CN109888394A - A kind of novel serondary lithium battery electrolyte - Google Patents
A kind of novel serondary lithium battery electrolyte Download PDFInfo
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- CN109888394A CN109888394A CN201910254459.7A CN201910254459A CN109888394A CN 109888394 A CN109888394 A CN 109888394A CN 201910254459 A CN201910254459 A CN 201910254459A CN 109888394 A CN109888394 A CN 109888394A
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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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- Y02E60/10—Energy storage using batteries
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Abstract
The invention belongs to electrochemical energy source fields, are related to a kind of novel serondary lithium battery electrolyte.Lithium battery electrolytes of the invention, which is characterized in that electrolyte is the liquid electrolyte containing organic solvent, lithium salts or additive.The organic solvent is carbonate-based solvent；Lithium salts is at least one of bis- (fluorine sulphonyl) imine lithiums, bis- (fluoroform sulphonyl) imine lithiums, dioxalic acid lithium borate, difluorine oxalic acid boracic acid lithium；Additive be lithium hexafluoro phosphate, LiBF4, lithium perchlorate, vinylene carbonate, ethyl sulfate, fluorinated ethylene carbonate be at least one of.Electrolyte of the invention is applied to serondary lithium battery, can significantly improve the cycle performance of battery, have a good application prospect.
Description
Technical field
The invention belongs to electrochemical energy source fields, are related to a kind of novel serondary lithium battery electrolyte.
Background technique
The storage that battery generates electricity in consumption electronic product, electric car, the intermittent renewable energy (such as wind energy or solar energy)
It deposits most important.However, be currently available that commercial batteries (such as plumbic acid, nickel-metal hydride battery) be not able to satisfy portable electronic device,
The stringent or growing demand of electric car and power grid energy-storage system.Exploitation energy density is higher, cycle life is longer, peace
The battery that complete horizontal acceptable, cost can be born is very important.
With the commercialized lithium ion battery of Sony's invention first item in 1991, lithium ion battery was just set in portable electronic
It is widely used in standby.In recent years, lithium ion battery also has extensive use in electric car and extensive energy storage.But mesh
Lithium salts in the electrolyte of preceding commercialized lithium ion battery is mainly 1mol/L or 1.2mol/L lithium hexafluoro phosphate (LiPF6),
Solvent is the mixed solvent of ethylene carbonate (EC) and diethyl carbonate (DEC), or is ethylene carbonate (EC) and carbonic acid first
The mixed solvent of vinyl acetate (EMC).A large amount of lithium hexafluoro phosphate (LiPF6) noxious materials such as HF can be generated when encounter water,
The cycle performance of battery can be not only reduced, but also great harm can be will cause to human body.
Compared with lithium hexafluoro phosphate (LiPF6), bis- (fluorine sulphonyl) imine lithiums (LiFSI), bis- (fluoroform sulphonyl) imine lithiums
(LiTFSI), the lithium salts such as dioxalic acid lithium borate (LiBOB) and difluorine oxalic acid boracic acid lithium (LiDFOB) are stronger to the tolerance of water, no
Significant impact can be caused to the cycle performance of battery.Dioxalic acid lithium borate (LiBOB), bis- (fluoroform sulphonyl) imines simultaneously
Decomposition product of the lithium (LiTFSI) during circulating battery stable solid electrolyte interface easy to form is conducive to improve electricity
The cycle performance in pond.
Summary of the invention
The technical problem to be solved in the present invention is to provide a kind of electrolyte for serondary lithium battery, can effectively improve
The cyclical stability of serondary lithium battery.
The present invention relates to a kind of serondary lithium battery electrolyte, which is characterized in that electrolyte be containing organic solvent, lithium salts or
The liquid electrolyte of additive is used for rechargeable lithium battery.
The organic solvent is carbonate-based solvent, can be ethylene carbonate (EC), dimethyl carbonate (DMC), carbonic acid
Diethylester (DEC), propene carbonate (PC), methyl ethyl carbonate enester (EMC), methyl propyl carbonate (MPC), carbonic acid first isopropyl ester
(MiPC) at least two in.
Lithium salts in the electrolyte is bis- (fluorine sulphonyl) imine lithiums (LiFSI), bis- (fluoroform sulphonyl) imine lithiums
(LiTFSI), at least one of dioxalic acid lithium borate (LiBOB), difluorine oxalic acid boracic acid lithium (LiDFOB).
The additive is lithium hexafluoro phosphate (LiPF6), LiBF4 (LiBF4), lithium perchlorate (LiClO4), carbonic acid
At least one of vinylene (VC), ethyl sulfate (DTD), fluorinated ethylene carbonate (FEC).
The concentration range of the lithium salts in organic solvent is 0.1~10mol/L, preferably 1~4mol/L.
The content of the additive is no more than the 10% of electrolyte quality.
The aqueous electrolyte is for that can effectively improve the cyclical stability of serondary lithium battery in serondary lithium battery.
Detailed description of the invention
Fig. 1 is the constant current charge-discharge curve graph of the embodiment of the present invention 1.
Fig. 2 is the cycle performance figure of the embodiment of the present invention 1.
Fig. 3 is the constant current charge-discharge curve graph of the embodiment of the present invention 2.
Fig. 4 is the cycle performance figure of the embodiment of the present invention 2.
Fig. 5 is the constant current charge-discharge curve graph of the embodiment of the present invention 3.
Fig. 6 is the cycle performance figure of the embodiment of the present invention 3.
Fig. 7 is the constant current charge-discharge curve graph of the embodiment of the present invention 4.
Fig. 8 is the cycle performance figure of the embodiment of the present invention 4.
Fig. 9 is the constant current charge-discharge curve graph of the embodiment of the present invention 5.
Figure 10 is the cycle performance figure of the embodiment of the present invention 5.
Figure 11 is the constant current charge-discharge curve graph of comparative example 1 of the present invention.
Figure 12 is the cycle performance figure of comparative example 1 of the present invention.
Figure 13 is the constant current charge-discharge curve graph of comparative example 2 of the present invention.
Figure 14 is the cycle performance figure of comparative example 2 of the present invention.
Specific embodiment
The present invention will be further described in detail below with reference to the accompanying drawings and specific embodiments, but protection of the invention
Range is not limited thereto.
Embodiment 1
The dioxalic acid lithium borate (LiBOB) of bis- (fluoroform sulphonyl) imine lithiums (LiTFSI) of 0.6mol/L, 0.4mol/L
It is dissolved in ethylene carbonate (EC) and propene carbonate (PC) with the lithium hexafluoro phosphate (LiPF6) of 0.05mol/L, wherein carbonic acid second
Enester (EC) and the volume ratio of propene carbonate (PC) are 7:3.
It is according to mass ratio by positive electrode active materials LiMn2O4 and conductive carbon black, binder Kynoar (PVDF) respectively
80:10:10 is uniformly mixed, and is sized mixing with N-Methyl pyrrolidone (NMP), is then coated on aluminium foil, anode is made in 110 DEG C of dryings
Material.It uses polypropylene (PP) as diaphragm, above-mentioned electrolyte is added, assembled battery, carries out constant current charge-discharge and cycle performance is surveyed
Examination.
Fig. 1 is the constant current charge-discharge curve graph in the current density condition of 0.15A/g, and first circle specific discharge capacity is
132.5mAh/g, its specific capacity remains to reach 99mAh/g after circulation 400 is enclosed.
Fig. 2 is the cycle performance figure in 0.15A/g, and after recycling 400 times, capacity remains to reach 99mAh/g, and capacity is protected
Holdup is 74.7%, and average coulombic efficiency is 99.6%, embodies good cyclical stability.
Embodiment 2
The dioxalic acid lithium borate (LiBOB) of 0.6mol/L bis- (fluoroform sulphonyl) imine lithiums (LiTFSI) and 0.4mol/L
It is dissolved in ethylene carbonate (EC) and diethyl carbonate (DEC), wherein the body of ethylene carbonate (EC) and diethyl carbonate (DEC)
Product is than being 5:5.Additive is the lithium hexafluoro phosphate (LiPF of 0.05mol/L6)。
Respectively by positive electrode active materials ternary lithium (NMC111) and conductive carbon black, binder Kynoar (PVDF) according to
Mass ratio is uniformly mixed for 80:10:10, is sized mixing with N-Methyl pyrrolidone (NMP), is then coated on aluminium foil, 110 DEG C of dryings,
Positive electrode is made.It uses polyethylene (PE) as diaphragm, above-mentioned electrolyte is added, assembled battery carries out constant current charge-discharge and follows
Ring performance test.
Fig. 3 is the constant current charge-discharge curve graph in the current density condition of 0.15A/g, and first circle specific discharge capacity is
146.3mAh/g, its specific capacity remains to reach 134.7mAh/g after circulation 100 is enclosed.
Fig. 4 is the cycle performance figure in 0.15A/g, and after recycling 200 times, capacity remains to reach 134.7mAh/g, is held
Measuring conservation rate is 92.1%, and average coulombic efficiency is 99.3%, embodies good cyclical stability.
Embodiment 3
The dioxalic acid lithium borate (LiBOB) of bis- (fluorine sulphonyl) imine lithiums (LiFSI) of 1mol/L and 1mol/L are dissolved in carbonic acid second
In enester (EC) and propene carbonate (PC), wherein the volume ratio of ethylene carbonate (EC) and propene carbonate (PC) is 7:3.Add
Adding agent is the lithium hexafluoro phosphate (LiPF of 0.1mol/L6)。
Respectively by positive electrode active materials ternary lithium (NMC111) and conductive carbon black, binder Kynoar (PVDF) according to
Mass ratio is uniformly mixed for 80:10:10, is sized mixing with N-Methyl pyrrolidone (NMP), is then coated on aluminium foil, 110 DEG C of dryings,
Positive electrode is made.It uses polypropylene (PP) as diaphragm, above-mentioned electrolyte is added, assembled battery carries out constant current charge-discharge and follows
Ring performance test.
Fig. 5 is the constant current charge-discharge curve graph in the current density condition of 0.15A/g, and first circle specific discharge capacity is
139.5mAh/g, its specific capacity remains to reach 105.9mAh/g after circulation 200 is enclosed.
Fig. 6 is the cycle performance figure in 0.15A/g, and after recycling 200 times, capacity remains to reach 105.9mAh/g, is held
Measuring conservation rate is 75.9%, and average coulombic efficiency is 99.6%, embodies preferable cyclical stability.
Embodiment 4
Bis- (fluoroform sulphonyl) imine lithiums (LiTFSI) of 1mol/L, the difluorine oxalic acid boracic acid lithium (LiDFOB) of 1mol/L are molten
In ethylene carbonate (EC) and diethyl carbonate (DEC), the wherein volume of ethylene carbonate (EC) and diethyl carbonate (DEC)
Than for 7:3.The fluorinated ethylene carbonate (FEC) of 2% mass fraction is added simultaneously.
Respectively by positive electrode active materials ternary lithium (NMC111) and conductive carbon black, binder Kynoar (PVDF) according to
Mass ratio is uniformly mixed for 80:10:10, is sized mixing with N-Methyl pyrrolidone (NMP), is then coated on aluminium foil,
Positive electrode is made in 110 DEG C of dryings.It uses polyethylene (PE) as diaphragm, above-mentioned electrolyte is added, assembled battery carries out
Constant current charge-discharge and cycle performance test.
Fig. 7 is the constant current charge-discharge curve graph in the current density condition of 0.15A/g, and first circle specific discharge capacity is
132.7mAh/g, its specific capacity remains to reach 106mAh/g after circulation 100 is enclosed.
Fig. 8 is the cycle performance figure in 0.15A/g, and after recycling 100 times, capacity remains to reach 106mAh/g,
Capacity retention ratio is 79.9%, and average coulombic efficiency is 99.9%, embodies preferable cyclical stability.
Embodiment 5
The dioxalic acid lithium borate (LiBOB) of 0.6mol/L bis- (fluoroform sulphonyl) imine lithiums (LiTFSI) and 0.4mol/L
It is dissolved in ethylene carbonate (EC), methyl ethyl carbonate enester (EMC) and diethyl carbonate (DEC), wherein ethylene carbonate (EC), carbon
The volume ratio of sour first and second enesters (EMC) and diethyl carbonate (DEC) is 4:2:2.Additive is the lithium hexafluoro phosphate of 0.05mol/L
(LiPF6)。
Respectively by positive electrode active materials ternary lithium (NMC111) and conductive carbon black, binder Kynoar (PVDF) according to
Mass ratio is uniformly mixed for 80:10:10, is sized mixing with N-Methyl pyrrolidone (NMP), is then coated on aluminium foil, 110 DEG C of dryings,
Positive electrode is made.It uses polyethylene (PE) as diaphragm, above-mentioned electrolyte is added, assembled battery carries out constant current charge-discharge and follows
Ring performance test
Fig. 9 is the constant current charge-discharge curve graph in the current density condition of 0.15A/g, and first circle specific discharge capacity is
146.3mAh/g, its specific capacity remains to reach 134.7mAh/g after circulation 100 is enclosed.
Figure 10 is the cycle performance figure in 0.15A/g, and after recycling 200 times, capacity remains to reach 134.7mAh/g, is held
Measuring conservation rate is 92.1%, and average coulombic efficiency is 99.3%, embodies good cyclical stability.
Comparative example 1
The dioxalic acid lithium borate (LiBOB) of 0.6mol/L bis- (fluoroform sulphonyl) imine lithiums (LiTFSI) and 0.4mol/L
It is dissolved in ethylene carbonate (EC) and propene carbonate (PC), wherein the volume of ethylene carbonate (EC) and propene carbonate (PC)
Than for 7:3.
It is according to mass ratio by positive electrode active materials LiMn2O4 and conductive carbon black, binder Kynoar (PVDF) respectively
80:10:10 is uniformly mixed, and is sized mixing with N-Methyl pyrrolidone (NMP), is then coated on aluminium foil, anode is made in 110 DEG C of dryings
Material.It uses polypropylene (PP) as diaphragm, above-mentioned electrolyte is added, assembled battery, carries out constant current charge-discharge and cycle performance is surveyed
Examination.
Figure 11 is the constant current charge-discharge curve graph under the current density of 0.15A/g, and first circle specific discharge capacity is
133.9mAh/g, 100 circle after its capacity there was only 50.2mAh/g.
Figure 12 is the cycle performance figure in 0.15A/g, and after recycling 100 times, capacity retention ratio only has 37.5%, circulation
Performance is poor.
Comparative example 2
The dioxalic acid lithium borate (LiBOB) of 0.6mol/L bis- (fluoroform sulphonyl) imine lithiums (LiTFSI) and 0.4mol/L
It is dissolved in ethylene carbonate (EC) and diethyl carbonate (DEC), wherein the body of ethylene carbonate (EC) and diethyl carbonate (DEC)
Product is than being 7:3.
Respectively by positive electrode active materials ternary lithium (NMC111) and conductive carbon black, binder Kynoar (PVDF) according to
Mass ratio is uniformly mixed for 80:10:10, is sized mixing with N-Methyl pyrrolidone (NMP), is then coated on aluminium foil,
Positive electrode is made in 110 DEG C of dryings.It uses polyethylene (PE) as diaphragm, above-mentioned electrolyte is added, assembled battery carries out
Constant current charge-discharge and cycle performance test.
Figure 13 is the constant current charge-discharge curve graph in the current density condition of 0.15A/g, and first circle specific discharge capacity is
130.9mAh/g, its specific capacity only has 76mAh/g after circulation 100 is enclosed.
Figure 14 is the cycle performance figure in 0.15A/g, and after recycling 100 times, capacity retention ratio 58.1%, circulation is surely
It is qualitative poor.
Embodiment of above is only for interpreting the claims, and protection scope of the present invention is not limited to specification.
Anyone skilled in the art within the technical scope of the present disclosure, the variation that can readily occur in or replaces
It changes, is included within the scope of the present invention.
Claims (7)
1. a kind of novel serondary lithium battery electrolyte, which is characterized in that electrolyte is to contain organic solvent, lithium salts or additive
Liquid electrolyte, be used for rechargeable lithium battery.
2. serondary lithium battery electrolyte according to claim 1, which is characterized in that the organic solvent is that carbonates are molten
Agent can be ethylene carbonate (EC), dimethyl carbonate (DMC), diethyl carbonate (DEC), propene carbonate (PC), carbonic acid first
Vinyl acetate (EMC), methyl propyl carbonate (MPC), carbonic acid first isopropyl ester (MiPC) at least two.
3. serondary lithium battery electrolyte according to claim 1, which is characterized in that the lithium salts in the electrolyte is double
(fluorine sulphonyl) imine lithium (LiFSI), bis- (fluoroform sulphonyl) imine lithiums (LiTFSI), dioxalic acid lithium borate (LiBOB), difluoro
At least one of Lithium bis (oxalate) borate (LiDFOB).
4. serondary lithium battery electrolyte according to claim 1, which is characterized in that additive is hexafluoro in the electrolyte
Lithium phosphate (LiPF6), LiBF4 (LiBF4), lithium perchlorate (LiClO4), vinylene carbonate (VC), ethyl sulfate
(DTD), at least one of fluorinated ethylene carbonate (FEC).
5. serondary lithium battery electrolyte according to any one of claims 1 to 4, it is characterised in that: the lithium salts is having
Concentration range in solvent is 0.1~10mol/L, preferably 1~4mol/L.
6. serondary lithium battery electrolyte according to claim 1 or 4, which is characterized in that the content of the additive does not surpass
Cross the 10% of electrolyte quality.
7. serondary lithium battery electrolyte according to any one of claims 1 to 6, which is characterized in that the electrolyte is used for
The cyclical stability of serondary lithium battery can be effectively improved in serondary lithium battery.
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Cited By (5)
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| CN112349962A (en) * | 2019-08-08 | 2021-02-09 | 宁德时代新能源科技股份有限公司 | Lithium ion battery |
| CN112670584A (en) * | 2020-12-24 | 2021-04-16 | 湖南艾华集团股份有限公司 | Electrolyte with good safety performance, lithium ion battery and preparation method |
| CN114421008A (en) * | 2020-10-28 | 2022-04-29 | 陕西泽邦环境科技有限公司 | Wettability-enhanced lithium ion battery electrolyte and application thereof |
| CN114421010A (en) * | 2020-10-28 | 2022-04-29 | 陕西泽邦环境科技有限公司 | Lithium-supplement type lithium ion battery electrolyte and application thereof |
| WO2022133926A1 (en) * | 2020-12-24 | 2022-06-30 | 宁德时代新能源科技股份有限公司 | Lithium-ion secondary battery and preparation method therefor, battery module, battery pack, and device |
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