CN117941117A - Electrolyte, secondary battery, battery module, battery pack, and electricity device - Google Patents
Electrolyte, secondary battery, battery module, battery pack, and electricity device Download PDFInfo
- Publication number
- CN117941117A CN117941117A CN202280056212.4A CN202280056212A CN117941117A CN 117941117 A CN117941117 A CN 117941117A CN 202280056212 A CN202280056212 A CN 202280056212A CN 117941117 A CN117941117 A CN 117941117A
- Authority
- CN
- China
- Prior art keywords
- orthocarbonate
- lithium
- electrolyte
- secondary battery
- salt
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Pending
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- 239000003792 electrolyte Substances 0.000 title claims abstract description 103
- 230000005611 electricity Effects 0.000 title description 3
- 159000000002 lithium salts Chemical class 0.000 claims abstract description 54
- 229910003002 lithium salt Inorganic materials 0.000 claims abstract description 53
- 150000001875 compounds Chemical class 0.000 claims abstract description 28
- 125000000217 alkyl group Chemical group 0.000 claims abstract description 25
- 239000002131 composite material Substances 0.000 claims description 60
- -1 tetradecyl fluoroorthocarbonate Chemical compound 0.000 claims description 54
- 229910052744 lithium Inorganic materials 0.000 claims description 43
- 239000000945 filler Substances 0.000 claims description 42
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 claims description 32
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims description 30
- 239000000919 ceramic Substances 0.000 claims description 29
- 229910001416 lithium ion Inorganic materials 0.000 claims description 28
- 239000010416 ion conductor Substances 0.000 claims description 21
- 125000001188 haloalkyl group Chemical group 0.000 claims description 14
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims description 10
- CWLNAJYDRSIKJS-UHFFFAOYSA-N triethoxymethoxyethane Chemical compound CCOC(OCC)(OCC)OCC CWLNAJYDRSIKJS-UHFFFAOYSA-N 0.000 claims description 9
- 125000000008 (C1-C10) alkyl group Chemical group 0.000 claims description 8
- AHJWSRRHTXRLAQ-UHFFFAOYSA-N tetramethoxymethane Chemical compound COC(OC)(OC)OC AHJWSRRHTXRLAQ-UHFFFAOYSA-N 0.000 claims description 7
- GFBZPRXNUFHLKG-UHFFFAOYSA-N 1-(tributoxymethoxy)butane Chemical compound CCCCOC(OCCCC)(OCCCC)OCCCC GFBZPRXNUFHLKG-UHFFFAOYSA-N 0.000 claims description 6
- YMSQYBJUXYMMKN-UHFFFAOYSA-N 1-(triheptoxymethoxy)heptane Chemical compound C(OCCCCCCC)(OCCCCCCC)(OCCCCCCC)OCCCCCCC YMSQYBJUXYMMKN-UHFFFAOYSA-N 0.000 claims description 6
- UNZRWCGQFKEJLF-UHFFFAOYSA-N 1-(trihexoxymethoxy)hexane Chemical compound CCCCCCOC(OCCCCCC)(OCCCCCC)OCCCCCC UNZRWCGQFKEJLF-UHFFFAOYSA-N 0.000 claims description 6
- IXGIQHBYIVKIFL-UHFFFAOYSA-N 1-(tripentoxymethoxy)pentane Chemical compound CCCCCOC(OCCCCC)(OCCCCC)OCCCCC IXGIQHBYIVKIFL-UHFFFAOYSA-N 0.000 claims description 6
- LFMXSZSVDQJYDU-UHFFFAOYSA-N 1-(tripropoxymethoxy)propane Chemical compound CCCOC(OCCC)(OCCC)OCCC LFMXSZSVDQJYDU-UHFFFAOYSA-N 0.000 claims description 6
- QVEMMGJRDYQAGQ-UHFFFAOYSA-N CCCCCCCCCOC(OCCCCCCCCC)(OCCCCCCCCC)OCCCCCCCCC Chemical compound CCCCCCCCCOC(OCCCCCCCCC)(OCCCCCCCCC)OCCCCCCCCC QVEMMGJRDYQAGQ-UHFFFAOYSA-N 0.000 claims description 6
- NIWKSRAYCGCPFC-UHFFFAOYSA-N CCCCCCCCOC(OCCCCCCCC)(OCCCCCCCC)OCCCCCCCC Chemical compound CCCCCCCCOC(OCCCCCCCC)(OCCCCCCCC)OCCCCCCCC NIWKSRAYCGCPFC-UHFFFAOYSA-N 0.000 claims description 6
- UQSXHKLRYXJYBZ-UHFFFAOYSA-N Iron oxide Chemical compound [Fe]=O UQSXHKLRYXJYBZ-UHFFFAOYSA-N 0.000 claims description 6
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 claims description 6
- AMWRITDGCCNYAT-UHFFFAOYSA-L hydroxy(oxo)manganese;manganese Chemical compound [Mn].O[Mn]=O.O[Mn]=O AMWRITDGCCNYAT-UHFFFAOYSA-L 0.000 claims description 6
- BDUXVICNCUWRIT-UHFFFAOYSA-N tetradecoxymethanetriol Chemical compound CCCCCCCCCCCCCCOC(O)(O)O BDUXVICNCUWRIT-UHFFFAOYSA-N 0.000 claims description 6
- RIUWBIIVUYSTCN-UHFFFAOYSA-N trilithium borate Chemical compound [Li+].[Li+].[Li+].[O-]B([O-])[O-] RIUWBIIVUYSTCN-UHFFFAOYSA-N 0.000 claims description 6
- CPLXHLVBOLITMK-UHFFFAOYSA-N Magnesium oxide Chemical compound [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 claims description 5
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 5
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 5
- UCKMPCXJQFINFW-UHFFFAOYSA-N Sulphide Chemical compound [S-2] UCKMPCXJQFINFW-UHFFFAOYSA-N 0.000 claims description 4
- 150000004820 halides Chemical class 0.000 claims description 4
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 claims description 4
- VDVLPSWVDYJFRW-UHFFFAOYSA-N lithium;bis(fluorosulfonyl)azanide Chemical compound [Li+].FS(=O)(=O)[N-]S(F)(=O)=O VDVLPSWVDYJFRW-UHFFFAOYSA-N 0.000 claims description 4
- MCVFFRWZNYZUIJ-UHFFFAOYSA-M lithium;trifluoromethanesulfonate Chemical compound [Li+].[O-]S(=O)(=O)C(F)(F)F MCVFFRWZNYZUIJ-UHFFFAOYSA-M 0.000 claims description 4
- BTBUEUYNUDRHOZ-UHFFFAOYSA-N Borate Chemical compound [O-]B([O-])[O-] BTBUEUYNUDRHOZ-UHFFFAOYSA-N 0.000 claims description 3
- QPLDLSVMHZLSFG-UHFFFAOYSA-N Copper oxide Chemical compound [Cu]=O QPLDLSVMHZLSFG-UHFFFAOYSA-N 0.000 claims description 3
- 239000005751 Copper oxide Substances 0.000 claims description 3
- WGLPBDUCMAPZCE-UHFFFAOYSA-N Trioxochromium Chemical compound O=[Cr](=O)=O WGLPBDUCMAPZCE-UHFFFAOYSA-N 0.000 claims description 3
- BRPQOXSCLDDYGP-UHFFFAOYSA-N calcium oxide Chemical compound [O-2].[Ca+2] BRPQOXSCLDDYGP-UHFFFAOYSA-N 0.000 claims description 3
- 239000000292 calcium oxide Substances 0.000 claims description 3
- ODINCKMPIJJUCX-UHFFFAOYSA-N calcium oxide Inorganic materials [Ca]=O ODINCKMPIJJUCX-UHFFFAOYSA-N 0.000 claims description 3
- 229910000423 chromium oxide Inorganic materials 0.000 claims description 3
- 229910000428 cobalt oxide Inorganic materials 0.000 claims description 3
- IVMYJDGYRUAWML-UHFFFAOYSA-N cobalt(ii) oxide Chemical compound [Co]=O IVMYJDGYRUAWML-UHFFFAOYSA-N 0.000 claims description 3
- 229910000431 copper oxide Inorganic materials 0.000 claims description 3
- 125000003709 fluoroalkyl group Chemical group 0.000 claims description 3
- 150000003949 imides Chemical class 0.000 claims description 3
- DEUISMFZZMAAOJ-UHFFFAOYSA-N lithium dihydrogen borate oxalic acid Chemical compound B([O-])(O)O.C(C(=O)O)(=O)O.C(C(=O)O)(=O)O.[Li+] DEUISMFZZMAAOJ-UHFFFAOYSA-N 0.000 claims description 3
- MHCFAGZWMAWTNR-UHFFFAOYSA-M lithium perchlorate Chemical compound [Li+].[O-]Cl(=O)(=O)=O MHCFAGZWMAWTNR-UHFFFAOYSA-M 0.000 claims description 3
- 229910001486 lithium perchlorate Inorganic materials 0.000 claims description 3
- 239000000395 magnesium oxide Substances 0.000 claims description 3
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- GNRSAWUEBMWBQH-UHFFFAOYSA-N oxonickel Chemical compound [Ni]=O GNRSAWUEBMWBQH-UHFFFAOYSA-N 0.000 claims description 3
- 239000011787 zinc oxide Substances 0.000 claims description 3
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 2
- 239000000377 silicon dioxide Substances 0.000 claims description 2
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 claims 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 claims 1
- 239000004033 plastic Substances 0.000 abstract description 73
- 239000007784 solid electrolyte Substances 0.000 abstract description 12
- 150000002500 ions Chemical class 0.000 description 30
- 210000004027 cell Anatomy 0.000 description 19
- 239000000463 material Substances 0.000 description 18
- 238000000034 method Methods 0.000 description 18
- 239000010410 layer Substances 0.000 description 17
- 230000003647 oxidation Effects 0.000 description 16
- 238000007254 oxidation reaction Methods 0.000 description 16
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 14
- 239000011888 foil Substances 0.000 description 12
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- 239000004743 Polypropylene Substances 0.000 description 10
- 229910052751 metal Inorganic materials 0.000 description 10
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- 229920001155 polypropylene Polymers 0.000 description 10
- 239000004698 Polyethylene Substances 0.000 description 9
- 229910052782 aluminium Inorganic materials 0.000 description 9
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 9
- 125000005843 halogen group Chemical group 0.000 description 9
- 239000007788 liquid Substances 0.000 description 9
- 229920000573 polyethylene Polymers 0.000 description 9
- 230000008859 change Effects 0.000 description 8
- 239000007774 positive electrode material Substances 0.000 description 8
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- 239000006258 conductive agent Substances 0.000 description 7
- 229910052799 carbon Inorganic materials 0.000 description 6
- 239000002904 solvent Substances 0.000 description 6
- 239000002033 PVDF binder Substances 0.000 description 5
- 239000006183 anode active material Substances 0.000 description 5
- 230000000052 comparative effect Effects 0.000 description 5
- 239000011267 electrode slurry Substances 0.000 description 5
- 230000008595 infiltration Effects 0.000 description 5
- 238000001764 infiltration Methods 0.000 description 5
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- 229920001707 polybutylene terephthalate Polymers 0.000 description 5
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- 229910045601 alloy Inorganic materials 0.000 description 4
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- 125000001153 fluoro group Chemical group F* 0.000 description 4
- 229920000139 polyethylene terephthalate Polymers 0.000 description 4
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- 238000002360 preparation method Methods 0.000 description 4
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- 125000001424 substituent group Chemical group 0.000 description 4
- 239000000758 substrate Substances 0.000 description 4
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 3
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- GELKBWJHTRAYNV-UHFFFAOYSA-K lithium iron phosphate Chemical compound [Li+].[Fe+2].[O-]P([O-])([O-])=O GELKBWJHTRAYNV-UHFFFAOYSA-K 0.000 description 3
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- IXPNQXFRVYWDDI-UHFFFAOYSA-N 1-methyl-2,4-dioxo-1,3-diazinane-5-carboximidamide Chemical compound CN1CC(C(N)=N)C(=O)NC1=O IXPNQXFRVYWDDI-UHFFFAOYSA-N 0.000 description 2
- 229910001316 Ag alloy Inorganic materials 0.000 description 2
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 2
- 229910000990 Ni alloy Inorganic materials 0.000 description 2
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- NRJJZXGPUXHHTC-UHFFFAOYSA-N [Li+].[O--].[O--].[O--].[O--].[Zr+4].[La+3] Chemical compound [Li+].[O--].[O--].[O--].[O--].[Zr+4].[La+3] NRJJZXGPUXHHTC-UHFFFAOYSA-N 0.000 description 2
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- FQBJEOBTOBNOOV-UHFFFAOYSA-N [S].[P].[Li] Chemical compound [S].[P].[Li] FQBJEOBTOBNOOV-UHFFFAOYSA-N 0.000 description 1
- 238000010521 absorption reaction Methods 0.000 description 1
- DPXJVFZANSGRMM-UHFFFAOYSA-N acetic acid;2,3,4,5,6-pentahydroxyhexanal;sodium Chemical compound [Na].CC(O)=O.OCC(O)C(O)C(O)C(O)C=O DPXJVFZANSGRMM-UHFFFAOYSA-N 0.000 description 1
- 239000002671 adjuvant Substances 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
- 229910021383 artificial graphite Inorganic materials 0.000 description 1
- 238000000429 assembly Methods 0.000 description 1
- 230000000712 assembly Effects 0.000 description 1
- 230000000903 blocking effect Effects 0.000 description 1
- 229910052796 boron Inorganic materials 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
- 239000001768 carboxy methyl cellulose Substances 0.000 description 1
- 125000002057 carboxymethyl group Chemical group [H]OC(=O)C([H])([H])[*] 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
- 229910052801 chlorine Inorganic materials 0.000 description 1
- 125000001309 chloro group Chemical group Cl* 0.000 description 1
- 229920001577 copolymer Polymers 0.000 description 1
- 229910052802 copper Inorganic materials 0.000 description 1
- 239000010949 copper Substances 0.000 description 1
- 239000011889 copper foil Substances 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 230000001351 cycling effect Effects 0.000 description 1
- 125000001995 cyclobutyl group Chemical group [H]C1([H])C([H])([H])C([H])(*)C1([H])[H] 0.000 description 1
- 125000001559 cyclopropyl group Chemical group [H]C1([H])C([H])([H])C1([H])* 0.000 description 1
- 239000008367 deionised water Substances 0.000 description 1
- 229910021641 deionized water Inorganic materials 0.000 description 1
- 230000008021 deposition Effects 0.000 description 1
- 238000001514 detection method Methods 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- ZFTFAPZRGNKQPU-UHFFFAOYSA-N dicarbonic acid Chemical compound OC(=O)OC(O)=O ZFTFAPZRGNKQPU-UHFFFAOYSA-N 0.000 description 1
- 238000000113 differential scanning calorimetry Methods 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 239000011737 fluorine Substances 0.000 description 1
- ZYMKZMDQUPCXRP-UHFFFAOYSA-N fluoro prop-2-enoate Chemical compound FOC(=O)C=C ZYMKZMDQUPCXRP-UHFFFAOYSA-N 0.000 description 1
- 229910052733 gallium Inorganic materials 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
- 239000010931 gold Substances 0.000 description 1
- 229910021385 hard carbon Inorganic materials 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
- 239000008240 homogeneous mixture Substances 0.000 description 1
- 125000004435 hydrogen atom Chemical group [H]* 0.000 description 1
- CPSYWNLKRDURMG-UHFFFAOYSA-L hydron;manganese(2+);phosphate Chemical compound [Mn+2].OP([O-])([O-])=O CPSYWNLKRDURMG-UHFFFAOYSA-L 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
- 239000011256 inorganic filler Substances 0.000 description 1
- 229910003475 inorganic filler Inorganic materials 0.000 description 1
- 229910052740 iodine Inorganic materials 0.000 description 1
- 230000037427 ion transport Effects 0.000 description 1
- 125000004491 isohexyl group Chemical group C(CCC(C)C)* 0.000 description 1
- 238000010030 laminating Methods 0.000 description 1
- 239000001989 lithium alloy Substances 0.000 description 1
- 229910000664 lithium aluminum titanium phosphates (LATP) Inorganic materials 0.000 description 1
- CEMTZIYRXLSOGI-UHFFFAOYSA-N lithium lanthanum(3+) oxygen(2-) titanium(4+) Chemical compound [Li+].[O--].[O--].[O--].[O--].[Ti+4].[La+3] CEMTZIYRXLSOGI-UHFFFAOYSA-N 0.000 description 1
- 229910021437 lithium-transition metal oxide Inorganic materials 0.000 description 1
- DVATZODUVBMYHN-UHFFFAOYSA-K lithium;iron(2+);manganese(2+);phosphate Chemical compound [Li+].[Mn+2].[Fe+2].[O-]P([O-])([O-])=O DVATZODUVBMYHN-UHFFFAOYSA-K 0.000 description 1
- 229910052749 magnesium Inorganic materials 0.000 description 1
- 239000011777 magnesium Substances 0.000 description 1
- AXZKOIWUVFPNLO-UHFFFAOYSA-N magnesium;oxygen(2-) Chemical compound [O-2].[Mg+2] AXZKOIWUVFPNLO-UHFFFAOYSA-N 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- 230000008018 melting Effects 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- 230000005012 migration Effects 0.000 description 1
- 238000013508 migration Methods 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 125000004108 n-butyl group Chemical group [H]C([H])([H])C([H])([H])C([H])([H])C([H])([H])* 0.000 description 1
- 125000001280 n-hexyl group Chemical group C(CCCCC)* 0.000 description 1
- 125000000740 n-pentyl group Chemical group [H]C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])* 0.000 description 1
- 125000004123 n-propyl group Chemical group [H]C([H])([H])C([H])([H])C([H])([H])* 0.000 description 1
- 229910021382 natural graphite Inorganic materials 0.000 description 1
- 239000004745 nonwoven fabric Substances 0.000 description 1
- 239000010450 olivine Substances 0.000 description 1
- 229910052609 olivine Inorganic materials 0.000 description 1
- 238000005457 optimization Methods 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- 125000001147 pentyl group Chemical group C(CCCC)* 0.000 description 1
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 description 1
- 239000010452 phosphate Substances 0.000 description 1
- 150000003013 phosphoric acid derivatives Chemical class 0.000 description 1
- 230000010287 polarization Effects 0.000 description 1
- 229920001495 poly(sodium acrylate) polymer Polymers 0.000 description 1
- 229920002961 polybutylene succinate Polymers 0.000 description 1
- 239000004631 polybutylene succinate Substances 0.000 description 1
- 239000011148 porous material Substances 0.000 description 1
- 238000005036 potential barrier Methods 0.000 description 1
- 230000001737 promoting effect Effects 0.000 description 1
- 125000001436 propyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])[H] 0.000 description 1
- 230000009257 reactivity Effects 0.000 description 1
- 230000001105 regulatory effect Effects 0.000 description 1
- 239000011347 resin Substances 0.000 description 1
- 229920005989 resin Polymers 0.000 description 1
- 229910052814 silicon oxide Inorganic materials 0.000 description 1
- 239000002153 silicon-carbon composite material Substances 0.000 description 1
- 229910052709 silver Inorganic materials 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- 239000002356 single layer Substances 0.000 description 1
- 239000002002 slurry Substances 0.000 description 1
- 239000011734 sodium Substances 0.000 description 1
- 235000019812 sodium carboxymethyl cellulose Nutrition 0.000 description 1
- 229920001027 sodium carboxymethylcellulose Polymers 0.000 description 1
- 229910001415 sodium ion Inorganic materials 0.000 description 1
- NNMHYFLPFNGQFZ-UHFFFAOYSA-M sodium polyacrylate Chemical compound [Na+].[O-]C(=O)C=C NNMHYFLPFNGQFZ-UHFFFAOYSA-M 0.000 description 1
- 229910021384 soft carbon Inorganic materials 0.000 description 1
- 239000010959 steel Substances 0.000 description 1
- 229920003048 styrene butadiene rubber Polymers 0.000 description 1
- 125000001973 tert-pentyl group Chemical group [H]C([H])([H])C([H])([H])C(*)(C([H])([H])[H])C([H])([H])[H] 0.000 description 1
- GIUKDPYJMVJMDZ-UHFFFAOYSA-N tetralithium methanetetrolate Chemical compound C([O-])([O-])([O-])[O-].[Li+].[Li+].[Li+].[Li+] GIUKDPYJMVJMDZ-UHFFFAOYSA-N 0.000 description 1
- 239000002562 thickening agent Substances 0.000 description 1
- XOLBLPGZBRYERU-UHFFFAOYSA-N tin dioxide Chemical compound O=[Sn]=O XOLBLPGZBRYERU-UHFFFAOYSA-N 0.000 description 1
- 229910001887 tin oxide Inorganic materials 0.000 description 1
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 description 1
- 238000012546 transfer Methods 0.000 description 1
- 239000006163 transport media Substances 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
- 229910052725 zinc Inorganic materials 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
- 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
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
-
- 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
- H01M10/0568—Liquid materials characterised by the solutes
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Landscapes
- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Inorganic Chemistry (AREA)
- Physics & Mathematics (AREA)
- Condensed Matter Physics & Semiconductors (AREA)
- General Physics & Mathematics (AREA)
- Materials Engineering (AREA)
- Secondary Cells (AREA)
Abstract
The embodiment of the application provides an electrolyte, a secondary battery, a battery module, a battery pack and an electric device. The electrolyte comprises a plastic crystal compound, wherein the plastic crystal compound comprises orthocarbonate and lithium salt, the orthocarbonate comprises one or more of compounds shown in a formula I, and R1 to R4 respectively and independently represent alkyl or halogenated alkyl. According to the embodiment of the application, the orthocarbonate and the lithium salt form the plastic crystal compound, so that the ion conductivity of the electrolyte can be improved, and the cycle performance of the secondary battery is improved. Since the solid electrolyte is not easily burned, the safety performance of the secondary battery can be ensured.
Description
The application relates to the field of batteries, in particular to an electrolyte, a secondary battery, a battery module, a battery pack and an electric device.
The secondary battery has characteristics of high capacity, long life, and the like, and thus is widely used in electronic devices such as mobile phones, notebook computers, battery cars, electric automobiles, electric airplanes, electric ships, electric toy cars, electric toy ships, electric toy airplanes, electric tools, and the like. As the secondary battery has made great progress, there is a higher demand for the performance of the secondary battery. In order to improve the performance of the secondary battery, optimization and improvement of materials such as electrolytes in the secondary battery are generally performed. The electrolyte, which serves as a transport medium for metal ions in the secondary battery, has a non-negligible effect on the performance of the secondary battery.
However, currently improved electrolytes have yet to be improved in cycle performance and safety performance when applied to secondary batteries.
Disclosure of Invention
The present application has been made in view of the above problems, and an object thereof is to provide an electrolyte, a secondary battery, a battery module, a battery pack, and an electric device.
The first aspect of the present application provides an electrolyte for a secondary battery, the electrolyte comprising a plastic crystal composite including an orthocarbonate and a lithium salt, the orthocarbonate including one or more of compounds represented by formula I,
In formula I, R1 to R4 each independently represent an alkyl group or a haloalkyl group.
Therefore, the embodiment of the application can improve the ion conductivity of the electrolyte by forming the plastic crystal compound by the orthocarbonate and the lithium salt. When the electrolyte is applied to the secondary battery, the electrolyte has better infiltration performance with the positive electrode plate and/or the negative electrode plate, and can be matched with the high-voltage positive electrode plate due to relatively higher oxidation stability, so that the cycle performance of the secondary battery is improved. Since the solid electrolyte is not easily burned, the safety performance of the secondary battery can be ensured.
In any embodiment, alkyl is C1-C10 alkyl. The miscibility of the orthocarbonate and the lithium salt is relatively better, which is favorable for forming a plastic crystal compound.
In any embodiment, the haloalkyl is a C1-C10 haloalkyl. The miscibility of the orthocarbonate and the lithium salt is relatively better, which is favorable for forming a plastic crystal compound.
In any embodiment, the haloalkyl is fluoroalkyl. The electrolyte can be further inhibited from being oxidized due to the strong electron-withdrawing effect of the fluorine group, and the electrochemical window of the electrolyte is improved.
In any embodiment, the orthocarbonate comprises tetramethyl orthocarbonate, tetraethyl orthocarbonate, tetrapropyl orthocarbonate, tetrabutyl orthocarbonate, tetrapentyl orthocarbonate, tetrahexyl orthocarbonate, tetraheptyl orthocarbonate, tetraoctyl orthocarbonate, tetranonyl orthocarbonate, tetradecyl orthocarbonate, tetramethyl orthofluoro-carbonate, tetraethyl fluoroorthocarbonate, tetrapropyl fluoroorthocarbonate, tetrabutyl fluoroorthocarbonate, tetrapentyl fluoroorthocarbonate, tetrahexyl fluoroorthocarbonate, tetraheptyl fluoroorthocarbonate, tetraoctyl fluoroorthocarbonate, tetranonyl fluoroorthocarbonate, tetradecyl fluoroorthocarbonate, tetratrifluoromethoxy methane, tetrakis- (2, 2-trifluoroethoxy) -methane, tetrakis- (3, 3-trifluoropropoxy) -methane, methyltriethyl orthocarbonate, dimethyldiethyl orthocarbonate, ethyltrimethyl orthocarbonate, methyltrimethyl orthocarbonate, dimethylpropyl orthocarbonate, propyltrimethyl orthocarbonate, ethyltripropylethyl orthocarbonate, diethyldipropyl orthocarbonate, trimethyldipropyl orthocarbonate, and tributyl orthobutyl dicarbonate. The orthocarbonate has stronger mixing capability with lithium salt, and the formed plastic-crystal composite is easier to form because the phase change transformation entropy of the plastic-crystal composite from a plastic crystal state to a liquid state is lower.
In any embodiment, the orthocarbonate comprises one or more of tetramethyl orthocarbonate, tetraethyl orthocarbonate, tetrapropyl orthocarbonate, tetrabutyl orthocarbonate, tetrapentyl orthocarbonate, tetrahexyl orthocarbonate, tetraheptyl orthocarbonate, tetraoctyl orthocarbonate, tetranonyl orthocarbonate, and tetradecyl orthocarbonate. The orthocarbonates and lithium salts are easier to form plastic crystal composites.
In any embodiment, the lithium salt comprises one or more of a lithium sulfonimide salt, a lithium borate salt, lithium hexafluorophosphate, lithium perchlorate, lithium hexafluoroarsenate, and lithium trifluoromethane sulfonate.
Therefore, the lithium salt of the embodiment of the application can easily form a plastic crystal compound with the orthocarbonate, and can also form a solid electrolyte interface (Solid Electrolyte Interphase, SEI) film on the negative electrode plate of the secondary battery, so that the negative electrode plate can be protected, the structural stability of the negative electrode plate is ensured, and the risk of side reaction between the negative electrode plate and electrolyte is reduced.
In any embodiment, the lithium sulfonimide salt comprises one or more of lithium bis-fluorosulfonimide, lithium bis-fluoromethylsulfonimide, and lithium bis-pentafluoroethylsulfonimide; further alternatively, the lithium sulfonimide salt comprises lithium bis (fluorosulfonyl) imide and/or lithium bis (fluoromethylsulfonyl) imide; further alternatively, the lithium sulfonimide salt comprises lithium bis-fluorosulfonimide.
In any embodiment, the lithium borate salt comprises one or more of lithium tetrafluoroborate, lithium dioxalate borate, and lithium difluorooxalato borate.
In any embodiment, the molar amount x of orthocarbonate and the molar amount y of lithium salt satisfy: x is more than or equal to 0.5 and y is more than or equal to 3; alternatively, 1.ltoreq.x.ltoreq.y.ltoreq.2.
Thus, when the molar amounts of the orthocarbonate and the lithium salt in the embodiments of the present application satisfy the above ranges, the participation of the orthocarbonate around lithium ions can be reduced, the risk of decomposition of the orthocarbonate can be reduced, and the oxidation stability of the electrolyte can be further improved.
In any embodiment, the mole percent of orthocarbonate is 30% to 80% based on the total mass of orthocarbonate and lithium salt; alternatively, 50% -70%. When the mole percentage of the orthocarbonate satisfies the above range, the mixing ability of the orthocarbonate and the lithium salt is relatively good, so that the molding compound is more easily formed.
In any embodiment, the mole percent of lithium salt is 20% to 70% based on the total mass of orthocarbonate and lithium salt; alternatively, 30% -50%. When the mole percentage of the lithium salt satisfies the above range, the participation degree of the orthocarbonate around lithium ions can be further reduced, and the risk of decomposition of the orthocarbonate can be reduced; and can participate in the formation of SEI film, further improve the barrier propterty to the negative pole piece.
In any embodiment, the electrolyte further comprises an inorganic ceramic-based filler; optionally, the inorganic ceramic-based filler is selected from inorganic ceramic-based inert fillers and/or inorganic ceramic-based lithium ion conductor fillers.
Therefore, the inorganic ceramic inert filler and the plastic crystal composite are compounded to form the electrolyte, the inorganic ceramic inert filler can improve the integral mechanical strength of the electrolyte, and can promote the transmission of metal ions at the interface between the plastic crystal composite and the inorganic ceramic inert filler, so that the cycle performance of the secondary battery is improved.
According to the embodiment of the application, the inorganic ceramic lithium ion conductor filler and the plastic crystal compound are compounded to form the electrolyte, so that the mechanical strength of the whole electrolyte can be improved, the ion conductivity of the whole electrolyte can be improved, and the cycle performance of the secondary battery can be improved.
In any embodiment, the inorganic ceramic-based inert filler is selected from one or more of alumina, silica, titania, zinc oxide, magnesia, iron oxide, copper oxide, calcium oxide, chromium oxide, manganese oxide, cobalt oxide, and nickel oxide.
In any embodiment, the inorganic ceramic-based lithium ion conductor filler is selected from one or more of an oxide-based lithium ion conductor filler, a sulfide-based lithium ion conductor filler, and a halide-based lithium ion conductor filler.
The second aspect of the present application also provides a secondary battery comprising the electrolyte of any one of the embodiments of the first aspect of the present application.
In any embodiment, the secondary battery further comprises a negative electrode tab comprising a lithium element.
The third aspect of the application also provides a battery module comprising the secondary battery as the embodiment of the second aspect of the application.
The fourth aspect of the application also provides a battery pack comprising a battery module as an embodiment of the third aspect of the application.
The fifth aspect of the present application also provides an electric device comprising the secondary battery as the embodiment of the second aspect of the present application, the battery module as the embodiment of the third aspect of the present application, or the battery pack as the embodiment of the fourth aspect of the present application.
In order to more clearly illustrate the technical solutions of the embodiments of the present application, the drawings that are needed in the embodiments of the present application will be briefly described below, and it is obvious that the drawings described below are only some embodiments of the present application, and other drawings may be obtained according to the drawings without inventive effort for a person skilled in the art.
Fig. 1 is a schematic view of a secondary battery according to an embodiment of the present application.
Fig. 2 is an exploded view of the secondary battery according to an embodiment of the present application shown in fig. 1.
Fig. 3 is a schematic view of a battery module according to an embodiment of the present application.
Fig. 4 is a schematic view of a battery pack according to an embodiment of the present application.
Fig. 5 is an exploded view of the battery pack of the embodiment of the present application shown in fig. 4.
FIG. 6 is a schematic diagram of an electrical device according to an embodiment of the present application;
FIG. 7 is a DSC curve of the plastic composite of example 1 of the present application;
FIG. 8 is a graph showing the change trend of the ion conductivity of the plastic crystal composite according to example 1 of the present application with temperature;
FIG. 9 is a graph showing the change trend of the ion conductivity of the plastic crystal composite according to example 2 of the present application with temperature;
FIG. 10 is a graph of the sweep voltammogram of a button cell composed of the plastic-crystalline composite of example 1 of the present application;
FIG. 11 is a cycle chart of button cell composed of the plastic-crystalline composite material of example 1 of the present application;
fig. 12 is a graph showing the first cycle of the secondary battery composed of the plastic crystal composite according to example 1 of the present application.
The reference numerals are explained as follows:
1. A secondary battery; 11. and (3) outer packaging; 111. a top cover assembly; 112. a housing; 12. an electrode assembly; 10. a battery module; 20. a battery pack; 21. an upper case; 22. a lower box body; 30. and (5) an electric device.
The following detailed description specifically discloses embodiments of a secondary battery, a battery module, a battery pack, and an electric device of the present application. However, unnecessary detailed description may be omitted. For example, detailed descriptions of well-known matters and repeated descriptions of the actual same structure may be omitted. This is to avoid that the following description becomes unnecessarily lengthy, facilitating the understanding of those skilled in the art. Furthermore, the drawings and the following description are provided for a full understanding of the present application by those skilled in the art, and are not intended to limit the subject matter recited in the claims.
The "range" disclosed herein is defined in terms of lower and upper limits, with the given range being defined by the selection of a lower and an upper limit, the selected lower and upper limits defining the boundaries of the particular range. Ranges that are defined in this way can be inclusive or exclusive of the endpoints, and any combination can be made, i.e., any lower limit can be combined with any upper limit to form a range. For example, if ranges of 60-120 and 80-110 are listed for a particular parameter, it is understood that ranges of 60-110 and 80-120 are also contemplated. Furthermore, if the minimum range values 1 and 2 are listed, and if the maximum range values 3,4 and 5 are listed, the following ranges are all contemplated: 1-3, 1-4, 1-5, 2-3, 2-4 and 2-5. In the present application, unless otherwise indicated, the numerical range "a-b" represents a shorthand representation of any combination of real numbers between a and b, where a and b are both real numbers. For example, the numerical range "0-5" means that all real numbers between "0-5" have been listed throughout, and "0-5" is simply a shorthand representation of a combination of these values. When a certain parameter is expressed as an integer of 2 or more, it is disclosed that the parameter is, for example, an integer of 2,3,4, 5, 6, 7, 8, 9, 10, 11, 12 or the like.
All embodiments of the application and alternative embodiments may be combined with each other to form new solutions, unless otherwise specified. All technical features and optional technical features of the application may be combined with each other to form new technical solutions, unless specified otherwise.
All the steps of the present application may be performed sequentially or randomly, preferably sequentially, unless otherwise specified. For example, the method may include steps (a) and (b), and the method may include steps (a) and (b) performed sequentially, or may include steps (b) and (a) performed sequentially. For example, it is mentioned that the method may further comprise step (c), meaning that step (c) may be added to the method in any order, e.g. the method may comprise steps (a), (b) and (c), may also comprise steps (a), (c) and (b), may also comprise steps (c), (a) and (b), etc.
The terms "comprising" and "including" as used herein mean open ended or closed ended, unless otherwise noted. For example, "comprising" and "including" may mean that other components not listed may also be included or included, or that only listed components may be included or included.
The term "or" is inclusive in this application, unless otherwise specified. For example, the phrase "a or B" means "a, B, or both a and B. More specifically, either of the following conditions satisfies the condition "a or B": a is true (or present) and B is false (or absent); a is false (or absent) and B is true (or present); or both A and B are true (or present).
The term "alkyl" encompasses both straight and branched chain alkyl groups. For example, alkyl may be C1-C50 alkyl, C1-C40 alkyl, C1-C30 alkyl, C1-C20 alkyl, C1-C12 alkyl, C1-C10 alkyl, C1-C6 alkyl, C1-C4 alkyl. In some embodiments, alkyl groups include methyl, ethyl, propyl, isopropyl, butyl, isobutyl, sec-butyl, tert-butyl, cyclobutyl, pentyl, isopentyl, neopentyl, tert-pentyl, cyclopentyl, hexyl, cyclohexyl, heptyl, cycloheptyl, octyl, cyclooctyl, nonyl, decyl and the like. In addition, the alkyl group may be optionally substituted. The term "haloalkyl" means an alkyl group in which hydrogen atoms are partially or entirely substituted with halogen atoms, and the term "halogen atom" means a fluorine atom, a chlorine atom, a bromine atom, an iodine atom, or the like.
Throughout this specification, substituents of a compound are disclosed in groups or ranges. It is expressly intended that such description include each individual subcombination of the members of these groups and ranges. For example, the term "C1-C10 alkyl" is expressly contemplated to disclose C1、C2、C3、C4、C5、C6、C7、C8、C9、C10、C1～C10、C1～C9、C1～C8、C1～C7、C1～C6、C1～C5、C1～C4、C1～C3、C1～C2、C2～C10、C2～C9、C2～C8、C2～C7、C2～C6、C2～C5、C2～C4、C2～C3、C3～C10、C3～C9、C3～C8、C3～C7、C3～C6、C3～C5、C3～C4、C4～C10、C4～C9、C4～C8、C4～C7、C4～C6、C4～C5、C5～C10、C5～C9、C5～C8、C5～C7、C5～C6、C6～C10、C6～C9、C6～C8、C6～C7、C7～C10、C7～C9、C7～C8、C8～C10 and C8-C9 alkyl groups separately.
When the above groups are substituted, the substituents may be independently selected from halogen atoms.
In the related art, solid electrolyte is adopted as electrolyte of a secondary battery, and the solid electrolyte can not provide a smooth migration channel for metal ions well in the charging and discharging process of the secondary battery, so that the metal ions can not move between the positive electrode plate and the negative electrode plate smoothly, and the ion conductivity of the solid electrolyte is poor.
In view of this, the present inventors have improved the composition of the electrolyte from the viewpoint of increasing the ion conductivity of the electrolyte, and have proposed an electrolyte suitable for use in a secondary battery, and the present application will be described in detail.
Electrolyte composition
In a first aspect, embodiments of the present application provide an electrolyte comprising a plastic composite comprising an orthocarbonate and a lithium salt, the orthocarbonate comprising one or more of the compounds of formula I,
In formula I, R1 to R4 each independently represent an alkyl group or a haloalkyl group.
The orthocarbonate has solvent performance and can be mixed with lithium salt to form a plastic crystal compound, so that the ion conductivity can be improved, and although the reason for the improvement is not clear, the reason for the improvement of the ion conductivity may be that the plastic crystal compound has the characteristics of ordered positions and disordered orientations between a crystal state and a liquid state, and the plastic crystal compound has space defects due to the characteristics, and metal ions can be conducted in the space defects, so that the ion transmission efficiency can be improved.
The molecules of the plastic crystal composite have rotational freedom degree, which is beneficial to reducing the energy barrier of metal ion transition and promoting the plastic crystal composite to have higher ion conductivity at room temperature. The plastic crystal compound has relatively low rotation potential barrier, and the sliding between molecules is easy to realize, so that the plastic crystal compound has plasticity, and the ion transmission efficiency of the electrolyte can be further improved. In addition, the plasticity can ensure that the electrolyte can better infiltrate the positive electrode plate and/or the negative electrode plate when being applied to the secondary battery, and form good interface infiltration and contact with the positive electrode plate and/or the negative electrode plate, thereby improving the capacity release capability.
For example, when the electrolyte including the plastic-crystal composite is applied to the secondary battery, a relatively high temperature may be set to melt and place the plastic-crystal composite in a liquid state, the electrolyte is in a liquid state, the electrolyte in the liquid state is injected into the secondary battery, the electrolyte is gradually infiltrated on the positive electrode tab and/or the negative electrode tab, and after the electrolyte forms good interface infiltration with the positive electrode tab and/or the negative electrode tab, the temperature may be reduced to convert the plastic-crystal composite in the liquid state into the plastic state, thereby making the electrolyte appear in a solid state.
In addition, the oxidation stability of the electrolyte is relatively high and can reach 5V, so that the electrolyte can be matched with a high-voltage positive electrode plate when applied to a secondary battery, and the energy density of the secondary battery is further improved.
In view of the fact that the electrolyte is solid, when the electrolyte is applied to a secondary battery, side reactions are not easy to occur with the negative electrode plate, and therefore the cycle life of the secondary battery can be guaranteed; and the solid electrolyte is not easy to burn, and the safety performance is high.
According to the electrolyte provided by the embodiment of the application, the plastic crystal compound is formed by the orthocarbonate and the lithium salt, so that the ion conductivity of the electrolyte can be improved. When the electrolyte is applied to the secondary battery, the electrolyte has better infiltration performance with the positive electrode plate and/or the negative electrode plate, and can be matched with the high-voltage positive electrode plate due to relatively higher oxidation stability, so that the cycle performance of the secondary battery is improved. Since the solid electrolyte is not easily burned, the safety performance of the secondary battery can be ensured.
In some embodiments, R1 to R4 each independently represent an alkyl group, and the alkyl group may be a C1-C10 alkyl group. When R1 to R4 each independently represent a C1-C10 alkyl group, the kind of the alkyl group is not particularly limited and may be selected according to practical requirements, for example, a chain alkyl group and a cyclic alkyl group, and the chain alkyl group includes a straight chain alkyl group and a branched alkyl group. The cyclic alkyl group may have a substituent or may not have a substituent. The C1-C10 alkyl group may be one selected from the group consisting of methyl, ethyl, n-propyl, isopropyl, cyclopropyl, n-butyl, isobutyl, sec-butyl, tert-butyl, n-pentyl, isopentyl, neopentyl, cyclopentyl, n-hexyl, isohexyl, cyclohexyl, heptyl, cycloheptyl, octyl, cyclooctyl, nonyl and decyl.
The miscibility of the orthocarbonate and the lithium salt is relatively better, which is favorable for forming a plastic crystal compound.
In some embodiments, when the above-mentioned alkyl group having 1 to 10 carbon atoms is partially or completely substituted with one or more halogen atoms, a haloalkyl group having 1 to 10 carbon atoms is formed, and the number of halogen atoms and the substitution positions thereof are not particularly limited and may be selected according to practical requirements. For example, the number of substitution of halogen atoms may be 1,2, 3 or 4. When the number of halogen atoms substituted is 2 or more, the types of halogen atoms may be the same, may be completely different, or may be partially the same.
When the haloalkyl is C1-C10 haloalkyl, the miscibility of the orthocarbonate and lithium salt is relatively better, and the orthocarbonate and the lithium salt are favorable for forming a plastic crystal compound.
In some embodiments, the halogen atom is selected from one or both of F, cl; illustratively, the haloalkyl may be a fluoroalkyl. The electrolyte can be further inhibited from being oxidized due to the strong electron-withdrawing effect of the fluorine group, and the electrochemical window of the electrolyte is improved.
In some embodiments, the orthocarbonate comprises one or more of tetramethyl orthocarbonate, tetraethyl orthocarbonate, tetrapropyl orthocarbonate, tetrabutyl orthocarbonate, tetrapentyl orthocarbonate, tetrahexyl orthocarbonate, tetraheptyl orthocarbonate, tetraoctyl orthocarbonate, tetranonyl orthocarbonate, tetradecyl orthocarbonate, tetramethyl fluoroorthocarbonate, tetraethyl fluoroorthocarbonate, tetrapropyl fluoroorthocarbonate, tetrabutyl fluoroorthocarbonate, tetrapentyl fluoroorthocarbonate, tetrahexyl fluoroorthocarbonate, tetraheptyl fluoroorthocarbonate, tetraoctyl fluoroorthocarbonate, tetranonyl fluoroorthocarbonate, tetradecyl fluoroorthocarbonate, tetratrifluoromethoxy methane, tetrakis- (2, 2-trifluoroethoxy) -methane, and tetrakis- (3, 3-trifluoropropoxy) -methane.
The orthocarbonate has stronger mixing capability with lithium salt, and the formed plastic-crystal composite is easier to form because the phase change transformation entropy of the plastic-crystal composite from a plastic crystal state to a liquid state is lower.
In some embodiments, the orthocarbonate comprises one or more of tetramethyl orthocarbonate, tetraethyl orthocarbonate, tetrapropyl orthocarbonate, tetrabutyl orthocarbonate, tetrapentyl orthocarbonate, tetrahexyl orthocarbonate, tetraheptyl orthocarbonate, tetraoctyl orthocarbonate, tetranonyl orthocarbonate, tetradecyl orthocarbonate. The orthocarbonates and lithium salts are easier to form plastic crystal composites.
In some embodiments, the lithium salt includes one or more of a lithium sulfonimide salt, a lithium borate salt, lithium hexafluorophosphate, lithium perchlorate, lithium hexafluoroarsenate, and lithium trifluoromethane sulfonate.
The lithium salt can form a plastic crystal compound with the orthocarbonate easily, and can form a solid electrolyte interface (Solid Electrolyte Interphase, SEI) film on the negative electrode plate of the secondary battery, so that the negative electrode plate can be protected, the structural stability of the negative electrode plate is ensured, and the risk of side reaction between the negative electrode plate and electrolyte is reduced.
In some embodiments, the lithium sulfonimide salt includes one or more of lithium bis-fluorosulfonimide, lithium bis-fluoromethylsulfonimide, and lithium bis-pentafluoroethylsulfonimide. Optionally, the lithium sulfonimide salt comprises lithium bis-fluorosulfonimide and/or lithium bis-fluoromethylsulfonimide. Further alternatively, the lithium sulfonimide salt comprises lithium bis-fluorosulfonimide.
In some embodiments, the lithium borate salt includes one or more of lithium tetrafluoroborate, lithium dioxalate borate, and lithium difluorooxalato borate.
In some embodiments, the molar amount x of orthocarbonate and the molar amount y of lithium salt satisfy: x is more than or equal to 0.5 and y is more than or equal to 3.
When the molar amounts of the orthocarbonate and the lithium salt satisfy the above ranges, the participation of the orthocarbonate around lithium ions can be reduced, the risk of decomposition of the orthocarbonate can be reduced, and the oxidation stability of the electrolyte can be further improved. The molar amounts of orthocarbonate and lithium salt satisfy 0.5.ltoreq.x.ltoreq.y.ltoreq.3, alternatively 1.ltoreq.x.ltoreq.y.ltoreq.2. Illustratively, the ratio x of the molar amounts of orthocarbonate and lithium salt: y is 0.5, 0.6, 0.8, 0.9, 1, 1.2, 1.5, 1.6, 1.8, 2, 2.2, 2.5, 2.6, 2.8, 2.9, or 2, or may be a combination of any two of the foregoing values.
In some embodiments, the mole percent of orthocarbonate is 30% to 80% based on the total mass of orthocarbonate and lithium salt.
When the mole percentage of the orthocarbonate satisfies the above range, the mixing ability of the orthocarbonate and the lithium salt is relatively good, so that the molding compound is more easily formed. The mole percentage of the orthocarbonate is 30% -80%, alternatively 50% -70%. Illustratively, the mole percent of orthocarbonate is 30%, 35%, 38%, 40%, 45%, 50%, 55%, 60%, 65%, 70%, 75% or 80%, or may be a combination of any two of the foregoing values.
In some embodiments, the mole percent of lithium salt is 20% to 70% based on the total mass of the orthocarbonate and lithium salt; alternatively, 30% -50%.
When the mole percentage of the lithium salt satisfies the above range, the participation degree of the orthocarbonate around lithium ions can be further reduced, and the risk of decomposition of the orthocarbonate can be reduced; and can participate in the formation of SEI film, further improve the barrier propterty to the negative pole piece. The mole percent of the lithium salt is 20% -70%, alternatively 30% -50%. Illustratively, the mole percent of lithium salt is 20%, 25%, 30%, 35%, 40%, 45%, 50%, 55%, 60%, 65%, or 70%, or may be a combination of any two of the foregoing values.
In some embodiments, the electrolyte further comprises an inorganic ceramic-based filler. The inorganic ceramic filler has more defects, and is beneficial to the transmission of metal ions, so that the ion transmission efficiency of the electrolyte can be further improved; and the mechanical strength of the electrolyte can be improved.
Optionally, the inorganic ceramic-based filler is selected from inorganic ceramic-based inert fillers and/or inorganic ceramic-based lithium ion conductor fillers.
The inorganic ceramic inert filler and the plastic crystal composite are compounded to form the electrolyte, the inorganic ceramic inert filler can improve the integral mechanical strength of the electrolyte, and can promote the transmission of metal ions at the interface between the plastic crystal composite and the inorganic ceramic inert filler, so that the cycle performance of the secondary battery is improved.
The inorganic ceramic lithium ion conductor filler and the plastic crystal compound are compounded to form the electrolyte, and the inorganic ceramic lithium ion conductor filler can improve the integral mechanical strength of the electrolyte and the integral ion conductivity of the electrolyte, so that the cycle performance of the secondary battery is improved.
Illustratively, the inorganic ceramic-based inert filler is selected from one or more of aluminum oxide, silicon oxide, titanium oxide, zinc oxide, magnesium oxide, iron oxide, copper oxide, calcium oxide, chromium oxide, manganese oxide, cobalt oxide, and nickel oxide.
Illustratively, the inorganic ceramic-based lithium ion conductor filler is selected from one or more of an oxide-based lithium ion conductor filler, a sulfide-based lithium ion conductor filler, and a halide-based lithium ion conductor filler. For example, the oxide-based lithium ion conductor filler is selected from at least one of Lithium Lanthanum Zirconium Oxide (LLZO), lithium Lanthanum Titanium Oxide (LLTO), and lithium germanium aluminum phosphate (LATP). The sulfide type lithium ion conductor filler is at least one of lithium phosphorus sulfur (LiPS), lithium germanium phosphorus sulfur (LiGPS), lithium phosphorus sulfur chlorine (LiPSCl) and lithium germanium phosphorus sulfur chlorine (LiGPSCl). The halide lithium ion conductor filler is at least one of lithium indium chloride (LiInCl), lithium iridium chloride (LiYCl), lithium indium bromide (LiInBr) and lithium iridium bromide (LiYBa).
Secondary battery
In a second aspect, the present application provides a secondary battery. The secondary battery includes the electrolyte of any one of the embodiments of the first aspect of the present application.
According to the secondary battery provided by the embodiment of the application, the orthocarbonate and the lithium salt in the electrolyte can form a plastic crystal compound, so that the ion conductivity of the electrolyte is improved. The electrolyte has better infiltration performance with the positive electrode plate and/or the negative electrode plate, and can be matched with the high-voltage positive electrode plate due to relatively higher oxidation stability, so that the cycle performance of the secondary battery is improved. Since the solid electrolyte is not easily burned, the safety performance of the secondary battery can be ensured.
In some embodiments, the secondary battery has high metal ion transfer efficiency and is less prone to side reactions during cyclic charge and discharge at 10 ℃ to 80 ℃, especially at 40 ℃ to 50 ℃.
In some embodiments, when the charge-discharge current density of the secondary battery is 0.05mA/cm2 to 0.5mA/cm2, the current density is relatively high, and the charge-discharge time of the secondary battery can be shortened; and the electrolyte can provide a matched ion transport capacity to improve its cycling performance.
The secondary battery of the embodiment of the application further comprises a negative electrode plate, a positive electrode plate and a separation film. The isolating film is arranged between the positive pole piece and the negative pole piece to separate the positive pole piece and the negative pole piece.
[ Negative electrode sheet ]
The negative electrode plate comprises a negative electrode current collector and a negative electrode film layer arranged on at least one surface of the negative electrode current collector, wherein the negative electrode film layer comprises a negative electrode active material.
As an example, the anode current collector has two surfaces opposing in its own thickness direction, and the anode film layer is provided on either one or both of the two surfaces opposing the anode current collector.
In some embodiments, the negative electrode current collector may employ a metal foil or a composite current collector. For example, as the metal foil, copper foil may be used. The composite current collector may include a polymeric material base layer and a metal layer formed on at least one surface of the polymeric material base material. The composite current collector may be formed by forming a metal material (copper, copper alloy, nickel alloy, titanium alloy, silver alloy, etc.) on a polymer material substrate (such as a substrate of polypropylene (PP), polyethylene terephthalate (PET), polybutylene terephthalate (PBT), polystyrene (PS), polyethylene (PE), etc.).
In some embodiments, the anode active material may employ an anode active material for a battery, which is well known in the art. As an example, the anode active material may include at least one of the following materials: artificial graphite, natural graphite, soft carbon, hard carbon, silicon-based materials, tin-based materials, lithium titanate, metallic lithium, lithium alloys, sodium alloys, and the like. The silicon-based material may be at least one selected from elemental silicon, silicon oxygen compounds, silicon carbon composites, silicon nitrogen composites, and silicon alloys. The tin-based material may be at least one selected from elemental tin, tin oxide, and tin alloys. However, the present application is not limited to these materials, and other conventional materials that can be used as a battery anode active material may be used. These negative electrode active materials may be used alone or in combination of two or more.
Optionally, the negative electrode sheet comprises lithium element. In the process of charging and discharging the secondary battery, lithium ions are used as active ions and can stably migrate between the positive electrode plate and the negative electrode plate, so that the electrochemical performance of the secondary battery is ensured. The plastic crystal compound in the electrolyte has lower reactivity to the negative electrode plate, so that the risk of side reaction between the electrolyte and the negative electrode plate can be reduced, and the risk of lithium dendrite on the negative electrode plate is further reduced; and the electrolyte is injected into the secondary battery at a relatively high temperature to be matched with the isolating film, and the electrolyte is in a solid state, so that the risk that lithium dendrites pierce the isolating film can be further reduced, the occurrence of internal short circuit can be blocked to a certain extent, and the safety performance of the secondary battery is improved.
The lithium element may be in the form of a metal simple substance or an alloy as the anode active material. Optionally, the alloy may also include one or more of tin, zinc, aluminum, magnesium, silver, gold, gallium, indium, and foil; further optionally, the alloy further comprises one or more of boron, carbon and silicon. The alloy not only can ensure conductivity, but also can improve the stability between the negative electrode plate and electrolyte.
In some embodiments, the negative electrode film layer further optionally includes a binder. The binder may be at least one selected from Styrene Butadiene Rubber (SBR), polyacrylic acid (PAA), sodium Polyacrylate (PAAs), polyacrylamide (PAM), polyvinyl alcohol (PVA), sodium Alginate (SA), polymethacrylic acid (PMAA) and carboxymethyl chitosan (CMCS).
In some embodiments, the negative electrode film layer further optionally includes a conductive agent. The conductive agent is at least one selected from superconducting carbon, acetylene black, carbon black, ketjen black, carbon dots, carbon nanotubes, graphene and carbon nanofibers.
In some embodiments, the negative electrode film layer may optionally further include other adjuvants, such as thickening agents (e.g., sodium carboxymethyl cellulose (CMC-Na)), and the like.
In some embodiments, the negative electrode sheet may be prepared by: dispersing the above components for preparing the negative electrode sheet, such as a negative electrode active material, a conductive agent, a binder and any other components, in a solvent (e.g., deionized water) to form a negative electrode slurry; and coating the negative electrode slurry on a negative electrode current collector, and obtaining a negative electrode plate after the procedures of drying, cold pressing and the like.
[ Positive electrode sheet ]
The positive pole piece comprises a positive current collector and a positive film layer arranged on at least one surface of the positive current collector, wherein the positive film layer comprises a positive active material.
As an example, the positive electrode current collector has two surfaces opposing in its own thickness direction, and the positive electrode film layer is provided on either one or both of the two surfaces opposing the positive electrode current collector.
In some embodiments, the positive current collector may employ a metal foil or a composite current collector. For example, as the metal foil, aluminum foil may be used. The composite current collector may include a polymeric material base layer and a metal layer formed on at least one surface of the polymeric material base layer. The composite current collector may be formed by forming a metal material (aluminum, aluminum alloy, nickel alloy, titanium alloy, silver alloy, etc.) on a polymer material substrate (such as a substrate of polypropylene (PP), polyethylene terephthalate (PET), polybutylene terephthalate (PBT), polystyrene (PS), polyethylene (PE), etc.).
In some embodiments, the positive electrode active material may employ a positive electrode active material for a battery, which is well known in the art. As an example, the positive electrode active material may include at least one of the following materials: olivine structured lithium-containing phosphates, lithium transition metal oxides and their respective modified compounds. However, the present application is not limited to these materials, and other conventional materials that can be used as a battery positive electrode active material may be used. These positive electrode active materials may be used alone or in combination of two or more. Examples of the olivine-structured lithium-containing phosphate may include, but are not limited to, at least one of lithium iron phosphate (e.g., liFePO 4 (also simply LFP)), a composite of lithium iron phosphate and carbon, a composite of lithium manganese phosphate (e.g., liMnPO 4), a composite of lithium manganese phosphate and carbon, a composite of lithium iron phosphate and manganese phosphate, and a composite of lithium manganese iron phosphate and carbon.
In some embodiments, the positive electrode film layer further optionally includes a binder. As an example, the binder may include at least one of polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), a vinylidene fluoride-tetrafluoroethylene-propylene terpolymer, a vinylidene fluoride-hexafluoropropylene-tetrafluoroethylene terpolymer, a tetrafluoroethylene-hexafluoropropylene copolymer, and a fluoroacrylate resin.
In some embodiments, the positive electrode film layer further optionally includes a conductive agent. As an example, the conductive agent may include at least one of superconducting carbon, acetylene black, carbon black, ketjen black, carbon dots, carbon nanotubes, graphene, and carbon nanofibers.
In some embodiments, the positive electrode sheet may be prepared by: dispersing the above components for preparing the positive electrode sheet, such as the positive electrode active material, the conductive agent, the binder and any other components, in a solvent (such as N-methylpyrrolidone) to form a positive electrode slurry; and (3) coating the positive electrode slurry on a positive electrode current collector, and obtaining a positive electrode plate after the procedures of drying, cold pressing and the like.
[ Isolation Membrane ]
In some embodiments, a separator is further included in the secondary battery. The type of the separator is not particularly limited, and any known porous separator having good chemical stability and mechanical stability can be used.
In some embodiments, the material of the isolation film may be at least one selected from glass fiber, non-woven fabric, polyethylene, polypropylene and polyvinylidene fluoride. The separator may be a single-layer film or a multilayer composite film, and is not particularly limited. When the separator is a multilayer composite film, the materials of the respective layers may be the same or different, and are not particularly limited.
In some embodiments, the positive electrode tab, the negative electrode tab, and the separator may be manufactured into an electrode assembly through a winding process or a lamination process.
In some embodiments, the secondary battery may include an outer package. The outer package may be used to encapsulate the electrode assembly and electrolyte described above.
In some embodiments, the outer package of the secondary battery may be a hard case, such as a hard plastic case, an aluminum case, a steel case, or the like. The exterior package of the secondary battery may also be a pouch type pouch, for example. The material of the flexible bag may be plastic, and examples of the plastic include polypropylene, polybutylene terephthalate, and polybutylene succinate. The shape of the secondary battery is not particularly limited in the present application, and may be cylindrical, square, or any other shape. For example, fig. 1 and 2 are secondary batteries 1 of a square structure as one example.
In some embodiments, secondary battery 1 includes an outer package 11. The overpack 11 includes a top cover assembly 111 and a housing 112. The positive electrode sheet, the negative electrode sheet, and the separator constitute the electrode assembly 12, which is housed in the case 112, and the electrolyte is also housed in the case 112. The positive pole piece or the negative pole piece comprises a pole lug. During the charge and discharge of the secondary battery 1, metal ions are inserted and extracted back and forth between the positive electrode tab and the negative electrode tab. The electrolyte plays a role in ion conduction between the positive electrode plate and the negative electrode plate. The isolating film is arranged between the positive pole piece and the negative pole piece, and mainly plays a role in preventing the positive pole piece and the negative pole piece from being short-circuited, and meanwhile, active ions can pass through the isolating film. Specifically, the secondary battery 1 may be a wound or laminated battery such as a lithium ion battery, a sodium ion battery, but is not limited thereto.
Alternatively, the housing 112 may include a bottom plate and a side plate coupled to the bottom plate, the bottom plate and the side plate enclosing to form the receiving cavity. The housing 112 has an opening communicating with the accommodating chamber, and the cap assembly 111 can be cap-provided to the opening to close the accommodating chamber. The positive electrode sheet, the negative electrode sheet, and the separator may be formed into the electrode assembly 12 through a winding process or a lamination process. The electrode assembly 12 is packaged in the receiving chamber. Electrolyte is impregnated in the electrode assembly 12. The number of electrode assemblies 12 included in the secondary battery 1 may be one or more, and those skilled in the art may select according to specific practical requirements.
In some embodiments, the secondary battery 1 may be assembled into a battery. The battery may be a battery module or a battery includes. For example, the number of secondary batteries 1 included in the battery module may be one or more, and a specific number may be selected by those skilled in the art according to the application and capacity of the battery module.
Fig. 3 is a battery module 10 as one example. Referring to fig. 3, in the battery module 10, a plurality of secondary batteries 1 may be sequentially arranged in the longitudinal direction of the battery module 10. Of course, the arrangement may be performed in any other way. The plurality of secondary batteries 1 may be further fixed by fasteners. Alternatively, the battery module 10 may further include a case having an accommodating space in which the plurality of secondary batteries 1 are accommodated.
In some embodiments, the battery modules 10 may be assembled into a battery pack, and the number of battery modules 10 included in the battery pack may be one or more, and a specific number may be selected by those skilled in the art according to the application and capacity of the battery pack. Of course, the battery pack may be directly composed of a plurality of secondary batteries 1.
Fig. 4 and 5 are battery packs 20 as one example. Referring to fig. 4 and 5, a battery case and a plurality of battery modules 10 disposed in the battery case may be included in the battery pack 20. The battery case includes an upper case 21 and a lower case 22, and the upper case 21 can be covered on the lower case 22 and forms a closed space for accommodating the battery module 10. The plurality of battery modules 10 may be arranged in the battery case in any manner.
In addition, the application also provides an electric device which comprises at least one of the secondary battery, the battery module or the battery pack. The secondary battery, the battery module, or the battery pack may be used as a power source of the power consumption device, and may also be used as an energy storage unit of the power consumption device. The power utilization device may include mobile devices (e.g., cell phones, notebook computers, etc.), electric vehicles (e.g., electric-only vehicles, hybrid electric vehicles, plug-in hybrid electric vehicles, electric bicycles, electric scooters, electric golf carts, electric trucks, etc.), electric trains, ships and satellites, energy storage systems, etc., but is not limited thereto. As the electricity consumption device, a secondary battery, a battery module, or a battery pack may be selected according to the use requirements thereof.
Fig. 6 is an electrical device 30 as one example. The electric device 30 is a pure electric vehicle, a hybrid electric vehicle, a plug-in hybrid electric vehicle, or the like. In order to meet the high power and high energy density requirements of the secondary battery of the power consumption device 30, a battery pack or a battery module may be employed. As another example, the device may be a cell phone, tablet computer, notebook computer, or the like. The device is generally required to be light and thin, and a secondary battery can be used as a power source.
Examples
Hereinafter, embodiments of the present application are described. The following examples are illustrative only and are not to be construed as limiting the application. The examples are not to be construed as limiting the specific techniques or conditions described in the literature in this field or as per the specifications of the product. The reagents or apparatus used were conventional products commercially available without the manufacturer's attention.
Example 1
1. Preparation of positive electrode plate
Aluminum foil with a thickness of 8 μm was used as the positive electrode current collector. Fully stirring and mixing positive active material nickel cobalt lithium manganate (NMC), conductive agent acetylene black and binder polyvinylidene fluoride (PVDF) in a proper amount of N-methyl pyrrolidone (NMP) solvent according to a weight ratio of 98:1:1, so that uniform positive slurry is formed; and coating the positive electrode slurry on the surface of a positive electrode current collector, and drying to obtain a positive electrode plate.
2. Preparation of negative electrode plate
A50 μm metal lithium foil was used as the negative electrode tab.
3. Preparation of electrolyte
The lithium bis (fluorosulfonyl) imide salt Y is taken, tetraethyl orthocarbonate solvent X is added, and stirring is carried out at 60 ℃ until a colorless transparent solution is formed. Cooling to room temperature and standing for 2 hours, wherein the solution is solidified, and the molar quantity of the lithium difluorosulfimide salt Y is 1g/mol and the molar quantity of the tetraethyl orthocarbonate solvent X is 1.5g/mol.
4. Preparation of secondary battery
And sequentially laminating an anode plate, a separation film (PP/PE/PP composite film) and a cathode plate, wrapping the anode plate, the separation film (PP/PE/PP composite film) and the cathode plate in an aluminum plastic film to form a laminated cell, injecting 0.3g of electrolyte into the cell at 60 ℃, carrying out vacuum hot-pressing packaging on the aluminum plastic film, standing at 60 ℃ for at least 6 hours, cooling to 30 ℃, standing at 30 ℃ for at least 6 hours until the electrolyte is solidified, and then carrying out hot-pressing, formation and other procedures to obtain the secondary battery.
Examples 2 to 7
Unlike example 1, examples 2 to 7 employed different orthocarbonates.
Examples 8 to 10
Unlike example 1, examples 8 to 10 employ different lithium salts.
Examples 11 to 12
Unlike example 1, examples 11 to 12 add an inorganic ceramic filler to the electrolyte.
Examples 13 to 20
Unlike example 1, the molar percentage amounts of lithium salts of examples 13 to 20 are different.
Example 21
Unlike example 1, example 21 employed a different negative electrode sheet.
Comparative example 1
Unlike example 1, no lithium salt was added in comparative example 1.
Comparative example 2
Unlike example 1, comparative example 2 uses a different lithium salt, which does not form a plastic composite with orthocarbonate.
Table 1 shows the substances and the relevant parameters of the examples and comparative examples.
In table 1, liFSI represents lithium bis-fluorosulfonyl imide, liBF 4 represents lithium tetrafluoroborate, liPF 6 lithium hexafluorophosphate, CF 3SO 3 lithium trifluoromethylsulfonate, liBOB lithium dioxaborate; al 2O 3 represents aluminum oxide; LLZO represents lithium lanthanum zirconium oxide.
Test part
1. Electrolyte condition detection
The phase transition point and the heat of transformation of the plastic-crystal composite in the electrolyte were measured by differential calorimetric scanning (DIFFERENTIAL SCANNING calorimetry, DSC).
And (3) using STA449F3 test electrolyte produced by German fly-resistance instrument manufacturing company to start temperature rising experiment on homogeneous mixture of lithium salt and orthocarbonate from room temperature, wherein the temperature rising speed is 2 ℃/min until 100 ℃ is cut off, and recording heat release and absorption data in the temperature rising process to analyze the phase transition temperature and whether the transition temperature of the material is within the range of a plastic crystal material interval.
2. Determination of ion conductivity of electrolyte
Two stainless steel sheets SUS are used as blocking electrodes, and are placed on two sides of a circular polyimide film with known thickness and perforated middle to form the button cell. After melting the electrolyte at 60 ℃, the electrolyte was added to the pores of the cyclic polyimide film, and the volume between the stainless steel sheets SUS was filled.
The impedance test is carried out on the button cell formed by the method at different temperatures, the x-axis intercept is the bulk ion transmission resistance R, and the thickness t of the polyimide film and the mesoporous area S can be obtained by the following formula: σ=t/RS calculates the ion conductivity of the above electrolyte for lithium ions at different temperatures.
3. Determination of the oxidative stability of an electrolyte
The button cell was formed by injecting molten electrolyte into a separator film using a 50 μm metal lithium foil as a negative electrode, an aluminum foil as a positive electrode, and a polyethylene porous film as a separator film. The formed coin cell was allowed to stand for 3 hours at 40 ℃ before the sweep voltammogram (LSV) test was performed: the voltage interval was open-circuit voltage-6V, the voltage sweep rate was set to 1mV/s, and the corrosion current was recorded, but the voltage at which the corrosion current density reached 10. Mu.A/cm 2 was recorded as the oxidation stability threshold, which was used to evaluate the oxidation stability, the higher the threshold, the better the oxidation stability.
4. Cycle performance of secondary battery
4.1 Determination of the Voltage Chart
The button cell was formed by injecting molten electrolyte into a separator film using a 50 μm metal lithium foil as a negative electrode, an aluminum foil as a positive electrode, and a polyethylene porous film as a separator film. The formed coin cell was left to stand at 40 ℃ for 3 hours, after which the coin cell was cycled from low to high current density to obtain a voltage profile. Specifically, the coin cell was cycled 5 times at a current density of 0.1mA/cm 2、0.2mA/cm 2 and 0.4mA/cm 2, respectively, and a capacity density of 0.25mAh/cm 2, respectively.
4.2 Cycle life
The test conditions are normal temperature, the manufactured secondary battery is charged at 0.05C multiplying power and discharged at 0.05C multiplying power, full charge discharge cycle test is carried out until the capacity of the secondary battery is reduced to 80% of the initial capacity, the test is stopped, and the number of cycles is recorded.
Test results
The effect of the electrolyte of the present application on improving the cycle performance of the secondary battery is shown in table 2,
As can be seen from Table 2, examples 1 to 7 employ different orthocarbonates, which can form a plastic composite with lithium salt Y at room temperature. And the alkyl chain in the orthocarbonate is lengthened, the ion conductivity of the plastic crystal composite is reduced, the cycle performance of the secondary battery is reduced, but the oxidation stability of the plastic crystal composite is improved. In particular, when R1 to R4 in the orthocarbonate each independently represent a C1 to C10 alkyl group, the plastic crystal composite can achieve both ion conductivity and oxidation stability. When the alkyl chain in the orthocarbonate is substituted with fluorine, the oxidation stability of the electrolyte can be stabilized.
In examples 1, 8 to 10, different lithium salts Y and tetraethyl orthocarbonate are used to form a plastic crystal composite, and the plastic crystal composite has high ion conductivity and relatively high oxidation stability.
Examples 11 and 12, the addition of the inorganic filler to example 1, the filler can improve the mechanical properties of the electrolyte and can ensure the cycle performance of the secondary battery.
In examples 1, 13 to 20, the orthocarbonate and the lithium salt are used in different molar ratios, and the properties of the formed plastic-crystal composite can be adjusted by controlling the molar ratio. Especially when x is more than or equal to 0.5 and y is more than or equal to 3, the orthocarbonate and the lithium salt can form a plastic crystal structure more easily at room temperature.
In example 1, the use of metallic lithium as the negative electrode tab can ensure the cycle performance of the secondary battery as compared to example 21, thereby confirming that the electrolyte of example 1 can maintain the stability of the negative electrode tab and can reduce the risk of occurrence of lithium dendrites.
Fig. 7 shows the DSC curve of the plastic composite of example 1, and as can be seen from fig. 7, the plastic composite has a distinct endothermic peak at about 57 ℃, meaning that the temperature undergoes a phase transition from solid to liquid. The entropy of the process was calculated to be 17.96J/(mol.K), which is less than the critical value of 20J/(mol.K). This indicates that the material has a plastic crystal structure from room temperature to 57 ℃. In fig. 7, T represents temperature.
Fig. 8 shows a graph of the change of the ion conductivity of the plastic-crystal composite of example 1 with the change of temperature, fig. 9 shows a graph of the change of the ion conductivity of the plastic-crystal composite of example 2 with the change of temperature, and as can be seen from fig. 8 and 9, the ion conductivity of the button cell composed of the plastic-crystal composite of example 1 at different temperatures is different, and in a certain temperature range, the ion conductivity increases with the increase of temperature. In fig. 8 and 9, λ represents the ion conductivity, and T represents the temperature.
Fig. 10 shows a sweep voltammogram of a coin cell composed of the plastic crystal composite of example 1, and as can be seen from fig. 10, the coin cell composed of the plastic crystal composite of example 1 still has an oxidation corrosion current of less than 25 mua/cm 2 under conditions of 5V for metallic lithium potential, thereby demonstrating that the solid-state plastic crystal electrolyte has excellent oxidation stability.
Fig. 11 shows a cycle chart of the coin cell composed of the plastic composite of example 1, and it can be seen from fig. 11 that the coin cell composed of the plastic composite of example can stably cycle at a current density of 0.1mA/cm 2、0.2mA/cm 2, can generate more significant polarization at a current density of 0.4mA/cm 2, and has a more significant increase in overpotential with an increase in deposition capacity at 40 ℃.
Fig. 12 shows a first cycle chart of the secondary battery composed of the plastic crystal composite of example 1, and as can be seen from fig. 12, the secondary battery can stably circulate and release more than 95% of rated capacity, and the first cycle coulombic efficiency is relatively consistent with the authorized coulombic efficiency of the ternary positive electrode in a liquid system. In fig. 12, Q represents capacity, and U represents voltage.
According to the analysis, the ion conductivity and the oxidation stability of the plastic crystal composite can be improved by regulating and controlling the plastic crystal structure in the plastic crystal composite, so that the cycle performance of the secondary battery can be improved.
While the application has been described with reference to a preferred embodiment, various modifications may be made and equivalents may be substituted for elements thereof without departing from the scope of the application. In particular, the technical features mentioned in the respective embodiments may be combined in any manner as long as there is no structural conflict. The present application is not limited to the specific embodiments disclosed herein, but encompasses all technical solutions falling within the scope of the claims.
Claims (12)
- An electrolyte comprising a plastic-crystalline composite comprising an orthocarbonate and a lithium salt, the orthocarbonate comprising one or more of the compounds of formula I,In formula I, R1 to R4 each independently represent an alkyl group or a haloalkyl group.
- The electrolyte according to claim 1, wherein,The alkyl is C1-C10 alkyl; and/orThe haloalkyl is a C1-C10 haloalkyl.
- The electrolyte according to claim 1 or 2, wherein the haloalkyl is a fluoroalkyl.
- The electrolyte according to any one of claim 1 to 3, wherein,The orthocarbonates include tetramethyl orthocarbonate, tetraethyl orthocarbonate, tetrapropyl orthocarbonate, tetrabutyl orthocarbonate, tetrapentyl orthocarbonate, tetrahexyl orthocarbonate, tetraheptyl orthocarbonate, tetraoctyl orthocarbonate, tetranonyl orthocarbonate, tetradecyl orthocarbonate, tetramethyl orthocarbonate, tetraethyl fluoroorthocarbonate, tetrapropyl fluoroorthocarbonate, tetrabutyl fluoroorthocarbonate, tetrapentyl fluoroorthocarbonate, tetrahexyl fluoroorthocarbonate, tetraheptyl fluoroorthocarbonate, tetraoctyl fluoroorthocarbonate, tetranonyl fluoroorthocarbonate, tetradecyl fluoroorthocarbonate, tetratrifluoromethoxy methane, tetrakis- (2, 2-trifluoroethoxy) -methane, tetrakis- (3, 3-trifluoropropoxy) -methane, methyltriethyl orthocarbonate, dimethyldiethyl orthocarbonate, ethyltrimethyl orthocarbonate, methyltripropyl orthocarbonate, dimethylpropyl orthocarbonate, propyltrimethyl orthocarbonate, ethyltripropyl orthocarbonate, diethyldipropyl orthocarbonate, tripropyl orthodipropyl carbonate, and trimethyldibutyl orthocarbonate;optionally, the orthocarbonate comprises one or more of tetramethyl orthocarbonate, tetraethyl orthocarbonate, tetrapropyl orthocarbonate, tetrabutyl orthocarbonate, tetrapentyl orthocarbonate, tetrahexyl orthocarbonate, tetraheptyl orthocarbonate, tetraoctyl orthocarbonate, tetranonyl orthocarbonate and tetradecyl orthocarbonate.
- The electrolyte according to any one of claims 1 to 4, wherein,The lithium salt comprises one or more of lithium sulfonimide salt, lithium borate salt, lithium hexafluorophosphate, lithium perchlorate, lithium hexafluoroarsenate and lithium trifluoromethane sulfonate;Optionally, the lithium sulfonimide salt comprises one or more of lithium bis (fluorosulfonyl) imide, lithium bis (fluoromethylsulfonyl) imide and lithium bis (pentafluoroethylsulfonyl) imide; further alternatively, the lithium sulfonimide salt comprises lithium bis (fluorosulfonyl) imide and/or lithium bis (fluoromethylsulfonyl) imide; further alternatively, the lithium sulfonimide salt comprises lithium bis-fluorosulfonimide;Optionally, the lithium borate salt includes one or more of lithium tetrafluoroborate, lithium dioxalate borate, and lithium difluorooxalato borate.
- The electrolyte according to any one of claims 1 to 5, wherein,The molar amount x of the orthocarbonate and the molar amount y of the lithium salt satisfy: x is more than or equal to 0.5 and y is more than or equal to 3;alternatively, 1.ltoreq.x.ltoreq.y.ltoreq.2.
- The electrolyte according to any one of claims 1 to 6, wherein,The mole percentage of the orthocarbonate is 30% -80% based on the total mass of the orthocarbonate and the lithium salt; alternatively, 50% -70%; and/orThe mole percentage of the lithium salt is 20-70% based on the total mass of the orthocarbonate and the lithium salt; alternatively, 30% -50%.
- The electrolyte according to any one of claims 1 to 7, wherein,The electrolyte also comprises inorganic ceramic filler; optionally, the inorganic ceramic-based filler is selected from inorganic ceramic-based inert fillers and/or inorganic ceramic-based lithium ion conductor fillers;Further alternatively, the inorganic ceramic-based inert filler is selected from one or more of alumina, silica, titania, zinc oxide, magnesia, iron oxide, copper oxide, calcium oxide, chromium oxide, manganese oxide, cobalt oxide, and nickel oxide;Further alternatively, the inorganic ceramic-based lithium ion conductor filler is selected from one or more of an oxide-based lithium ion conductor filler, a sulfide-based lithium ion conductor filler, and a halide-based lithium ion conductor filler.
- A secondary battery comprising the electrolyte according to any one of claims 1 to 8;optionally, the secondary battery further comprises a negative electrode tab, wherein the negative electrode tab comprises lithium element.
- A battery module comprising the secondary battery according to claim 9.
- A battery pack comprising the battery module of claim 10.
- An electric device comprising the secondary battery according to claim 9, the battery module according to claim 10, or the battery pack according to claim 11.
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| PCT/CN2022/094196 WO2023221113A1 (en) | 2022-05-20 | 2022-05-20 | Electrolyte, secondary battery, battery module, battery pack, and electric device |
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| JP2012119151A (en) * | 2010-11-30 | 2012-06-21 | Sony Corp | Nonaqueous electrolyte secondary battery, and nonaqueous electrolyte |
| CN106816627A (en) * | 2016-11-29 | 2017-06-09 | 中国电子科技集团公司第十八研究所 | Composite plastic crystal polymer electrolyte material and preparation method thereof |
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