CN1819324A - Electrolyte and lithium ion battery using same - Google Patents
Electrolyte and lithium ion battery using same Download PDFInfo
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- CN1819324A CN1819324A CNA2006100496873A CN200610049687A CN1819324A CN 1819324 A CN1819324 A CN 1819324A CN A2006100496873 A CNA2006100496873 A CN A2006100496873A CN 200610049687 A CN200610049687 A CN 200610049687A CN 1819324 A CN1819324 A CN 1819324A
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- Prior art keywords
- cyclic
- electrolyte
- lithium ion
- carbonate
- battery
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- 239000003792 electrolyte Substances 0.000 title claims abstract description 52
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 36
- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 36
- -1 benzotriazole compound Chemical class 0.000 claims abstract description 64
- VAYTZRYEBVHVLE-UHFFFAOYSA-N 1,3-dioxol-2-one Chemical compound O=C1OC=CO1 VAYTZRYEBVHVLE-UHFFFAOYSA-N 0.000 claims abstract description 23
- BJWMSGRKJIOCNR-UHFFFAOYSA-N 4-ethenyl-1,3-dioxolan-2-one Chemical compound C=CC1COC(=O)O1 BJWMSGRKJIOCNR-UHFFFAOYSA-N 0.000 claims abstract description 15
- 125000004122 cyclic group Chemical group 0.000 claims abstract description 13
- LSNNMFCWUKXFEE-UHFFFAOYSA-M Bisulfite Chemical compound OS([O-])=O LSNNMFCWUKXFEE-UHFFFAOYSA-M 0.000 claims abstract description 11
- LSNNMFCWUKXFEE-UHFFFAOYSA-N Sulfurous acid Chemical compound OS(O)=O LSNNMFCWUKXFEE-UHFFFAOYSA-N 0.000 claims abstract description 11
- 239000007774 positive electrode material Substances 0.000 claims abstract description 6
- 239000007773 negative electrode material Substances 0.000 claims abstract description 4
- KZNICNPSHKQLFF-UHFFFAOYSA-N succinimide Chemical class O=C1CCC(=O)N1 KZNICNPSHKQLFF-UHFFFAOYSA-N 0.000 claims description 22
- 229960002317 succinimide Drugs 0.000 claims description 14
- 229910003002 lithium salt Inorganic materials 0.000 claims description 10
- 159000000002 lithium salts Chemical class 0.000 claims description 10
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 9
- 229910052799 carbon Inorganic materials 0.000 claims description 9
- 239000000463 material Substances 0.000 claims description 8
- 239000002904 solvent Substances 0.000 claims description 7
- PEEHTFAAVSWFBL-UHFFFAOYSA-N Maleimide Chemical class O=C1NC(=O)C=C1 PEEHTFAAVSWFBL-UHFFFAOYSA-N 0.000 claims description 6
- DNIAPMSPPWPWGF-UHFFFAOYSA-N Propylene glycol Chemical compound CC(O)CO DNIAPMSPPWPWGF-UHFFFAOYSA-N 0.000 claims description 6
- 125000001997 phenyl group Chemical group [H]C1=C([H])C([H])=C(*)C([H])=C1[H] 0.000 claims description 6
- 229910013870 LiPF 6 Inorganic materials 0.000 claims description 5
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims description 5
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 claims description 5
- 150000002148 esters Chemical class 0.000 claims description 5
- 239000013538 functional additive Substances 0.000 claims description 5
- 229910052744 lithium Inorganic materials 0.000 claims description 5
- 229910000314 transition metal oxide Inorganic materials 0.000 claims description 5
- 239000004698 Polyethylene Substances 0.000 claims description 4
- 125000000217 alkyl group Chemical group 0.000 claims description 4
- 125000001797 benzyl group Chemical group [H]C1=C([H])C([H])=C(C([H])=C1[H])C([H])([H])* 0.000 claims description 4
- 229920000573 polyethylene Polymers 0.000 claims description 4
- LZDKZFUFMNSQCJ-UHFFFAOYSA-N 1,2-diethoxyethane Chemical compound CCOCCOCC LZDKZFUFMNSQCJ-UHFFFAOYSA-N 0.000 claims description 3
- RRQYJINTUHWNHW-UHFFFAOYSA-N 1-ethoxy-2-(2-ethoxyethoxy)ethane Chemical compound CCOCCOCCOCC RRQYJINTUHWNHW-UHFFFAOYSA-N 0.000 claims description 3
- POAOYUHQDCAZBD-UHFFFAOYSA-N 2-butoxyethanol Chemical compound CCCCOCCO POAOYUHQDCAZBD-UHFFFAOYSA-N 0.000 claims description 3
- JWUJQDFVADABEY-UHFFFAOYSA-N 2-methyltetrahydrofuran Chemical compound CC1CCCO1 JWUJQDFVADABEY-UHFFFAOYSA-N 0.000 claims description 3
- PNGAWASQASFPNE-UHFFFAOYSA-N 4,5,6,7-tetrahydro-1,3-dioxonin-2-one Chemical compound C1(OCCCCC=CO1)=O PNGAWASQASFPNE-UHFFFAOYSA-N 0.000 claims description 3
- YEJRWHAVMIAJKC-UHFFFAOYSA-N 4-Butyrolactone Chemical compound O=C1CCCO1 YEJRWHAVMIAJKC-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
- XTHFKEDIFFGKHM-UHFFFAOYSA-N Dimethoxyethane Chemical compound COCCOC XTHFKEDIFFGKHM-UHFFFAOYSA-N 0.000 claims description 3
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 claims description 3
- RJUFJBKOKNCXHH-UHFFFAOYSA-N Methyl propionate Chemical compound CCC(=O)OC RJUFJBKOKNCXHH-UHFFFAOYSA-N 0.000 claims description 3
- XBDQKXXYIPTUBI-UHFFFAOYSA-M Propionate Chemical compound CCC([O-])=O XBDQKXXYIPTUBI-UHFFFAOYSA-M 0.000 claims description 3
- QOSMNYMQXIVWKY-UHFFFAOYSA-N Propyl levulinate Chemical compound CCCOC(=O)CCC(C)=O QOSMNYMQXIVWKY-UHFFFAOYSA-N 0.000 claims description 3
- WYURNTSHIVDZCO-UHFFFAOYSA-N Tetrahydrofuran Chemical compound C1CCOC1 WYURNTSHIVDZCO-UHFFFAOYSA-N 0.000 claims description 3
- GTDPSWPPOUPBNX-UHFFFAOYSA-N ac1mqpva Chemical compound CC12C(=O)OC(=O)C1(C)C1(C)C2(C)C(=O)OC1=O GTDPSWPPOUPBNX-UHFFFAOYSA-N 0.000 claims description 3
- KXKVLQRXCPHEJC-UHFFFAOYSA-N acetic acid trimethyl ester Natural products COC(C)=O KXKVLQRXCPHEJC-UHFFFAOYSA-N 0.000 claims description 3
- 230000002378 acidificating effect Effects 0.000 claims description 3
- 230000004888 barrier function Effects 0.000 claims description 3
- BVKZGUZCCUSVTD-UHFFFAOYSA-N carbonic acid Chemical compound OC(O)=O BVKZGUZCCUSVTD-UHFFFAOYSA-N 0.000 claims description 3
- 239000002131 composite material Substances 0.000 claims description 3
- FUGIIBWTNARRSF-UHFFFAOYSA-N decane-5,6-diol Chemical compound CCCCC(O)C(O)CCCC FUGIIBWTNARRSF-UHFFFAOYSA-N 0.000 claims description 3
- 229940019778 diethylene glycol diethyl ether Drugs 0.000 claims description 3
- SBZXBUIDTXKZTM-UHFFFAOYSA-N diglyme Chemical compound COCCOCCOC SBZXBUIDTXKZTM-UHFFFAOYSA-N 0.000 claims description 3
- RTZKZFJDLAIYFH-UHFFFAOYSA-N ether Substances CCOCC RTZKZFJDLAIYFH-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
- FPYJFEHAWHCUMM-UHFFFAOYSA-N maleic anhydride Chemical compound O=C1OC(=O)C=C1 FPYJFEHAWHCUMM-UHFFFAOYSA-N 0.000 claims description 3
- 229940017219 methyl propionate Drugs 0.000 claims description 3
- STCOOQWBFONSKY-UHFFFAOYSA-N tributyl phosphate Chemical compound CCCCOP(=O)(OCCCC)OCCCC STCOOQWBFONSKY-UHFFFAOYSA-N 0.000 claims description 3
- DQWPFSLDHJDLRL-UHFFFAOYSA-N triethyl phosphate Chemical compound CCOP(=O)(OCC)OCC DQWPFSLDHJDLRL-UHFFFAOYSA-N 0.000 claims description 3
- WVLBCYQITXONBZ-UHFFFAOYSA-N trimethyl phosphate Chemical compound COP(=O)(OC)OC WVLBCYQITXONBZ-UHFFFAOYSA-N 0.000 claims description 3
- ZPFAVCIQZKRBGF-UHFFFAOYSA-N 1,3,2-dioxathiolane 2,2-dioxide Chemical compound O=S1(=O)OCCO1 ZPFAVCIQZKRBGF-UHFFFAOYSA-N 0.000 claims description 2
- WNXJIVFYUVYPPR-UHFFFAOYSA-N 1,3-dioxolane Chemical compound C1COCO1 WNXJIVFYUVYPPR-UHFFFAOYSA-N 0.000 claims description 2
- 229910015015 LiAsF 6 Inorganic materials 0.000 claims description 2
- 229910013063 LiBF 4 Inorganic materials 0.000 claims description 2
- 229910013188 LiBOB Inorganic materials 0.000 claims description 2
- 229910013684 LiClO 4 Inorganic materials 0.000 claims description 2
- 229910013733 LiCo Inorganic materials 0.000 claims description 2
- 229910012735 LiCo1/3Ni1/3Mn1/3O2 Inorganic materials 0.000 claims description 2
- 229910012851 LiCoO 2 Inorganic materials 0.000 claims description 2
- 229910010707 LiFePO 4 Inorganic materials 0.000 claims description 2
- 229910015645 LiMn Inorganic materials 0.000 claims description 2
- 229910013330 LiNiO2 LiMnO2 Inorganic materials 0.000 claims description 2
- 239000004743 Polypropylene Substances 0.000 claims description 2
- 125000003368 amide group Chemical group 0.000 claims description 2
- 239000000919 ceramic Substances 0.000 claims description 2
- 125000004093 cyano group Chemical group *C#N 0.000 claims description 2
- 239000011152 fibreglass Substances 0.000 claims description 2
- 125000001153 fluoro group Chemical group F* 0.000 claims description 2
- 125000004435 hydrogen atom Chemical group [H]* 0.000 claims description 2
- 239000012528 membrane Substances 0.000 claims description 2
- 239000002931 mesocarbon microbead Substances 0.000 claims description 2
- 229910021382 natural graphite Inorganic materials 0.000 claims description 2
- 229920001155 polypropylene Polymers 0.000 claims description 2
- NVBMUOYFLVUZJU-UHFFFAOYSA-N propane-1,2-diol;sulfurous acid Chemical compound OS(O)=O.CC(O)CO NVBMUOYFLVUZJU-UHFFFAOYSA-N 0.000 claims description 2
- 125000001424 substituent group Chemical group 0.000 claims description 2
- RINCXYDBBGOEEQ-UHFFFAOYSA-N succinic anhydride Chemical compound O=C1CCC(=O)O1 RINCXYDBBGOEEQ-UHFFFAOYSA-N 0.000 claims description 2
- HXJUTPCZVOIRIF-UHFFFAOYSA-N sulfolane Chemical compound O=S1(=O)CCCC1 HXJUTPCZVOIRIF-UHFFFAOYSA-N 0.000 claims description 2
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 abstract description 15
- 239000011889 copper foil Substances 0.000 abstract description 15
- 230000007797 corrosion Effects 0.000 abstract description 10
- 238000005260 corrosion Methods 0.000 abstract description 10
- 229910052782 aluminium Inorganic materials 0.000 abstract description 3
- 239000011888 foil Substances 0.000 abstract description 3
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 abstract description 2
- 238000004519 manufacturing process Methods 0.000 abstract description 2
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 abstract 1
- 239000012964 benzotriazole Substances 0.000 abstract 1
- 230000015572 biosynthetic process Effects 0.000 abstract 1
- 230000000052 comparative effect Effects 0.000 description 27
- 239000005030 aluminium foil Substances 0.000 description 11
- 239000000654 additive Substances 0.000 description 10
- 238000003860 storage Methods 0.000 description 8
- 238000012360 testing method Methods 0.000 description 7
- 230000000996 additive effect Effects 0.000 description 6
- NIPNSKYNPDTRPC-UHFFFAOYSA-N N-[2-oxo-2-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)ethyl]-2-[[3-(trifluoromethoxy)phenyl]methylamino]pyrimidine-5-carboxamide Chemical compound O=C(CNC(=O)C=1C=NC(=NC=1)NCC1=CC(=CC=C1)OC(F)(F)F)N1CC2=C(CC1)NN=N2 NIPNSKYNPDTRPC-UHFFFAOYSA-N 0.000 description 3
- 230000008859 change Effects 0.000 description 3
- 150000005676 cyclic carbonates Chemical class 0.000 description 3
- 239000007789 gas Substances 0.000 description 3
- 206010027146 Melanoderma Diseases 0.000 description 2
- 239000000853 adhesive Substances 0.000 description 2
- 230000001070 adhesive effect Effects 0.000 description 2
- 238000006243 chemical reaction Methods 0.000 description 2
- 239000011248 coating agent Substances 0.000 description 2
- 238000000576 coating method Methods 0.000 description 2
- 239000006258 conductive agent Substances 0.000 description 2
- 230000006866 deterioration Effects 0.000 description 2
- 239000008151 electrolyte solution Substances 0.000 description 2
- 238000006056 electrooxidation reaction Methods 0.000 description 2
- 230000014759 maintenance of location Effects 0.000 description 2
- 230000007246 mechanism Effects 0.000 description 2
- 235000011837 pasties Nutrition 0.000 description 2
- MKRBAPNEJMFMHU-UHFFFAOYSA-N 1-benzylpyrrole-2,5-dione Chemical compound O=C1C=CC(=O)N1CC1=CC=CC=C1 MKRBAPNEJMFMHU-UHFFFAOYSA-N 0.000 description 1
- KYEACNNYFNZCST-UHFFFAOYSA-N 1-methylpyrrolidine-2,5-dione Chemical compound CN1C(=O)CCC1=O KYEACNNYFNZCST-UHFFFAOYSA-N 0.000 description 1
- 239000002033 PVDF binder Substances 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 239000011149 active material Substances 0.000 description 1
- 239000003575 carbonaceous material Substances 0.000 description 1
- 150000004649 carbonic acid derivatives Chemical class 0.000 description 1
- 239000004568 cement Substances 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 229910017052 cobalt Inorganic materials 0.000 description 1
- 239000010941 cobalt Substances 0.000 description 1
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 1
- 239000011258 core-shell material Substances 0.000 description 1
- 230000000875 corresponding effect Effects 0.000 description 1
- 238000007599 discharging Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 239000003112 inhibitor Substances 0.000 description 1
- JEIPFZHSYJVQDO-UHFFFAOYSA-N iron(III) oxide Inorganic materials O=[Fe]O[Fe]=O JEIPFZHSYJVQDO-UHFFFAOYSA-N 0.000 description 1
- 150000002576 ketones Chemical class 0.000 description 1
- 238000003475 lamination Methods 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 230000007774 longterm Effects 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- 230000008018 melting Effects 0.000 description 1
- 238000000034 method Methods 0.000 description 1
- 239000012046 mixed solvent Substances 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 238000012856 packing Methods 0.000 description 1
- 239000002985 plastic film Substances 0.000 description 1
- 229920006255 plastic film Polymers 0.000 description 1
- 229920000098 polyolefin Polymers 0.000 description 1
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- KCXFHTAICRTXLI-UHFFFAOYSA-N propane-1-sulfonic acid Chemical compound CCCS(O)(=O)=O KCXFHTAICRTXLI-UHFFFAOYSA-N 0.000 description 1
- 238000012797 qualification Methods 0.000 description 1
- 150000003839 salts Chemical class 0.000 description 1
- 239000011257 shell material Substances 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
Classifications
-
- 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
- Secondary Cells (AREA)
Abstract
The invention relates to an electrolyte containing a benzotriazole compound, and at least one of vinyl ethylene carbonate, vinylene carbonate, cyclic sulfonic acid, cyclic sulfate, cyclic sulfite, cyclic anhydride and cyclic imide and a lithium ion battery using the electrolyte, so as to form a thin and compact passive film on the surfaces of positive and negative active materials of the battery, reduce the gas production of the battery during formation, reduce the corrosion of a current collector copper foil and an aluminum foil, reduce the impedance of the whole battery, and improve the high capacity and the excellent charge/discharge cycle performance of the battery.
Description
Technical field
The present invention relates to comprise a kind of BTA compounds, also contain at least a electrolyte of vinyl ethylene carbonate, vinylene carbonate, ring-type sulfonic acid, cyclic sulfates, cyclic sulfite, cyclic acid anhydride, cyclic imide in addition and use the lithium ion battery of this electrolyte.
Background technology
Begin till now from the commercialization of lithium ion liquid two primary cells of Sony Co., because its high-energy-density, memory-less effect, lithium ion two primary cells have been widely applied in portable computer, the portable phone etc.Twice battery of lithium ion comprises negative pole and positive pole, negative pole generally adopts carbonaceous material as negative active core-shell material, anodal general employing transition metal oxides etc. are as positive electrode active materials, lithium ion two primary cells prepare in the following way: embed porous polyolefin base barrier film between negative pole and positive pole, inject then and contain LiPF
6The nonaqueous electrolytic solution of salt etc.When battery charge,, insert then in the carbon-coating of negative pole the lithium ion release of positive electrode active materials.When battery discharge, opposite reaction takes place, with the lithium ion release of negative pole carbon-coating, insert in the anodal active material then.
Nonaqueous electrolytic solution plays the instrumentality of mobile lithium ion between negative pole and positive pole.Electrolyte should be stablized in the operating voltage range of lithium ion battery, and can move fast enough by lithium ion under the multiplying power discharging condition.As electrolyte, cyclic carbonate has big polarity and the lithium salts that therefore can dissociate, but viscosity is bigger, must be aided with the less solvent of viscosity and comprise dimethyl carbonate, diethyl carbonate, methyl ethyl carbonate, carbonic acid first propyl ester, methyl acetate, methyl propionate, oxolane, methyltetrahydrofuran, glycol dimethyl ether, diethylene glycol dimethyl ether, ethylene glycol diethyl ether, diethylene glycol diethyl ether, butyl cellosolve, dibutyl ethylene glycol ether, trimethyl phosphate, triethyl phosphate, tributyl phosphate, di(2-ethylhexyl)phosphate Methylethyl ester, di(2-ethylhexyl)phosphate methyl-propyl ester, di(2-ethylhexyl)phosphate methyl butyl ester etc.Different cyclic carbonates comprises ethylene carbonate, propylene carbonate ester, butylene, vinylene carbonate, gamma-butyrolacton etc.
The bottleneck that present lithium ion battery is used aspect electrokinetic cell is fail safe and cost, the present invention does not relate to fail safe, with regard to cost, refer to the ratio of performance to price, if the cycle life of lithium ion battery energy long enough, storage life surpass 10 years, the application of lithium ion battery on electric automobile, hybrid-electric car, electric bicycle becomes possibility so.In other words, existing lithium ion battery exactly at useful life, storage life, negative current collector Copper Foil in battery system, the aspects such as corrosion that long-term circulation causes exist not enough.
Summary of the invention
The purpose of this invention is to provide a kind of electrolyte, described electrolyte can improve the mechanism of lithium ion battery when changing into, and shows high power capacity and excellent charge/discharge cycle performance, reduces the corrosion of copper foil of affluxion body, aluminium foil.
Another object of the present invention provides a kind of lithium ion battery that comprises described electrolyte.
For realizing above purpose, electrolyte of the present invention comprises:
Nonaqueous solvents;
Lithium salts;
Functional additive;
Described functional additive comprises:
The BTA compounds of general formula (1) expression and vinyl ethylene carbonate, vinylene carbonate, ring-type sulfonic acid, cyclic sulfates, cyclic sulfite, cyclic acid anhydride, cyclic imide at least a;
R in the formula
1, R
2Can be expressed as hydrogen atom or carbon number independently of one another and be the group such as alkyl, phenyl or benzyl, cyano group, amido, sulfonic group of 1～4 alkyl, perfluoro or part fluoro.
Described lithium salt is the 0.5-2.0 molar concentration, preferred 0.8-1.5 molar concentration; The content of described BTA compounds is the 0.01-5% of electrolyte total weight, preferred 0.2-2%; At least a content of described vinyl ethylene carbonate, vinylene carbonate, ring-type sulfonic acid, cyclic sulfates, cyclic sulfite, cyclic acid anhydride, cyclic imide is 0.1-5%, preferred 0.5-2%.
Generally speaking, EC reaches 39 ℃ as the cyclic carbonate that is used in the battery that adopts the graphitized carbon negative pole because its fusing point is higher than room temperature, so it reduces the cryogenic property of electrolyte fast.For solving this contradiction, generally used to comprise electrolyte components with low melting point and low viscous linear carbonates.Then, because electrolyte can produce gas when battery changes into when being injected into battery, especially for plastic-aluminum flexible packing battery, aluminum-shell battery, electrokinetic cell, has bigger influence, in case gas because battery rises, and cause the increase of the deterioration, particularly battery impedance of battery performance, with the performance of deterioration battery greatly.
Rust inhibitor and corrosion inhibiter that BTA compounds of the present invention is copper foil of affluxion body, aluminium foil, the film forming agent of surface of positive electrode active material cooperates the film forming of at least a material of vinyl ethylene carbonate, vinylene carbonate, ring-type sulfonic acid, cyclic sulfates, cyclic sulfite, cyclic acid anhydride, cyclic imide on the negative electrode active material surface simultaneously.Reach thus on both positive and negative polarity active matter surface and all form the thin and fine and close passivating film of one deck, the gas production of minimizing battery when changing into, the corrosion of minimizing copper foil of affluxion body, aluminium foil.The present invention can reduce the impedance of entire cell in this way, improves the capacity and the excellent charge/discharge cycle performance of battery.
In addition, lithium salts of the present invention provides lithium ion in battery, and can make lithium ion battery can realize basic function, can include but not limited to: LiPF
6, LiBF
4, LiClO
4, LiAsF
6, LiCF
3SO
3, LiN (CF
3SO
2)
2At least a with LiBOB.
Described nonaqueous solvents serves as medium, by this medium the lithium ion that participates in chemical reaction in the battery can be moved, can include but not limited at least two kinds of following material: ethylene carbonate, propylene carbonate ester, butylene, vinylene carbonate, dimethyl carbonate, diethyl carbonate, methyl ethyl carbonate, carbonic acid first propyl ester, gamma-butyrolacton, dioxolane, oxolane, methyltetrahydrofuran, sulfolane, methyl acetate, methyl propionate, glycol dimethyl ether, ethylene glycol diethyl ether, butyl cellosolve, diethylene glycol dimethyl ether, diethylene glycol diethyl ether, dibutyl ethylene glycol ether, trimethyl phosphate, triethyl phosphate, tributyl phosphate, di(2-ethylhexyl)phosphate Methylethyl ester, di(2-ethylhexyl)phosphate methyl-propyl ester, di(2-ethylhexyl)phosphate methyl butyl ester.
Described ring-type sulfonic acid can include but not limited to: 1, and 3-N-morpholinopropanesulfonic acid lactone, 1,4-butyl sultone, 1,3-butyl sultone, 1,3-propene sulfonic acid lactone at least a;
Described cyclic sulfates can include but not limited to: glycol sulfate, propylene glycol sulfuric ester at least a;
Described cyclic sulfite can include but not limited to: glycol sulfite ester, propylene glycol sulfite at least a;
Described cyclic acid anhydride can include but not limited to: succinyl oxide, maleic anhydride, benzo succinyl oxide, 1,4,5,8-naphthalenetetracarbacidic acidic dianhydride, cyclohexane dicarboxylic acid acid anhydride at least a;
Described cyclic imide can include but not limited to: succinimide, maleimide, benzo succinimide, carbon number be can be with the phenyl of different substituents group, benzyl substituted succinimide, maleimide, benzo succinimide on N-alkyl substituted succinimide, maleimide, benzo succinimide and the phenyl ring of 1-4 at least a.
The described lithium ion battery of another purpose of the present invention comprises:
Electrolyte as claimed in claim 1;
Can reversibly store and discharge the graphitized carbon as the negative electrode active material material of lithium ion;
Can reversibly store and discharge the lithium-containing transition metal oxide as the positive electrode active material material of lithium ion;
Place the porous septum between negative pole and the positive pole.
Aforesaid lithium ion battery can form element cell well known by persons skilled in the art, has the double cell of negative pole/dividing plate/positive plate/diaphragm structure, or the lamination battery of the structure repeated several times of element cell wherein
Described graphitized carbon can include but not limited to: regular Delanium, modified natural graphite, wherein said Delanium is preferably: MCMB, MPCF, CMS's is wherein a kind of.
Described lithium-containing transition metal oxide can include but not limited to: LiCoO
2, LiNiO
2LiMnO
2, LiMn
2O
4, LiFePO
4, LiCo
xNi
1-xO
2, LiCo
1/3Ni
1/3Mn
1/3O
2Wherein a kind of.
Described porous septum can include but not limited to: polyethylene film, polypropylene film, polyethylene and polyacrylic composite membrane, paper barrier film, fibreglass diaphragm, ceramic diaphragm wherein a kind of.
In sum, the present invention uses the functional additive BTA compounds by general formula (1) expression, the lithium ion battery that also has at least a electrolyte preparation of vinyl ethylene carbonate, vinylene carbonate, ring-type sulfonic acid, cyclic sulfates, cyclic sulfite, cyclic acid anhydride, cyclic imide in addition, can make the mechanism of electrolyte improvement when battery changes into, reduce discharge quantity, improve the storage life of battery, and show high power capacity and excellent charge/discharge cycle performance.
Embodiment
Below by suitable embodiment the present invention is described, but the present invention is not subjected to any qualification of these embodiment, in the scope that does not change principal character of the present invention, can carries out suitable change and implement.
In embodiment 1-12 and comparative example 1-3, the lithium ion battery of assembling adopts: positive pole is made as follows, active matter cobalt acid lithium 90%, adhesive PVDF 5%, conductive agent 5% is modulated into pasty state with N-crassitude ketone solvent, be coated in then on the aluminium foil that thickness is 25 μ m, the press roll-in of 10kg is adopted in dry back, and the thickness that makes pole piece is 110 μ m, and surface density is 0.9mAh/cm
2Negative pole is made as follows, active matter CMS93%, adhesive water-base cement 3%, conductive agent 4% is modulated into pasty state in the water, be coated in then on the Copper Foil that thickness is 18 μ m, the press roll-in of 10kg is adopted in dry back, and the thickness that makes pole piece is 105 μ m, and surface density is 0.9mAh/cm
2Barrier film adopts three layers of composite porous film; It is EC/DMC/EMC=1/1/1 that electrolyte adopts mass ratio, LiPF
6Be 1.0M.
Adopt above-mentioned material, make the test cell of embodiment 1-12 and comparative example 1-3, battery is the aluminum plastic film flexible package, and the battery nominal capacity is 500mAh.
Add BTA (BTA) 1% (percentage by weight) and vinylene carbonate (VC) 1% (percentage by weight) in embodiment one, the electrolyte.
Add BTA (BTA) 1% (percentage by weight) and vinyl ethylene carbonate (VEC) 1% (percentage by weight) in embodiment two, the electrolyte.
Add BTA (BTA) 1% (percentage by weight) and glycol sulfite ester (ES) 1% (percentage by weight) in embodiment three, the electrolyte.
Add BTA (BTA) 1% (percentage by weight) and maleic anhydride 1% (percentage by weight) in embodiment four, the electrolyte.
Add BTA (BTA) 1% (percentage by weight) and 1,4,5 in embodiment five, the electrolyte, 8-naphthalenetetracarbacidic acidic dianhydride 1% (percentage by weight).
Add BTA (BTA) 1% (percentage by weight) and succinimide 1% (percentage by weight) in embodiment six, the electrolyte.
Add BTA (BTA) 1% (percentage by weight) and N methyl succinimide 1% (percentage by weight) in embodiment seven, the electrolyte.
Add BTA (BTA) 1% (percentage by weight) and N-benzyl maleimide 1% (percentage by weight) in embodiment eight, the electrolyte.
Add BTA (BTA) 1% (percentage by weight) in embodiment nine, the electrolyte, vinylene carbonate (VC) 0.5% (percentage by weight) and vinyl ethylene carbonate (VEC) 0.5% (percentage by weight).
Add BTA (BTA) 1% (percentage by weight) in embodiment ten, the electrolyte, vinylene carbonate (VC) 1% (percentage by weight) and vinyl ethylene carbonate (VEC) 1% (percentage by weight).
Add BTA (BTA) 1% (percentage by weight) in embodiment 11, the electrolyte, vinylene carbonate (VC) 1% (percentage by weight) and glycol sulfite ester (ES) 1% (percentage by weight).
Add BTA (BTA) 1% (percentage by weight) in embodiment 12, the electrolyte, vinylene carbonate (VC) 1% (percentage by weight) and succinimide 1% (percentage by weight).
Comparative example one, do not add any additives.
Add vinylene carbonate (VC) 1% (percentage by weight) in comparative example two, the electrolyte.
Comparative example three, glycol sulfite ester (ES) 1% (percentage by weight).
Embodiment 1-12 and the comparative example 1-3 lithium ion battery made for said method, change in room temperature and promptly carry out under 25 ℃ of conditions, adopt 0.1C head to be charged to 4.2V, 0.2C head is put into 2.7V, (be charged to 4.2V 0.2C circulate for the second time and for the third time, discharge into 3V) finish, investigate the chemistry of cycle performance (capacity), storage life (70 ℃ of high-temperature storage), Copper Foil of battery and electrochemical corrosion situation etc. then.
Be the measurement result table below:
Table one, cycle performance of battery test (1C100%DOD):
| Additive capacity % | First run capacity mAh | The 500th circulation time capacity/mAh | The 1500th circulation time capacity/mAh | ||
| BTA | Other | ||||
| Embodiment one | 1 | 1 | 500.1 | 450.3 | 401.1 |
| Embodiment two | 1 | 1 | 500.5 | 455.2 | 408.4 |
| Embodiment three | 1 | 1 | 501.2 | 449.7 | 405.7 |
| Embodiment four | 1 | 1 | 501.5 | 453.2 | 402.2 |
| Embodiment five | 1 | 1 | 500.7 | 456.3 | 389.6 |
| Embodiment six | 1 | 1 | 502.0 | 452.8 | 399.8 |
| Embodiment seven | 1 | 1 | 500.6 | 458.1 | 388.6 |
| Embodiment eight | 1 | 1 | 500.7 | 453.6 | 395.7 |
| Embodiment nine | 1 | 0.5+0.5 | 500.0 | 449.9 | 405.9 |
| Embodiment ten | 1 | 1+1 | 502.5 | 459.7 | 411.8 |
| Embodiment 11 | 1 | 1+1 | 500.9 | 458.6 | 409.3 |
| Embodiment 12 | 1 | 1+1 | 500.7 | 456.8 | 410.2 |
| Comparative example one | 0 | 0 | 500.8 | 351.3 | -- |
| Comparative example two | 0 | 1 | 500.1 | 403.5 | -- |
| Comparative example three | 0 | 1 | 500.6 | 400.9 | -- |
As can be seen from Table I, do not add comparative example one battery of any additives in electrolyte, it the 500th takes turns 70.15% of wheel capacity headed by the circulation, and battery can't be recycled to 1500 at all and take turns circulation; Add comparative example two batteries of vinylene carbonate (VC) 1% (percentage by weight) in electrolyte, it the 500th takes turns 80.68% of wheel capacity headed by the circulation, and battery also can't be recycled to 1500 and take turns circulation, but slightly stronger than comparative example one; Comparative example three is similar to comparative example two.For the test cell of embodiment 1-12, the 500th takes turns the circulation time capacity about 90%, and the 1500th takes turns the circulation time capacity about 80%, and different additive difference is less.
Table two, battery storage life test
| Additive capacity % | First run capacity mAh | 70 ℃ store a month capacity mAh | 70 ℃ store 1 year capacity mAh | ||
| BTA | Other | ||||
| Embodiment one | 1 | 1 | 500.3 | 495 | 445 |
| Embodiment two | 1 | 1 | 500.1 | 493 | 449 |
| Embodiment three | 1 | 1 | 501.2 | 494 | 441 |
| Embodiment four | 1 | 1 | 501.5 | 496 | 440 |
| Embodiment five | 1 | 1 | 500.5 | 493 | 451 |
| Embodiment six | 1 | 1 | 502.0 | 492 | 453 |
| Embodiment seven | 1 | 1 | 500.9 | 496 | 449 |
| Embodiment eight | 1 | 1 | 500.7 | 493 | 449 |
| Embodiment nine | 1 | 0.5+0.5 | 500.5 | 496 | 443 |
| Embodiment ten | 1 | 1+1 | 502.3 | 497 | 452 |
| Embodiment 11 | 1 | 1+1 | 500.6 | 493 | 450 |
| Embodiment 12 | 1 | 1+1 | 500.7 | 495 | 452 |
| Comparative example one | 0 | 0 | 500.8 | 415 | 150 |
| Comparative example two | 0 | 1 | 501.3 | 428 | 163 |
| Comparative example three | 0 | 1 | 500.6 | 430 | 171 |
As can be seen from Table I, do not add comparative example one battery of any additives in electrolyte, its 70 ℃ store one month, capacity attenuation 17.2%; 70 ℃ store 1 year, capacity attenuation 70%; Comparative example two and comparative example three batteries are compared with comparative example one battery and to be omited, and its 70 ℃ store month capacity and 70 ℃ and store 1 year capacity and all slightly improve; For the test cell of embodiment 1-12, a month capacity of its 70 ℃ storages and 1 year capacity of 70 ℃ of storages all are significantly increased, and different additive difference is less.
The chemistry of table three, Copper Foil, aluminium foil and electrochemical corrosion test
| Additive capacity % | Copper Foil, aluminium foil initial condition | The 500th circulation time Copper Foil, aluminium foil | The 1500th circulation time Copper Foil, aluminium foil | ||
| BTA | Other | ||||
| Embodiment one | 1 | 1 | Light | No any unusual, light as new | Almost not corrosion |
| Embodiment two | 1 | 1 | Light | ||
| Embodiment three | 1 | 1 | Light | ||
| Embodiment four | 1 | 1 | Light | ||
| Embodiment five | 1 | 1 | Light | ||
| Embodiment six | 1 | 1 | Light | ||
| Embodiment seven | 1 | 1 | Light | ||
| Embodiment eight | 1 | 1 | Light | ||
| Embodiment nine | 1 | 0.5+0.5 | Light | ||
| Embodiment ten | 1 | 1+1 | Light | ||
| Embodiment 11 | 1 | 1+1 | Light | ||
| Embodiment 12 | 1 | 1+1 | Light | ||
| Comparative example one | 0 | 0 | Light | Slight corrosion is arranged, have a spot of stain to occur | Seriously corroded, a large amount of blackspots are arranged, become discontinuous paillon foil |
| Comparative example two | 0 | 1 | Light | ||
| Comparative example three | 0 | 1 | Light |
As can be seen from Table I, in electrolyte, do not add comparative example one, comparative example two and comparative example three batteries of BTA, the 500th circulation time, slight corrosion is arranged on the Copper Foil as collector, there is a spot of stain to occur, and serious at the 1500th circulation time Copper Foil, aluminium foil corrosion, a large amount of blackspots are arranged, become discontinuous paillon foil.And for the test cell of embodiment 1-12, it is any unusual that 500 circulation time Copper Foils, aluminium foil do not have, light as new; 1500 circulation time Copper Foils, aluminium foil be not corrosion almost.
Should illustrate that electrolyte adopts different additives ratio, adopts the mixing of above-mentioned described additive; Do not use above-mentioned mixed solvent (mass ratio is EC/DMC/EMC=1/1/1), but adopt other solvent of mentioning among the present invention; Lithium salts LiPF
6Concentration in the 0.5-2.0 molar concentration, perhaps adopt other lithium salts of mentioning among the present invention, also can obtain corresponding effects.
Claims (15)
1, a kind of electrolyte, it comprises:
Nonaqueous solvents;
Lithium salts;
Functional additive;
Described functional additive comprises:
The BTA compounds of general formula (1) expression and vinyl ethylene carbonate, vinylene carbonate, ring-type sulfonic acid, cyclic sulfates, cyclic sulfite, cyclic acid anhydride, cyclic imide at least a;
R1, R2 can be expressed as groups such as alkyl, phenyl or benzyl that hydrogen atom or carbon number are alkyl, perfluoro or the part fluoro of 1-4, cyano group, amido, sulfonic group independently of one another in the formula.
2, electrolyte as claimed in claim 1, wherein said lithium salt are the 0.5-2.0 molar concentration; The content of described BTA compounds is the 0.01-5% of electrolyte total weight; At least a content of described vinyl ethylene carbonate, vinylene carbonate, ring-type sulfonic acid, cyclic sulfates, cyclic sulfite, cyclic acid anhydride, cyclic imide is 0.1-5%.
3, electrolyte as claimed in claim 2, wherein said lithium salt are the 0.8-1.5 molar concentration; The content of described BTA compounds is the 0.2-2% of electrolyte total weight; At least a content of described vinyl ethylene carbonate, vinylene carbonate, ring-type sulfonic acid, cyclic sulfates, cyclic sulfite, cyclic acid anhydride, cyclic imide is 0.5-2%.
4, electrolyte as claimed in claim 1, wherein said lithium salts is selected from LiPF
6, LiBF
4, LiClO
4, LiAsF
6, LiCF
3SO
3, LiN (CF
3SO
2)
2At least a with LiBOB.
5, electrolyte as claimed in claim 1, wherein said nonaqueous solvents are to be selected from least two kinds of following material: ethylene carbonate, propylene carbonate ester, butylene, vinylene carbonate, dimethyl carbonate, diethyl carbonate, methyl ethyl carbonate, carbonic acid first propyl ester, gamma-butyrolacton, dioxolane, oxolane, methyltetrahydrofuran, sulfolane, methyl acetate, methyl propionate, glycol dimethyl ether, ethylene glycol diethyl ether, butyl cellosolve, diethylene glycol dimethyl ether, diethylene glycol diethyl ether, dibutyl ethylene glycol ether, trimethyl phosphate, triethyl phosphate, tributyl phosphate, di(2-ethylhexyl)phosphate Methylethyl ester, di(2-ethylhexyl)phosphate methyl-propyl ester, di(2-ethylhexyl)phosphate methyl butyl ester.
6, as claim 1 or 2 or 3 described electrolyte, wherein said ring-type sulfonic acid is for being selected from 1,3-N-morpholinopropanesulfonic acid lactone, 1,4-butyl sultone, 1,3-butyl sultone, 1,3-propene sulfonic acid lactone at least a.
7, as claim 1 or 2 or 3 described electrolyte, wherein said cyclic sulfates is selected from least a of glycol sulfate, propylene glycol sulfuric ester.
8, as claim 1 or 2 or 3 described electrolyte, wherein said cyclic sulfite is be selected from glycol sulfite ester, propylene glycol sulfite at least a.
9, as claim 1 or 2 or 3 described electrolyte, wherein said cyclic acid anhydride is for being selected from succinyl oxide, maleic anhydride, benzo succinyl oxide, 1,4,5,8-naphthalenetetracarbacidic acidic dianhydride, cyclohexane dicarboxylic acid acid anhydride at least a.
10, as claim 1 or 2 or 3 described electrolyte, wherein said cyclic imide be selected from N-alkyl substituted succinimide, maleimide, benzo succinimide and the phenyl ring that succinimide, maleimide, benzo succinimide, carbon number are 1-4 can be with the phenyl of different substituents group, benzyl substituted succinimide, maleimide, benzo succinimide at least a.
11, a kind of lithium ion battery, it comprises:
Electrolyte as claimed in claim 1;
Can reversibly store and discharge the graphitized carbon as the negative electrode active material material of lithium ion;
Can reversibly store and discharge the lithium-containing transition metal oxide as the positive electrode active material material of lithium ion;
Place the porous septum between positive pole and the negative pole.
12, lithium ion battery as claimed in claim 11, wherein said graphitized carbon is for to be selected from: regular Delanium, modified natural graphite.
13, lithium ion battery as claimed in claim 12, wherein said Delanium is for to be selected from: MCMB, MPCF, CMS's is wherein a kind of.
14, lithium ion battery as claimed in claim 11, wherein said lithium-containing transition metal oxide is for being selected from: LiCoO
2, LiNiO
2LiMnO
2, LiMn
2O
4, LiFePO
4, LiCo
xNi
4-xO
2, LiCo
1/3Ni
1/3Mn
1/3O
2Wherein a kind of.
15, lithium ion battery as claimed in claim 11, wherein said porous septum is for being selected from: polyethylene film, polypropylene film, polyethylene and polyacrylic composite membrane, paper barrier film, fibreglass diaphragm, ceramic diaphragm wherein a kind of.
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| CNA2006100496873A CN1819324A (en) | 2006-03-03 | 2006-03-03 | Electrolyte and lithium ion battery using same |
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CNA2006100496873A CN1819324A (en) | 2006-03-03 | 2006-03-03 | Electrolyte and lithium ion battery using same |
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