CN114267881A - Battery with a battery cell - Google Patents
Battery with a battery cell Download PDFInfo
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- CN114267881A CN114267881A CN202111566903.2A CN202111566903A CN114267881A CN 114267881 A CN114267881 A CN 114267881A CN 202111566903 A CN202111566903 A CN 202111566903A CN 114267881 A CN114267881 A CN 114267881A
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- electrolyte
- battery
- negative plate
- carbonate
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- 239000003792 electrolyte Substances 0.000 claims abstract description 82
- 239000012528 membrane Substances 0.000 claims abstract description 9
- -1 nitrogen-containing compound Chemical class 0.000 claims description 36
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 10
- FKRCODPIKNYEAC-UHFFFAOYSA-N ethyl propionate Chemical compound CCOC(=O)CC FKRCODPIKNYEAC-UHFFFAOYSA-N 0.000 claims description 10
- 239000011356 non-aqueous organic solvent Substances 0.000 claims description 10
- 239000000654 additive Substances 0.000 claims description 8
- 230000000996 additive effect Effects 0.000 claims description 8
- 229910052799 carbon Inorganic materials 0.000 claims description 8
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 claims description 7
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 claims description 7
- 229910003002 lithium salt Inorganic materials 0.000 claims description 7
- 159000000002 lithium salts Chemical class 0.000 claims description 7
- BTBUEUYNUDRHOZ-UHFFFAOYSA-N Borate Chemical compound [O-]B([O-])[O-] BTBUEUYNUDRHOZ-UHFFFAOYSA-N 0.000 claims description 6
- 125000003118 aryl group Chemical group 0.000 claims description 6
- 150000007942 carboxylates Chemical class 0.000 claims description 6
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 claims description 5
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 claims description 5
- 150000003949 imides Chemical class 0.000 claims description 5
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 claims description 4
- 125000000217 alkyl group Chemical group 0.000 claims description 4
- DKPFZGUDAPQIHT-UHFFFAOYSA-N butyl acetate Chemical compound CCCCOC(C)=O DKPFZGUDAPQIHT-UHFFFAOYSA-N 0.000 claims description 4
- 150000001721 carbon Chemical group 0.000 claims description 4
- OBNCKNCVKJNDBV-UHFFFAOYSA-N ethyl butyrate Chemical compound CCCC(=O)OCC OBNCKNCVKJNDBV-UHFFFAOYSA-N 0.000 claims description 4
- MLFHJEHSLIIPHL-UHFFFAOYSA-N isoamyl acetate Chemical compound CC(C)CCOC(C)=O MLFHJEHSLIIPHL-UHFFFAOYSA-N 0.000 claims description 4
- PGMYKACGEOXYJE-UHFFFAOYSA-N pentyl acetate Chemical compound CCCCCOC(C)=O PGMYKACGEOXYJE-UHFFFAOYSA-N 0.000 claims description 4
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 claims description 4
- 239000002904 solvent Substances 0.000 claims description 4
- 125000001424 substituent group Chemical group 0.000 claims description 4
- 150000001733 carboxylic acid esters Chemical class 0.000 claims description 3
- YKYONYBAUNKHLG-UHFFFAOYSA-N n-Propyl acetate Natural products CCCOC(C)=O YKYONYBAUNKHLG-UHFFFAOYSA-N 0.000 claims description 3
- 229940090181 propyl acetate Drugs 0.000 claims description 3
- NQPDZGIKBAWPEJ-UHFFFAOYSA-N valeric acid Chemical compound CCCCC(O)=O NQPDZGIKBAWPEJ-UHFFFAOYSA-N 0.000 claims description 3
- PXGOKWXKJXAPGV-UHFFFAOYSA-N Fluorine Chemical compound FF PXGOKWXKJXAPGV-UHFFFAOYSA-N 0.000 claims description 2
- JGFBQFKZKSSODQ-UHFFFAOYSA-N Isothiocyanatocyclopropane Chemical compound S=C=NC1CC1 JGFBQFKZKSSODQ-UHFFFAOYSA-N 0.000 claims description 2
- 125000003342 alkenyl group Chemical group 0.000 claims description 2
- 125000003545 alkoxy group Chemical group 0.000 claims description 2
- PWLNAUNEAKQYLH-UHFFFAOYSA-N butyric acid octyl ester Natural products CCCCCCCCOC(=O)CCC PWLNAUNEAKQYLH-UHFFFAOYSA-N 0.000 claims description 2
- 150000004649 carbonic acid derivatives Chemical group 0.000 claims description 2
- 125000004185 ester group Chemical group 0.000 claims description 2
- 229910052736 halogen Inorganic materials 0.000 claims description 2
- 150000002367 halogens Chemical class 0.000 claims description 2
- GJRQTCIYDGXPES-UHFFFAOYSA-N iso-butyl acetate Natural products CC(C)COC(C)=O GJRQTCIYDGXPES-UHFFFAOYSA-N 0.000 claims description 2
- 229940117955 isoamyl acetate Drugs 0.000 claims description 2
- FGKJLKRYENPLQH-UHFFFAOYSA-M isocaproate Chemical compound CC(C)CCC([O-])=O FGKJLKRYENPLQH-UHFFFAOYSA-M 0.000 claims description 2
- OQAGVSWESNCJJT-UHFFFAOYSA-N isovaleric acid methyl ester Natural products COC(=O)CC(C)C OQAGVSWESNCJJT-UHFFFAOYSA-N 0.000 claims description 2
- UUIQMZJEGPQKFD-UHFFFAOYSA-N n-butyric acid methyl ester Natural products CCCC(=O)OC UUIQMZJEGPQKFD-UHFFFAOYSA-N 0.000 claims description 2
- MCSINKKTEDDPNK-UHFFFAOYSA-N propyl propionate Chemical compound CCCOC(=O)CC MCSINKKTEDDPNK-UHFFFAOYSA-N 0.000 claims description 2
- 239000000126 substance Substances 0.000 claims description 2
- 230000000052 comparative effect Effects 0.000 description 18
- 239000007773 negative electrode material Substances 0.000 description 10
- 238000011056 performance test Methods 0.000 description 10
- 238000002360 preparation method Methods 0.000 description 10
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 9
- 229920001577 copolymer Polymers 0.000 description 9
- 229910052744 lithium Inorganic materials 0.000 description 9
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 8
- 229910052782 aluminium Inorganic materials 0.000 description 8
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 8
- 239000011889 copper foil Substances 0.000 description 8
- 239000011888 foil Substances 0.000 description 8
- 238000002156 mixing Methods 0.000 description 8
- 239000000203 mixture Substances 0.000 description 8
- 239000002002 slurry Substances 0.000 description 8
- 239000011230 binding agent Substances 0.000 description 7
- 239000011521 glass Substances 0.000 description 7
- 230000014759 maintenance of location Effects 0.000 description 7
- 238000000034 method Methods 0.000 description 7
- 239000010410 layer Substances 0.000 description 6
- 230000008569 process Effects 0.000 description 6
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- 239000002033 PVDF binder Substances 0.000 description 5
- 239000006258 conductive agent Substances 0.000 description 5
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 5
- 238000011160 research Methods 0.000 description 5
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 4
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 4
- 230000009471 action Effects 0.000 description 4
- 239000011248 coating agent Substances 0.000 description 4
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- 239000007774 positive electrode material Substances 0.000 description 4
- 239000002109 single walled nanotube Substances 0.000 description 4
- 238000009736 wetting Methods 0.000 description 4
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 3
- 239000004698 Polyethylene Substances 0.000 description 3
- DPXJVFZANSGRMM-UHFFFAOYSA-N acetic acid;2,3,4,5,6-pentahydroxyhexanal;sodium Chemical class [Na].CC(O)=O.OCC(O)C(O)C(O)C(O)C=O DPXJVFZANSGRMM-UHFFFAOYSA-N 0.000 description 3
- 229910021383 artificial graphite Inorganic materials 0.000 description 3
- 239000002041 carbon nanotube Substances 0.000 description 3
- 239000001768 carboxy methyl cellulose Substances 0.000 description 3
- 150000001768 cations Chemical class 0.000 description 3
- 238000005056 compaction Methods 0.000 description 3
- 125000000524 functional group Chemical group 0.000 description 3
- 229910001416 lithium ion Inorganic materials 0.000 description 3
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 3
- 229920000573 polyethylene Polymers 0.000 description 3
- 238000009781 safety test method Methods 0.000 description 3
- 235000019812 sodium carboxymethyl cellulose Nutrition 0.000 description 3
- 229920001027 sodium carboxymethylcellulose Polymers 0.000 description 3
- 238000004804 winding Methods 0.000 description 3
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 2
- 239000013543 active substance Substances 0.000 description 2
- 229910052786 argon Inorganic materials 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- 125000004432 carbon atom Chemical group C* 0.000 description 2
- 125000003178 carboxy group Chemical group [H]OC(*)=O 0.000 description 2
- 239000008367 deionised water Substances 0.000 description 2
- 229910021641 deionized water Inorganic materials 0.000 description 2
- 229910002804 graphite Inorganic materials 0.000 description 2
- 239000010439 graphite Substances 0.000 description 2
- 239000011244 liquid electrolyte Substances 0.000 description 2
- QSZMZKBZAYQGRS-UHFFFAOYSA-N lithium;bis(trifluoromethylsulfonyl)azanide Chemical compound [Li+].FC(F)(F)S(=O)(=O)[N-]S(=O)(=O)C(F)(F)F QSZMZKBZAYQGRS-UHFFFAOYSA-N 0.000 description 2
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen group Chemical group [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 description 2
- 229920001343 polytetrafluoroethylene Polymers 0.000 description 2
- 239000004810 polytetrafluoroethylene Substances 0.000 description 2
- 238000003825 pressing Methods 0.000 description 2
- 238000005096 rolling process Methods 0.000 description 2
- 238000007493 shaping process Methods 0.000 description 2
- 239000011734 sodium Substances 0.000 description 2
- 239000000243 solution Substances 0.000 description 2
- 238000001179 sorption measurement Methods 0.000 description 2
- 238000003756 stirring Methods 0.000 description 2
- 229920003048 styrene butadiene rubber Polymers 0.000 description 2
- 229910052723 transition metal Inorganic materials 0.000 description 2
- 150000003624 transition metals Chemical class 0.000 description 2
- 238000009461 vacuum packaging Methods 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- 229910019142 PO4 Inorganic materials 0.000 description 1
- 239000005062 Polybutadiene Substances 0.000 description 1
- 229920002873 Polyethylenimine Polymers 0.000 description 1
- 239000004642 Polyimide Substances 0.000 description 1
- 239000004743 Polypropylene Substances 0.000 description 1
- 239000004372 Polyvinyl alcohol Substances 0.000 description 1
- 229920002125 Sokalan® Polymers 0.000 description 1
- HMDDXIMCDZRSNE-UHFFFAOYSA-N [C].[Si] Chemical compound [C].[Si] HMDDXIMCDZRSNE-UHFFFAOYSA-N 0.000 description 1
- 239000006230 acetylene black Substances 0.000 description 1
- 229920006231 aramid fiber Polymers 0.000 description 1
- 239000012752 auxiliary agent Substances 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 229910021393 carbon nanotube Inorganic materials 0.000 description 1
- 239000011247 coating layer Substances 0.000 description 1
- 229920001940 conductive polymer Polymers 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 238000007599 discharging Methods 0.000 description 1
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- 239000008151 electrolyte solution Substances 0.000 description 1
- 238000003912 environmental pollution Methods 0.000 description 1
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- 229910021389 graphene Inorganic materials 0.000 description 1
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- 229910052809 inorganic oxide Inorganic materials 0.000 description 1
- 239000003273 ketjen black Substances 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 229910001947 lithium oxide Inorganic materials 0.000 description 1
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 description 1
- ACFSQHQYDZIPRL-UHFFFAOYSA-N lithium;bis(1,1,2,2,2-pentafluoroethylsulfonyl)azanide Chemical compound [Li+].FC(F)(F)C(F)(F)S(=O)(=O)[N-]S(=O)(=O)C(F)(F)C(F)(F)F ACFSQHQYDZIPRL-UHFFFAOYSA-N 0.000 description 1
- QVXQYMZVJNYDNG-UHFFFAOYSA-N lithium;bis(trifluoromethylsulfonyl)methylsulfonyl-trifluoromethane Chemical compound [Li+].FC(F)(F)S(=O)(=O)[C-](S(=O)(=O)C(F)(F)F)S(=O)(=O)C(F)(F)F QVXQYMZVJNYDNG-UHFFFAOYSA-N 0.000 description 1
- IGILRSKEFZLPKG-UHFFFAOYSA-M lithium;difluorophosphinate Chemical compound [Li+].[O-]P(F)(F)=O IGILRSKEFZLPKG-UHFFFAOYSA-M 0.000 description 1
- 229910052748 manganese Inorganic materials 0.000 description 1
- 230000003446 memory effect Effects 0.000 description 1
- 239000002923 metal particle Substances 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 229910021382 natural graphite Inorganic materials 0.000 description 1
- 229910052759 nickel Inorganic materials 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
- 229920000058 polyacrylate Polymers 0.000 description 1
- 239000004584 polyacrylic acid Substances 0.000 description 1
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Abstract
The invention provides a battery, and belongs to the technical field of batteries. The battery comprises a positive plate, a negative plate, an isolating membrane and electrolyte, wherein the contact angle theta of the electrolyte is more than or equal to 60 degrees, and the negative plate meets the following requirements: thickness of negative plate<200 mu m and/or the single-side surface density of the negative plate is less than or equal to 0.013g/cm2(ii) a According to the invention, the contact angle of the electrolyte is improved, the thickness of the negative plate is reduced, so that the electrolyte of the battery achieves very good wettability to the negative plate, and the cycle performance and the safety performance of the battery are obviously improved.
Description
Technical Field
The invention relates to a battery and application thereof, and belongs to the technical field of batteries.
Background
The lithium ion battery has the advantages of high working voltage, large specific energy density, long cycle life, low self-discharge rate, no memory effect, small environmental pollution and the like, is widely applied to various electronic consumer product markets, and is an ideal power source for future electric vehicles and various electric tools.
The electrolyte of the lithium ion battery which is commercialized at present is completely liquid, and the liquid electrolyte in the battery is dispersed in each gap of the isolating membrane, the pole piece and the battery shell, and the liquid electrolyte mainly plays a role in transferring lithium ions.
Research shows that when the wettability of the electrolyte is poor, or when the thickness or the surface density of the negative electrode plate is large, some gaps in the internal part of the battery are not fully filled with the electrolyte, so that the cycle performance of the battery is poor, and even more, the lithium separation phenomenon occurs in the charging process of the battery, so that the safety problem occurs.
Disclosure of Invention
In order to overcome the defects of the prior art, the invention provides a battery, wherein the electrolyte in the battery has very good wettability to a negative plate, and the addition of the electrolyte can obviously improve the cycle performance and the safety performance of the battery.
The purpose of the invention is realized by the following technical scheme:
a battery comprises a positive plate, a negative plate, a separation film and electrolyte, wherein the contact angle theta of the electrolyte is more than or equal to 60 degrees, and the negative plate satisfies the following conditions: thickness of negative plate<200 mu m and/or the single-side surface density of the negative plate is less than or equal to 0.013g/cm2。
In the invention, the "contact angle of the electrolyte" refers to the contact angle of the electrolyte on the surface of the glass slide, which is an important parameter for measuring the wettability of the electrolyte on the surface of the negative electrode, as shown in fig. 1, and is the included angle between the electrolyte and the glass slide. The contact angle of the electrolyte on the surface of the glass slide is in positive correlation with the contact angle and wettability of the electrolyte on the surface of the negative electrode, namely the contact angle of the electrolyte on the surface of the glass slide is larger, which shows that the wettability of the electrolyte on the negative electrode sheet is better.
The inventor of the invention discovers, after research, that the thickness of the negative plate in the battery<200 mu m and/or the single-side surface density of the negative plate is less than or equal to 0.013g/cm2When the contact angle theta of the electrolyte is not less than 60 degrees, the wettability of the electrolyte on the negative plate is very excellent, the fluidity of the electrolyte is very good, and the electrolyte can be well filled into a gap inside the battery; when the thickness of the negative plate in the battery is more than or equal to 200 mu m and/or the single-side surface density of the negative plate>0.013g/cm2When, or when the contact angle theta of the electrolyte<At 60 ℃, the wettability of the electrolyte to the negative electrode sheet is poor, the fluidity of the electrolyte is poor, and the electrolyte cannot be sufficiently filled in the gaps inside the battery; further research shows that when the thickness of the negative plate in the battery is more than or equal to 200 mu m and/or the single-side surface density of the negative plate>0.013g/cm2In the process, even if the wetting angle theta of the electrolyte is more than or equal to 60 degrees, the wetting property of the electrolyte on the negative plate is insufficient, so that the problem of lithium precipitation of the battery in the circulating process is caused, and a safety accident can be caused in the serious process.
According to the invention, the contact angle theta of the electrolyte is greater than or equal to 60 degrees, and exemplarily, the contact angle theta of the electrolyte is 60 degrees, 70 degrees, 80 degrees, 90 degrees, 100 degrees, 110 degrees, 120 degrees, 130 degrees, 140 degrees, 150 degrees, 160 degrees, 170 degrees or 179 degrees.
According to the present invention, the thickness of the negative electrode sheet is <200 μm, and illustratively, the thickness of the negative electrode sheet is 10 μm, 20 μm, 30 μm, 40 μm, 50 μm, 60 μm, 70 μm, 80 μm, 90 μm, 100 μm, 110 μm, 120 μm, 130 μm, 140 μm, 150 μm, 160 μm, 170 μm, 180 μm, or 190 μm.
According to the invention, the single-side surface density of the negative plate is less than or equal to 0.013g/cm2E.g.. ltoreq.0.010 g/cm2And also for example ≦ 0.009g/cm2Illustratively, the single-sided surface density of the negative plate is 0.005g/cm2、0.006g/cm2、0.007g/cm2、0.008g/cm2、0.009g/cm2、0.010g/cm2、0.011g/cm2Or 0.012g/cm2。
According to the present invention, the electrolyte includes a lithium salt, a non-aqueous organic solvent, and an additive including a nitrogen-containing compound.
According to the invention, the structural formula of the nitrogen-containing compound is shown as the formula (1):
wherein R is substituted or unsubstituted alkyl, substituted or unsubstituted ester group, substituted or unsubstituted alkenyl, substituted or unsubstituted aryl; m is at least one of hexafluorophosphate, tetrafluoroborate, difluorine oxalato borate, bisoxalato borate, bisfluorosulfonyl imide and bistrifluoromethanyl imide; when containing a substituent group, the substituent group is an alkyl, halogen, or alkoxy group.
According to the invention, R is-C1-6Alkyl, -C1-6alkylene-COO-C1-6Alkyl, -C2-6Alkenyl, -C6-12And (4) an aryl group. Preferably, R is-C1-3Alkyl, -C1-3alkylene-COO-C1-3Alkyl, -C2-4Alkenyl, -C6-8And (4) an aryl group.
According to the invention, the nitrogen-containing compound may be specifically at least one of the following two substances:
the cations in the nitrogen-containing compound provided by the invention can reduce the surface tension of the electrolyte, so that the contact angle of the electrolyte is increased, and the wettability of the electrolyte on a negative plate is obviously improved. In addition, the cation can produce adsorption with some active functional groups on the surface of the negative active material, such as: the surface of the graphite contains some carboxyl functional groups, and cations in the nitrogen-containing compound can generate certain adsorption effect with the carboxyl functional groups, so that the electrolyte is guided to fully wet the negative active material. Meanwhile, the nitrogen-containing compound can also form an SEI film on the surface of the negative electrode, and the SEI film has high strength and low impedance and can improve the low-temperature discharge capacity of the battery.
According to the invention, the mass percentage of the addition of the nitrogen-containing compound in the total mass of the electrolyte is Bwt%, wherein the B wt% is less than or equal to 2 wt%; that is, the nitrogen-containing compound is added in an amount of 2 wt% or less, illustratively 0.01 wt% or less and 1 wt% or less, based on the total mass of the electrolyte, for example, 0.01 wt%, 0.02 wt%, 0.03 wt%, 0.04 wt%, 0.05 wt%, 0.1 wt%, 0.15 wt%, 0.2 wt%, 0.3 wt%, 0.4 wt%, 0.5 wt%, 0.6 wt%, 0.7 wt%, 0.8 wt%, 0.9 wt%, or 1 wt% of B wt%.
According to the invention, the adding amount of the nitrogen-containing compound accounts for the total mass of the electrolyte and is Bwt%, wherein the numerical ratio of B to the thickness (unit mum) of the negative plate is more than or equal to 0.0001, and preferably, the numerical ratio is more than or equal to 0.0005. According to the invention, through research, a certain amount of the additive is needed for improving the wettability of the electrolyte to the negative pole pieces with different thicknesses, and when the numerical ratio of the B to the thickness (unit mum) of the negative pole piece is more than or equal to 0.0001, the optimal relation between the thickness of the negative pole piece and the content of the additive in the electrolyte can be obtained.
According to the invention, the mass percentage of the addition amount of the nitrogen-containing compound in the total mass of the electrolyte is Bwt%, wherein the single-side surface density (unit g/cm) of B and the negative plate2) The numerical ratio of (b) is equal to or greater than 6, preferably equal to or greater than 10. According to the invention, researches show that negative plates with different single-side surface densities need a certain amount of the additive to improve the wettability of the electrolyte, and when B is equal to the single-side surface density (unit g/cm) of the negative plate2) The numerical ratio of (2) is more than or equal to 6, and the optimal relation between the single-side surface density of the negative plate and the content of the additive in the electrolyte can be obtained.
According to the invention, the non-aqueous organic solvent is selected from carbonates and/or carboxylates.
Wherein the carbonate is selected from one or more of the following solvents: ethylene carbonate, propylene carbonate, dimethyl carbonate, diethyl carbonate, and ethyl methyl carbonate. The carboxylic ester is selected from one or more of the following solvents: propyl acetate, n-butyl acetate, isobutyl acetate, n-pentyl acetate, isoamyl acetate, ethyl propionate, n-propyl propionate, methyl butyrate, ethyl n-butyrate.
According to the invention, the non-aqueous organic solvent comprises a linear carbonate with a number of carbon atoms of 5 or less and/or a linear carboxylate with a number of carbon atoms of 5 or less.
Preferably, the linear carbonate with the carbon number less than or equal to 5 is selected from at least one of dimethyl carbonate, ethyl methyl carbonate and diethyl carbonate.
Preferably, the linear carboxylic acid ester with the carbon number of less than or equal to 5 is selected from at least one of ethyl propionate and propyl acetate.
Preferably, the mass percentage of the mass of the linear carbonate with the carbon atom number of less than or equal to 5 and/or the mass of the linear carboxylate with the carbon atom number of less than or equal to 5 to the total mass of the electrolyte is greater than or equal to 10 wt%, preferably 10 to 70 wt%, for example 10 wt%, 20 wt%, 30 wt%, 40 wt%, 50 wt%, 60 wt% or 70 wt%. The nonaqueous organic solvent provided by the invention has smaller molecular chains, and when the content of the nonaqueous organic solvent is more than or equal to 10 wt%, the wettability of the electrolyte on the negative plate can be further improved.
According to the present invention, the lithium salt is selected from one or two or more of lithium hexafluorophosphate, lithium difluorophosphate, lithium difluorooxalato borate, lithium difluorosulfonimide, lithium bistrifluoromethylsulfonyl imide, lithium difluorobis-oxalato phosphate, lithium tetrafluoroborate, lithium bisoxalato borate, lithium hexafluoroantimonate, lithium hexafluoroarsenate, lithium bis (trifluoromethylsulfonyl) imide, lithium bis (pentafluoroethylsulfonyl) imide, lithium tris (trifluoromethylsulfonyl) methide or lithium bis (trifluoromethylsulfonyl) imide.
According to the invention, the lithium salt has a concentration of 2mol/L or less, for example 0.5mol/L, 0.6mol/L, 0.7mol/L, 0.8mol/L, 0.9mol/L, 1mol/L, 1.1mol/L, 1.2mol/L, 1.3mol/L, 1.4mol/L, 1.5mol/L, 1.6mol/L, 1.7mol/L, 1.8mol/L or 2 mol/L. The inventors found that when the concentration of the conductive lithium salt is more than 2mol/L, the contact angle of the electrolyte becomes significantly small, greatly affecting the wettability of the electrolyte.
According to the present invention, the negative electrode sheet comprises a negative electrode current collector and a negative electrode active material layer coated on one or both surfaces of the negative electrode current collector, the negative electrode active material layer comprises a negative electrode active material, a conductive agent, a binder and an auxiliary agent,
according to the invention, the negative electrode active material layer comprises the following components in percentage by mass:
90-99.6 wt% of negative electrode active material, 0.2-5 wt% of conductive agent and 0.2-5 wt% of binder.
Illustratively, the mass percentage of the negative active material is 90 wt%, 91 wt%, 92 wt%, 93 wt%, 94 wt%, 95 wt%, 96 wt%, 97 wt%, 98 wt%, 99 wt%, 99.6 wt%.
Illustratively, the conductive agent is present in an amount of 0.2 wt%, 0.3 wt%, 0.4 wt%, 0.5 wt%, 0.6 wt%, 0.7 wt%, 0.8 wt%, 0.9 wt%, 1 wt%, 2 wt%, 3 wt%, 4 wt%, 5 wt% by mass.
Illustratively, the binder is present in an amount of 0.2 wt%, 0.3 wt%, 0.4 wt%, 0.5 wt%, 0.6 wt%, 0.7 wt%, 0.8 wt%, 0.9 wt%, 1 wt%, 2 wt%, 3 wt%, 4 wt%, 5 wt% by mass.
According to the present invention, the negative active material is selected from at least one of artificial graphite, natural graphite, hard carbon, soft carbon, silica or silicon carbon negative electrode materials.
According to the invention, the conductive agent is selected from one or more of conductive carbon black, Ketjen black, conductive fibers, conductive polymers, acetylene black, carbon nanotubes, graphene, flake graphite, conductive oxides and metal particles.
According to the invention, the binder is selected from at least one of polyvinylidene fluoride and its copolymer derivative, polytetrafluoroethylene and its copolymer derivative, polyacrylic acid and its copolymer derivative, polyvinyl alcohol and its copolymer derivative, polystyrene-butadiene rubber and its copolymer derivative, polyimide and its copolymer derivative, polyethyleneimine and its copolymer derivative, polyacrylate and its copolymer derivative, and sodium carboxymethylcellulose and its copolymer derivative.
In one embodiment of the invention, the porosity of the negative electrode sheet is 20-55%.
In one aspect of the present inventionIn the method, the compaction density of the negative plate is 1.2-1.9 g/cm3。
In one embodiment of the invention, the OI value of the negative plate is 4.3-34.
In one embodiment of the present invention, the negative electrode sheet has a capacity per unit thickness of 26.9 to 123mAh/μm.
In one scheme of the invention, the D/D range of the negative electrode sheet is more than or equal to 1.04 and less than or equal to 1.1, wherein D is the thickness of the rolled negative electrode sheet after standing for 48 hours, and D is the thickness of the rolled negative electrode sheet.
According to the present invention, the thickness of the negative electrode sheet and the thickness of the positive electrode sheet satisfy the following relationship: the thickness of the positive electrode sheet/the thickness of the negative electrode sheet is (0.93-1.48): 1.
The invention has the beneficial effects that:
(1) according to the invention, the contact angle of the electrolyte is improved, the thickness of the negative plate and/or the single-side surface density of the negative plate are/is reduced, so that the electrolyte of the battery achieves very good wettability to the negative plate, and the cycle performance and the safety performance of the battery are obviously improved. (2) In order to improve the contact angle of the electrolyte, the nitrogen-containing compound is further used as an additive, and meanwhile, in order to optimize the electrolyte to the maximum extent, the wettability of the electrolyte on the negative plate is greatly improved by adjusting the relation between the content of the nitrogen-containing compound and the thickness of the negative plate and/or adjusting the relation between the content of the nitrogen-containing compound and the single-side surface density of the negative plate.
(3) The N-containing additive disclosed by the invention can be adsorbed on the surface of a negative electrode, and the side reaction of electrolyte components on the surface of the negative electrode is reduced, so that the impedance performance of a battery is reduced, and the low-temperature discharge performance of the battery is obviously improved.
Drawings
FIG. 1 is an analysis diagram of contact angle.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention clearer, the technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the embodiments of the present invention. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
It is understood that the battery of the present invention includes a negative electrode tab and an electrolyte. The battery also comprises a positive plate, an isolating membrane and an outer package. The battery of the invention can be obtained by stacking the positive plate, the isolating film and the negative plate to obtain the battery core or stacking the positive plate, the isolating film and the negative plate, then winding to obtain the battery core, placing the battery core in an outer package, and injecting electrolyte into the outer package. The specific structure of the positive electrode plate, the separator and the outer package is not particularly limited, and may be selected from conventional positive electrode plates, separators and outer packages in the art.
In the present invention, the functional surfaces refer to two surfaces of the current collector having the largest area and being oppositely disposed.
The positive plate can be obtained by arranging the positive active layer on one functional surface of the positive current collector, and can also be obtained by arranging the positive active layers on the two functional surfaces of the positive current collector.
The positive electrode active layer of the present invention includes a positive electrode active material, a conductive agent, and a binder. Wherein the positive electrode active material may be a lithium oxide compound including a transition metal, and the transition metal may be selected from at least one of Co, Mn, Ni, or Al.
The isolating membrane can be a polypropylene porous membrane, a polyethylene porous membrane or an aramid fiber porous membrane; the porous membrane may be coated with a coating layer containing an inorganic oxide or polytetrafluoroethylene.
Brief introduction to the test method for contact angle of electrolyte:
using a contact angle testing apparatus model JC2000D1, test environment: the temperature is 20-30 ℃, and the humidity is less than or equal to 70 percent RH; the testing steps are as follows: putting a clean glass slide on the sample table; using a sampler to extract 1 microliter of electrolyte sample and dripping the electrolyte sample on a glass slide; after the electrolyte sample is dropped on the glass slide for 5 seconds, the picture is taken by a computer, the test result shown in figure 1 is obtained, and the size of the contact angle is analyzed.
Examples and comparative examples
The batteries of examples 1-13 and comparative examples 1-5 were prepared by the following steps:
1) preparation of positive plate
Mixing the positive electrode active material lithium cobaltate (Li)1.05CoO2) Mixing polyvinylidene fluoride (PVDF) as a binder, SP (super P) and Carbon Nanotubes (CNTs) according to a mass ratio of 96:2:1.5:0.5, adding N-methyl pyrrolidone (NMP), and stirring under the action of a vacuum stirrer until a mixed system becomes positive active slurry with uniform fluidity; uniformly coating the positive active slurry on two functional surfaces of the aluminum foil; and drying the coated aluminum foil, and then rolling and slitting to obtain the required positive plate, wherein the thickness of the positive plate is 98 microns, and the thickness of the aluminum foil is 10 microns.
2) Preparation of negative plate
Mixing the negative active substance artificial graphite, sodium carboxymethylcellulose (CMC-Na), styrene butadiene rubber, conductive carbon black (SP) and single-walled carbon nanotubes (SWCNTs) according to the mass ratio of 96:1.5:1.5:0.9:0.1, adding deionized water, and obtaining negative active slurry under the action of a vacuum stirrer; uniformly coating the negative active slurry on two functional surfaces of the copper foil; airing the coated copper foil at room temperature, transferring the copper foil to an oven at 80 ℃ for drying for 10h, and then performing cold pressing and slitting to obtain the negative plate, wherein the thickness of the negative plate is shown in tables 1 and 3, the thickness of the copper foil is 6 mu m, and the compaction density of the negative plate is 1.78g/cm3。
3) Preparation of the electrolyte
In a glove box filled with argon (H)2O＜0.1ppm，O2Less than 0.1ppm), uniformly mixing the nonaqueous organic solvent according to the mass percentage to obtain a mixed solution, and then quickly adding the fully dried lithium salt with the specific concentration into the mixed solution to form a basic electrolyte; the basic electrolyte is added with nitrogen-containing compounds with different mass percentage contents to obtain the electrolyte (the specific composition of the electrolyte is shown in tables 1 and 3, wherein PC is propylene carbonate, EC is ethylene carbonate, DMC is dimethyl carbonate, EP is ethyl propionate, EMC is ethyl methyl carbonate, and DEC is diethyl carbonate).
4) Preparation of the Battery
Stacking the positive plate obtained in the step 1), the negative plate obtained in the step 2) and a separation film (a polyethylene porous film with the thickness of 12 mu m) in the order of the positive plate, the separation film and the negative plate, and then winding to obtain a battery cell; placing the battery core in an aluminum foil for external packaging, injecting the electrolyte obtained in the step 3) into the external packaging, and carrying out vacuum packaging, standing, formation, shaping, sorting and other processes to obtain the battery, wherein specific preparation parameters are shown in tables 1 and 3.
The batteries of examples 14 to 26 and comparative examples 6 to 10 were prepared by the following steps:
1) preparation of positive plate
Mixing the positive electrode active material lithium cobaltate (Li)1.05CoO2) Mixing polyvinylidene fluoride (PVDF) as a binder, SP (super P) and Carbon Nanotubes (CNTs) according to a mass ratio of 96:2:1.5:0.5, adding N-methyl pyrrolidone (NMP), and stirring under the action of a vacuum stirrer until a mixed system becomes positive active slurry with uniform fluidity; uniformly coating the positive active slurry on two functional surfaces of the aluminum foil; and drying the coated aluminum foil, and then rolling and slitting to obtain the required positive plate, wherein the thickness of the positive plate is 98 microns, and the thickness of the aluminum foil is 10 microns.
2) Preparation of negative plate
Mixing the negative active substance artificial graphite, sodium carboxymethylcellulose (CMC-Na), styrene butadiene rubber, conductive carbon black (SP) and single-walled carbon nanotubes (SWCNTs) according to the mass ratio of 96:1.5:1.5:0.9:0.1, adding deionized water, and obtaining negative active slurry under the action of a vacuum stirrer; uniformly coating the negative active slurry on two functional surfaces of the copper foil; airing the coated copper foil at room temperature, transferring the copper foil to an oven at 80 ℃ for drying for 10h, and then performing cold pressing and slitting to obtain the negative plate, wherein the single-side surface density of the negative plate is shown in tables 5 and 7, the thickness of the copper foil is 6 mu m, and the compaction density of the negative plate is 1.65g/cm3。
3) Preparation of the electrolyte
In a glove box filled with argon (H)2O＜0.1ppm，O2＜0.1ppm)，Uniformly mixing a non-aqueous organic solvent according to mass percentage to obtain a mixed solution, and quickly adding a fully dried lithium salt with a specific concentration into the mixed solution to form a basic electrolyte; the nitrogen-containing compounds with different mass percentage contents were added to the basic electrolyte to obtain an electrolyte (the specific composition of the electrolyte is shown in tables 5 and 7, wherein PC is propylene carbonate, EC is ethylene carbonate, DMC is dimethyl carbonate, EP is ethyl propionate, EMC is ethyl methyl carbonate, and DEC is diethyl carbonate).
4) Preparation of the Battery
Stacking the positive plate obtained in the step 1), the negative plate obtained in the step 2) and a separation film (a polyethylene porous film with the thickness of 12 mu m) in the order of the positive plate, the separation film and the negative plate, and then winding to obtain a battery cell; placing the battery core in an aluminum foil for external packaging, injecting the electrolyte obtained in the step 3) into the external packaging, and carrying out vacuum packaging, standing, formation, shaping, sorting and other processes to obtain the battery, wherein specific preparation parameters are shown in tables 5 and 7.
The following tests were performed on the batteries obtained in the above examples and comparative examples, respectively, and the test results are shown in tables 2, 4, 6, and 8.
1) Cycle performance test
The batteries obtained in examples and comparative examples were subjected to charge-discharge cycles at 25 ℃ for 100 weeks at a rate of 1C in the range of 3.0V to 4.4V, and the discharge capacity at 1 week and the discharge capacity at 100 weeks were tested; the capacity at week 100 was divided by the capacity at week 1 to obtain the cycle capacity retention.
2) Safety testing
After the circulation, the mixture is charged to 4.4V at constant current and constant voltage according to the multiplying power of 1C, and the current is cut off at 0.05C. Then, the mixture was stored at 130 ℃ for 30 min. And (5) observing whether the battery is ignited or not.
3) Low temperature discharge performance test
The batteries obtained in examples and comparative examples were subjected to 5 charge-discharge cycles at 1C rate at room temperature, and then charged to 4.45V at 1C rate, and 1C capacity Q was recorded0. Laying the battery at-20 deg.C for 4h, discharging to 3V at 0.2C rate, and recording discharge capacity Q3Is calculated byObtaining the retention rate of discharge capacity at-20 ℃;
the low-temperature discharge capacity retention rate is calculated by the following formula:
table 1 cell compositions and performance test results of examples and comparative examples
Table 2 results of performance test of batteries of examples and comparative examples
As can be seen from Table 2, when the contact angle of the electrolyte is <60 deg., or the thickness of the negative electrode sheet is greater than or equal to 200 μm, the cycle performance and safety performance of the battery are sharply reduced.
Table 3 cell compositions and performance test results of examples and comparative examples
Table 4 results of performance test of batteries of examples and comparative examples
| Serial number | Capacity retention at 25 ℃ for 100 weeks | Safety testing | Retention of discharge capacity at-20 DEG C |
| Comparative example 4 | 52.46％ | On fire | 10.9％ |
| Example 10 | 71.55％ | PASS | 25.7％ |
| Example 11 | 81.71％ | PASS | 51.2％ |
| Comparative example 5 | 47.51％ | On fire | 25.7％ |
| Example 12 | 79.18％ | PASS | 49.2％ |
| Example 13 | 85.79％ | PASS | 51.3％ |
As can be seen from table 4, the addition of the nitrogen-containing compound can significantly improve the wetting property of the electrolyte to the negative electrode plate, thereby improving the cycle performance of the battery and simultaneously improving the low-temperature discharge performance of the battery.
Table 5 cell compositions and performance test results of examples and comparative examples
Table 6 results of performance test of batteries of examples and comparative examples
As can be seen from Table 6, the contact angle when the electrolyte solution was used<60 degrees, or the single-side surface density of the negative plate is more than or equal to 0.013g/cm2In time, the cycle performance and safety performance of the battery are drastically reduced.
Table 7 cell compositions and performance test results of examples and comparative examples
Table 8 results of performance test of batteries of examples and comparative examples
| Serial number | Capacity retention at 25 ℃ for 100 weeks | Safety testing | Retention of discharge capacity at-20 DEG C |
| Comparative example 9 | 53.06％ | On fire | 11.4％ |
| Example 23 | 73.61％ | PASS | 24.3％ |
| Example 24 | 82.26％ | PASS | 53.7％ |
| Comparative example 10 | 49.10％ | On fire | 24.9％ |
| Example 25 | 80.91％ | PASS | 50.3％ |
| Example 26 | 84.52％ | PASS | 52.0％ |
As can be seen from table 8, the addition of the nitrogen-containing compound can significantly improve the wetting property of the electrolyte to the negative electrode sheet, thereby improving the cycle performance of the battery and simultaneously improving the low-temperature discharge performance of the battery.
The embodiments of the present invention have been described above. However, the present invention is not limited to the above embodiment. Any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the protection scope of the present invention.
Claims (10)
1. The battery comprises a positive plate, a negative plate, an isolating membrane and electrolyte, and is characterized in that the contact angle theta of the electrolyte is not less than 60 degrees, and the negative plate satisfies the following conditions: thickness of negative plate<200 mu m and/or the single-side surface density of the negative plate is less than or equal to 0.013g/cm2。
2. The battery of claim 1, wherein the electrolyte comprises a lithium salt, a non-aqueous organic solvent, and an additive comprising a nitrogen-containing compound;
the structural formula of the nitrogen-containing compound is shown as the formula (1):
wherein R is substituted or unsubstituted alkyl, substituted or unsubstituted ester group, substituted or unsubstituted alkenyl, substituted or unsubstituted aryl; m is at least one of hexafluorophosphate, tetrafluoroborate, difluorine oxalato borate, bisoxalato borate, bisfluorosulfonyl imide and bistrifluoromethanyl imide; when containing a substituent group, the substituent group is an alkyl, halogen, or alkoxy group.
3. The battery according to claim 2, wherein the battery further comprises a battery cell,wherein R is-C1-6Alkyl, -C1-6alkylene-COO-C1-6Alkyl, -C2-6Alkenyl, -C6-12And (4) an aryl group.
4. The battery of claim 3, wherein R is-C1-3Alkyl, -C1-3alkylene-COO-C1-3Alkyl, -C2-4Alkenyl, -C6-8And (4) an aryl group.
5. The battery according to any one of claims 2 to 4, wherein the nitrogen-containing compound is at least one of the following two substances:
6. the battery according to any one of claims 2 to 4, wherein the nitrogen-containing compound is added in an amount of B wt% based on the total mass of the electrolyte, wherein B wt% is less than or equal to 2 wt%.
7. The battery according to claim 6, wherein the nitrogen-containing compound is added in an amount of B wt% based on the total mass of the electrolyte, wherein the numerical ratio of B to the thickness (in μm) of the negative electrode sheet is 0.0001 or more;
and/or the mass percentage of the addition amount of the nitrogen-containing compound in the total mass of the electrolyte is B wt%, wherein the single-side surface density (unit g/cm) of B and the negative plate2) The numerical ratio of (A) is 6 or more.
8. The cell according to any one of claims 2 to 4, wherein the non-aqueous organic solvent is selected from carbonates and/or carboxylates;
the carbonate is selected from one or more of the following solvents: ethylene carbonate, propylene carbonate, dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate; the carboxylic ester is selected from one or more of the following solvents: propyl acetate, n-butyl acetate, isobutyl acetate, n-pentyl acetate, isoamyl acetate, ethyl propionate, n-propyl propionate, methyl butyrate, ethyl n-butyrate.
9. The battery according to claim 8, wherein the non-aqueous organic solvent comprises a linear carbonate having a carbon number of 5 or less and/or a linear carboxylate having a carbon number of 5 or less.
10. The battery according to claim 9, wherein the mass of the linear carbonate having a carbon atom number of 5 or less and/or the linear carboxylate having a carbon atom number of 5 or less accounts for 10 to 70 wt% of the total mass of the electrolyte.
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