivatives represented by S1 to S7 were added under low temperature conditions significantly improved the comparative ratio of the 0.2C discharge capacity after 1C charge at 0 ℃ to the 0.2C discharge capacity after 5C charge at 0 ℃. Further, by adding the carboxylate derivatives represented by S1 to S7 and the electrolytes of the aromatic compounds represented by F1 to F8 at the same time, the 0.2C discharge capacity after 0 ℃ 1C charge and the 0.2C discharge capacity after 0 ℃ 5C charge are both further improved. In the embodiment, the highest 0.2C discharge capacity can reach 0.905Ah after 0 ℃ 1C charging, and the highest 0.2C discharge capacity/Ah can reach 0.805Ah after 0 ℃ 5C charging. The examples show that the electrolyte solution containing the carboxylate derivatives represented by S1 to S7 or the electrolyte solution containing both the carboxylate derivatives represented by S1 to S7 and the aromatic compounds represented by F1 to F8 has a high low-temperature charge/discharge capacity and a reduced phenomenon of lithium deposition in the negative electrode.
As can be seen from the above table, the batteries of the examples according to the present invention all performed better than the batteries of the comparative examples. The carboxylate derivative additives shown in S1-S7 or the carboxylate derivative shown in S1-S7 and the aromatic compound combined additive shown in F1-F8 can improve the thermal stability and electrochemical stability of the anode and the cathode of the lithium ion battery, further improve the charge and discharge characteristics of the lithium ion battery, improve the capacity retention rate of the battery at normal temperature and high temperature, inhibit the swelling and internal resistance increase of the battery at high temperature, and reduce the lithium precipitation phenomenon of the cathode of the battery at low temperature, and the prepared battery has excellent comprehensive performance.
The above embodiments are merely illustrative of the technical concept and features of the present invention, and the purpose thereof is to enable those skilled in the art to understand the content of the present invention and implement the invention, and not to limit the scope of the invention, and all equivalent changes or modifications made according to the spirit of the present invention should be covered by the scope of the present invention.
Claims (12)
1. An electrolyte comprising a lithium salt, an organic solvent and an additive, wherein: the additive comprises carboxylic ester derivatives, wherein the carboxylic ester derivatives are one or more compounds shown in a structural formula (I), and the structural formula (I) is
R1 and R2 are independently C 1 -C 6 Alkyl or
Wherein G is 1 Is a bond, C 1 -C 5 Alkylene or substituent containing hetero atoms, G 2 Is C 1 -C 5 Alkyl or a substituent group containing a hetero atom, and, G 1 、G 2 At least one of which is a substituent group containing a hetero atom, and at least one of R1 and R2 is
2. The electrolyte of claim 1, wherein: the structural formula of the substituent group containing the heteroatom is-R 5 OR 6 ，-OR 6 ，-R 5 SR 6 ，-SR 6 ，-S i R 6 R 7 R 8 or-R 5 S i R 6 R 7 R 8 Wherein R is 5 Is C 1 -C 5 Alkylene radical, R 6 、R 7 、R 8 Independently is C 1 -C 5 An alkyl group.
3. The electrolyte of claim 2, wherein: the carboxylic ester derivative is selected from one or more of the substances shown in the following structural formula:
4. the electrolyte as claimed in any one of claims 1 to 3, wherein: the additive also comprises aromatic compounds, wherein the aromatic compounds are one or more of compounds shown in a structural formula (II), and the structural formula (II) is
R3 and R4 are independently C 1 -C 6 Alkyl, unsubstituted or substituted phenyl, the substituents being halo, alkyl, haloalkyl, alkenyl, haloalkenyl, alkynyl, haloalkynyl, phenyl, halophenyl, carbonyl, nitro, amino, cyano, thio, at least one of R3 and R4 being unsubstituted or substituted phenyl.
5. The electrolyte of claim 4, wherein: the aromatic compound is selected from one or more of the following substances shown in the structural formula:
6. the electrolyte of claim 1, wherein: the carboxylic ester derivative accounts for 0.01-5.0% of the total mass of the electrolyte.
7. The electrolyte of claim 4, wherein: the combination of the carboxylic ester derivative and the aromatic compound accounts for 0.01-5.0% of the total mass of the electrolyte.
8. The electrolyte of claim 7, wherein: the mass ratio of the carboxylate derivative to the aromatic compound is 0.5 to 8.
9. The electrolyte of claim 1, wherein: the organic solvent is one or more of carbonate, carboxylate, ether and sulfone; the organic solvent accounts for 50-85% of the total amount of the electrolyte.
10. The electrolyte of claim 1, wherein: the lithium salt is LiPF 6 、LiBF 4 、LiAsF 6 、LiClO 4 、LiCF 3 SO 3 、LiC 4 F 9 SO 3 、Li(CF 3 SO 2 ) 2 N、Li(SO 2 F) 2 N、Li(CF 3 SO 2 ) 3 C、Li(C 6 F 5 ) 4 B、Li(C 2 F 5 SO 2 ) 2 N、LiBF 3 C 2 F 5 、LiPF 3 (C2F 5 ) 3 One or more of (a); the lithium salt accounts for 8-25% of the total mass of the electrolyte.
11. The electrolyte of claim 1, wherein: the electrolyte also comprises other additives, wherein the other additives are one or more of cyclic carbonate containing double bonds, sulfonate, sultone, sulfate, sulfite, a benzene-containing compound, a halogenated compound, a nitrile compound, a boron-containing compound, a cyclic ether compound, a phosphazene compound, phosphate, phosphite, an amine compound, an isocyanate compound, a silicon-containing compound, a lithium salt type compound and a fluoroether compound; the other additives account for 0.5-15% of the total mass of the electrolyte.
12. The utility model provides a lithium ion battery, includes electric core and electrolyte, its characterized in that: the electrolyte solution according to any one of claims 1 to 11.
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