CN109659614A - A kind of lithium-ion battery electrolytes and the lithium ion battery with high energy density using the electrolyte - Google Patents
A kind of lithium-ion battery electrolytes and the lithium ion battery with high energy density using the electrolyte Download PDFInfo
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- CN109659614A CN109659614A CN201811557427.6A CN201811557427A CN109659614A CN 109659614 A CN109659614 A CN 109659614A CN 201811557427 A CN201811557427 A CN 201811557427A CN 109659614 A CN109659614 A CN 109659614A
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- China
- Prior art keywords
- lithium
- additive
- ion battery
- acid
- anhydride
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- 239000003792 electrolyte Substances 0.000 title claims abstract description 46
- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 46
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 45
- 239000000654 additive Substances 0.000 claims abstract description 49
- 230000000996 additive effect Effects 0.000 claims abstract description 47
- -1 ether nitrile compounds Chemical class 0.000 claims abstract description 47
- 229910003002 lithium salt Inorganic materials 0.000 claims abstract description 19
- 159000000002 lithium salts Chemical class 0.000 claims abstract description 19
- 150000002148 esters Chemical class 0.000 claims abstract description 17
- 230000015572 biosynthetic process Effects 0.000 claims abstract description 12
- RTZKZFJDLAIYFH-UHFFFAOYSA-N ether Substances CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 claims abstract description 12
- 150000002825 nitriles Chemical class 0.000 claims abstract description 8
- VAYTZRYEBVHVLE-UHFFFAOYSA-N 1,3-dioxol-2-one Chemical compound O=C1OC=CO1 VAYTZRYEBVHVLE-UHFFFAOYSA-N 0.000 claims abstract description 7
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 claims abstract description 6
- 239000003960 organic solvent Substances 0.000 claims abstract description 6
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 4
- 125000001153 fluoro group Chemical group F* 0.000 claims abstract description 4
- 239000000956 alloy Substances 0.000 claims abstract description 3
- 229910052799 carbon Inorganic materials 0.000 claims abstract description 3
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims description 12
- 229910052744 lithium Inorganic materials 0.000 claims description 12
- BTGRAWJCKBQKAO-UHFFFAOYSA-N adiponitrile Chemical compound N#CCCCCC#N BTGRAWJCKBQKAO-UHFFFAOYSA-N 0.000 claims description 9
- DGTVXEHQMSJRPE-UHFFFAOYSA-M difluorophosphinate Chemical group [O-]P(F)(F)=O DGTVXEHQMSJRPE-UHFFFAOYSA-M 0.000 claims description 8
- 239000008151 electrolyte solution Substances 0.000 claims description 8
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- 150000008064 anhydrides Chemical class 0.000 claims description 6
- 150000007942 carboxylates Chemical group 0.000 claims description 6
- 150000001875 compounds Chemical class 0.000 claims description 6
- 229910052731 fluorine Inorganic materials 0.000 claims description 6
- QRMHDYCPNIVCBO-UHFFFAOYSA-N [SH2]=N.[F] Chemical compound [SH2]=N.[F] QRMHDYCPNIVCBO-UHFFFAOYSA-N 0.000 claims description 5
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- 239000011737 fluorine Substances 0.000 claims description 4
- MLFHJEHSLIIPHL-UHFFFAOYSA-N isoamyl acetate Chemical compound CC(C)CCOC(C)=O MLFHJEHSLIIPHL-UHFFFAOYSA-N 0.000 claims description 4
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- NDZWKTKXYOWZML-UHFFFAOYSA-N trilithium;difluoro oxalate;borate Chemical compound [Li+].[Li+].[Li+].[O-]B([O-])[O-].FOC(=O)C(=O)OF NDZWKTKXYOWZML-UHFFFAOYSA-N 0.000 claims description 4
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- BJWMSGRKJIOCNR-UHFFFAOYSA-N 4-ethenyl-1,3-dioxolan-2-one Chemical compound C=CC1COC(=O)O1 BJWMSGRKJIOCNR-UHFFFAOYSA-N 0.000 claims description 3
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 claims description 3
- 229910019142 PO4 Inorganic materials 0.000 claims description 3
- 229910052782 aluminium Inorganic materials 0.000 claims description 3
- SIXOAUAWLZKQKX-UHFFFAOYSA-N carbonic acid;prop-1-ene Chemical compound CC=C.OC(O)=O SIXOAUAWLZKQKX-UHFFFAOYSA-N 0.000 claims description 3
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 claims description 3
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 claims description 3
- PQIOSYKVBBWRRI-UHFFFAOYSA-N methylphosphonyl difluoride Chemical group CP(F)(F)=O PQIOSYKVBBWRRI-UHFFFAOYSA-N 0.000 claims description 3
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- 239000007774 positive electrode material Substances 0.000 claims description 3
- TWQULNDIKKJZPH-UHFFFAOYSA-K trilithium;phosphate Chemical compound [Li+].[Li+].[Li+].[O-]P([O-])([O-])=O TWQULNDIKKJZPH-UHFFFAOYSA-K 0.000 claims description 3
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- JPSKCQCQZUGWNM-UHFFFAOYSA-N 2,7-Oxepanedione Chemical compound O=C1CCCCC(=O)O1 JPSKCQCQZUGWNM-UHFFFAOYSA-N 0.000 claims description 2
- UHOPWFKONJYLCF-UHFFFAOYSA-N 2-(2-sulfanylethyl)isoindole-1,3-dione Chemical compound C1=CC=C2C(=O)N(CCS)C(=O)C2=C1 UHOPWFKONJYLCF-UHFFFAOYSA-N 0.000 claims description 2
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- 239000002131 composite material Substances 0.000 description 1
- 239000002482 conductive additive Substances 0.000 description 1
- 238000005520 cutting process Methods 0.000 description 1
- 238000000354 decomposition reaction Methods 0.000 description 1
- 238000009831 deintercalation Methods 0.000 description 1
- 239000008367 deionised water Substances 0.000 description 1
- 229910021641 deionized water Inorganic materials 0.000 description 1
- 230000006866 deterioration Effects 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 239000012530 fluid Substances 0.000 description 1
- 239000000446 fuel Substances 0.000 description 1
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 1
- 229910052737 gold Inorganic materials 0.000 description 1
- 239000010931 gold Substances 0.000 description 1
- 239000010439 graphite Substances 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 238000002347 injection Methods 0.000 description 1
- 239000007924 injection Substances 0.000 description 1
- 230000003993 interaction Effects 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 150000002596 lactones Chemical class 0.000 description 1
- 230000007774 longterm Effects 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- 150000004702 methyl esters Chemical class 0.000 description 1
- 239000003921 oil Substances 0.000 description 1
- 238000005457 optimization Methods 0.000 description 1
- 238000000643 oven drying Methods 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 238000012856 packing Methods 0.000 description 1
- 229920001155 polypropylene Polymers 0.000 description 1
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 1
- 238000003825 pressing Methods 0.000 description 1
- 239000001294 propane Substances 0.000 description 1
- 239000011814 protection agent Substances 0.000 description 1
- 239000003223 protective agent Substances 0.000 description 1
- 238000012797 qualification Methods 0.000 description 1
- 238000011084 recovery Methods 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 238000007493 shaping process Methods 0.000 description 1
- 235000019812 sodium carboxymethyl cellulose Nutrition 0.000 description 1
- 229920001027 sodium carboxymethylcellulose Polymers 0.000 description 1
- 230000000087 stabilizing effect Effects 0.000 description 1
- 238000003756 stirring Methods 0.000 description 1
- 230000002195 synergetic effect Effects 0.000 description 1
- 239000002562 thickening agent Substances 0.000 description 1
- 230000007704 transition Effects 0.000 description 1
- 229910052723 transition metal Inorganic materials 0.000 description 1
- 150000003624 transition metals Chemical class 0.000 description 1
- 238000004804 winding Methods 0.000 description 1
Classifications
-
- 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
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
- H01M10/4235—Safety or regulating additives or arrangements in electrodes, separators or electrolyte
-
- 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
Landscapes
- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Physics & Mathematics (AREA)
- Condensed Matter Physics & Semiconductors (AREA)
- General Physics & Mathematics (AREA)
- Inorganic Chemistry (AREA)
- Materials Engineering (AREA)
- Secondary Cells (AREA)
Abstract
A kind of lithium-ion battery electrolytes and the lithium ion battery with high energy density using the electrolyte.The lithium-ion electrolyte includes non-aqueous including organic solvent, lithium salts and additive.The additive includes cathode film formation additive, nitrile or ether nitrile compounds and anhydride compound and lithium salts type additive.The cathode film formations additive such as the vinylene carbonate of 0.3-20wt% and/or fluoro carbonic ester in the present invention can form excellent SEI film containing Carbon anode or the alloy anodes containing silicium cathode or silicon-carbon etc., stablize cathode, guarantee excellent battery performance；The nitrile of 0.2-6.5wt% or ether nitrile compound and anhydride compound and combinations thereof in the present invention can be complexed the metal ion of anode or form protective film in positive electrode surface, to stablize anode, improve battery performance.The impedance that the lithium salts type additive of 0.5-3wt% can reduce battery in the present invention improves the cryogenic property of battery or improves the high-temperature behavior of battery.
Description
Technical field
The invention belongs to lithium ion battery material technical fields, and in particular to a kind of lithium-ion battery electrolytes and using should
The lithium ion battery with high energy density of electrolyte.
Background technique
Requirement with world community to environment is higher and higher, and the requirement to car exhaust gas is more and more harsh, wherein
The discharge standards such as the carbon dioxide and nitrogen oxides generated in fossil energy are especially paid attention to.New-energy automobile comes into being, and
There is provided its power is that lithium ion battery or partial power replace moving using oil electricity is mixed with lithium battery, reduces exhaust emissions.Mesh
The type of the new-energy automobile of preceding mainstream on the market is as follows: pure electric automobile (BEV), hybrid electric vehicle (HEV), plug-in mixing
Power car (PHEV), fuel electric vehicle (FCEV), extended-range electric vehicle (REEV) etc..
Requirement with client to electronic car kilometer is higher and higher, and this requires the corresponding lithium battery for providing power is continuous
Energy density is improved, to meet the needs of client's mileage.And the mode for improving energy density has following two aspect, it on the one hand can be with
Improve the charging voltage of battery, using the higher anode of charging voltage or using the better nickelic positive electrode of capacity；Another party
It face can be using the silicon-carbon cathode material of high-energy density or the combination of both fronts.But improve voltage one side positive electrode surface
Unstable, electrolyte can be oxidized；The SEI of another aspect negative terminal surface may be destroyed, and performance is caused to deteriorate.In addition silicon-carbon
The SEI film of cathode is unstable, in cyclic process due to removal lithium embedded bring stress make cathode SEI constantly destroy and constantly
It generates, film for additive can be constantly consumed, this just needs cathode film formation stronger or at the better additive of film toughness.
The positive and negative electrode of stabilizing material allows its interface to form more preferable more stable protective film, electrolyte serve it is key,
An important factor for being influence lithium ion battery electrical property, and additive is wherein extremely crucial component, it is one or more kinds of
Additive can significantly improve the various aspects of performance of lithium ion battery.Such as: application No. is the inventions of CN201610653856.8
" a kind of nickelic ternary power battery electrolyte and nickelic ternary lithium-ion-power cell ", discloses using conductive additive difluoro
Lithium phosphate (LiPO2F2), film for additive sulfuric acid vinyl ester (DTD), size be fluoro phosphonitrile and fluorinated ethylene carbonate
At least one of (FEC), by the interaction of the above three classes additive, excellent SEI film is formed in electrode surface, is promoted
Inside lithium ion cell dynamic process, guarantee power battery high power characteristic and good cycle performance, while also having
Higher safety.However, power battery at high temperature circulation and high-temperature storage performance are higher, high temperature protection agent therein is less, long
Phase high temperature storage and high temperature cyclic performance may can not guarantee, require further improvement optimization.
High-voltage anode or nickelic positive or main silicon-carbon cathode problem are as follows: high-voltage anode or nickelic anode, full
Positive electrode surface transition metal ions is in high oxidation state when electric state, is easy to capture the electronics in solvent or additive, make solvent or
Additive is oxidized decomposition, so as to cause gas, additive failure etc. is produced as a result, furthermore the transition metal ions of high oxidation state is unstable
It is fixed, it is easy the effect by HF, causes transition metal ions to dissolve out, to move to cathode by electrolyte, destroys cathode
SEI；Furthermore silicon-carbon cathode major problem is that, in charge and discharge or long-term cyclic process, since removal lithium embedded and material are in deintercalation
The variation that lithium overcharges middle structure causes the SEI on silicium cathode surface unstable, can constantly be destroyed in cyclic process, then and not
Medium well is at needing to consume more cathode film formation agent.
Summary of the invention
The purpose of the present invention is to solve current lithium ion battery high voltage appearance anode or nickelic positive electrode surface transition gold
Belong to ion high activity and is easy to provide a kind of lithium ion battery electrolysis by the problem of HF burn into silicon-carbon cathode SEI membrane stability difference
Liquid and the lithium ion battery with high energy density for using the electrolyte.
To achieve the above object, the technical solution adopted by the present invention is as follows:
A kind of lithium-ion battery electrolytes, including organic solvent, lithium salts and additive, the additive include cathode at
Film additive, anhydride additive and lithium salts type additive, in addition, further including nitrile compounds or ether nitrile compounds.
A kind of lithium ion battery with high energy density comprising above-mentioned electrolyte, the lithium ion battery include containing just
The positive plate of pole active material, the negative electrode tab containing negative electrode active material, diaphragm, binder and electrolyte.
The beneficial effect of the present invention compared with the existing technology is:
(1) it is directed to high-voltage anode or nickelic anode, the main combination for passing through nitrile and acid anhydrides, and positive protective agent,
By complexing or the effect of physical bond or bonding, stablizes the transition metal of positive electrode surface well, reduce or inhibit its oxidation molten
Agent or additive stablize anode and its interface, to guarantee the electrical property of battery, nitrile compares propylene sulphur with anhydride additive
The characteristic that acid lactone (RPS) has impedance low, cryogenic property are more excellent.
(2) be directed to silicon-carbon cathode, the percentage according to contained by wherein silicon, reasonably optimizing cathode film formation additive therein and
Its content, vinylene carbonate are good cathode film formation additives, can be formed a film well in graphite cathode, and fluoro carbonic acid
Ester can form a film well in silicon-carbon cathode, and at film have certain toughness, can preferably support to a certain extent
It is anti-due to silicon-carbon cathode during removal lithium embedded bring volume change.
(3) lithium salts type additive, which is added, can further improve high temperature or reduce battery impedance, further promote battery
Electrical property.In summary the effect of multiple additives can improve lithium ion battery with high energy density by their synergistic effect
The electrical properties such as high temperature storage, circulation and low temperature discharge.
Specific embodiment
Below with reference to embodiment, further description of the technical solution of the present invention, and with nickelic positive nickle cobalt lithium manganate
(NMC811) anode does specific description with silicon-carbon cathode battery, and positive and negative electrode of the invention, electrolyte are not limited thereto, all
It is that modifying or equivalently replacing the technical solution of the present invention, without departing from the spirit and scope of the technical solution of the present invention,
It should cover within the protection scope of the present invention.
Specific embodiment 1: present embodiment record is a kind of lithium-ion battery electrolytes, including organic solvent, lithium
Salt and additive, the additive includes cathode film formation additive, anhydride additive and lithium salts type additive, in addition, also
Including nitrile compounds or ether nitrile compounds.
Cathode film formation additive can form the SEI of stable negative terminal surface, nitrile compounds or ether nitrile compounds in cathode
With anhydride compound, anode can be complexed or form stable protective film in positive electrode surface, lithium salts type additive can improve
High-temperature behavior and/or reduction impedance.
Specific embodiment 2: a kind of lithium-ion battery electrolytes described in specific embodiment one, described is organic molten
Agent includes A and/or B, and the A is carbonic ester or fluoro carbonic ester, and the B is carboxylate or alpha-fluorocarboxylate ester；Described
Carbonic ester is one or more of ethylene carbonate, propene carbonate, dimethyl carbonate, diethyl carbonate, methyl ethyl carbonate；
The fluoro carbonic ester is one or more of the corresponding fluoric compound of carbonic ester；The carboxylate is second
Sour methyl esters, ethyl acetate, propyl acetate, n-butyl acetate, isobutyl acetate, n-amyl acetate, isoamyl acetate, propionic acid first
One or more of ester, ethyl propionate, propyl propionate, methyl butyrate, ethyl butyrate；The alpha-fluorocarboxylate ester is described
One or more of corresponding fluoric compound of carboxylate.
Specific embodiment 3: a kind of lithium-ion battery electrolytes described in specific embodiment one, the electrolyte
Shared mass fraction is 10wt%~20wt% to middle lithium salts in the electrolytic solution, preferably 12%~16%；The lithium salts is
Lithium hexafluoro phosphate (LiPF6), LiBF4 (LiBF4), bis- (oxalic acid) lithium borates (LiBOB), difluoro (oxalic acid) lithium borate
(LiODFB), difluoro dioxalic acid lithium phosphate (LiDFOP), tetrafluoro oxalic acid lithium phosphate (LiTFOP), bis trifluoromethyl sulfimide
(LiTFSI), trifluoromethyl sulfonic acid lithium (LiSO3CF3One or more of).
Specific embodiment 4: a kind of lithium-ion battery electrolytes described in specific embodiment one, the nitrile
Conjunction object is succinonitrile (SN), glutaronitrile, adiponitrile (ADN), pimelic dinitrile, hexamethylene dicyanide, certain herbaceous plants with big flowers dintrile, 1,3,6- hexane, three nitrile
(HTCN), one or more of (2- cyanoethoxyl) ethane of 1,2- bis- (DENE)；When adding nitrile compounds, nitrile chemical combination
Shared mass fraction is 0.2~6.5%, preferably 0.2~3% in the electrolytic solution for both object and anhydride compound；It is described
Ether nitrile compounds be bis- (propionitrile) ethers of ethylene glycol, 1,2- bis- (2- cyanoethoxyl) ethane, 1,2,3- tri--(2- cyanoethoxyls)
One or more of propane；When adding ether nitrile compounds, both ether nitrile compounds and anhydride compound are being electrolysed
Shared mass fraction is 0.2~6.5%, preferably 0.2~3% in liquid.
Specific embodiment 5: a kind of lithium-ion battery electrolytes described in specific embodiment one, the anhydride
Additive is succinic anhydride, glutaric anhydride, adipic anhydride, pimelic acid acid anhydride, phthalic anhydride, maleic anhydride, citraconic acid
One of fluoric compound of one or more of acid anhydride, citric anhydride, perfluoroglutaric acid acid anhydride or the acid anhydrides is several
Kind.
Specific embodiment 6: a kind of lithium-ion battery electrolytes described in specific embodiment one, the cathode at
Film additive is vinylene carbonate (VC), vinyl ethylene carbonate (VEC), fluorinated ethylene carbonate (FEC), sulfuric acid ethylene
Ester (DTD), 1,3-propane sultone (1,3-PS), ethylene sulfite (ES), one in methane-disulfonic acid methylene ester (MMDS)
Kind is several；Shared ratio is 0.3~20wt% to the cathode film formation additive in the electrolytic solution, preferably 0.3~
15wt%.
Specific embodiment 7: a kind of lithium-ion battery electrolytes described in specific embodiment one, the lithium salts type
Additive is difluorophosphate (LiPO2F2), difluoro (oxalic acid) lithium borate (LiODFB), double fluorine sulfimide lithiums (LiFSI), two
One or more of fluorine dioxalic acid lithium phosphate (LiDFOP), bis trifluoromethyl sulfimide (LiTFSI)；The lithium salts type
Shared ratio is 0.3wt.%~8wt.%, preferably 1wt.%~3wt.% to additive in the electrolytic solution.
Specific embodiment 8: a kind of include electrolysis described in specific embodiment any in specific embodiment one to seven
The lithium ion battery with high energy density of liquid, the lithium ion battery include the positive plate containing positive electrode active materials, containing negative
Negative electrode tab, diaphragm, binder and the electrolyte of pole active material.
Specific embodiment 9: lithium ion battery described in specific embodiment eight, the positive plate is Layered Lithium
Composite oxides, general formula Li1+xNiyCozM(1-y-z)Y2, wherein -0.1≤x≤0.5,0≤y≤1,0≤z≤1, and 0≤y+z
≤1；M is one or more of Mg, Zn, Ga, Ba, Al, Fe, Cr, Sn, V, Mn, Sc, Ti, Nb, Mo, Zr；Y is in O, F, P
It is one or more of.
Specific embodiment 10: lithium ion battery described in specific embodiment eight, the negative electrode tab be carbon materials,
Silica-base material, tin-based material or their alloy material；Contain one of carbon, silicon, tin element in the negative electrode active material
Or it is several.
The operating voltage range of lithium ion battery of the present invention is 4.2V and the above voltage.
(1) prepared by positive plate
Positive electrode active materials nickle cobalt lithium manganate (811 type), conductive agent carbon black, binder Kynoar (PVDF) are pressed into matter
Amount is than (96~98): (3~1): 1 is mixed, and N-Methyl pyrrolidone (NMP) is added and makees solvent, stirs under vacuum conditions
Obtain the good anode sizing agent of mixing uniform flow；The anode sizing agent is coated uniformly in current collector aluminum foil, through 120 DEG C of baking ovens
Drying 6~10 hours, then roll-in cut to obtain anode pole piece.
(2) prepared by negative electrode tab
By negative electrode active material silicon-carbon (5%SiO), thickener sodium carboxymethylcellulose (CMC), binder, butadiene-styrene rubber,
Conductive agent is mixed according to weight ratio 97:1:1:1, and deionized water is added, and obtains negative electrode slurry under de-airing mixer effect；
Negative electrode slurry is coated uniformly on copper foil of affluxion body；It is small that copper foil is transferred to 120 DEG C of oven dryings 8~13 after room temperature is dried
When, then negative electrode tab is obtained by cold pressing, cutting.
(3) prepared by electrolyte
Full of argon gas water oxygen content qualification glove box in, by ethylene carbonate, propene carbonate, diethyl carbonate,
Methyl ethyl carbonate is uniformly mixed according to the ratio of mass ratio 25:5:50:20, then rapidly joins the abundant of 12.5wt% thereto
Dry lithium hexafluoro phosphate (LiPF6), it is dissolved in organic solvent, is eventually adding and accounts for electrolyte total amount weight 0.3wt% carbonic acid
Vinylene (VC), 2wt%1,3-N-morpholinopropanesulfonic acid lactone (1,3-PS), 6.5wt% fluorinated ethylene carbonate (FEC), 0.5wt%
Adiponitrile (ADN), 0.5wt% difluorophosphate (LiPO2F2) it is uniformly mixing to obtain the electrolyte in embodiment 1.
(4) preparation of isolation film
The polypropylene isolation film (being provided by Celgard company) of 6~13 μ m-thicks is provided.
(5) preparation of lithium ion battery
The positive plate, isolation film, negative electrode tab of above-mentioned preparation are successively stacked in order, guarantee that isolation film is in always
Play the role of isolation between positive and negative plate, the naked battery core of non-fluid injection is then obtained by winding；Naked battery core is placed in outer packing
In foil, by the above-mentioned electrolyte prepared be injected into it is dry after naked battery core in, by Vacuum Package, standing, chemical conversion, shaping,
The production process such as sorting, obtain required lithium ion battery.
Electrolyte is substantially according to the preparation in above-mentioned electrolyte quota, here the area of the electrolyte of embodiment and comparative example
It is not listed as follows:
| Type | Adiponitrile | Propene sultone | Citraconic anhydride | Difluorophosphate | Double fluorine Huang imide lis |
| Embodiment 1 | 0.5 | 0.5 | |||
| Embodiment 2 | 0.5 | 1 | |||
| Embodiment 3 | 0.5 | 0.5 | 0.5 | ||
| Embodiment 4 | 0.5 | 0.5 | 1 | ||
| Embodiment 5 | 0.5 | 1 | 1 | ||
| Embodiment 6 | 0.2 | 0.5 | |||
| Embodiment 7 | 0.2 | 1 | |||
| Embodiment 8 | 0.2 | 0.5 | 1 | ||
| Embodiment 9 | 0.2 | 1 | 1 | ||
| Embodiment 10 | 0.3 | 0.2 | 0.5 | ||
| Embodiment 11 | 0.3 | 0.2 | 0.5 | 1 | |
| Embodiment 12 | 0.3 | 0.2 | 1 | 1 | |
| Comparative example 1 | |||||
| Comparative example 2 | 0.5 | ||||
| Comparative example 3 | 0.5 | 1 | |||
| Comparative example 4 | 0.5 | 1 | 1 |
Dependence test is described as follows:
High temperature storage experiment:
Embodiment 1~12 and 1~3 gained battery of comparative example are subjected to 5 charge and discharges at room temperature with the charge-discharge magnification of 1C
Electric loop test, then 1C multiplying power is charged to full power state.1C capacity Q is recorded respectively0With thickness D0.The battery of full power state is existed
It is stored 30 days at 60 DEG C, records cell thickness D1With 1C discharge capacity Q1, then by battery at room temperature with the multiplying power charge and discharge 5 of 1C
Record 1C discharge capacity Q in week2, it is real that battery high-temperature memory capacity conservation rate, capacity restoration rate and thickness change etc. is calculated
Data are tested, result such as table 1 is recorded.
The calculation formula wherein used is as follows:
Thickness change (%)=(D1-D0)/D0* 100%
Capacity retention ratio (%)=Q1/Q0* 100%
Capacity restoration rate (%)=Q2/Q0* 100%
45 DEG C of high temperature circulation experiments:
By 1~4 gained battery of embodiment 1~12 and comparative example, the initial full electric thickness D of battery is tested0, shelved at 45 DEG C
1-3 hours, after battery body reaches environment temperature, 4.2V is then charged to 1C constant current, then 4.2V constant pressure is charged to 0.05C,
Then 1C constant-current discharge recycles 5 weeks to 2.75V, records discharge capacity Q0, then record is recycled to the discharge capacity of certain all numbers
Q1, the fully charged leave from office of battery is then tested the thickness D of the full electricity of battery to battery recovery to room temperature1, calculated thickness change rate and
Capacity retention ratio records result such as table 1.
Thickness change (%)=(D1-D0)/D0* 100%
Capacity retention ratio (%)=Q1/Q0* 100%
Low temperature discharge experiment:
The battery of comparative example and embodiment is subjected to 5 charge and discharge cycles at room temperature with 1C multiplying power, then with 1C multiplying power
It is charged to full power state, records 1C capacity Q0.After battery under full power state is shelved 4-6 hours at -20 DEG C, with 0.2C multiplying power
3V is discharged into, discharge capacity Q is recorded1, can be calculated low temperature discharge capacity conservation rate, record result such as table 1.
Low temperature discharge capacity conservation rate calculation is following formula:
Capacity retention ratio (%)=Q1/Q0* 100%
The comparison of 1 embodiment and comparative example experimental result of table
It is compared by comparative example 1,2,3, illustrates that propene sultone (RPS), which is added, can obviously inhibit normal temperature circulation and height
The expansion of temperature circulation thickness, but since propene sultone (RPS) additive internal resistance is larger, hence it is evident that deterioration low temperature performance.
It is compared by comparative example 3,4 and embodiment 2,5, illustrates adiponitrile (ADN) and difluorophosphate (LiPO2F2) and/or double fluorine sulphonyl
Imine lithium (LiFSI) can be obviously improved the expansion of normal temperature circulation and high temperature circulation thickness, while their combination compares propylene
Sultones (RPS) and difluorophosphate (LiPO2F2) and/or double fluorine sulfimide lithiums (LiFSI) combination, impedance is lower, can
To improve low temperature performance, high-temperature storage performance is quite even more excellent.It is compared by comparative example 3,4 and embodiment 7,9, explanation
Citraconic anhydride and difluorophosphate (LiPO2F2) and/or double fluorine sulfimide lithiums (LiFSI) can be obviously improved normal temperature circulation and
The expansion of high temperature circulation thickness, while improving low temperature performance.Pass through comparative example 1,2, embodiment 1,2, embodiment 4,5, reality
It applies example 8,9 and embodiment 11,12 and compares discovery two-by-two, increase difluorophosphate (LiPO2F2) content can improve low temperature discharge property
Can, battery impedance can be reduced by being primarily due to it.It is compared two-by-two by comparison comparative example 3,4, embodiment 3,4, discovery increases
The content of double fluorine sulfimide lithiums (LiFSI) can improve circulating battery, thickness and high temperature storage thickness.By embodiment 6,7,
8 and embodiment 10,11,12 comparison discovery, adiponitrile (ADN), citraconic anhydride and difluorophosphate (LiPO2F2) and/or double fluorine sulphurs
The combined cycle performance and circulation thickness and high temperature storage thickness of imide li (LiFSI) are smaller, compared to single combination
Effect is more preferable.
It is to be illustrated for possible embodiments of the invention above, but positive and negative electrode of the invention, electrolyte not office
It is limited to this, all modifying or equivalently replacing the technical solution of the present invention, without departing from the spirit of the technical scheme of the invention
And range, it should all cover within the protection scope of the present invention.
Claims (10)
1. a kind of lithium-ion battery electrolytes, including organic solvent, lithium salts and additive, it is characterised in that: the additive
Including cathode film formation additive, anhydride additive and lithium salts type additive, in addition, further including nitrile compounds or ether nitrile
Close object.
2. a kind of lithium-ion battery electrolytes according to claim 1, it is characterised in that: the organic solvent includes A
And/or B, the A are carbonic ester or fluoro carbonic ester, the B is carboxylate or alpha-fluorocarboxylate ester；The carbonic ester is
One or more of ethylene carbonate, propene carbonate, dimethyl carbonate, diethyl carbonate, methyl ethyl carbonate；The fluorine
It is one or more of the corresponding fluoric compound of carbonic ester for carbonic ester；The carboxylate be methyl acetate,
Ethyl acetate, propyl acetate, n-butyl acetate, isobutyl acetate, n-amyl acetate, isoamyl acetate, methyl propionate, propionic acid second
One or more of ester, propyl propionate, methyl butyrate, ethyl butyrate；The alpha-fluorocarboxylate ester is the carboxylate pair
One or more of fluoric compound answered.
3. a kind of lithium-ion battery electrolytes according to claim 1, it is characterised in that: lithium salts exists in the electrolyte
Shared mass fraction is 10wt%~20wt% in electrolyte；The lithium salts is lithium hexafluoro phosphate, LiBF4, double
(oxalic acid) lithium borate, difluoro (oxalic acid) lithium borate, difluoro dioxalic acid lithium phosphate, tetrafluoro oxalic acid lithium phosphate, bis trifluoromethyl sulphonyl
One or more of imines, trifluoromethyl sulfonic acid lithium.
4. a kind of lithium-ion battery electrolytes according to claim 1, it is characterised in that: the nitrile compounds are fourth
Dintrile, glutaronitrile, adiponitrile, pimelic dinitrile, hexamethylene dicyanide, certain herbaceous plants with big flowers dintrile, 1,3,6- hexane, three nitrile, 1,2- bis- (2- cyanoethoxyl) ethane
One or more of；When adding nitrile compounds, both nitrile compounds and anhydride compound are shared in the electrolytic solution
Mass fraction be 0.2~6.5%；The ether nitrile compounds are bis- (propionitrile) ethers of ethylene glycol, (the 2- cyanogen ethoxy of 1,2- bis-
Base) ethane, 1, one or more of 2,3- tri--(2- cyanoethoxyl) propane；When adding ether nitrile compounds, ether nitrile
Closing both object and anhydride compound, shared mass fraction is 0.2~6.5% in the electrolytic solution.
5. a kind of lithium-ion battery electrolytes according to claim 1, it is characterised in that: the anhydride additive is
Succinic anhydride, glutaric anhydride, adipic anhydride, pimelic acid acid anhydride, phthalic anhydride, maleic anhydride, citraconic acid acid anhydride, citric acid
One or more of acid anhydride, perfluoroglutaric acid acid anhydride or one or more of the fluoric compound of the acid anhydrides.
6. a kind of lithium-ion battery electrolytes according to claim 1, it is characterised in that: the cathode film formation additive
For vinylene carbonate, vinyl ethylene carbonate, fluorinated ethylene carbonate, sulfuric acid vinyl ester, 1,3-propane sultone, sulfurous
One or more of vinyl acetate, methane-disulfonic acid methylene ester；The cathode film formation additive is shared in the electrolytic solution
Ratio is 0.3~20wt%.
7. a kind of lithium-ion battery electrolytes according to claim 1, it is characterised in that: the lithium salts type additive is
Difluorophosphate, difluoro (oxalic acid) lithium borate, double fluorine sulfimide lithiums, difluoro dioxalic acid lithium phosphate, bis trifluoromethyl sulphonyl are sub-
One or more of amine；Shared ratio is 0.3wt.%~8wt.% to the lithium salts type additive in the electrolytic solution.
8. a kind of lithium ion battery with high energy density comprising electrolyte described in claim 1~7 any claim, special
Sign is: the lithium ion battery include the positive plate containing positive electrode active materials, the negative electrode tab containing negative electrode active material,
Diaphragm, binder and electrolyte.
9. lithium ion battery according to claim 8, it is characterised in that: the positive plate is Layered Lithium combined oxidation
Object, general formula Li1+xNiyCozM(1-y-z)Y2, wherein -0.1≤x≤0.5,0≤y≤1,0≤z≤1, and 0≤y+z≤1；M is
One or more of Mg, Zn, Ga, Ba, Al, Fe, Cr, Sn, V, Mn, Sc, Ti, Nb, Mo, Zr；Y be one of O, F, P or
It is several.
10. lithium ion battery according to claim 8, it is characterised in that: the negative electrode tab is carbon materials, silicon substrate
Material, tin-based material or their alloy material.Contain one or more of carbon, silicon, tin element in the negative electrode active material.
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Application publication date: 20190419 |