TWI395361B - Nonaqueous electrolytes, batteries and electrochemical capacitors - Google Patents
Nonaqueous electrolytes, batteries and electrochemical capacitors Download PDFInfo
- Publication number
- TWI395361B TWI395361B TW095130822A TW95130822A TWI395361B TW I395361 B TWI395361 B TW I395361B TW 095130822 A TW095130822 A TW 095130822A TW 95130822 A TW95130822 A TW 95130822A TW I395361 B TWI395361 B TW I395361B
- Authority
- TW
- Taiwan
- Prior art keywords
- group
- carbonate
- modified
- aqueous electrolyte
- decane
- Prior art date
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- 239000011255 nonaqueous electrolyte Substances 0.000 title claims description 26
- 239000003990 capacitor Substances 0.000 title claims description 14
- DIOQZVSQGTUSAI-NJFSPNSNSA-N decane Chemical class CCCCCCCCC[14CH3] DIOQZVSQGTUSAI-NJFSPNSNSA-N 0.000 claims description 25
- 239000003792 electrolyte Substances 0.000 claims description 20
- 239000008151 electrolyte solution Substances 0.000 claims description 16
- 125000000217 alkyl group Chemical group 0.000 claims description 14
- 229910052744 lithium Inorganic materials 0.000 claims description 14
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims description 13
- 239000000203 mixture Substances 0.000 claims description 12
- 125000004432 carbon atom Chemical group C* 0.000 claims description 11
- 150000003839 salts Chemical class 0.000 claims description 10
- 125000003118 aryl group Chemical group 0.000 claims description 8
- 125000005587 carbonate group Chemical group 0.000 claims description 8
- 125000003710 aryl alkyl group Chemical group 0.000 claims description 7
- 125000005843 halogen group Chemical group 0.000 claims description 7
- 150000002924 oxiranes Chemical class 0.000 claims description 7
- 125000003277 amino group Chemical group 0.000 claims description 4
- 229910052731 fluorine Chemical group 0.000 claims description 4
- KPUWHANPEXNPJT-UHFFFAOYSA-N disiloxane Chemical class [SiH3]O[SiH3] KPUWHANPEXNPJT-UHFFFAOYSA-N 0.000 claims description 3
- 239000007788 liquid Substances 0.000 claims description 3
- 229910003002 lithium salt Inorganic materials 0.000 claims description 3
- 159000000002 lithium salts Chemical group 0.000 claims description 3
- 239000011737 fluorine Chemical group 0.000 claims description 2
- 239000007864 aqueous solution Substances 0.000 claims 1
- BVKZGUZCCUSVTD-UHFFFAOYSA-N carbonic acid Chemical compound OC(O)=O BVKZGUZCCUSVTD-UHFFFAOYSA-N 0.000 claims 1
- 238000005868 electrolysis reaction Methods 0.000 claims 1
- 229910052736 halogen Inorganic materials 0.000 claims 1
- 150000002367 halogens Chemical class 0.000 claims 1
- DIOQZVSQGTUSAI-UHFFFAOYSA-N decane Chemical compound CCCCCCCCCC DIOQZVSQGTUSAI-UHFFFAOYSA-N 0.000 description 31
- -1 3-aminopropyl group Chemical group 0.000 description 22
- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 description 21
- 239000002904 solvent Substances 0.000 description 14
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 13
- 150000001875 compounds Chemical class 0.000 description 11
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 10
- 229910052799 carbon Inorganic materials 0.000 description 9
- 229910052751 metal Inorganic materials 0.000 description 9
- 239000010410 layer Substances 0.000 description 8
- 229910001416 lithium ion Inorganic materials 0.000 description 8
- 239000002184 metal Substances 0.000 description 8
- VLKZOEOYAKHREP-UHFFFAOYSA-N n-Hexane Chemical compound CCCCCC VLKZOEOYAKHREP-UHFFFAOYSA-N 0.000 description 8
- 150000002923 oximes Chemical class 0.000 description 8
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 7
- 238000007259 addition reaction Methods 0.000 description 7
- 239000002131 composite material Substances 0.000 description 7
- RTZKZFJDLAIYFH-UHFFFAOYSA-N Diethyl ether Chemical compound CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 description 6
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 6
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 6
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 description 6
- 229910045601 alloy Inorganic materials 0.000 description 6
- 239000000956 alloy Substances 0.000 description 6
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- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 5
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- 239000010949 copper Substances 0.000 description 5
- 230000000694 effects Effects 0.000 description 5
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- 238000010992 reflux Methods 0.000 description 5
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- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 description 4
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 description 4
- IAYPIBMASNFSPL-UHFFFAOYSA-N Ethylene oxide Chemical compound C1CO1 IAYPIBMASNFSPL-UHFFFAOYSA-N 0.000 description 4
- WYURNTSHIVDZCO-UHFFFAOYSA-N Tetrahydrofuran Chemical compound C1CCOC1 WYURNTSHIVDZCO-UHFFFAOYSA-N 0.000 description 4
- 239000002253 acid Substances 0.000 description 4
- 125000003545 alkoxy group Chemical group 0.000 description 4
- 229910052782 aluminium Inorganic materials 0.000 description 4
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 4
- 238000006243 chemical reaction Methods 0.000 description 4
- 239000006258 conductive agent Substances 0.000 description 4
- 229910052802 copper Inorganic materials 0.000 description 4
- 125000001495 ethyl group Chemical group [H]C([H])([H])C([H])([H])* 0.000 description 4
- 239000007789 gas Substances 0.000 description 4
- 229910052752 metalloid Inorganic materials 0.000 description 4
- 238000000034 method Methods 0.000 description 4
- 125000002496 methyl group Chemical group [H]C([H])([H])* 0.000 description 4
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 4
- 239000000243 solution Substances 0.000 description 4
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- 239000010935 stainless steel Substances 0.000 description 4
- 238000003756 stirring Methods 0.000 description 4
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- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 description 3
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- 125000004104 aryloxy group Chemical group 0.000 description 3
- 229910017052 cobalt Inorganic materials 0.000 description 3
- 239000010941 cobalt Substances 0.000 description 3
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 3
- 230000000052 comparative effect Effects 0.000 description 3
- 238000004821 distillation Methods 0.000 description 3
- RIFGWPKJUGCATF-UHFFFAOYSA-N ethyl chloroformate Chemical compound CCOC(Cl)=O RIFGWPKJUGCATF-UHFFFAOYSA-N 0.000 description 3
- 125000004435 hydrogen atom Chemical group [H]* 0.000 description 3
- RAXXELZNTBOGNW-UHFFFAOYSA-N imidazole Natural products C1=CNC=N1 RAXXELZNTBOGNW-UHFFFAOYSA-N 0.000 description 3
- 150000002500 ions Chemical class 0.000 description 3
- 230000014759 maintenance of location Effects 0.000 description 3
- 239000007773 negative electrode material Substances 0.000 description 3
- 239000007774 positive electrode material Substances 0.000 description 3
- 238000011084 recovery Methods 0.000 description 3
- YEJRWHAVMIAJKC-UHFFFAOYSA-N 4-Butyrolactone Chemical compound O=C1CCCO1 YEJRWHAVMIAJKC-UHFFFAOYSA-N 0.000 description 2
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 description 2
- COQYUAJAXLUAHF-UHFFFAOYSA-N CC(CCCCCCCCCOC)(C)C Chemical compound CC(CCCCCCCCCOC)(C)C COQYUAJAXLUAHF-UHFFFAOYSA-N 0.000 description 2
- 239000004215 Carbon black (E152) Substances 0.000 description 2
- XDTMQSROBMDMFD-UHFFFAOYSA-N Cyclohexane Chemical compound C1CCCCC1 XDTMQSROBMDMFD-UHFFFAOYSA-N 0.000 description 2
- XTHFKEDIFFGKHM-UHFFFAOYSA-N Dimethoxyethane Chemical compound COCCOC XTHFKEDIFFGKHM-UHFFFAOYSA-N 0.000 description 2
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 description 2
- QIGBRXMKCJKVMJ-UHFFFAOYSA-N Hydroquinone Chemical compound OC1=CC=C(O)C=C1 QIGBRXMKCJKVMJ-UHFFFAOYSA-N 0.000 description 2
- 229910012851 LiCoO 2 Inorganic materials 0.000 description 2
- AFVFQIVMOAPDHO-UHFFFAOYSA-N Methanesulfonic acid Chemical compound CS(O)(=O)=O AFVFQIVMOAPDHO-UHFFFAOYSA-N 0.000 description 2
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- 229910003617 SiB Inorganic materials 0.000 description 2
- PMZURENOXWZQFD-UHFFFAOYSA-L Sodium Sulfate Chemical compound [Na+].[Na+].[O-]S([O-])(=O)=O PMZURENOXWZQFD-UHFFFAOYSA-L 0.000 description 2
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- 239000006230 acetylene black Substances 0.000 description 2
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- HSFWRNGVRCDJHI-UHFFFAOYSA-N alpha-acetylene Natural products C#C HSFWRNGVRCDJHI-UHFFFAOYSA-N 0.000 description 2
- RDOXTESZEPMUJZ-UHFFFAOYSA-N anisole Chemical compound COC1=CC=CC=C1 RDOXTESZEPMUJZ-UHFFFAOYSA-N 0.000 description 2
- 229910052787 antimony Inorganic materials 0.000 description 2
- WATWJIUSRGPENY-UHFFFAOYSA-N antimony atom Chemical compound [Sb] WATWJIUSRGPENY-UHFFFAOYSA-N 0.000 description 2
- PACOTQGTEZMTOT-UHFFFAOYSA-N bis(ethenyl) carbonate Chemical compound C=COC(=O)OC=C PACOTQGTEZMTOT-UHFFFAOYSA-N 0.000 description 2
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- KYGISWNEHOVNRN-UHFFFAOYSA-N decane Polymers CCCCCCCCCC.CCCCCCCCCC.CCCCCCCCCC.CCCCCCCCCC KYGISWNEHOVNRN-UHFFFAOYSA-N 0.000 description 2
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- 229910052783 alkali metal Inorganic materials 0.000 description 1
- 229910052784 alkaline earth metal Inorganic materials 0.000 description 1
- AZDRQVAHHNSJOQ-UHFFFAOYSA-N alumane Chemical class [AlH3] AZDRQVAHHNSJOQ-UHFFFAOYSA-N 0.000 description 1
- 150000001450 anions Chemical class 0.000 description 1
- 239000012300 argon atmosphere Substances 0.000 description 1
- 150000004945 aromatic hydrocarbons Chemical class 0.000 description 1
- 229910052785 arsenic Inorganic materials 0.000 description 1
- RQNWIZPPADIBDY-UHFFFAOYSA-N arsenic atom Chemical compound [As] RQNWIZPPADIBDY-UHFFFAOYSA-N 0.000 description 1
- 229910021383 artificial graphite Inorganic materials 0.000 description 1
- 239000012298 atmosphere Substances 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 229910052788 barium Inorganic materials 0.000 description 1
- DSAJWYNOEDNPEQ-UHFFFAOYSA-N barium atom Chemical compound [Ba] DSAJWYNOEDNPEQ-UHFFFAOYSA-N 0.000 description 1
- RFRXIWQYSOIBDI-UHFFFAOYSA-N benzarone Chemical compound CCC=1OC2=CC=CC=C2C=1C(=O)C1=CC=C(O)C=C1 RFRXIWQYSOIBDI-UHFFFAOYSA-N 0.000 description 1
- 125000001797 benzyl group Chemical group [H]C1=C([H])C([H])=C(C([H])=C1[H])C([H])([H])* 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 239000004305 biphenyl Substances 0.000 description 1
- 235000010290 biphenyl Nutrition 0.000 description 1
- 238000009835 boiling Methods 0.000 description 1
- 229910052796 boron Inorganic materials 0.000 description 1
- YRAZAPPRLGWDNZ-UHFFFAOYSA-N but-1-ene;carbonic acid Chemical compound CCC=C.OC(O)=O YRAZAPPRLGWDNZ-UHFFFAOYSA-N 0.000 description 1
- 125000000484 butyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])C([H])([H])[H] 0.000 description 1
- 229910052793 cadmium Inorganic materials 0.000 description 1
- BDOSMKKIYDKNTQ-UHFFFAOYSA-N cadmium atom Chemical compound [Cd] BDOSMKKIYDKNTQ-UHFFFAOYSA-N 0.000 description 1
- TVFDJXOCXUVLDH-UHFFFAOYSA-N caesium atom Chemical group [Cs] TVFDJXOCXUVLDH-UHFFFAOYSA-N 0.000 description 1
- WUKWITHWXAAZEY-UHFFFAOYSA-L calcium difluoride Chemical compound [F-].[F-].[Ca+2] WUKWITHWXAAZEY-UHFFFAOYSA-L 0.000 description 1
- CREMABGTGYGIQB-UHFFFAOYSA-N carbon carbon Chemical compound C.C CREMABGTGYGIQB-UHFFFAOYSA-N 0.000 description 1
- 235000011089 carbon dioxide Nutrition 0.000 description 1
- 239000004917 carbon fiber Substances 0.000 description 1
- 150000004649 carbonic acid derivatives Chemical class 0.000 description 1
- SIXOAUAWLZKQKX-UHFFFAOYSA-N carbonic acid;prop-1-ene Chemical compound CC=C.OC(O)=O SIXOAUAWLZKQKX-UHFFFAOYSA-N 0.000 description 1
- 125000003178 carboxy group Chemical group [H]OC(*)=O 0.000 description 1
- 150000001768 cations Chemical class 0.000 description 1
- 239000000919 ceramic Substances 0.000 description 1
- ZMIGMASIKSOYAM-UHFFFAOYSA-N cerium Chemical compound [Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce] ZMIGMASIKSOYAM-UHFFFAOYSA-N 0.000 description 1
- 239000003610 charcoal Substances 0.000 description 1
- 229910052804 chromium Inorganic materials 0.000 description 1
- 239000011651 chromium Substances 0.000 description 1
- 239000003426 co-catalyst Substances 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- 239000011889 copper foil Substances 0.000 description 1
- 125000004122 cyclic group Chemical group 0.000 description 1
- MWKFXSUHUHTGQN-UHFFFAOYSA-N decan-1-ol Chemical group CCCCCCCCCCO MWKFXSUHUHTGQN-UHFFFAOYSA-N 0.000 description 1
- 238000000354 decomposition reaction Methods 0.000 description 1
- 230000007423 decrease Effects 0.000 description 1
- 125000002704 decyl group Chemical group [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])* 0.000 description 1
- 230000018044 dehydration Effects 0.000 description 1
- 238000006297 dehydration reaction Methods 0.000 description 1
- 238000007033 dehydrochlorination reaction Methods 0.000 description 1
- VUPKGFBOKBGHFZ-UHFFFAOYSA-N dipropyl carbonate Chemical compound CCCOC(=O)OCCC VUPKGFBOKBGHFZ-UHFFFAOYSA-N 0.000 description 1
- 230000005611 electricity Effects 0.000 description 1
- 150000002148 esters Chemical class 0.000 description 1
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 description 1
- 230000005496 eutectics Effects 0.000 description 1
- 239000003925 fat Substances 0.000 description 1
- 239000010436 fluorite Substances 0.000 description 1
- 239000011888 foil Substances 0.000 description 1
- 229910052733 gallium Inorganic materials 0.000 description 1
- 239000011245 gel electrolyte Substances 0.000 description 1
- 229910052732 germanium Inorganic materials 0.000 description 1
- GNPVGFCGXDBREM-UHFFFAOYSA-N germanium atom Chemical compound [Ge] GNPVGFCGXDBREM-UHFFFAOYSA-N 0.000 description 1
- 210000004907 gland Anatomy 0.000 description 1
- 239000003365 glass fiber Substances 0.000 description 1
- 229910021397 glassy carbon 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
- 150000008282 halocarbons Chemical class 0.000 description 1
- 125000003187 heptyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])[H] 0.000 description 1
- 125000004051 hexyl group Chemical group [H]C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])* 0.000 description 1
- 150000002430 hydrocarbons Chemical class 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 230000007062 hydrolysis Effects 0.000 description 1
- 238000006460 hydrolysis reaction Methods 0.000 description 1
- 230000003301 hydrolyzing effect Effects 0.000 description 1
- 229910052738 indium Inorganic materials 0.000 description 1
- APFVFJFRJDLVQX-UHFFFAOYSA-N indium atom Chemical compound [In] APFVFJFRJDLVQX-UHFFFAOYSA-N 0.000 description 1
- 238000009413 insulation Methods 0.000 description 1
- 229910000765 intermetallic Inorganic materials 0.000 description 1
- 229920003049 isoprene rubber Polymers 0.000 description 1
- 125000003253 isopropoxy group Chemical group [H]C([H])([H])C([H])(O*)C([H])([H])[H] 0.000 description 1
- 229910052746 lanthanum Inorganic materials 0.000 description 1
- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 description 1
- 229910052749 magnesium Inorganic materials 0.000 description 1
- 159000000003 magnesium salts Chemical class 0.000 description 1
- 239000011572 manganese Substances 0.000 description 1
- 150000002697 manganese compounds Chemical class 0.000 description 1
- WPBNNNQJVZRUHP-UHFFFAOYSA-L manganese(2+);methyl n-[[2-(methoxycarbonylcarbamothioylamino)phenyl]carbamothioyl]carbamate;n-[2-(sulfidocarbothioylamino)ethyl]carbamodithioate Chemical compound [Mn+2].[S-]C(=S)NCCNC([S-])=S.COC(=O)NC(=S)NC1=CC=CC=C1NC(=S)NC(=O)OC WPBNNNQJVZRUHP-UHFFFAOYSA-L 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- 230000008018 melting Effects 0.000 description 1
- 239000002905 metal composite material Substances 0.000 description 1
- 239000007769 metal material Substances 0.000 description 1
- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 229910052976 metal sulfide Inorganic materials 0.000 description 1
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 1
- 229940098779 methanesulfonic acid Drugs 0.000 description 1
- 125000000956 methoxy group Chemical group [H]C([H])([H])O* 0.000 description 1
- UZKWTJUDCOPSNM-UHFFFAOYSA-N methoxybenzene Substances CCCCOC=C UZKWTJUDCOPSNM-UHFFFAOYSA-N 0.000 description 1
- ARYZCSRUUPFYMY-UHFFFAOYSA-N methoxysilane Chemical class CO[SiH3] ARYZCSRUUPFYMY-UHFFFAOYSA-N 0.000 description 1
- KKQAVHGECIBFRQ-UHFFFAOYSA-N methyl propyl carbonate Chemical compound CCCOC(=O)OC KKQAVHGECIBFRQ-UHFFFAOYSA-N 0.000 description 1
- 229910021382 natural graphite Inorganic materials 0.000 description 1
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen group Chemical group [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 description 1
- 239000004745 nonwoven fabric Substances 0.000 description 1
- 125000002347 octyl group Chemical group [H]C([*])([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
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- UJMWVICAENGCRF-UHFFFAOYSA-N oxygen difluoride Chemical group FOF UJMWVICAENGCRF-UHFFFAOYSA-N 0.000 description 1
- 239000003002 pH adjusting agent Substances 0.000 description 1
- 125000001147 pentyl group Chemical group C(CCCC)* 0.000 description 1
- 239000002006 petroleum coke Substances 0.000 description 1
- 239000011334 petroleum pitch coke Substances 0.000 description 1
- 239000005011 phenolic resin Substances 0.000 description 1
- 125000000951 phenoxy group Chemical group [H]C1=C([H])C([H])=C(O*)C([H])=C1[H] 0.000 description 1
- 125000001997 phenyl group Chemical group [H]C1=C([H])C([H])=C(*)C([H])=C1[H] 0.000 description 1
- 229920000767 polyaniline Polymers 0.000 description 1
- 229920002857 polybutadiene Polymers 0.000 description 1
- 229920000573 polyethylene Polymers 0.000 description 1
- 229920000642 polymer Polymers 0.000 description 1
- 229920000098 polyolefin Polymers 0.000 description 1
- 229920001155 polypropylene Polymers 0.000 description 1
- 239000005077 polysulfide Substances 0.000 description 1
- 229920001021 polysulfide Polymers 0.000 description 1
- 150000008117 polysulfides Polymers 0.000 description 1
- 229920000123 polythiophene Polymers 0.000 description 1
- 229920000131 polyvinylidene Polymers 0.000 description 1
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 1
- 239000005373 porous glass Substances 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- 125000002572 propoxy group Chemical group [*]OC([H])([H])C(C([H])([H])[H])([H])[H] 0.000 description 1
- 125000001436 propyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])[H] 0.000 description 1
- QQONPFPTGQHPMA-UHFFFAOYSA-N propylene Natural products CC=C QQONPFPTGQHPMA-UHFFFAOYSA-N 0.000 description 1
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 description 1
- 125000004805 propylene group Chemical group [H]C([H])([H])C([H])([*:1])C([H])([H])[*:2] 0.000 description 1
- UMJSCPRVCHMLSP-UHFFFAOYSA-N pyridine Natural products COC1=CC=CN=C1 UMJSCPRVCHMLSP-UHFFFAOYSA-N 0.000 description 1
- JUJWROOIHBZHMG-UHFFFAOYSA-O pyridinium Chemical compound C1=CC=[NH+]C=C1 JUJWROOIHBZHMG-UHFFFAOYSA-O 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 239000011347 resin Substances 0.000 description 1
- 229920005989 resin Polymers 0.000 description 1
- 238000007789 sealing Methods 0.000 description 1
- 229910052711 selenium Inorganic materials 0.000 description 1
- 239000011669 selenium Substances 0.000 description 1
- 229910052709 silver Inorganic materials 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- 238000005245 sintering Methods 0.000 description 1
- 239000002002 slurry Substances 0.000 description 1
- 239000001632 sodium acetate Substances 0.000 description 1
- 235000017281 sodium acetate Nutrition 0.000 description 1
- NLJMYIDDQXHKNR-UHFFFAOYSA-K sodium citrate Chemical compound O.O.[Na+].[Na+].[Na+].[O-]C(=O)CC(O)(CC([O-])=O)C([O-])=O NLJMYIDDQXHKNR-UHFFFAOYSA-K 0.000 description 1
- 239000001509 sodium citrate Substances 0.000 description 1
- 159000000000 sodium salts Chemical class 0.000 description 1
- 239000007784 solid electrolyte Substances 0.000 description 1
- 238000010532 solid phase synthesis reaction Methods 0.000 description 1
- 239000006104 solid solution Substances 0.000 description 1
- 229910052596 spinel Inorganic materials 0.000 description 1
- 239000011029 spinel Substances 0.000 description 1
- HXJUTPCZVOIRIF-UHFFFAOYSA-N sulfolane Chemical compound O=S1(=O)CCCC1 HXJUTPCZVOIRIF-UHFFFAOYSA-N 0.000 description 1
- 229910052717 sulfur Inorganic materials 0.000 description 1
- 239000011593 sulfur Substances 0.000 description 1
- 238000003786 synthesis reaction Methods 0.000 description 1
- 229910052714 tellurium Inorganic materials 0.000 description 1
- PORWMNRCUJJQNO-UHFFFAOYSA-N tellurium atom Chemical compound [Te] PORWMNRCUJJQNO-UHFFFAOYSA-N 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
- YLQBMQCUIZJEEH-UHFFFAOYSA-N tetrahydrofuran Natural products C=1C=COC=1 YLQBMQCUIZJEEH-UHFFFAOYSA-N 0.000 description 1
- 238000005979 thermal decomposition reaction Methods 0.000 description 1
- 229910052719 titanium Inorganic materials 0.000 description 1
- 239000010936 titanium Substances 0.000 description 1
- 125000003944 tolyl group Chemical group 0.000 description 1
- 238000009834 vaporization Methods 0.000 description 1
- 230000008016 vaporization Effects 0.000 description 1
- 125000000391 vinyl group Chemical group [H]C([*])=C([H])[H] 0.000 description 1
- 238000005406 washing Methods 0.000 description 1
- 239000002023 wood Substances 0.000 description 1
- 239000008096 xylene Substances 0.000 description 1
- 229910052726 zirconium Inorganic materials 0.000 description 1
Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
- H01M10/0566—Liquid materials
- H01M10/0567—Liquid materials characterised by the additives
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/54—Electrolytes
- H01G11/58—Liquid electrolytes
- H01G11/64—Liquid electrolytes characterised by additives
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
- H01G9/00—Electrolytic capacitors, rectifiers, detectors, switching devices, light-sensitive or temperature-sensitive devices; Processes of their manufacture
- H01G9/004—Details
- H01G9/022—Electrolytes; Absorbents
- H01G9/035—Liquid electrolytes, e.g. impregnating materials
-
- 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
- H01M10/0587—Construction or manufacture of accumulators having only wound construction elements, i.e. wound positive electrodes, wound negative electrodes and wound separators
-
- 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
- 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
- Y02E60/13—Energy storage using capacitors
-
- 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
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- Chemical & Material Sciences (AREA)
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- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- Manufacturing & Machinery (AREA)
- Power Engineering (AREA)
- General Chemical & Material Sciences (AREA)
- Microelectronics & Electronic Packaging (AREA)
- Materials Engineering (AREA)
- Physics & Mathematics (AREA)
- Condensed Matter Physics & Semiconductors (AREA)
- General Physics & Mathematics (AREA)
- Inorganic Chemistry (AREA)
- Secondary Cells (AREA)
- Electric Double-Layer Capacitors Or The Like (AREA)
Description
本發明係關於含碳酸酯改性矽烷及/或矽氧烷之非水電解液,及使用該電解液之各種能源設備,特別為蓄電池、電二重層電容器等之電化學電容器,尤其係關於鋰離子蓄電池。
近年,作為筆記型電腦、行動電話、數位相機或數位攝像機之可充電之攜帶式電源,使用具高能量密度之鋰離子蓄電池者漸增。此外,從環境面考量,作為不排放氣體於大氣中之汽車,實用化漸增之電動汽車、混合汽車用之輔助電源亦正研討使用非水電解液之鋰離子蓄電池或電二重層電容器。
然而,鋰離子蓄電池雖然性能高,但於惡劣環境下(特別為低溫環境下)之放電特性及短時間內需大量電之高輸出下之放電特性並不足夠。另一方面,電二重層電容器中其耐電壓不足夠,且存在電容量經時間變化而降低之問題。此外,使用二甲基碳酸酯、二乙基碳酸酯等為代表之低引火點溶劑為主成分之非水電解液居多,電池內一旦發生熱猛增現象,則會引起電解液之氣化、分解,可能引起電池之破裂及起火之情形。因此,通常裝入IC回路作為電池內異常時之電流遮斷裝置,為避免碳氫氣體產生時電池內部壓力增高安裝安全閥。為增加安全性與輕量化及降低成本,一直尋求更優良之電解液。
諸如化學安定性高、與電解液之相容性高之聚醚改性矽氧烷一直研究至今。此物不但可使LiPF6
等電解質充分溶解,且自聚醚改性矽氧烷原本具有之界面活性能,可改善電極或分離器之潤濕性效果。此外,眾說周知在電解液中添加數%可改善充放電循環特性。然而,以上之效果亦不足夠,聚醚改性矽氧烷缺乏熱安定性,另一方面因為熔點較高所以於低溫時使用會產生問題。再尋求與安定性高之電解液更相容之添加劑正開發中。
此外,與本發明相關之先前文獻,列舉如下述。
〔專利文獻1〕特開平11-214032號公報〔專利文獻2〕特開2000-58123號公報〔專利文獻3〕特開2001-110455號公報〔專利文獻4〕特開2003-142157號公報
本發明有鑒於上述狀況,旨在提供充放電特性增強、安全性提高之非水電解液及使用其之各種能源設備為目的(電池及電容器)。
本發明者們為達成上述課題專心致力研討之結果,當作非水電解液,籍由使用特定之含碳酸酯改性矽烷及/或矽氧烷之非水電解液,發現其充放電特性增強、安全性提高,完成本發明。
亦即,本發明之特徵為提供以非水溶劑、電解質鹽類及下述式(1)及(2)所示之碳酸酯改性矽烷及/或矽氧烷中選擇一種或兩種以上之混合物為必要成分之非水電解液。
R
1
(4-x)
R
2
x
Si (1) R
1
a
R
2
b
SiO
(4-a-b)/2
(2)
但是,上述式中R1
係可以氫氧基及部分鹵原子取代之碳數1~30之烷基、芳基、芳烷基、氨基取代烷基、羧基取代烷基、烷氧基、芳氧基之中選擇同一或相異之基,R2
為下述一般式(3)所示之碳酸酯基。
然而,R3
係碳數1~30之烷基、芳基、芳烷基,部分可以鹵素原子取代、A為含醚鍵結或酯鍵結亦可之碳數2~20之二價有機基。
x為1~4之整數,a、b各為1.0≦a≦2.5、0.001≦b≦1.5之正數,1.001≦a+b≦3。
此外,本發明提供上述含非水電解液之蓄電池、電化學電容器、鋰離子蓄電池。
本發明係含有碳酸酯改性矽烷及/或矽氧烷之非水電解液,具有效溶解電解質鹽類,提高充放電特性之效果。
本發明之非水溶劑中所使用之碳酸酯改性矽烷及矽氧烷為下述式(1)、(2)所示。
R
1
(4-x)
R
2
x
Si (1) R
1
a
R
2
b
SiO
(4-a-b)/2
(2)
上述式(1)、(2)中之R1
可相同或相異,以氫氧基或部分鹵素原子取代亦可之碳數1~30,最好為1~12,更好為1~6之烷基、芳基、芳烷基、氨基取代烷基、羧基取代烷基、烷氧基或芳氧基。該等之具體例列舉如,甲基、乙基、丙基、丁基、戊烷基、己基、庚基、辛基、壬醇、癸基等之烷基、苯基、甲苯基等之芳基、苄基、苯乙基等之芳烷基等之外,列舉如3-氨丙基、3-〔(2-氨乙基)氨基〕丙基等之氨基取代烷基、3-羧丙基等之羧基取代烷基等。此外,亦可列舉如三氟丙烷基及九氟辛烷基等之部分氫原子被氟原子等之鹵原子所取代之鹵化烷基。烷氧基可列舉如甲氧基、乙氧基、丙氧基、異丙氧基等。芳氧基可列舉苯氧基。該等之中最好為碳數1~6之烷基及氟取代烷基,更好為甲基或乙基。尤其,R1
之80莫耳%以上為甲基或乙基更好。
上述式(1)、(2)中之R2
為下述一般式(3)所示之直鏈狀構造的碳酸酯基。
R3
係碳數1~30,最好1~12,更好1~6之烷基、芳基或芳烷基,部分可以鹵素原子取代,例示與上述R1
同樣之物。該等之中最好為碳數1~6之烷基及氟取代烷基,更好為甲基或乙基。A為碳數2~20,最好為2~11之醚鍵結(-O-)及酯鍵結(-COO-)亦可為含直鏈或分支鏈之烷基等二價有機基。具體列舉如,-(CH2
)2
-、-(CH2
)3
-、-(CH2
)4
-、-CH2
CH(CH3
)CH2
-、-(CH2
)5
-、-(CH2
)6
-、-(CH2
)7
-、-(CH2
)8
-、-(CH2
)1 1
-、-(CH2
)2
-CH(CH2
CH2
CH3
)-、-CH2
-CH(CH2
CH3
)-、-(CH2
)3
-O-CH2
-、-(CH2
)3
-O-(CH2
)2
-、-(CH2
)3
-O-(CH2
)2
-O-(CH2
)2
-、-(CH2
)3
-O-CH2
CH(CH3
)-、-CH2
-CH(CH3
)-COO(CH2
)2
-等。該等之中的一部分或全部之氫原子以氟原子取代之氟醚基、全氟醚基亦可。最好為乙烯基或三甲基,更好為三甲基。
x為1~4之整數,x為3或4時相對的碳酸酯基之含有量增加因此矽之特徵減弱,較佳為1或2。最佳為1。
前述a為1.0≦a≦2.5、最好為1.5≦a≦2.5之正數。a小於1.0時碳酸酯改性矽氧烷黏度增加,電解液中離子移動度有時會降低,且無法期待潤濕性的提高。另一方面,大於2.5時與電解液之相容性變差,難以安定地溶解電解質。b為0.001≦b≦1.5之正數。最好為0.1≦b≦1.0,b小於0.001時碳酸酯改性矽氧烷中的碳酸酯含有量會降低,與電解液之相容性差,難以安定地溶解電解質。大於1.5時碳酸酯改性矽氧烷之黏度會增加,電解液中離子移動度降低,且無法期待潤濕性的提高。此時,a+b為1.001≦a+b≦3,最好為1.1≦a+b≦2.7,更好為1.5≦a+b≦2.5。
再者,上述式(2)中之矽氧烷為直鏈狀、環狀、分支狀、三次元網狀構造等之任一分子構造均可,此外上述式(2)中之矽氧烷中,矽原子數量為2~200,為2~60最好。
本發明之碳酸酯改性矽烷(1)及碳酸酯改性矽氧烷(2)如詳細表示,可列舉下述所示之化合物〔I〕~〔Ⅸ〕。
本發明之碳酸酯改性矽烷(1)及矽氧烷(2),為各自矽原子中鍵結氫原子(SiH基)之有機氫矽烷及有機氫聚矽氧烷時,可由具碳-碳雙鍵碳酸酯之加成反應所得。例如:
上述之碳酸酯基所改性之矽氧烷(化合物)〔Ⅱ〕時,具SiH基之矽氧烷可由與五甲基二矽氧烷及芳基乙基碳酸酯之加成反應所取得。此外,芳基乙基碳酸酯可由市售之氯代碳酸乙酯及芳基醇之脫鹽酸反應簡單合成。
上述加成反應最好於白金催化劑或銠催化劑存在下進行,具體為適宜使用氯化白金酸、乙醇改性氯化白金酸、氯化白金酸-乙烯基矽氧烷錯合體等之催化劑。
此外,作為助催化劑與pH調整劑,可添加乙酸鈉及檸檬酸鈉。
再者,催化劑之使用量可為催化劑量,但對於SiH基含有矽氧烷及具碳-碳雙鍵之碳酸酯之總量白金或銠數量50ppm以下為佳,20ppm以下更佳。
上述加成反應視需要可於有機溶劑中進行。有機溶劑列舉如,甲醇、乙醇、2-丙醇、丁醇等之脂肪族醇,甲苯、二甲苯等之芳香族碳氫化合物,n-戊烷、n-己烷、環己烷等之脂肪族或脂環式碳氫化合物,二氯甲烷、三氯甲烷、四氯化碳等之鹵化碳氫化合物等。加成反應條件並無特別限定,回流下使其反應一至十個小時。
本發明之碳酸酯改性矽氧烷(2)亦可由其他方法籍由烷氧矽烷與鹵化矽烷之加水分解而合成。例如,由三甲氧矽烷(H(MeO)3
Si)、甲基二甲氧矽烷(HMe(MeO)2
Si)及/或二甲基甲氧矽烷(H Me2
(MeO)Si)與芳基乙基碳酸酯,依前述之加成反應合成碳酸酯改性矽烷,該等與四甲氧矽烷、甲基三甲氧矽烷、二甲基二甲氧矽烷及三甲基甲氧矽烷中所選擇之烷氧矽烷於硫酸或甲磺酸存在下進行加水分解。烷氧基、乙氧基亦相同。另一方面,使用鹵化矽烷時,碳酸酯改性鹵化矽烷依前述加成反應合成後,與適宜選擇之氯矽烷同時滴入大量水進行合成。再者,任一反應中均可使用乙醇等之溶劑作為相溶化劑。
本發明之碳酸酯改性矽烷及矽氧烷於非水電解液中須含有0.001體積%以上。如未達0.001體積%時,本發明之效果不能充分發揮。最好含0.1體積%以上。此外,關於含有量之上限,依所使用之非水電解液用溶劑而不同,但非水電解液內Li離子之移動不到實用標準以下程度之含有量。通常80體積%以下,最好為60體積%以下,50體積%以下更好。另一方面,完全不使用揮發性非水電解液用溶劑時,非水電解液中之矽烷及矽氧烷含有量可為100體積%。
本發明之碳酸酯改性矽烷及矽氧烷之黏度並無特別限制,但若顧及非水電解液內使Li離子可順利移動時,例如依回轉式黏度計測定黏度,25℃下之黏度為2,000 mPa.s以下,最好為1,000 mmPa.s以下。
本發明之非水電解液含有電解質鹽類及非水溶劑。電解質鹽類類列舉如輕金屬鹽。輕金屬鹽類如鋰鹽、鈉鹽、鈣鹽等之鹼金屬鹽,鎂鹽、鈣鹽等之鹼土類金屬鹽,或鋁鹽等,可依目的選擇一種或多種。例如,鋰鹽列舉如LiBF4
、LiClO4
、LiPF6
、LiAsF6
、CF3
SO3
Li、(CF3
SO2
)2
NLi、C4
F9
SO3
Li、CF3
CO2
Li、(CF3
CO2
)2
NLi、C6
F5
SO3
Li、C8
F1 7
SO3
Li、(C2
F5
SO2
)2
NLi、(C4
F9
SO2
)(CF3
SO2
)NLi、(F SO2
C6
F4
)(CF3
SO2
)NLi、((CF3
)2
CHOSO2
)2
NLi、(CF3
SO2
)3
CLi、(3,5-(CF3
)2
C6
F3
)4
BLi、LiCF3
、LiAlCl4
或C4
BO8
Li,該等中可任一種或兩種以上混合使用。
非水電解液之電解質鹽類濃度,從電傳導性方面來看,最好為0.5~2.0 mol/L。此外,該非水電解液之溫度於25℃之導電率最好為0.01 S/m以上,依電解質鹽類之種類或其濃度調整。
本發明所使用之非水電解液用溶劑,只要可作為非水電解液者均無特別限制。一般列舉如碳酸乙烯酯、碳酸丙烯酯、碳酸丁烯酯、γ-丁酸內酯等之非質子性高導電率溶劑,及二甲基碳酸酯、乙基甲基碳酸酯、二乙基碳酸酯、甲基丙基碳酸酯、二丙基碳酸酯、二乙基醚、四氫呋喃、1,2-二甲氧基乙烷、1,2-二乙氧基乙烷、1,3-二氧雜戊環、環丁碼(sulfolane)、甲基環丁碼、乙睛、丙睛、茴香醚、甲基乙酸鹽等之乙酸酯類或丙酸乙酯類等之非質子性低黏度溶劑。此等之非質子性高導電率溶劑及非質子性低黏度溶劑以適當混合比並用為佳。此外可使用具咪唑、銨、及吡啶鎓型陽離子之離子性液體。對陰離子無特別限定,列舉如BF4 -
、PF6 -
、(CF3
SO2
)2
N-
等。離子性液體可與前述之非水電解液溶劑混合使用。
當作固體電解質及凝膠電解質時,高分子材料可含有矽凝膠、矽聚醚凝膠、丙烯基凝膠、丙烯晴凝膠、聚(乙烯叉螢石)等。再者,該等可不預先聚合,可注入液體後再聚合。該等可單獨或作為混合物使用。
此外,本發明之非水電解液亦可視需要添加各種添加劑。例如,旨在提高循環壽命之碳酸乙烯酯、甲基碳酸乙烯酯、乙基碳酸乙烯酯、4-丁二烯碳酸酯等,及旨在防止過度充電之聯苯、烷基聯苯、環己苯、t-丁苯、二苯醚、苯呋喃等,及旨在脫氧及脫水之各種碳酸酯化合物、各種碳酸酐、各種含氮及含硫黃化合物。
與本發明相關之非水電解液,可於備有正極、負極、分離器、電解液之蓄電池中使用。
正極活性物質列舉,可使用能吸收及脫附鋰離子之氧化物或硫化物等之任一種或兩種以上。具體列舉如TiS2
、MoS2
、NbS2
、ZrS2
、VS2
或V2
O5
、MoO3
及Mg(V3
O8
)2
等之未含鋰之金屬硫化物或氧化物,或鋰及含鋰之鋰複合氧化物,此外,列舉NbSe2
等之複合金屬。其中為增加能量密度,以Lip
MetO2
為主體之鋰複合氧化物為佳。再者,此時之Met具體為鈷、鎳、鐵及錳之中至少一種為佳,p通常為0.05≦p≦1.10範圍內之數值。諸如此類之鋰複合氧化物的具體例列舉如備有層構造之LiCoO2
、LiNi O2
、LiFeO2
、Liq
Nir
Co1 - r
O2
(但是,q及r之數值依電池之充放電狀態而異,通常0<q<1,0.7<r≦1)、尖晶石構造之LiMn2
O4
及斜方晶LiMnO2
。此外亦可使用作為高電壓對應型之取代尖晶石錳化合物LiMets
Mn1 - s
O4
(0<s<1),此時之Met列舉如鈦、鉻、鐵、鈷、鎳、銅及鋅等。
再者,上述之鋰複合氧化物與,例如鋰之碳氧鹽、硝酸鹽、氧化物或氫氧化物及過度金屬之碳氧鹽、硝酸鹽、氧化物或氫氧化物依所期望之組成粉碎混合,於氧氣環境中以600~1,000℃之溫度範圍內燒結調製。
此外正極活性物質亦可使用有機物。列舉如聚乙炔、聚吡咯、聚對苯基、聚苯胺、聚噻吩、聚並苯(polyacene)、聚硫化物化合物等。
可吸收及脫附鋰離子之負極材料列舉如碳材料、金屬元素或類金屬材料、金屬複合氧化物或聚乙炔或聚吡咯等之高分子材料等。
碳材料列舉如經碳化過程之乙炔碳黑、熱分解碳、天然石墨等之以氣相法合成之碳類與人造石墨類,石油焦炭或瀝青焦炭等含焦炭類之以液相法合成之碳類,高分子、木質原料、苯酚樹脂、碳膠片燒結而成之熱分解碳、木炭、玻璃狀碳類、碳纖維等之以固相法合成之碳類。
可吸收及脫附鋰之負極材料亦可列舉如可形成鋰與合金之金屬元素或類金屬元素之單體、合金或化合物。其形態存在固溶體、共晶、金屬間化合物或該等之中兩種以上共存。該等之任一種或兩種以上亦可混用。
諸如此類之金屬元素或類金屬,列舉如錫、鉛、鋁、銦、矽、鋅、銅、鈷、銻、鉍、鎘、鎂、硼、鎵、鍺、砷、硒、碲、銀、鉿、鋯及釔。其中,4B族之金屬元素或類金屬元素之單體、合金或化合物為佳,最好為矽或錫、或該等之合金或化合物。該等可為結晶質或非晶體化(amorphous)。
諸如此類之合金或化合物,具體可列舉如LiAl、AlSb、CuMgSb、SiB4
、SiB6
、Mg2
Si、Mg2
Sn、Ni2
Si、TiSi2
、Mo Si2
、CoSi2
、NiSi2
、CaSi2
、CrSi2
、Cu5
Si、FeSi2
、MnSi2
、NbSi2
、TaSi2
、VSi2
、WSi2
、ZnSi2
、SiC、Si/SiC複合物、Si3
N4
、Si2
N2
O、SiOv
(0<v≦2)、SiO/C複合物、SnOw
(0<w≦2)、SnSiO3
、LiSiO或LiSnO等。
正極、負極之製作方法無特別限制。一般為溶劑中加入活性物質、接著劑、導電劑等使其呈泥漿狀,於集電體板上塗佈、乾燥、壓著製作。
接著劑一般列舉如聚氟化亞乙烯基、聚四氟乙烯、苯乙烯、丁二烯橡膠、異戊二烯橡膠、各種聚醯亞胺樹脂等。
導電劑一般列舉如石墨、炭黑等碳系材料及銅、鎳等金屬材料。
集電體列舉如正極用為鋁或其合金,負極用如銅、不鏽鋼、鎳等之金屬或該等之合金等。
正極與負極間使用之分離器如對於電解液之安定、保液性優良則無特別限制,一般列舉如聚乙烯、聚丙烯等之聚烯系多孔質板或不織布。此外亦可使用多孔質玻璃、陶瓷等。
蓄電池之形狀為任意形狀,並無特別限制。一般列舉如衝壓硬幣形狀之電極及分離器積層而成之硬幣型、電極板與分離器呈螺旋狀之圓筒型等。
與本發明相關之非水電解液,係備有電極、分離器、電解液之電化學電容器,特別可使用電二重層電容器或類似電二重層電容器、非對稱電容器、氧化還原電容器等。
電容器中使用之電極中至少一方為以碳質物質為主成分之分極性電極。分極性電極一般由碳質物質、導電劑、接著劑所構成,相關之分極正電極之製法與上述之鋰蓄電池以完全相同方法製作。例如,主要混合粉末狀或纖維狀活性炭及炭黑及乙炔碳黑等之導電劑,加入接著劑之聚四氟乙烯,將此混合物塗佈於不鏽鋼及鋁等之集電體上或使用壓蓋物。同樣分離器及電解液最好與鋰蓄電池所使用之材料近乎相同使用離子穿透性高之材料。此外形狀可列舉如硬幣型、圓筒型、角型等。
以下明示實施例及比較例,具體說明本發明,但本發明並不侷限於下述之實施例。再者,黏度為依回轉式黏度計於25℃時所測量之數值。
合成具碳-碳雙鍵鍵結之碳酸酯備有攪拌機、溫度計及回流管之反應器中,加入芳基醇469g、吡啶693g及THF 1,200g,一邊攪拌一邊控制內溫為-5℃,滴入氯碳酸乙酯797g進行反應。氯碳酸乙酯滴下結束後,於室溫下進行2小時熟成。反應液中加入鹽酸水溶液進行中和。該中加入己烷1,000mL水洗,分離己烷層,加入無水硫酸鈉乾燥。進行精密蒸餾,籍由提取沸點149-150℃之餾分,得到芳基乙基碳酸酯769g。回收率為81%。依氣象層析分析純度為99.5%。重氯仿中測定1
H-NMR為1.28ppm(3 H,t)、4.14ppm(2H,q)、4.57ppm(2H,d)、5.3ppm(2H,m)、5.9ppm(1H,m)。此外,重丙酮中測定1 3
C-NMR為14.4ppm、64.2ppm、68.4ppm、118.2ppm、133.2ppm、155.5ppm之中觀測到訊號。再以IR測定1748cm- 1
中觀測到羰基之強烈信號,因此可確認為芳基乙基碳酸酯。
以碳酸酯基合成改性矽氧烷(i)下述式中所示之矽氧烷(亦即,前述化合物〔Ⅱ))依以下順序合成。
備有攪拌機、溫度計及回流管之反應器中加入芳基乙基碳酸酯118g、甲苯100g及氯化白金酸0.5質量%之甲苯溶液0.05g,一邊攪拌一邊於80℃滴入五甲基二矽氧烷134g。相對於SiH基之末端不飽和基之莫耳比約為1.0。滴下結束後,於2小時、80℃下熟成,反應液於減壓下進行精密蒸餾,藉由85℃/100Pa之餾分,得到42%回收率之下述式〔Ⅱ〕所示碳酸酯基之改性矽氧烷。
黏度為7mPa.s,比重為0.926。依氣象層析分析純度為99.5%。
(ii)下述式中所示之矽氧烷(亦即,前述化合物〔V Ⅲ))依以下順序合成。
備有攪拌機、溫度計及回流管之反應器中,加入芳基乙基碳酸酯98g、甲苯100g及氯化白金酸0.5質量%之甲苯溶液0.05g,一邊攪拌一邊於80℃滴入甲基甲氧矽烷110g。相對於SiH基之末端不飽和基之莫耳比約為0.83。滴下結束後,於2小時、80℃下熟成,反應液於減壓下進行精密蒸餾,藉由到103℃/100Pa之餾分,得到碳酸酯改性甲氧矽烷。回收率為66%。接著,於備有攪拌機、溫度計及回流管之反應器中,加入碳酸酯改性甲氧矽烷100g、三甲基甲氧矽烷124g及甲醇60g,於-10℃下冷卻,添加濃硫酸4g。於-10℃之冷卻狀態下緩慢添加離子交換水30g,進行加水分解。攪拌2小時後,恢復至室溫,添加甲苯進行水洗。分離甲苯層後,加入無水硫酸鈉乾燥。100℃/50Pa之條件下進行2小時減壓去除,得到希望之碳酸酯改性矽氧烷。黏度為12mPa.s,比重為0.971。
(非水電解液之調製)碳酸乙烯酯(EC)及碳酸二乙烯酯(DEC)中碳酸酯改性矽烷或矽氧烷之前述化合物〔I〕~〔Ⅸ〕以表1之比例溶解。接著,LiPF6
於1mol/L濃度下溶解,形成非水電解液。此外,作為比較例,非水電解液中不含矽氧烷時添加3%及6%之聚醚改性矽烷時亦進行同樣之評量。
(電池材料之製作)正極材料使用LiCoO2
為活性物質,集電體為鋁箔單層板(Pionics(股)製,商品名:Pioxcel C-100)。此外,負極材料使用石墨為活性物質,集電體為銅箔單層板(Pionics(股)製,商品名:Pioxcel A-100)。分離器使用玻璃纖維濾紙(Toyo Advantec(股)製,商品名:GC50)。
(電池之組裝)於氬環境下之乾燥箱內,使用具前述電池材料與正極導電體之不鏽鋼罐及具負極導電體之不鏽鋼封口板及絕緣用墊片組裝2032硬幣型電池。
(電池性能之評量;循環特徵)於0℃及25℃下充電(0.6mA一定電流下至4.2V)及放電(0.6mA一定電流下至2.5V)重複操作一百次循環。但是,進行0℃之充放電試驗時,須預先進行於25℃下充放電循環三次後,切換至0℃進行充放電。評量以第100次循環之放電容量除以初期放電容量之數值以%列表比較。結果如表2所示。
比較一百次循環後之放電容量維持率時,將碳酸酯改性矽烷及矽氧烷之任一與無添加矽氧烷時及添加聚醚改性矽烷時比較,得知放電容量維持率上升。
Claims (9)
- 一種非水電解液,其特徵為於非水溶液、電解質鹽類,以及一種或兩種以上選自下述式(1)所示之碳酸酯改性矽烷及下述式(2)所示之碳酸酯改性矽氧烷之混合物為必要成分者,R1 (4-x )R2 x Si (1) R1 a R2 b SiO(4-a-b)/2 (2)(式中,R1 為選自部分可以鹵素原子取代之碳數1~30之烷基、芳基、芳烷基、氨基取代烷基,以及羧基取代烷基中之同一或相異之基,R2 為下述一般式(3)所示之碳酸酯基,
- 如申請專利範圍第1項所記載之非水電解液,其中前述碳酸酯改性矽烷(1)及碳酸酯改性矽氧烷(2)中之R1 為碳數1~6之烷基或氟取代烷基。
- 如申請專利範圍第1項或第2項所記載之非水電解液,其中前述碳酸酯基(3)中之A係三伸甲基。
- 如申請專利範圍第1項或第2項所記載之非水電解液,其中前述一種或兩種以上選自碳酸酯改性矽烷及碳酸酯改性矽氧烷之混合物的含有量為非水電解液全部之0.001體積%以上。
- 如申請專利範圍第1項或第2項所記載之非水電解液,其中電解質鹽類為鋰鹽。
- 一種蓄電池,其特徵為含有申請專利範圍第1項至第5項中任一項所記載之非水電解液。
- 一種電化學電容器,其特徵含有申請專利範圍第1項至第5項中任一項所記載之非水電解液。
- 一種鋰蓄電池,其特徵含有申請專利範圍第1項至第5項之任一項所記載之非水電解液。
- 如申請專利範圍第1項所記載之非水電解液,其中前述至少一種混合物係選自由具有式〔I〕、〔II〕、〔III〕、〔IV〕、〔V〕、〔VI〕、〔VII〕、〔VIII〕以及〔IX〕之混合物所組成的群組中之一種混合物:
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