CN105261790A - Electrolyte and lithium-ion battery including same - Google Patents
Electrolyte and lithium-ion battery including same Download PDFInfo
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- CN105261790A CN105261790A CN201510735600.7A CN201510735600A CN105261790A CN 105261790 A CN105261790 A CN 105261790A CN 201510735600 A CN201510735600 A CN 201510735600A CN 105261790 A CN105261790 A CN 105261790A
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- electrolyte
- lithium
- additive
- ion battery
- lithium ion
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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
-
- 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
-
- 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
-
- 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 invention relates to an electrolyte and a lithium-ion battery including the same. The electrolyte comprises an organic solvent, a lithium salt and an additive, wherein the additive comprises an additive A and fluoroethylene carbonate; and the additive A is triethylene cyanuric acid ester and/or triallyl cyanuric acid ester. The electrolyte provided by the invention is capable of lastingly and efficiently repairing an SEI film, which is located on a silicon-based anode in a circulating process, and of which the surface is continuously broken, and effectively inhibiting a side reaction between the silicon-based anode and the electrolyte, so that the cycle performance of the lithium-ion battery, particularly a silicon-based anode lithium-ion battery is improved.
Description
Technical field
The application relates to field of lithium ion battery, especially, relates to a kind of electrolyte and the lithium ion battery comprising this electrolyte and preparation method thereof.
Background technology
Lithium ion battery has the excellent feature such as high-energy-density, long circulation life, wide operating temperature range and environmental protection, has become the main energy sources of current mobile electronic device.Such as, but mobile electronic device in recent years, smart mobile phone, especially gentlier, the develop rapidly of thinner mobile phone, also propose higher demand to the energy density of lithium ion battery.
In order to improve the energy density of lithium ion battery, two kinds of conventional at present methods are the operating voltage of raising positive electrode respectively and use the negative material with more high discharge capacity.Wherein, silicon based anode material makes it become an important development direction of improving lithium ion battery energy density because it has far above the theoretical specific capacity of graphite cathode material.But compared with graphite cathode, huge bulk effect is there is in silicon-based anode in cyclic process, the solid electrolyte interface on silicon-based anode surface (being called for short SEI) film is broken in circulating battery process, cause electrolyte generation reduction decomposition, generate a large amount of accessory substances, thus worsen cycle performance.Simultaneously, due to the anti-life of side reaction, in lithium ion battery charge and discharge process, a large amount of reducibility gas can be produced, destroy the physical contact of inside battery, sharply worsen cycle performance, and to a certain degree may make battery explosion when the reducibility gas of inside battery runs up to, also can bring potential safety hazard.
In view of this, necessaryly provide a kind of electrolyte, be especially applicable to the electrolyte of the lithium ion battery of silicon-based anode, this electrolyte can improve the cycle performance of lithium ion battery.
Summary of the invention
In order to solve the problem, the applicant has carried out studying with keen determination, found that: will the electrolyte of additive A and fluorinated ethylene carbonate be included, wherein additive A is trivinyl fulminuric acid ester and/or iso-cyanuric acid triallyl ester, be applied to after in lithium ion battery, can lithium ion battery be improved, especially improve the cycle performance of silicon-based anode lithium ion battery, thus complete the application.
The object of the application is to provide a kind of electrolyte, comprises organic solvent, lithium salts and additive, and described additive comprises additive A and fluorinated ethylene carbonate, and wherein, additive A is trivinyl fulminuric acid ester and/or iso-cyanuric acid triallyl ester.
Another object of the application is to provide a kind of lithium ion battery, comprises the positive plate containing positive electrode active materials, electrolyte that negative plate, lithium battery diaphragm and the application containing negative active core-shell material provides.
The electrolyte that the application provides can continue efficient repairing and reset in the SEI film of the continuous breakage of negative terminal surface, especially the SEI film efficiently repairing the continuous breakage being positioned at the surface of silicon-based anode in cyclic process is continued, the generation of side reaction between effective suppression negative pole and electrolyte, improve lithium ion battery, especially improve the cycle performance of silicon-based anode lithium ion battery.
Embodiment
Be described in detail below by the application, the feature of the application and advantage will illustrate along with these and become more clear, clear and definite.
The object of the application is to provide a kind of electrolyte, comprises organic solvent, lithium salts and additive, and described additive comprises additive A and fluorinated ethylene carbonate, and wherein, additive A is trivinyl fulminuric acid ester and/or iso-cyanuric acid triallyl ester.
In above-mentioned electrolyte, described trivinyl fulminuric acid ester is as shown in the formula shown in (I).
In above-mentioned electrolyte, described iso-cyanuric acid triallyl ester is as shown in the formula shown in (II).
In above-mentioned electrolyte, described fluorinated ethylene carbonate is as shown in the formula shown in (III).
In above-mentioned electrolyte, preferably, the content of described fluorinated ethylene carbonate is 10% ~ 40% of the total weight of electrolyte, and further preferably, the content of described fluorinated ethylene carbonate is 20 ~ 40% of the total weight of electrolyte.When the content of the fluorinated ethylene carbonate in electrolyte is too low, the active interface of negative pole can be caused, particularly the active interface of silicon-based anode cannot be effectively protected and a large amount of side reactions occurs and cause cycle performance of battery sharply to worsen, therefore effectively can not improve the cycle performance of lithium ion battery, especially effectively can not improve the cycle performance of silicon-based anode lithium ion battery; When the too high levels of the fluorinated ethylene carbonate in electrolyte, especially under the high temperature conditions, make electrolyte and positive electrode generation side reaction, positive electrode active materials is damaged, also can cause the deterioration of the cycle performance of battery.
In above-mentioned electrolyte, preferably, the content of described additive A is 0.05% ~ 3% of the total weight of electrolyte, further preferably, the content of described additive A is 0.1% ~ 2% of the gross weight of electrolyte, wherein, " content of described additive A is 0.05% ~ 3% of the total weight of electrolyte " should be understood to " when additive A is trivinyl fulminuric acid ester, the content of described trivinyl fulminuric acid ester is 0.05% ~ 3% of the total weight of electrolyte, when additive A is iso-cyanuric acid triallyl ester, the content of described iso-cyanuric acid triallyl ester is 0.05% ~ 3% of the total weight of electrolyte, when additive A is the mixture of trivinyl fulminuric acid ester and iso-cyanuric acid triallyl ester, the total content of described trivinyl fulminuric acid ester and described iso-cyanuric acid triallyl ester is 0.05% ~ 3% of the total weight of electrolyte.”
Find after deliberation, if when the content of the described additive A in electrolyte is too low, electrolyte cannot form fine and close SEI film, not obvious to the improvement result of cycle performance; If during the too high levels of the described additive A in electrolyte, then can because of the interface impedance significantly increasing negative terminal surface, especially the interface impedance on silicon-based anode surface, same, also can worsen the cycle performance of battery.
In above-mentioned electrolyte, owing to comprising fluorinated ethylene carbonate and additive A in electrolyte simultaneously, due to the synergy of said two devices, electrolyte on the surface of the negative pole of battery, especially can form the SEI film of dense uniform on the surface of the silicon-based anode of battery, and the pliability of the SEI film formed is good and film forming efficiency is high, simultaneously in battery charge and discharge process, lithium ion can pass SEI film smoothly, and effectively reduce the polarization of battery, the interface impedance of the SEI film formed in addition is less; In addition, the electrolyte comprising said two devices can consume the hydrofluoric acid (HF) of trace in electrolyte, avoid the reaction of HF and silicon-based anode surface SEI film, the generation of effective minimizing side reaction, and this electrolyte can continue efficiently to repair the continuous damaged SEI film in surface of silicon-based anode, thus effectively suppresses the generation of side reaction between silicon-based anode and electrolyte; Can learn thus, the electrolyte of the application can improve the cycle performance of lithium ion battery, especially improves silicon-based anode cycle performance of lithium ion battery.
In this application, described " silicon-based anode " should be understood to include silica-base material in the negative pole of lithium ion battery, the kind of wherein mentioned silica-base material is a lot, and the oxide of such as silicon materials, silicon, Si-C composite material and aluminosilicate alloy material etc. all can be used as silica-base material.
In above-mentioned electrolyte, can comprise ethylene carbonate in described organic solvent, also can not comprise ethylene carbonate, wherein, described ethylene carbonate is as shown in the formula shown in (IV).
When comprising ethylene carbonate, the content of described ethylene carbonate is preferably 0 ~ 10% of the total weight of organic solvent, wherein, in the number range of described 0 ~ 10%, do not comprise 0, what the content of described ethylene carbonate was preferably the total weight of organic solvent is preferably 1.5 ~ 5%.Preferably, ethylene carbonate is not contained in described organic solvent.When not comprising described ethylene carbonate in the organic solvent in electrolyte, the interface impedance of SEI film can be reduced further, improving lithium ion battery, the especially cycle performance of silicon-based anode lithium ion battery.
General containing ethylene carbonate in organic solvent selected by the electrolyte of existing routine, the conductivity of electrolyte can be improved.
In above-mentioned electrolyte, preferably, at least one in propene carbonate, diethyl carbonate, methyl ethyl carbonate is also comprised in described organic solvent.Further preferably, described organic solvent is propene carbonate and/or diethyl carbonate.
In above-mentioned electrolyte, required lithium salts can be selected according to the actual requirements, such as, in organic lithium salt, inorganic lithium salt.
Preferably, at least one in fluorine element, boron element, P elements is contained in described lithium salts.Preferably, described lithium salts is selected from lithium hexafluoro phosphate LiPF
6, LiBF4 LiBF
4, two trifluoromethanesulfonimide lithium LiN (CF
3sO
2)
2(being abbreviated as LiTFSI), di-oxalate lithium borate LiB (C
2o
4)
2(being abbreviated as LiBOB) and difluorine oxalic acid boracic acid lithium LiBF
2(C
2o
4) at least one in (being abbreviated as LiDFOB).Preferably, in described organic electrolyte, the concentration of lithium salts is 0.9mol/L ~ 1.2mol/L.
Another object of the application is to provide a kind of lithium ion battery, comprises the positive plate containing positive electrode active materials, electrolyte that negative plate, lithium battery diaphragm and the application containing negative active core-shell material provides.
In above-mentioned lithium ion battery, preferably, described negative active core-shell material comprises silica-base material, and the oxide of such as silicon, Si-C composite material, aluminosilicate alloy material all can be used as silica-base material, specifically can enumerate nano Si material, SiO material, Si/C composite material, Mg
2si alloy material, Fe
2si alloy material, especially, selects the oxide of silicon as silica-base material, in addition, in described silica-base material, can also comprise material with carbon element, such as graphite etc.When not only having comprised silica-base material but also comprised material with carbon element in negative active core-shell material, in described negative active core-shell material, at least included the silica-base material of 10wt%.
In above-mentioned lithium ion battery, preferably, described positive electrode active materials is selected from least one in lithium and cobalt oxides, lithium nickel oxide, lithium manganese oxide, Li, Ni, Mn oxide, lithium nickel cobalt manganese oxide and lithium nickel cobalt aluminum oxide.
Because above-mentioned lithium ion battery comprises the electrolyte that the application provides, the electrolyte that the application provides can continue efficiently to repair the continuous damaged SEI film in the surface being positioned at silicon-based anode in cyclic process, the generation of side reaction between effective suppression silicon-based anode and electrolyte, improve lithium ion battery, especially improve the cycle performance of silicon-based anode lithium ion battery.
Embodiment
The application is further described below by way of instantiation.But these examples are only exemplary, do not form any restriction to the protection range of the application.
In following embodiment, comparative example and test example, the reagent used, material and instrument, as not having special explanation, are conventional reagent, conventional material and conventional instrument, all commercially available acquisition.
In following embodiment, comparative example and test example, used material is as follows:
Organic solvent: ethylene carbonate (EC), diethyl carbonate (DEC), propene carbonate (PC).
Lithium salts: lithium hexafluoro phosphate (LiPF
6).
Additive: fluorinated ethylene carbonate (FEC);
Additive A: trivinyl fulminuric acid ester (additive A 1), iso-cyanuric acid triallyl ester (additive A 2).
Silica-base material: SiO.
Lithium battery diaphragm: PE porous polymer film.
The preparation of embodiment 1 ~ 13 lithium ion battery 1 ~ 13
Lithium ion battery (abbreviation battery) 1 ~ 13 is prepared all by the following method:
(1) preparation of electrolyte:
Electrolyte 1 ~ 13 is prepared all by the following method:
After being mixed with certain weight ratio by PC and DEC, add EC, lithium salts, additive, additive A, mix, obtain electrolyte, wherein lithium salts concentration is in the electrolytic solution 1.1mol/L.
(2) preparation of anode pole piece:
By cobalt acid lithium, conductive agent SuperP, binding agent polyvinylidene fluoride (PVDF) by weight cobalt acid lithium: after conductive agent conductive black SuperP: binding agent polyvinylidene fluoride=97: 1.4: 1.6 mixing, add 1-METHYLPYRROLIDONE (NMP), be mixed evenly and prepare lithium ion battery anode glue size; Be coated on by anode sizing agent in current collector aluminum foil, cold pressing after drying at 85 DEG C, after then carrying out trimming, cut-parts, itemize, under the vacuum condition of 85 DEG C, dry 4h, soldering polar ear, prepares anode slice of lithium ion battery.
(3) preparation of cathode pole piece:
Be graphite using graphite and SiO according to weight ratio: the mixture of SiO=70: 30 is as negative active core-shell material, with conductive agent conductive black SuperP, thickener sodium carboxymethylcellulose (CMC), bonding agent polyacrylic acid (PAA) by weight being negative active core-shell material: conductive agent conductive black SuperP: thickener sodium carboxymethylcellulose (CMC): after bonding agent polyacrylic acid (PAA)=90: 1.0: 1.0: 8 mixes, adding pure water mixing and preparing cathode size; Cathode size to be coated on copper foil of affluxion body and to dry at 85 DEG C, after then carrying out trimming, cut-parts, itemize, under 120 DEG C of vacuum conditions, drying 12h, soldering polar ear, prepare lithium ion battery negative electrode.
(4) preparation of lithium ion battery (abbreviation battery):
The positive plate prepared above-mentioned, negative plate, lithium battery diaphragm are folded in order, make lithium battery diaphragm be in the middle of positive/negative plate, and winding obtains naked battery core; Naked battery core is placed in external packing, the electrolyte of above-mentioned preparation is injected in dried battery, encapsulate, leave standstill, change into, shaping, volume test, prepare the soft bag lithium ionic cell (abbreviation battery) of thickness 4.2mm, width 32mm, length 82mm, the condition wherein changed into be 0.02C constant current charge to 3.4V, then with 0.1C constant current charge to 3.85V.
In the preparation process of above-mentioned battery, the content of EC, FEC used in electrolyte selected in each battery, each electrolyte and the kind of additive A and content, as shown in Table 1 below.
In Table 1, the content of described additive A is the percetage by weight obtained based on the total weight of electrolyte, the content of institute FEC is the percetage by weight obtained based on the total weight of electrolyte, and the content of described EC is the percetage by weight obtained based on the total weight of organic solvent.
Table 1
Comparative example 1 ~ 4 lithium ion battery (abbreviation battery) 1
#~ 4
#preparation
Battery 1
#~ 4
#be prepared all by the following method:
Repeat the preparation of battery 1 in embodiment 1, wherein change the content of EC, PC, DEC and additive A, all the other conditions are all constant.
In the preparation process of above-mentioned battery, the content of EC, FEC used in electrolyte selected in each battery, each electrolyte and the kind of additive A and content, as shown in Table 2 below.
In table 2, the content of described additive A is the percetage by weight obtained based on the total weight of electrolyte, the content of institute FEC is the percetage by weight obtained based on the total weight of electrolyte, and the content of described EC is the percetage by weight obtained based on the total weight of organic solvent.
Table 2
Test example
the cycle performance test of battery
The battery prepared is carried out following test respectively:
Respectively at 25 DEG C, 45 DEG C, by battery with the constant current charge of 0.7C to 4.45V, then with 4.45V constant voltage charge to electric current for 0.05C, again with 1C constant-current discharge to 3.0V, this is for circulate first, carries out 300 cycle charging/electric discharges respectively according to above-mentioned condition, calculates battery respectively and to circulate at 25 DEG C, 45 DEG C the capability retention after 300 times, wherein, the capability retention after circulation calculates according to the following formula.The relevant test data obtained in each battery is see table 3.
Capability retention after circulation=(discharge capacity after corresponding cycle-index/circulate first discharge capacity) × 100%
Table 3
Can learn from the related data above-mentioned table 3, compare battery 1
#~ 4
#, battery 1 ~ 13 respectively at 25 DEG C, 45 DEG C through 300 times circulation after, battery 1 ~ 13 all has higher capability retention.
Can learn that electrolyte the application provided is applied to after in lithium ion battery thus, the cycle performance of lithium ion battery can be improved, especially, lithium ion battery can be improved, especially the cycle performance of silicon-based anode lithium battery under the high voltage of more than 4.45V.
The announcement of book according to the above description, the application those skilled in the art can also carry out suitable change and amendment to above-mentioned execution mode.Therefore, the application is not limited to embodiment disclosed and described above, also should fall in the protection range of claim of the application some modifications and changes of the application.
Claims (10)
1. an electrolyte, is characterized in that, comprises organic solvent, lithium salts and additive, and described additive comprises additive A and fluorinated ethylene carbonate, and wherein, additive A is trivinyl fulminuric acid ester and/or iso-cyanuric acid triallyl ester.
2. electrolyte according to claim 1, is characterized in that, the content of described fluorinated ethylene carbonate is 10% ~ 40% of the total weight of electrolyte.
3. electrolyte according to claim 1, is characterized in that, the content of described additive A is 0.05% ~ 3% of the total weight of electrolyte.
4. electrolyte according to claim 1, is characterized in that, also comprises ethylene carbonate in described organic solvent, and the content of described ethylene carbonate is 0 ~ 10% of the total weight of organic solvent, wherein, in the number range of 0 ~ 10%, does not comprise 0.
5. electrolyte according to claim 1, is characterized in that, does not comprise ethylene carbonate in described organic solvent.
6. electrolyte according to claim 1, is characterized in that, described organic solvent also comprise in propene carbonate, diethyl carbonate and methyl ethyl carbonate one or more.
7. electrolyte according to claim 1, is characterized in that, described lithium salts be selected from lithium hexafluoro phosphate, LiBF4, two trifluoromethanesulfonimide lithium, di-oxalate lithium borate and difluorine oxalic acid boracic acid lithium one or more.
8. a lithium ion battery, is characterized in that, comprises the positive plate containing positive electrode active materials, the electrolyte according to any one of negative plate, lithium battery diaphragm and claim 1 ~ 7 containing negative active core-shell material.
9. lithium ion battery according to claim 8, is characterized in that, described negative active core-shell material comprises silica-base material, described silica-base material be selected from silicon materials, the oxide of silicon, Si-C composite material and aluminosilicate alloy material one or more.
10. lithium ion battery according to claim 9, is characterized in that, described silica-base material is for being selected from nano Si material, SiO material, Si/C composite material, Mg
2si alloy material, Fe
2one or more in Si alloy material.
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|---|---|---|---|
| CN201510735600.7A CN105261790A (en) | 2015-11-03 | 2015-11-03 | Electrolyte and lithium-ion battery including same |
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| CN109155426A (en) * | 2016-05-26 | 2019-01-04 | 日本电气株式会社 | Lithium ion secondary battery |
| WO2019018435A1 (en) | 2017-07-17 | 2019-01-24 | NOHMs Technologies, Inc. | Modified triazine functional compounds |
| CN109937508A (en) * | 2016-12-22 | 2019-06-25 | 松下知识产权经营株式会社 | Non-aqueous electrolyte secondary battery |
| CN110190331A (en) * | 2019-06-18 | 2019-08-30 | 郑州中科新兴产业技术研究院 | A kind of electrolyte, preparation and its application on firm lithium ion battery silicon-carbon surface |
| CN110957532A (en) * | 2019-12-25 | 2020-04-03 | 惠州市豪鹏科技有限公司 | Electrolyte for lithium ion battery and lithium ion battery comprising same |
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| CN112331914A (en) * | 2019-08-05 | 2021-02-05 | 杉杉新材料（衢州）有限公司 | Non-aqueous electrolyte of lithium ion battery without ethylene carbonate solvent and battery |
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Application publication date: 20160120 |