CN104285330B - Lithium secondary battery - Google Patents
Lithium secondary battery Download PDFInfo
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- CN104285330B CN104285330B CN201480001221.9A CN201480001221A CN104285330B CN 104285330 B CN104285330 B CN 104285330B CN 201480001221 A CN201480001221 A CN 201480001221A CN 104285330 B CN104285330 B CN 104285330B
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- Prior art keywords
- monomer
- secondary battery
- lithium secondary
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- 229910052744 lithium Inorganic materials 0.000 title claims abstract description 47
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 title claims abstract description 46
- 239000000203 mixture Substances 0.000 claims abstract description 68
- 239000000178 monomer Substances 0.000 claims abstract description 55
- 239000005518 polymer electrolyte Substances 0.000 claims abstract description 42
- 125000000524 functional group Chemical group 0.000 claims abstract description 32
- 229910021645 metal ion Inorganic materials 0.000 claims abstract description 17
- 230000004888 barrier function Effects 0.000 claims abstract description 11
- 239000007773 negative electrode material Substances 0.000 claims abstract description 7
- 239000003792 electrolyte Substances 0.000 claims description 27
- NIXOWILDQLNWCW-UHFFFAOYSA-N 2-Propenoic acid Natural products OC(=O)C=C NIXOWILDQLNWCW-UHFFFAOYSA-N 0.000 claims description 21
- 150000001875 compounds Chemical class 0.000 claims description 17
- 239000002904 solvent Substances 0.000 claims description 16
- 239000003505 polymerization initiator Substances 0.000 claims description 13
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 12
- 150000002148 esters Chemical class 0.000 claims description 12
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- 238000000034 method Methods 0.000 claims description 9
- 239000007774 positive electrode material Substances 0.000 claims description 9
- 239000000126 substance Substances 0.000 claims description 9
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- 125000004494 ethyl ester group Chemical group 0.000 claims description 7
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- 229910052760 oxygen Inorganic materials 0.000 claims description 2
- 229910052720 vanadium Inorganic materials 0.000 claims description 2
- 229910052727 yttrium Inorganic materials 0.000 claims description 2
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- 208000018459 dissociative disease Diseases 0.000 description 1
- 239000012153 distilled water Substances 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 229920001971 elastomer Polymers 0.000 description 1
- 238000003487 electrochemical reaction Methods 0.000 description 1
- 230000005518 electrochemistry Effects 0.000 description 1
- 239000008151 electrolyte solution Substances 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 229940093499 ethyl acetate Drugs 0.000 description 1
- 239000004744 fabric Substances 0.000 description 1
- 239000000835 fiber Substances 0.000 description 1
- 238000003682 fluorination reaction Methods 0.000 description 1
- 239000011737 fluorine Substances 0.000 description 1
- 229910052733 gallium Inorganic materials 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- 239000011245 gel electrolyte Substances 0.000 description 1
- 239000003365 glass fiber 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
- 229910052735 hafnium Inorganic materials 0.000 description 1
- VBJZVLUMGGDVMO-UHFFFAOYSA-N hafnium atom Chemical compound [Hf] VBJZVLUMGGDVMO-UHFFFAOYSA-N 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 150000002431 hydrogen Chemical class 0.000 description 1
- 150000002432 hydroperoxides Chemical class 0.000 description 1
- 125000002887 hydroxy group Chemical group [H]O* 0.000 description 1
- 239000001863 hydroxypropyl cellulose Substances 0.000 description 1
- 235000010977 hydroxypropyl cellulose Nutrition 0.000 description 1
- APFVFJFRJDLVQX-UHFFFAOYSA-N indium atom Chemical compound [In] APFVFJFRJDLVQX-UHFFFAOYSA-N 0.000 description 1
- 238000003475 lamination Methods 0.000 description 1
- 125000000400 lauroyl group Chemical group O=C([*])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])[H] 0.000 description 1
- 229910001547 lithium hexafluoroantimonate(V) Inorganic materials 0.000 description 1
- 229910001540 lithium hexafluoroarsenate(V) Inorganic materials 0.000 description 1
- PAZHGORSDKKUPI-UHFFFAOYSA-N lithium metasilicate Chemical compound [Li+].[Li+].[O-][Si]([O-])=O PAZHGORSDKKUPI-UHFFFAOYSA-N 0.000 description 1
- MHCFAGZWMAWTNR-UHFFFAOYSA-M lithium perchlorate Chemical compound [Li+].[O-]Cl(=O)(=O)=O MHCFAGZWMAWTNR-UHFFFAOYSA-M 0.000 description 1
- 229910001486 lithium perchlorate Inorganic materials 0.000 description 1
- 229910052912 lithium silicate Inorganic materials 0.000 description 1
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 description 1
- ACFSQHQYDZIPRL-UHFFFAOYSA-N lithium;bis(1,1,2,2,2-pentafluoroethylsulfonyl)azanide Chemical compound [Li+].FC(F)(F)C(F)(F)S(=O)(=O)[N-]S(=O)(=O)C(F)(F)C(F)(F)F ACFSQHQYDZIPRL-UHFFFAOYSA-N 0.000 description 1
- QSZMZKBZAYQGRS-UHFFFAOYSA-N lithium;bis(trifluoromethylsulfonyl)azanide Chemical compound [Li+].FC(F)(F)S(=O)(=O)[N-]S(=O)(=O)C(F)(F)F QSZMZKBZAYQGRS-UHFFFAOYSA-N 0.000 description 1
- 150000002734 metacrylic acid derivatives Chemical class 0.000 description 1
- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 150000004706 metal oxides Chemical class 0.000 description 1
- 125000000956 methoxy group Chemical group [H]C([H])([H])O* 0.000 description 1
- 229940017219 methyl propionate Drugs 0.000 description 1
- PQIOSYKVBBWRRI-UHFFFAOYSA-N methylphosphonyl difluoride Chemical group CP(F)(F)=O PQIOSYKVBBWRRI-UHFFFAOYSA-N 0.000 description 1
- 229910052750 molybdenum Inorganic materials 0.000 description 1
- 239000011733 molybdenum Substances 0.000 description 1
- YKYONYBAUNKHLG-UHFFFAOYSA-N n-Propyl acetate Natural products CCCOC(C)=O YKYONYBAUNKHLG-UHFFFAOYSA-N 0.000 description 1
- QYZFTMMPKCOTAN-UHFFFAOYSA-N n-[2-(2-hydroxyethylamino)ethyl]-2-[[1-[2-(2-hydroxyethylamino)ethylamino]-2-methyl-1-oxopropan-2-yl]diazenyl]-2-methylpropanamide Chemical compound OCCNCCNC(=O)C(C)(C)N=NC(C)(C)C(=O)NCCNCCO QYZFTMMPKCOTAN-UHFFFAOYSA-N 0.000 description 1
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 description 1
- 239000011255 nonaqueous electrolyte Substances 0.000 description 1
- 239000004745 nonwoven fabric Substances 0.000 description 1
- 238000010606 normalization Methods 0.000 description 1
- 239000010450 olivine Substances 0.000 description 1
- 229910052609 olivine Inorganic materials 0.000 description 1
- 239000005486 organic electrolyte Substances 0.000 description 1
- 150000001451 organic peroxides Chemical group 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 238000010422 painting Methods 0.000 description 1
- 239000011574 phosphorus Substances 0.000 description 1
- 229920000058 polyacrylate Polymers 0.000 description 1
- 229920006254 polymer film Polymers 0.000 description 1
- 229920000098 polyolefin Polymers 0.000 description 1
- 229920002451 polyvinyl alcohol Polymers 0.000 description 1
- 229940090181 propyl acetate Drugs 0.000 description 1
- 238000010526 radical polymerization reaction Methods 0.000 description 1
- 150000003254 radicals Chemical class 0.000 description 1
- 239000004627 regenerated cellulose Substances 0.000 description 1
- 229910052702 rhenium Inorganic materials 0.000 description 1
- WUAPFZMCVAUBPE-UHFFFAOYSA-N rhenium atom Chemical compound [Re] WUAPFZMCVAUBPE-UHFFFAOYSA-N 0.000 description 1
- 239000011435 rock Substances 0.000 description 1
- 239000005060 rubber Substances 0.000 description 1
- DCKVNWZUADLDEH-UHFFFAOYSA-N sec-butyl acetate Chemical compound CCC(C)OC(C)=O DCKVNWZUADLDEH-UHFFFAOYSA-N 0.000 description 1
- 239000011257 shell material Substances 0.000 description 1
- 239000000377 silicon dioxide Substances 0.000 description 1
- 229910052814 silicon oxide Inorganic materials 0.000 description 1
- 229910052709 silver Inorganic materials 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- 239000007784 solid electrolyte Substances 0.000 description 1
- 229910052596 spinel Inorganic materials 0.000 description 1
- 239000011029 spinel Substances 0.000 description 1
- 239000008107 starch Substances 0.000 description 1
- 235000019698 starch Nutrition 0.000 description 1
- 229910052682 stishovite Inorganic materials 0.000 description 1
- 229920005608 sulfonated EPDM Polymers 0.000 description 1
- 229910052715 tantalum Inorganic materials 0.000 description 1
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 description 1
- JBQYATWDVHIOAR-UHFFFAOYSA-N tellanylidenegermanium Chemical compound [Te]=[Ge] JBQYATWDVHIOAR-UHFFFAOYSA-N 0.000 description 1
- UWNNZXDNLPNGQJ-UHFFFAOYSA-N tert-butyl 2-ethylhexanoate Chemical class CCCCC(CC)C(=O)OC(C)(C)C UWNNZXDNLPNGQJ-UHFFFAOYSA-N 0.000 description 1
- BFKJFAAPBSQJPD-UHFFFAOYSA-N tetrafluoroethene Chemical compound FC(F)=C(F)F BFKJFAAPBSQJPD-UHFFFAOYSA-N 0.000 description 1
- 239000010409 thin film Substances 0.000 description 1
- 229910052718 tin Inorganic materials 0.000 description 1
- 230000007704 transition Effects 0.000 description 1
- 229910052905 tridymite Inorganic materials 0.000 description 1
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 description 1
- 229910052721 tungsten Inorganic materials 0.000 description 1
- 239000010937 tungsten Substances 0.000 description 1
- NQPDZGIKBAWPEJ-UHFFFAOYSA-N valeric acid Chemical compound CCCCC(O)=O NQPDZGIKBAWPEJ-UHFFFAOYSA-N 0.000 description 1
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
- 229920001285 xanthan gum Polymers 0.000 description 1
- VWQVUPCCIRVNHF-UHFFFAOYSA-N yttrium atom Chemical compound [Y] VWQVUPCCIRVNHF-UHFFFAOYSA-N 0.000 description 1
- 239000011701 zinc Substances 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
- H01M10/052—Li-accumulators
-
- 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
- H01M10/0565—Polymeric materials, e.g. gel-type or solid-type
-
- 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
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/058—Construction or manufacture
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/362—Composites
- H01M4/364—Composites as mixtures
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/362—Composites
- H01M4/366—Composites as layered products
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
- H01M4/386—Silicon or alloys based on silicon
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
- H01M4/485—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of mixed oxides or hydroxides for inserting or intercalating light metals, e.g. LiTi2O4 or LiTi2OxFy
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
- H01M4/52—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron
- H01M4/525—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron of mixed oxides or hydroxides containing iron, cobalt or nickel for inserting or intercalating light metals, e.g. LiNiO2, LiCoO2 or LiCoOxFy
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
- H01M4/583—Carbonaceous material, e.g. graphite-intercalation compounds or CFx
- H01M4/587—Carbonaceous material, e.g. graphite-intercalation compounds or CFx for inserting or intercalating light metals
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M2220/00—Batteries for particular applications
- H01M2220/30—Batteries in portable systems, e.g. mobile phone, laptop
-
- 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
- H01M2300/0085—Immobilising or gelification of electrolyte
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
- H01M4/50—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese
- H01M4/505—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese of mixed oxides or hydroxides containing manganese for inserting or intercalating light metals, e.g. LiMn2O4 or LiMn2OxFy
-
- 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
-
- 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
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
Landscapes
- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Inorganic Chemistry (AREA)
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Composite Materials (AREA)
- Condensed Matter Physics & Semiconductors (AREA)
- Dispersion Chemistry (AREA)
- General Physics & Mathematics (AREA)
- Physics & Mathematics (AREA)
- Materials Engineering (AREA)
- Secondary Cells (AREA)
- Battery Electrode And Active Subsutance (AREA)
- Addition Polymer Or Copolymer, Post-Treatments, Or Chemical Modifications (AREA)
Abstract
The invention provides a kind of lithium secondary battery, it includes positive pole, negative pole, barrier film and gel polymer electrolyte, it is characterized in that, i) negative pole includes silicon (Si) base negative electrode active material, ii) gel polymer electrolyte is formed by making to polymerize comprising the composition with the monomer of functional group that can be combined with metal ion, and iii) charge voltage range of the battery is 3.0V to 5.0V.It can be prevented from being moved to the precipitation of negative pole or reduction metal in negative pole from the metal ion that positive pole dissolves according to the lithium secondary battery of the present invention, thus battery life can be not only improved, and the volumetric properties of battery are also excellent when being charged under high voltage and normal voltage.
Description
Technical field
The present invention relates to a kind of lithium secondary battery, it includes positive pole, negative pole, barrier film and gel polymer electrolyte, and
More specifically, it is related to a kind of lithium secondary battery, wherein, negative pole includes silicon (Si) base negative electrode active material, gelatin polymer electricity
Solution matter is formed by polymerizeing the composition comprising the monomer with the functional group that can be combined with metal ion, and battery
Charge voltage range is 3.0V to 5.0V.
Background technology
Recently, with the trend of the portable of electronic equipment, miniaturization, lightweight and high performance, electronic equipment, information
With communications industry rapid growth.Therefore, power source of the high performance lithium secondary battery as these mancarried electronic aids, and because
This demand rapid growth.The secondary cell that can be used with recharge and electric discharge is for for information and communication, electric car or electricity
It is required for the power source of the mancarried electronic aid of electrical automobile.Especially, because the performance of these products can be depended on
As the battery of critical component, so the consumer demand to high-capacity battery is improved constantly.
In general, known battery security is sequentially increased according to following：Liquid electrolyte ＜ gel polymer electrolytes
＜ solid polymer electrolytes, but battery performance is reduced with same order.
The electrolyte of liquid condition, especially, (wherein salt is dissolved in and non-aqueous had ionic conduction type liquid organic electrolyte
In machine solvent) electrolyte of electrochemical apparatus has been mainly used as, such as using the conventional of electrochemical reaction and double layer capacitor
The electrolyte of battery.However, when the electrolyte using liquid condition, electrode material can be degraded and organic solvent may be waved
Hair.Similarly, since the temperature rise of environment temperature and battery in itself, may there is security flaw (such as burning).
It is known as battery performance poor, solid polymer electrolyte is not commercialized yet at present.
Because gel polymer electrolyte can have excellent electrochemistry security, it is possible to consistently maintain battery
Thickness.Further, since the intrinsic adhesiveness of gel phase allows the contact between electrode and electrolyte good, therefore, can
To prepare film type battery.Therefore, the exploitation of various gel polymer electrolytes is being expanded.
In gel polymer electrolyte, because the size of lithium ion can be smaller, so directly mobile not only relative appearance
Easily, and due to jump (hopping) phenomenon as shown in Figure 1, lithium ion is also easy to move in the electrolytic solution.
When metal ion dissolves, metal ion can be reduced into the metallic state of negative pole to block the anti-of (block) negative pole
Answer site.When new metal is precipitated in negative terminal surface, electrolyte generates new solid electrolyte on the metal surface
Interface (SEI) layer, therefore, electrolyte is persistently consumed.Further, since the thickness of the SEI layers in negative pole it is sustainable increase and increase
Big resistance, therefore, it is possible to decrease lithium secondary battery life performance.Accordingly, it would be desirable to improve above-mentioned limitation.
The content of the invention
Technical problem
The present invention provides a kind of lithium secondary battery, and it can be by preventing from being moved to negative pole from the metal ion that positive pole dissolves
Or reduction translational speed, precipitation of the metal in negative pole is thus reduced, therefore, battery life can be not only improved, and battery
Volumetric properties are excellent under normal voltage and high voltage.
Technical scheme
According to an aspect of the invention, there is provided a kind of lithium secondary battery, it includes positive pole, negative pole, barrier film and gel
Polymer dielectric, it is characterised in that
I) negative pole includes silicon (Si) base negative electrode active material,
Ii) gel polymer electrolyte is by making comprising the monomer with the functional group that can be combined with metal ion
Composition polymerize to be formed, and
Iii) charge voltage range of the battery is 3.0V to 5.0V.
There is provided a kind of method for preparing lithium secondary battery according to another aspect of the present invention, it is characterised in that it is wrapped
Include：The step of electrode assembly including positive pole, the barrier film of negative pole and setting between a positive electrode and a negative electrode is inserted into battery case；
Composition for a gel polymer electrolyte is injected into battery case and makes composition polymerization to form gelatin polymer electricity
The step of solving matter, wherein, the composition for a gel polymer electrolyte includes electrolyte solvent, ionizable lithium
Salt, polymerization initiator and the monomer with the functional group that can be combined with metal ion.
Beneficial effect
Lithium secondary battery according to an embodiment of the invention, can be moved by the metal ion for preventing from dissolving from positive pole
Move to negative pole or reduce the translational speed of metal ion and reduce precipitation of the metal in negative pole, and therefore, can not only improve
Battery life, and the volumetric properties of battery are excellent under normal voltage and high voltage.
Brief description of the drawings
Fig. 1 is the figure for the motion principle for representing lithium ion when using gel polymer electrolyte.
Fig. 2 is to compared for using metal when conventional electrolysis liquid and the electrolyte of one embodiment of the invention in negative pole
On precipitation degree figure.
Fig. 3 is the high voltage for showing the lithium secondary battery that is prepared in embodiment 1 to 4 and comparative example 1 to 4 in 4.3V
Under capacity curve map.
Embodiment
Hereinafter, the present invention will be described in further detail, to enable the invention to be more clearly understood.
It should be understood that the word or term that use in the specification and in the claims should not be construed as being limited to it is general
Implication in dictionary.It should also be understood that reasonably defining the meaning of word or term in the present inventor in order to most preferably illustrate the present invention
On the principle basis of think of, word or term should be interpreted as having and meet it in correlation technique and the technological thought situation of the present invention
Lower the had meaning.
The present invention lithium secondary battery be characterised by, it include positive pole (cathode), negative pole (anode), barrier film and
Gel polymer electrolyte, wherein, i) negative pole includes silicon (Si) base negative electrode active material, ii) the gelatin polymer electricity
Solution matter is formed by polymerizeing the composition comprising the monomer with the functional group that can be combined with metal ion, and iii) institute
The charge voltage range for stating battery is 3.0V to 5.0V.
In the electrolyte of lithium secondary battery according to an embodiment of the invention, the composition is as gel
The composition of polymer dielectric can be included：Electrolyte solvent, ionizable lithium salts, polymerization initiator；With as can be with
Monomer monomer, with the functional group that can be combined with metal ion of gelatin polymer is formed by polymerisation.
Monomer with the functional group is acrylonitrile or for the monomer based on acrylate, and preferably, functional group
Any one selected from following functional group can be included：
The functional group is by C1-C5It is that alkyl or halogen replace or unsubstituted；Or its two or more mixing
Thing.
The representational example of the monomer with the functional group according to an embodiment of the invention can be selected from
Any one of following compound or two or more mixtures：
(1) 2 cyanoethyl acrylate；
(2) acrylic acid 2- cyanoethoxies ethyl ester；
(3) acrylonitrile；
(4) (E) -3- (pyridine -2- bases)-ethyl acrylate；
(5) (E) -3- (4- pyridine radicals) -2- ethyl acrylates；
(6) 2- acrylic acid 3,3 '-[2,2 '-bipyridyl] -4,4 '-diyl pair-dimethyl esters；
(7) 2- acrylic acid 2- [2,2 '-bipyridyl] -6- base ethyl esters；
(8) 2- acrylic acid 2- [2,2 '-bipyridyl] -5- base ethyl esters；
(9) 2- acrylic acid 2- [2,2 '-bipyridyl] -4- base ethyl esters；
(10) 2- acrylic acid 1,1 '-[[2,2 '-bipyridyl] -4,4 '-diyl is double (methylene)] ester；
(11) 2- acrylic acid, double (methylene) esters of 1,10- phenanthroline -2,9- diyls；
(12) 2- acrylic acid 3- (1,10- phenanthroline -2- bases)-phenyl methyl esters；With
(13) 2- acrylic acid 2- [[(1- oxo -2- acrylic) epoxide] methyl] -2- [(1,10- phenanthroline -5- base methoxies
Base) methyl] -1,3- glyceryl esters.
In these compounds, particularly preferably using selected from 2 cyanoethyl acrylate, acrylic acid 2- cyanoethoxy second
Any one of ester, acrylonitrile and (E) -3- (pyridine -2- bases)-ethyl acrylate or its two or more mixture.
According to one embodiment of the invention, because the monomer with functional group includes the functional group in monomer, so
Functional group can be stably fixed in the gel structure of gel polymer electrolyte.
For example, by the way that cyano group and acrylate are added to composition for a gel polymer electrolyte respectively
(gel electrolyte) and in the case of being polymerize and forming compound (complex), compound in itself can be for coagulating
Moved in the composition of xanthan polymer electrolyte, so that reduction reaction can occurs at negative pole and metal can be precipitated.So
And, according to one embodiment of the invention, in the case where 2 cyanoethyl acrylate is used as the monomer with functional group,
It is included in due to cyano group in the monomer with functional group, so cyano group can not be moved in gel structure in itself.
That is, according to one embodiment of the invention, as shown in Fig. 2 in composition for a gel polymer electrolyte
In the case of middle monomer of the use with functional group, the monomer with functional group can be combined with the metal ion dissolved from positive pole,
To reduce precipitation of the metal on negative pole, this is different from the use of the situation of conventional electrolysis liquid, the gold dissolved from positive pole in the situation
Belong to ion precipitation on negative pole.It therefore, it can improve the charge efficiency and discharging efficiency of lithium secondary battery, and can show
Good cycle specificity.In addition, being used for lithium two in the gel polymer electrolyte composition comprising the monomer with functional group
In the case of primary cell, the volumetric properties in normalization voltage range and high voltage range can be improved.
The term " normal voltage " used in this manual refers to, the charge voltage range of lithium secondary battery for 3.0V extremely
Situation less than 4.3V, and term " high voltage " refers to the situation that charge voltage range is 4.3V to 5.0V.
The content of monomer with functional group can be 0.1 weight % to 10 weight %, preferably 0.5 weight % to 5 weights
Measure %, the gross weight meter based on composition.When the amount of the monomer with functional group is less than 0.1 weight %, gelation becomes tired
Difficulty, and it is thus impossible to the performance of gel polymer electrolyte is presented.In the case that the amount of monomer is more than 10 weight %, by
The raising of resistance is excessively included and caused in monomer, and accordingly, it is possible to reduces battery performance.
Moreover, according to one embodiment of the invention, composition, which can also be included, has 2 to 6 acrylate groups
Monomer, and monomer can be branching type monomer.
Branching type monomer for example can be selected from following any one or its two or more mixture：Two (three hydroxyl first
Base) tetraacrylate, Dipentaerythritol Pentaacrylate, and dipentaerythritol acrylate.
The content of branching type monomer can be 0.1 weight % to 10 weight %, and preferably 0.5 weight % is based on to 5 weight %
Total restatement of composition.
According to one embodiment of the invention, in the case where composition also includes branching type monomer, with functional group
Monomer and branching type monomer mixing and under 30 DEG C to 100 DEG C of temperature range react 2 minutes to 12 hours, with prepare can
Polymerized monomer.In this case, the content ratio (weight ratio) of the monomer with functional group and branching type monomer may range from
Such as 1:0.1 to 1:10.However, the invention is not restricted to this.
The ionizable lithium salts included in the compositions of the present invention can be for example following any one or its two kinds
Mixture above：LiPF6、LiBF4、LiSbF6、LiAsF6、LiClO4、LiN(C2F5SO2)2、LiN(CF3SO2)2、CF3SO3Li、
LiC(CF3SO2)3And LiC4BO8.However, the invention is not restricted to this.
Moreover, the electrolyte solvent generally used in the electrolyte of lithium secondary battery can be used as this hair with without stint
The bright middle electrolyte solvent used, and such as ether, ester, acid amides, linear carbonate or cyclic carbonate can be used alone or
Used with the mixture that its is two or more.
In these materials, it can generally include cyclic carbonate, linear carbonate or the carbonic ester as its mixture
Compound.The instantiation of cyclic carbonate can be following any or its two or more mixture：Ethylene carbonate
(EC), the sub- pentyl ester of propylene carbonate (PC), carbonic acid 1,2- butylenes, carbonic acid 2,3- butylenes, carbonic acid 1,2-, carbonic acid 2,3- Asias penta
Ester, ethylene carbonate, and its halide.Moreover, the specific example of linear carbonate can for following any one or its
Two or more mixtures：Dimethyl carbonate (DMC), diethyl carbonate (DEC), dipropyl carbonate (DPC), ethyl methyl carbonate
(EMC), methyl ethyl ester (MPC) and carbonic acid ethylpropyl (EPC).However, the invention is not restricted to this.
Especially, because propylene carbonate and ethylene carbonate are used as the ring-type carbon in the electrolyte solvent based on carbonic ester
During acid esters, they are high-viscosity organic solvents and have high dielectric constant, so propylene carbonate and ethylene carbonate can
To dissociate the lithium salts in electrolyte well.It therefore, it can preferably use propylene carbonate and ethylene carbonate.When above-mentioned ring-type
Carbonic ester and low viscosity, the linear carbonate of low-k (such as ethyl methyl carbonate, diethyl carbonate and dimethyl carbonate)
When mixing in proper proportions, the electrolyte with high conductance can be prepared, it is possible to preferably use propylene carbonate
And ethylene carbonate.
Moreover, in methyl acetate, ethyl acetate, propyl acetate, methyl propionate, ethyl propionate, gamma-butyrolacton, γ-penta
Ester, γ-hexalactone, σ-any one of valerolactone and 6-caprolactone or its two or more mixture may be used as electrolyte
Ester in solvent.However, the invention is not restricted to this.
In the present invention, common polymerization initiator known in the art may be used as polymerization initiator.
The non-limiting examples of polymerization initiator can be organic peroxide or hydroperoxides, such as benzoyl peroxide
(benzoyl peroxide), acetyl peroxide (acetyl peroxide), the double lauroyl (dilauryl of peroxidating
Peroxide), di-tert-butyl peroxide (di-tert-butyl peroxide), the peroxidating 2- ethyl-hexanoic tert-butyl esters (t-
Butyl peroxy-2-ethyl--hexanoate), cumyl hydroperoxide (cumyl hydroperoxide) and peroxidating
Hydrogen, and azo-compound is for example, 2,2'- azos double (2- cyanobutanes), 2,2'- azos double (methylbutyronitrile), 2,2'- azos
Double (isobutyronitriles) (AIBN, 2,2'-Azobis (iso-butyronitrile)) and 2,2'- azo are double (methyl pentane nitrile)
(AMVN, 2,2'-Azobis (dimethylvaleronitrile)).However, the invention is not restricted to this.
Polymerization initiator can be dissociated by the heat in battery, and nonrestrictive example is for example at 30 DEG C to 100 DEG C
At a temperature of, or can at room temperature (5 DEG C to 30 DEG C) dissociations to form free radical, and can by radical polymerization with can
Polymerized monomer reacts to form gel polymer electrolyte.
Equally, the consumption of polymerization initiator can be 0.01 weight % to 2 weight %, total restatement based on composition.
In the case that the usage amount of polymerization initiator is more than 2 weight %, it is injected into by composition for a gel polymer electrolyte
Can carry out gelation during battery too quickly, or can remaining unreacted initiator then battery performance is produced it is unfavorable
Influence.Comparatively speaking, in the case where the usage amount of polymerization initiator is less than 0.01 weight %, it is impossible to carry out gel well
Change.
In addition to the above components, composition of the invention can optionally include other additives known in the art.
Equally, according to one embodiment of the invention, the present invention can provide the method for preparing lithium secondary battery, wrap
Include：The step of electrode assembly including positive pole, the barrier film of negative pole and setting between a positive electrode and a negative electrode is inserted into battery case；
Composition for a gel polymer electrolyte is injected into battery case and makes composition polymerization to form gelatin polymer electricity
The step of solving matter, wherein, composition for a gel polymer electrolyte includes electrolyte solvent, ionizable lithium salts, gathered
Close initiator and the monomer with the functional group that can be combined with metal ion.Gel according to an embodiment of the invention gathers
Polymer electrolyte, by will be polymerize for the above-mentioned composition of gel polymer electrolyte according to common method known in the art
To be formed.For example, gel polymer electrolyte can be polymerize for gel polymerisation by (in-situ) in situ in the secondary battery
The composition of thing electrolyte is formed.
According to one exemplary aspect of the invention, methods described may include：(a) will be by positive pole, negative pole and setting
The step of electrode assembly of barrier film between a positive electrode and a negative electrode is inserted into battery case；(b) gel polymer electrolyte will be used for
The composition of matter is injected into after battery case, makes the step of composition polymerization is to form electrolyte.
Original position (in-situ) polymerisation in lithium secondary battery can be carried out by thermal polymerization.In this case, institute
The polymerization time scope needed is about 2 minutes to 12 hours, and thermal polymerization temperature range can be 30 DEG C to 100 DEG C.
When carrying out the gelation based on polymerisation, gel polymer electrolyte is formed.Specifically, gel polymerisation is formed
Thing, wherein polymerisable monomer are cross-linked to each other by polymerisation, and the gelatin polymer being consequently formed can equably by
Liquid electrolyte is impregnated, and wherein electrolytic salt is dissociated in electrolyte solvent.
The electrode of lithium secondary battery of the present invention can be prepared by conventional method known in the art.For example, adhesive, leading
Electric agent and dispersant (if desired) and solvent are mixed and stirred with electrode active material to prepare slurry, and then golden
Category current-collector slurry is coated and compressed.Hereafter, electrode can be prepared by drying metal collector.
In the present invention, any compound may be used as positive electrode active materials in positive pole and without restriction, if its
It can be used under normal voltage and high voltage and can reversibly be embedded in/removal lithium embedded.
According to one embodiment of the invention, in positive pole, the positive electrode active materials example that can be used under normal voltage
It can such as include selected from following any one or its two or more mixture：LiCoO2、LiNiO2、LiMnO2、
LiMn2O4、LiNi1-yCoyO2(0≤y<1)、LiCo1-yMnyO2(0≤y<1)、LiNi1-yMnyO2(0≤y<And Li 1)
(NiaCobMnc)O2(0<A, b, c≤1, a+b+c=1).However, the invention is not restricted to this.Moreover, except above-mentioned oxide
(oxide) outside, sulfide (sulfide), selenides (selenide) and halide (halide) can also be included.
In lithium secondary battery according to another embodiment of the invention, the positive electrode active materials that can be used under high voltages
It can include selected from following any one or its two or more composite oxides：Hexagonal crystal system with high capacity characteristics
The spinel lithium transition of bedded salt rock (hexagonal layered rock-salt) structure, olivine structural and cubic structure
Metal oxide, V2O5, TiS and MoS.
Specifically, positive electrode active materials can for example include any or its two or more mixing in chemical formula 1 to 3
Thing.
<Chemical formula 1>
Li[LixNiaCobMnc]O2(wherein 0<x≤0.3、0.3≤c≤0.7、0<a+b<0.5 and x+a+b+c=1)；
<Chemical formula 2>
LiMn2-xMxO4(wherein M is selected from nickel (Ni), cobalt (Co), iron (Fe), phosphorus (P), sulphur (S), zirconium to be one or more
(Zr), the element of titanium (Ti) and aluminium (Al), and 0<x≤2)；
<Chemical formula 3>
Li1+aCoxM1-xAX4(wherein M is selected from Al, magnesium (Mg), Ni, Co, manganese (Mn), Ti, gallium (Ga), copper to be one or more
(Cu), the element of vanadium (V), niobium (Nb), Zr, cerium (Ce), indium (In), zinc (Zn) and yttrium (Y), X is selected from oxygen to be one or more
(O), the element of fluorine (F) and nitrogen (N), A is P, S or its complex element, 0≤a≤0.2 and 0.5≤x≤1).
In chemical formula 1, positive electrode active materials can meet 0.4≤c≤0.7 and 0.2≤a+b<0.5, and can be with
Including selected from LiNi0.5Mn1.5O4、LiCoPO4And LiFePO4Any one of or its two or more mixture,.
In the negative pole of lithium secondary battery according to an embodiment of the invention, negative active core-shell material can be used at this
Si base negative electrode active materials used in field, containing Si.For example, negative active core-shell material can include following any one
Or its two or more mixture：Single Si；Si and carbon material carry out Si-C compounds formed by mechanical alloying；Si with
Metal carries out compound formed by mechanical alloying；Carbon-Si nano-complexes；Si oxides (SiOx,1≤x≤2)；And painting
It is covered with Si the or Si oxides of carbon.Carbonaceous material in Si-C compounds can be selected from following any one or its two kinds with
On mixture：Native graphite, Delanium, carbonaceous mesophase spherules (mesocarbon microbeads (MCMB)), carbon fiber
And carbon black.In the case of using Si-C compounds, the proportion of silicon (Si) and carbon (C) in Si-C compounds can be 40
Parts by weight：60 parts by weight to 80 parts by weight：20 parts by weight.It is additionally, since the SiO or SiO as Si oxides2Reacted with lithium
During have by formation as inertia phase Li2O and lithium metasilicate and the cushioning effect for slowing down Si Volume Changes, so SiO
Or SiO2Volumetric properties can be improved.In addition, in Si and metal carry out compound formed by mechanical alloying, metal can be with
Selected from Ti, V, chromium (Cr), Mn, Fe, Co, Ni, Cu, Zr, Nb, molybdenum (Mo), tantalum (Ta), tungsten (W), hafnium (Hf), rhenium (Re), silver
(Ag), golden (Au), Al, Zn, tin (Sn), antimony (Sb) and its conjugate.
Negative pole in lithium secondary battery according to embodiments of the present invention can also include in Si base negative electrode active materials
Carbon-based material, such as graphite.
Pass through the dispersant for making negative pole or positive electrode active materials, adhesive, solvent and conductive agent and generally optionally using
It is mixed and stirred for and prepares slurry.It is then possible to by the way that slurry is coated into current-collector and compresses the current-collector of coating and prepares
Negative pole or positive pole.
Various types of binder polymers may be used as adhesive, and described adhesive polymer for example gathers inclined difluoro second
Alkene-hexafluoropropylene copolymer (PVDF-co-HEP), polyvinylidene fluoride (polyvinylidene fluoride), polyacrylonitrile
(polyacrylonitrile), polymethyl methacrylate (polymethylmethacrylate), polyvinyl alcohol, carboxymethyl
It is cellulose (CMC), starch, hydroxypropyl cellulose, regenerated cellulose, PVP, tetrafluoroethene, polyethylene, poly-
Propylene, polyacrylate, Ethylene-Propylene-Diene monomer (EPDM), sulfonated epdm, SBR styrene butadiene rubberses (SBR), fluorination
Rubber and various copolymers.
Moreover, the common porous polymer films as conventional separator, for example by the polymer based on polyolefin, (such as ethene is equal
Polymers, Noblen, ethylene/butylene copolymers, ethylene/hexene copolymer and ethylene/methacrylic acid ester copolymer) prepare
Apertured polymeric film, can be used alone or lamination is used as barrier film.In addition it is possible to use conventional porous non-woven
Cloth, such as non-woven fabrics by being formed with dystectic glass fibre or pet fiber.However, this hair
Bright not limited to this.
The shape of the lithium secondary battery of the present invention is not particularly limited, and for example, it may be uses the cylinder of shell, rib
Cylindricality, bag (pouch) shape or coin (coin) shape.
Hereinafter, the present invention is described in detail according to specific embodiment.However, the present invention can show as many not
With form and should not be construed as the embodiment that is limited to be proposed at this.And these embodiments are to provide so that originally
Specification is detailed and complete, and the scope of concept of the present invention is fully conveyed into those skilled in the art.
Embodiment
Hereinafter, the present invention will be described in more detail according to embodiment and EXPERIMENTAL EXAMPLE.However, the invention is not restricted to
This.
Embodiment 1
<The preparation of composition for a gel polymer electrolyte>
Electrolyte is by by LiPF6It is 1 to be dissolved in volume ratio:2 ethylene carbonate (EC) and ethyl methyl carbonate
(EMC) prepared in the non-aqueous electrolyte solvent of composition, to obtain LiPF6Concentration is 1M.For gel polymer electrolyte
Polymerisable monomer (the 2 cyanoethyl acrylate and 2.5 parts by weight of 2.5 parts by weight that the composition of matter passes through 5 parts by weight of addition
Two (trimethylolpropane) tetraacrylates) and 0.25 parts by weight the peroxide as polymerization initiator -2 ethyl hexanoic acid uncle
Butyl ester and prepare, the electrolyte meter based on 100 parts by weight.
<The preparation of coin-shaped secondary cell>
It is prepared by positive pole
Cathode mix slurry is prepared via a method which：Using the 94 weight % Li as positive electrode active materials
[Li0.29Ni0.14Co0.11Mn0.46]O2, 3 weight % carbon black (carbon black) as conductive agent and 3 weight % work
For adhesive polyvinylidene fluoride (PVdF) be added to as solvent METHYLPYRROLIDONE (NMP).It is about by thickness
20 μm aluminium (Al) thin film coated as cathode collector cathode mix slurry is simultaneously dried, then thin to aluminium
Film implements roll-in (roll press) and is prepared for positive pole.
It is prepared by negative pole
Using as the SiO and graphite that are coated with carbon of negative active core-shell material with 10:90 weight is than being mixed.By negative pole
Active material, as carbon black (carbon black), SBR and the CMC of conductive agent with 94:2:2:2 weight is than being mixed.System
Standby mixture is put into the distilled water as solvent, and is mixed and be prepared for uniform cathode size.
Cathode size is coated in thickness and is 10 μm copper (Cu) film as anode collector, and is dried and presses
System, then negative pole is prepared by making Cu film perforatings.
It is prepared by battery
Assembled using positive pole, negative pole and by the barrier film that three-layer polypropylene/polyethylene/polypropylene (PP/PE/PP) is formed
Battery, and the composition for a gel polymer electrolyte prepared is injected into the battery of assembling.Then, by nitrogen
Battery is heated with 80 DEG C 2 minutes to 30 minutes, be thus prepared for coin-shaped secondary cell under gas atmosphere.
Embodiment 2
Coin-shaped secondary cell is prepared in the same manner as example 1, difference is, preparing embodiment 1
In composition for a gel polymer electrolyte, acrylic acid 2- cyano group second is replaced using acrylic acid 2- cyanoethoxies ethyl ester
Ester.
Embodiment 3
Coin-shaped secondary cell is prepared in the same manner as example 1, difference is, preparing embodiment 1
In composition for a gel polymer electrolyte, 2 cyanoethyl acrylate is replaced using acrylonitrile.
Embodiment 4
Coin-shaped secondary cell is prepared in the same manner as example 1, difference is, preparing embodiment 1
In composition for a gel polymer electrolyte, acrylic acid 2- is replaced using (E) -3- (pyridine -2- bases)-ethyl acrylates
Cyanaoethyl methacrylate.
Comparative example 1
Coin-shaped secondary cell is prepared in the same manner as example 1, difference is, preparing embodiment 1
In composition for a gel polymer electrolyte, polymerisable monomer and polymerization initiator is not used.
Comparative example 2
Coin-shaped secondary cell is prepared in the same manner as example 1, difference is, preparing embodiment 1
In composition for a gel polymer electrolyte, using only two (trihydroxy methyl) tetraacrylates of 5 parts by weight, thus
Instead of using by the way that the 2 cyanoethyl acrylate of 2.5 parts by weight and (trihydroxy methyl) the propane tetrapropylene of 2.5 parts by weight two is sour
The polymerisable monomer for 5 parts by weight that ester is mixed and prepared.
Comparative example 3
Coin-shaped secondary cell is prepared in the same manner as example 1, difference is, preparing embodiment 1
In composition for a gel polymer electrolyte, using only the Dipentaerythritol Pentaacrylate of 5 parts by weight, thus instead of making
With by by 2.5 parts by weight of acrylic acid 2- cyanaoethyl methacrylates and the mixing of 2.5 parts by weight two (trihydroxy methyl) tetraacrylates
The polymerisable monomer of 5 parts by weight prepared.
Comparative example 4
Coin-shaped secondary cell is prepared in the same manner as example 1, difference is, preparing embodiment 1
In negative pole, using only graphite, thus instead of using being coated with the SiO of carbon and the mixture of graphite as negative active core-shell material.
EXPERIMENTAL EXAMPLE
Lithium secondary battery (the battery capacity prepared in embodiment 1 to 4 and comparative example 1 to 4：4.5mAh) at 55 DEG C
Using 0.7C constant current charge to voltage as 4.3V.Then, lithium secondary battery is charged with 4.3V constant voltage, and
And stop charging when charging current becomes 0.225mA.Afterwards, by battery standing 10 minutes, then with 0.5C constant current
Make battery discharge until voltage turns into 3.0V.The discharge and recharge is repeated into 40 circulations, battery capacity is then measured.Its
As a result figure 3 illustrates.
Specifically, as shown in figure 3, to the 5th circulate untill embodiment 1 to 4 and comparative example 1 to 4 capacity almost
It is mutually similar.However, after the about the 10th time circulates, the capacity of comparative example 1 to 4 starts reduction, and is followed at the 20th time
Drastically reduced after ring.Comparatively speaking, its volume change compared with comparative example 1 to 4 of embodiment 1 to 4 is relatively slow, and special
Not, more than 2 to 4 times of the capacity with comparative example 1 to 4 after embodiment 1 to 4 is even circulated at the 40th time.
It therefore, it can confirm：The battery prepared in embodiment 1 to 4 is charged and carried out under 4.3V high voltages
After 40 circulations, the discharge capacity of battery is significantly carried compared with the discharge capacity of the battery prepared in comparative example 1 to 4
It is high.
Industrial applicibility
Due to lithium secondary battery according to embodiments of the present invention not only increase battery life and also in normal voltage and
Also there are excellent volumetric properties, it is suitable to secondary cell under high voltage.
Claims (15)
1. a kind of lithium secondary battery, it includes：Positive pole, negative pole, barrier film and gel polymer electrolyte, it is characterised in that
The negative pole includes Si base negative electrode active materials,
The gel polymer electrolyte is by making comprising the composition with the monomer of functional group that can be combined with metal ion
It polymerize to be formed,
The charge voltage range of the battery be 3.0V to 5.0V,
The monomer with functional group is acrylate base monomer, and
The functional group included in the acrylate base monomer includes being selected from following any one：
The functional group is by C1-C5It is that alkyl or halogen replace or unsubstituted.
2. the lithium secondary battery of claim 1, it is characterised in that
The negative active core-shell material is any one in following material or its two or more mixture：Single Si；
Si and carbonaceous material carry out Si-C compounds formed by mechanical alloying；Si carries out multiple formed by mechanical alloying with metal
Compound；Carbon-Si nano-complexes；Si oxides；With Si the or Si oxides for being coated with carbon.
3. the lithium secondary battery of claim 2, it is characterised in that
The Si of the Si-C compounds is 40 parts by weight with C ratio scope：60 parts by weight to 80 parts by weight：20 parts by weight.
4. the lithium secondary battery of claim 2, it is characterised in that
The carbonaceous material is any one in following material or its two or more mixture：It is native graphite, artificial
Graphite, carbonaceous mesophase spherules, carbon fiber and carbon black.
5. the lithium secondary battery of claim 1, it is characterised in that
The monomer with functional group is selected from any one of following compound or its two or more mixture：
(1) (E) -3- (pyridine -2- bases)-ethyl acrylate；
(2) (E) -3- (4- pyridine radicals) -2- ethyl acrylates；
(3) 2- acrylic acid 3,3 '-[2,2 '-bipyridyl] -4,4 '-diyl pair-dimethyl esters；
(4) 2- acrylic acid 2- [2,2 '-bipyridyl] -6- base ethyl esters；
(5) 2- acrylic acid 2- [2,2 '-bipyridyl] -5- base ethyl esters；
(6) 2- acrylic acid 2- [2,2 '-bipyridyl] -4- base ethyl esters；
(7) 2- acrylic acid 1,1 '-[[2,2 '-bipyridyl] -4,4 '-diyl is double (methylene)] ester；
(8) double (methylene) esters of 2- acrylic acid 1,10- phenanthroline -2,9- diyls；
(9) 2- acrylic acid 3- (1,10- phenanthroline -2- bases)-phenyl methyl esters；With
(10) 2- acrylic acid 2- [[(1- oxo -2- acrylic) epoxide] methyl] -2- [(1,10- phenanthroline -5- ylmethoxies) first
Base] -1,3- glyceryl esters.
6. the lithium secondary battery of claim 1, it is characterised in that
The composition includes electrolyte solvent, ionizable lithium salts, polymerization initiator and with can be combined with metal ion
Functional group monomer.
7. the lithium secondary battery of claim 6, it is characterised in that
The composition also includes the monomer with 2 to 6 acrylate groups,
The monomer with 2 to 6 acrylate groups is branching type monomer.
8. the lithium secondary battery of claim 7, it is characterised in that
The branching type monomer is selected from any one of following monomer or its two or more mixture：Two (trihydroxy methyls)
Tetraacrylate, Dipentaerythritol Pentaacrylate and dipentaerythritol acrylate.
9. the lithium secondary battery of claim 6, it is characterised in that
The content of the monomer with functional group is 0.1 weight % to 10 weight %, total restatement based on composition.
10. the lithium secondary battery of claim 7, it is characterised in that
The content of the branching type monomer is 0.1 weight % to 10 weight %, total restatement based on composition.
11. the lithium secondary battery of claim 7, it is characterised in that
The weight ratio scope of the monomer and branching type monomer with functional group is 1:0.1 to 1:10.
12. the lithium secondary battery of claim 1, it is characterised in that
Positive electrode active materials for the positive pole are any in the compound of chemical formula 1 to 3 or its is two or more
Mixture：
<Chemical formula 1>
Li[LixNiaCobMnc]O2
Wherein 0<x≤0.3、0.3≤c≤0.7、0<a+b<0.5, and x+a+b+c=1；
<Chemical formula 2>
LiMn2-xMxO4
Wherein M is selected from Ni, Co, Fe, P, S, Zr, Ti and Al elements, and 0 for one or more<x≤2；
<Chemical formula 3>
Li1+aCoxM1-xAX4
Wherein M is one or more elements for being selected from Al, Mg, Ni, Co, Mn, Ti, Ga, Cu, V, Nb, Zr, Ce, In, Zn and Y, X
For one or more elements for being selected from O, F and N, A is P, S or its complex element, 0≤a≤0.2 and 0.5≤x≤1.
13. the lithium secondary battery of claim 1, it is characterised in that
Positive electrode active materials for the positive pole are the mixed of two kinds or more of any one or its in following material
Compound：LiCoO2、LiNiO2、LiMnO2、LiMn2O4、LiNi1-yCoyO2Wherein 0≤y<1、LiCo1-yMnyO2Wherein 0≤y<1、
LiNi1-yMnyO2Wherein 0≤y<1, and Li (NiaCobMnc)O2Wherein 0<A, b, c≤1, a+b+c=1.
14. a kind of method for the lithium secondary battery for preparing claim 1, it is characterised in that methods described includes：
Electrode assembly including positive pole, the barrier film of negative pole and setting between a positive electrode and a negative electrode is inserted into the step of battery case
Suddenly；
Composition for a gel polymer electrolyte is injected into battery case and composition polymerization is formed gel polymerisation
The step of thing electrolyte, wherein,
The composition for a gel polymer electrolyte comprising electrolyte solvent, ionizable lithium salts, polymerization initiator,
With the monomer with the functional group that can be combined with metal ion.
15. the method for claim 14, it is characterised in that
Described be aggregated under 30 DEG C to 100 DEG C of temperature range is carried out.
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| KR1020140009649A KR101545432B1 (en) | 2013-01-28 | 2014-01-27 | Lithium secondary battery |
| PCT/KR2014/000800 WO2014116085A1 (en) | 2013-01-28 | 2014-01-28 | Lithium secondary battery |
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| KR (1) | KR101545432B1 (en) |
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| JP6067844B2 (en) * | 2013-04-30 | 2017-01-25 | 日立オートモティブシステムズ株式会社 | Lithium ion secondary battery |
| US10326166B2 (en) * | 2016-08-15 | 2019-06-18 | GM Global Technology Operations LLC | Gel electrolytes and precursors thereof |
| US11710852B2 (en) | 2018-02-09 | 2023-07-25 | Lg Energy Solution, Ltd. | Separator for secondary battery and lithium secondary battery including same |
| JP7310118B2 (en) * | 2018-10-29 | 2023-07-19 | セイコーエプソン株式会社 | Manufacturing method of cathode material |
| CN111816925B (en) * | 2020-08-14 | 2022-11-29 | 中南大学 | Solid-state battery and preparation method thereof |
| CN117012910A (en) * | 2022-04-29 | 2023-11-07 | 华为技术有限公司 | Composite material, preparation method and application thereof |
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| KR20140097027A (en) | 2014-08-06 |
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| BR112014017510A2 (en) | 2017-06-13 |
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| KR101545432B1 (en) | 2015-08-18 |
| CN104285330A (en) | 2015-01-14 |
| JP2015524601A (en) | 2015-08-24 |
| BR112014017510A8 (en) | 2017-07-04 |
| BR112014017510B1 (en) | 2021-05-25 |
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