CN116314601A - Secondary battery and electric equipment - Google Patents
Secondary battery and electric equipment Download PDFInfo
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- CN116314601A CN116314601A CN202310352203.6A CN202310352203A CN116314601A CN 116314601 A CN116314601 A CN 116314601A CN 202310352203 A CN202310352203 A CN 202310352203A CN 116314601 A CN116314601 A CN 116314601A
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- 239000007774 positive electrode material Substances 0.000 claims abstract description 44
- 239000003792 electrolyte Substances 0.000 claims abstract description 41
- 239000002245 particle Substances 0.000 claims abstract description 21
- 229910000572 Lithium Nickel Cobalt Manganese Oxide (NCM) Inorganic materials 0.000 claims abstract description 14
- FBDMTTNVIIVBKI-UHFFFAOYSA-N [O-2].[Mn+2].[Co+2].[Ni+2].[Li+] Chemical compound [O-2].[Mn+2].[Co+2].[Ni+2].[Li+] FBDMTTNVIIVBKI-UHFFFAOYSA-N 0.000 claims abstract description 14
- 229910000616 Ferromanganese Inorganic materials 0.000 claims abstract description 6
- DALUDRGQOYMVLD-UHFFFAOYSA-N iron manganese Chemical compound [Mn].[Fe] DALUDRGQOYMVLD-UHFFFAOYSA-N 0.000 claims abstract description 6
- FUJCRWPEOMXPAD-UHFFFAOYSA-N lithium oxide Chemical compound [Li+].[Li+].[O-2] FUJCRWPEOMXPAD-UHFFFAOYSA-N 0.000 claims abstract description 6
- 229910001947 lithium oxide Inorganic materials 0.000 claims abstract description 6
- 239000013543 active substance Substances 0.000 claims abstract description 5
- 238000000926 separation method Methods 0.000 claims abstract 2
- XEOVADUHCWVXTA-UHFFFAOYSA-N [O-2].[Mn+2].[Li+].[Fe+2] Chemical compound [O-2].[Mn+2].[Li+].[Fe+2] XEOVADUHCWVXTA-UHFFFAOYSA-N 0.000 claims description 21
- 150000001875 compounds Chemical class 0.000 claims description 10
- 230000001186 cumulative effect Effects 0.000 claims description 6
- 239000011572 manganese Substances 0.000 claims description 6
- 229910052721 tungsten Inorganic materials 0.000 claims description 6
- XEEYBQQBJWHFJM-UHFFFAOYSA-N iron Substances [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims description 4
- 229910052738 indium Inorganic materials 0.000 claims description 3
- PXHVJJICTQNCMI-UHFFFAOYSA-N nickel Substances [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 3
- 229910052720 vanadium Inorganic materials 0.000 claims description 3
- 229910052727 yttrium Inorganic materials 0.000 claims description 3
- 229910052726 zirconium Inorganic materials 0.000 claims description 3
- 238000005056 compaction Methods 0.000 abstract description 9
- 238000009826 distribution Methods 0.000 abstract description 7
- 238000002360 preparation method Methods 0.000 abstract description 4
- 238000013461 design Methods 0.000 abstract description 3
- 230000000052 comparative effect Effects 0.000 description 11
- 239000000463 material Substances 0.000 description 10
- 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 8
- 238000000034 method Methods 0.000 description 7
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 6
- 239000011230 binding agent Substances 0.000 description 6
- 239000006258 conductive agent Substances 0.000 description 6
- 239000012528 membrane Substances 0.000 description 6
- 238000007599 discharging Methods 0.000 description 5
- 238000002156 mixing Methods 0.000 description 5
- 230000001105 regulatory effect Effects 0.000 description 5
- 239000000243 solution Substances 0.000 description 5
- 239000007773 negative electrode material Substances 0.000 description 4
- 239000003960 organic solvent Substances 0.000 description 4
- 238000012360 testing method Methods 0.000 description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 4
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 description 3
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 description 3
- 239000002033 PVDF binder Substances 0.000 description 3
- 239000000654 additive Substances 0.000 description 3
- 230000000996 additive effect Effects 0.000 description 3
- 229910052782 aluminium Inorganic materials 0.000 description 3
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 3
- 229910052799 carbon Inorganic materials 0.000 description 3
- 239000003575 carbonaceous material Substances 0.000 description 3
- 239000003153 chemical reaction reagent Substances 0.000 description 3
- 239000002131 composite material Substances 0.000 description 3
- 238000001035 drying Methods 0.000 description 3
- 239000011267 electrode slurry Substances 0.000 description 3
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 description 3
- 239000011888 foil Substances 0.000 description 3
- 239000010410 layer Substances 0.000 description 3
- 230000014759 maintenance of location Effects 0.000 description 3
- 238000011056 performance test Methods 0.000 description 3
- -1 polyethylene Polymers 0.000 description 3
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- 238000003825 pressing Methods 0.000 description 3
- 238000011160 research Methods 0.000 description 3
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 2
- 239000004743 Polypropylene Substances 0.000 description 2
- 239000006230 acetylene black Substances 0.000 description 2
- 239000010405 anode material Substances 0.000 description 2
- 239000011248 coating agent Substances 0.000 description 2
- 238000000576 coating method Methods 0.000 description 2
- 238000005520 cutting process Methods 0.000 description 2
- 239000008367 deionised water Substances 0.000 description 2
- 229910021641 deionized water Inorganic materials 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 238000000921 elemental analysis Methods 0.000 description 2
- 229910002804 graphite Inorganic materials 0.000 description 2
- 239000010439 graphite Substances 0.000 description 2
- 229910052744 lithium Inorganic materials 0.000 description 2
- 229910003002 lithium salt Inorganic materials 0.000 description 2
- 159000000002 lithium salts Chemical class 0.000 description 2
- 229920001155 polypropylene Polymers 0.000 description 2
- 150000003839 salts Chemical class 0.000 description 2
- 239000002210 silicon-based material Substances 0.000 description 2
- 238000005303 weighing Methods 0.000 description 2
- 229920000049 Carbon (fiber) Polymers 0.000 description 1
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- 229910015855 LiMn0.7Fe0.3PO4 Inorganic materials 0.000 description 1
- 229910012888 LiNi0.6Co0.1Mn0.3O2 Inorganic materials 0.000 description 1
- 229910015872 LiNi0.8Co0.1Mn0.1O2 Inorganic materials 0.000 description 1
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 1
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 1
- 239000004698 Polyethylene Substances 0.000 description 1
- 229910000676 Si alloy Inorganic materials 0.000 description 1
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 1
- HMDDXIMCDZRSNE-UHFFFAOYSA-N [C].[Si] Chemical compound [C].[Si] HMDDXIMCDZRSNE-UHFFFAOYSA-N 0.000 description 1
- OBNDGIHQAIXEAO-UHFFFAOYSA-N [O].[Si] Chemical compound [O].[Si] OBNDGIHQAIXEAO-UHFFFAOYSA-N 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
- 239000006183 anode active material Substances 0.000 description 1
- 239000006256 anode slurry Substances 0.000 description 1
- 239000012300 argon atmosphere Substances 0.000 description 1
- 229910021383 artificial graphite Inorganic materials 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 239000004917 carbon fiber Substances 0.000 description 1
- 239000001768 carboxy methyl cellulose Substances 0.000 description 1
- 230000015556 catabolic process Effects 0.000 description 1
- 239000011247 coating layer Substances 0.000 description 1
- 230000001276 controlling effect Effects 0.000 description 1
- 239000011889 copper foil Substances 0.000 description 1
- 238000006731 degradation reaction Methods 0.000 description 1
- 239000002270 dispersing agent Substances 0.000 description 1
- 229910021385 hard carbon Inorganic materials 0.000 description 1
- 238000002955 isolation Methods 0.000 description 1
- 238000011031 large-scale manufacturing process Methods 0.000 description 1
- GELKBWJHTRAYNV-UHFFFAOYSA-K lithium iron phosphate Chemical compound [Li+].[Fe+2].[O-]P([O-])([O-])=O GELKBWJHTRAYNV-UHFFFAOYSA-K 0.000 description 1
- 230000003446 memory effect Effects 0.000 description 1
- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 150000004706 metal oxides Chemical class 0.000 description 1
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 1
- 239000004005 microsphere Substances 0.000 description 1
- 239000011259 mixed solution Substances 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 229910021382 natural graphite Inorganic materials 0.000 description 1
- 229920000573 polyethylene Polymers 0.000 description 1
- 238000006479 redox reaction Methods 0.000 description 1
- 238000005096 rolling process Methods 0.000 description 1
- 229910052710 silicon Inorganic materials 0.000 description 1
- 239000010703 silicon Substances 0.000 description 1
- 235000019812 sodium carboxymethyl cellulose Nutrition 0.000 description 1
- 229920001027 sodium carboxymethylcellulose Polymers 0.000 description 1
- 229910021384 soft carbon Inorganic materials 0.000 description 1
- 239000002904 solvent Substances 0.000 description 1
- 238000003756 stirring Methods 0.000 description 1
- 229920003048 styrene butadiene rubber Polymers 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 239000002345 surface coating layer Substances 0.000 description 1
- 238000010998 test method Methods 0.000 description 1
- 239000002562 thickening agent 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
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/131—Electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
- H01M4/50—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese
- H01M4/505—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese of mixed oxides or hydroxides containing manganese for inserting or intercalating light metals, e.g. LiMn2O4 or LiMn2OxFy
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
- H01M4/52—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron
- H01M4/525—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron of mixed oxides or hydroxides containing iron, cobalt or nickel for inserting or intercalating light metals, e.g. LiNiO2, LiCoO2 or LiCoOxFy
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M2004/021—Physical characteristics, e.g. porosity, surface area
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
- H01M2004/028—Positive electrodes
-
- 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
Abstract
The invention provides a secondary battery and electric equipment. The secondary battery comprises a positive electrode plate, electrolyte, a separation film and a negative electrode plate, and is characterized in that the positive electrode plate comprises a positive electrode current collector and a positive electrode film which is arranged on at least one surface of the positive electrode current collector and comprises a positive electrode active substance, wherein the positive electrode active substance comprises ferromanganese lithium oxide and lithium nickel cobalt manganese oxide, and the secondary battery meets the following relation: 1<C LMFP ·PD·[(D v90 ‑D v10 )/D v50 ]·[(D n90 ‑D n10 )/D n50 ]·A EL And is less than or equal to 30. The invention meets the above conditions by reasonable collocation of the positive electrode active material, particle size distribution of the positive electrode active material, compaction density of the positive electrode plate and reasonable design of electrolyte, so that the energy density and cycle of the obtained secondary batteryThe ring performance is remarkably improved, and the preparation cost of the battery is remarkably reduced.
Description
Technical Field
The invention relates to the technical field of batteries, in particular to a secondary battery and electric equipment.
Background
The secondary battery has the outstanding advantages of high energy density, high power density, long service life, no memory effect and the like, and is widely applied to electric automobiles.
Compared with the lithium iron phosphate anode material, the lithium iron manganese phosphate anode material has a higher voltage platform and higher safety, and is widely paid attention to scientific researchers in the application field of power batteries and the like. Because the lithium iron manganese phosphate and the ternary material have similar electrochemical windows, the safety performance of the secondary battery can be improved to a certain extent by mixing the lower-cost lithium iron manganese phosphate material with the ternary material. However, how to improve the energy density and cycle performance of secondary batteries using lithium iron manganese phosphate ternary materials as positive electrode active materials, is still an important problem facing the whole power battery industry.
Disclosure of Invention
The invention aims to solve the problems that the energy density and the cycle performance of the existing secondary battery still need to be further improved and the cost is high, and provides a secondary battery. According to the invention, the particle size distribution of the composite positive electrode active material, the compaction density of the positive electrode plate and the parameters of the electrolyte are effectively regulated, so that the cycle performance and the energy density of the battery can be effectively improved under the condition of low ternary positive electrode active material content.
In order to achieve the above object, according to a first aspect of the present invention, there is provided a secondary battery including a positive electrode tab including a positive electrode current collector and a positive electrode tab disposed on at least one surface of the positive electrode current collector and including a positive electrode active material including lithium iron manganese oxide and lithium nickel cobalt manganese oxide, an electrolyte, a separator, and a negative electrode tab, the secondary battery satisfying the following relationship:
1<C LMFP ·PD·[(D v90 -D v10 )/D v50 ]·[(D n90 -D n10 )/D n50 ]·A EL ≤30；
wherein C is LMFP The weight ratio of the manganese iron lithium oxide in the positive electrode active material is as follows;
PD is the compacted density of the positive pole piece, and the unit is g/cm 3 ；
D v10 、D v50 、D v90 Particle sizes corresponding to the cumulative volume percentages of the positive electrode active materials reaching 10%, 50% and 90%, respectively, are expressed in micrometers;
D n10 、D n50 、D n90 particle size corresponding to the cumulative number percentage of the positive electrode active material reaching 10%, 50% and 90%, and the unit is mu m;
A EL the unit is g/Ah, which is the weight of electrolyte in the unit capacity of the secondary battery.
As an embodiment of the present invention, the secondary battery satisfies the following relationship: c is more than or equal to 9.5 LMFP ·PD·[(D v90 -D v10 )/D v50 ]·[(D n90 -D n10 )/D n50 ]·A EL ≤14。
As an embodiment of the present invention, the weight ratio of the manganese iron lithium oxide in the positive electrode active material is 10% or less than C LMFP ≤90％。
As an embodiment of the invention, the positive electrode plate has a compacted density of 2.2-3.7 g/cm 3 。
In the relation (D) as an embodiment of the present invention v90 -D v10 )/D v50 1.1 to 2.5.
In the relation (D) as an embodiment of the present invention n90 -D n10 )/D n50 0.5 to 2.5.
As an embodiment of the present invention, the electrolyte weight A per unit volume EL It is 2.0 to 5.0g/Ah, more preferably 2.5 to 4.5g/Ah.
As an embodiment of the present invention, the lithium iron manganese oxide includes a compound having the formula Li a Mn x Fe 1-x M 1-a PO 4 Wherein 0 is a compound of formula (I)<x<1,0.95 a is less than or equal to 1.1, and M comprises at least one of In, la, zr, ce, W, al, ti, sr, mg, sb, V, zn, cu, cr.
As an embodiment of the present invention, the lithium nickel cobalt manganese oxide includes a compound of the formula Li b (Ni y Co z Mn 1-y-z ) 1- c A c O 2 Is a compound of formula (I),wherein b is more than or equal to 0.95 and less than or equal to 1.1,0<y<1，0<z<C is more than or equal to 1 and less than or equal to 0.1, and A comprises at least one of Zr, sr, W, al, ti, mg, ce, Y, B elements.
In a second aspect of the present invention, there is provided an electric device comprising the above secondary battery.
Compared with the prior art, the invention has the beneficial effects that:
according to the invention, the particle size distribution of the composite positive electrode active material, the compaction density of the positive electrode plate and the parameters of the electrolyte are effectively regulated, so that the cycle performance and the energy density of the battery can be effectively improved under the condition of low ternary positive electrode active material content.
Detailed Description
For a better description of the objects, technical solutions and advantages of the present invention, the present invention will be further described with reference to the following specific examples, which are not intended to limit the present invention in any way. Unless specifically stated otherwise, the reagents, methods and apparatus employed in the present invention are those conventional in the art. The reagents and materials used in the present invention are commercially available unless otherwise specified.
An embodiment of the present invention provides a secondary battery including a positive electrode tab including a positive electrode current collector and a positive electrode sheet disposed on at least one surface of the positive electrode current collector and including a positive electrode active material including a lithium iron manganese oxide and a lithium nickel cobalt manganese oxide, an electrolyte, a separator, and a negative electrode tab, the secondary battery satisfying the following relationship:
1<C LMFP ·PD·[(D v90 -D v10 )/D v50 ]·[(D n90 -D n10 )/D n50 ]·A EL ≤30；
wherein C is LMFP The weight ratio of the manganese iron lithium oxide in the positive electrode active material is as follows;
PD is the compacted density of the positive pole piece, and the unit is g/cm 3 ；
D v10 、D v50 、D v90 Respectively, the cumulative volume percentage of the positive electrode active material reaches 10 percent, 50 percent,The corresponding particle size at 90% is in μm;
D n10 、D n50 、D n90 particle size corresponding to the cumulative number percentage of the positive electrode active material reaching 10%, 50% and 90%, and the unit is mu m;
A EL the unit is g/Ah, which is the weight of electrolyte in the unit capacity of the secondary battery.
The research of the invention shows that the capacity of the positive electrode active material plays a role of the ratio of the manganese iron lithium oxide in the positive electrode active material, the particle size distribution of the positive electrode active material, the compaction density of the positive electrode plate and the reasonable design of electrolyte (namely, C LMFP ·PD·[(D v90 -D v10 )/D v50 ]·[(D n90 -D n10 )/D n50 ]·A EL ") there is a clear correlation. By reasonable collocation of the materials, the energy density and the cycle stability of the battery can be obviously improved under the condition that a small amount of lithium nickel cobalt manganese oxide (also commonly called as a layered ternary positive electrode active material in the field) is added. Meanwhile, the addition of a small amount of lithium nickel cobalt manganese oxide can also greatly reduce the cost of the battery, and is suitable for large-scale production and application.
In the positive electrode active material in the secondary battery of the present invention, the ratio of lithium iron manganese phosphate can be calculated by ICP elemental analysis. The method comprises the following steps: 1) And (3) carrying out ICP elemental analysis on a positive electrode piece sample prepared by mixing the lithium nickel cobalt manganese oxide and the manganese iron lithium oxide to obtain the mass ratio of Li to P, so that the duty ratio of the manganese iron lithium oxide can be calculated.
In the present invention, reference to D is made to v10 、D v50 、D v90 、D n10 、D n50 、D n90 All refer to the particle size of the positive electrode active material mixture comprising lithium iron manganese oxide and lithium nickel cobalt manganese oxide.
In some embodiments of the present invention, the secondary battery satisfies the following relationship: c is more than or equal to 9.5 LMFP ·PD·[(D v90 -D v10 )/D v50 ]·[(D n90 -D n10 )/D n50 ]·A EL Within this range, the obtained secondary battery is more excellent in cycle performance and energy density.
In the secondary battery, the particle size distribution of the positive electrode active material, the duty ratio of the ferromanganese lithium oxide, the compacted density of the positive electrode plate and the electrolyte are mutually influenced, so that the energy density and the cycle performance of the battery are further influenced.
In some embodiments of the invention, (D) v90 -D v10 )/D v50 In the range of 1.1 to 2.5, e.g. (D) v90 -D v10 )/D v50 May be 1.1, 1.3, 1.5, 1.7, 1.9, 2.1, 2.3, 2.5 or a range consisting of any two of the foregoing values. Thus, the dynamic performance of the secondary battery is facilitated, and the energy density of the secondary battery is also considered.
In some embodiments of the invention, (D) n90 -D n10 )/D n50 In the range of 0.5 to 2.5. For example (D) n90 -D n10 )/D n50 May be 0.5, 0.7, 0.9, 1.1, 1.3, 1.5, 1.7, 1.9, 2.1, 2.3, 2.5 or a range consisting of any two of the foregoing values. When (D) n90 -D n10 )/D n50 And the dynamic performance of the secondary battery is favorably exerted within the range of 0.5-2.5, and the energy density of the battery is simultaneously considered.
In some embodiments of the invention, D v90 4-14 μm. For example D v90 May be 4 μm, 5 μm, 6 μm, 7 μm, 8 μm, 9 μm, 10 μm, 11 μm, 12 μm, 13 μm, 14 μm or a range consisting of any two of the foregoing values.
In some embodiments of the invention, D v10 0.7-1.8 μm. For example D v10 May be 0.7 μm, 0.8 μm, 0.9 μm, 1.0 μm, 1.1 μm, 1.2 μm, 1.3 μm, 1.4 μm, 1.5 μm, 1.6 μm, 1.7 μm, 1.8 μm or a range consisting of any two of the foregoing values.
In some embodiments of the invention, D v50 Is 2-10 mu m. For example D v50 May be 2 μm, 3 μm, 4 μm, 5 μm, 6 μm, 7 μm, 8 μm, 9 μm, 10 μm or a range consisting of any two of the foregoing values.
In some embodiments of the invention, D n90 0.5-1.4 μm. For example D n90 May be 0.5 μm, 0.6 μm, 0.7 μm, 0.8 μm, 0.9 μm, 1.0 μm, 1.1 μm, 1.2 μm, 1.3 μm, 1.4 μm or a range consisting of any two of the foregoing values.
In some embodiments of the invention, D n10 0.20 to 0.35 mu m. For example D n10 May be 0.20 μm, 0.22 μm, 0.24 μm, 0.26 μm, 0.28 μm, 0.30 μm, 0.33 μm, 0.35 μm or a range consisting of any two of the foregoing values.
In some embodiments of the invention, D n50 0.29 to 0.56 mu m. For example D n50 May be 0.29 μm, 0.32 μm, 0.35 μm, 0.38 μm, 0.41 μm, 0.43 μm, 0.46 μm, 0.49 μm, 0.52 μm, 0.56 μm or a range consisting of any two of the foregoing values.
The invention discovers that the mass ratio C of the manganese iron lithium oxide in the positive electrode active material LMFP Affecting the energy density of the battery and the watt-hour cost of the battery. In the positive electrode active material, the capacity of the ferromanganese lithium oxide is usually not as high as that of the layered ternary positive electrode active material (lithium nickel cobalt manganese oxide), but the cost of the ferromanganese lithium oxide is far lower than that of the layered ternary positive electrode active material. Thus, when C LMFP When the specific capacity of the battery is higher, the cost of the secondary battery can be reduced, but the specific capacity of the battery is also reduced; when C LMFP When the lithium iron manganese oxide is low, as the particles of the lithium iron manganese oxide are small, the particles of the ternary material are large, and in the rolling process, the lithium iron manganese phosphate particles can enter the gaps of the particles of the ternary material, so that the compaction density of the positive electrode plate can be improved to a certain extent, the compaction density of the positive electrode plate is improved, the energy density of the battery is also improved to a certain extent under the condition that the capacity is unchanged, but the effect of reducing the cost of the battery is limited. Thus, in some embodiments of the invention, the mass ratio of the lithium iron manganese oxide in the positive electrode active material satisfies 10% C LMFP Less than or equal to 90 percent. For example C LMFP May be 10%, 20%, 30%, 40%, 50%, 60%, 70%, 80%, 90% or consist ofA range consisting of any two of the foregoing values.
The research of the invention finds that the compaction density PD of the positive electrode plate also affects the exertion of the energy density of the battery. In some embodiments of the invention, the positive electrode sheet has a compacted density PD of 2.2 to 3.7g/cm 3 . For example, the compacted density PD of the positive electrode sheet may be 2.2g/cm 3 、2.4g/cm 3 、2.6g/cm 3 、2.8g/cm 3 、2.9g/cm 3 、3.1g/cm 3 、3.3g/cm 3 、3.5g/cm 3 、3.7g/cm 3 . Therefore, good wettability of the positive electrode active material and the electrolyte can be ensured, and a proper number of redox reaction sites can be ensured, so that positive electrode capacity can be ensured to be exerted, and the energy density of the battery can be improved.
The invention researches that the weight A of electrolyte in unit capacity EL The exertion of the energy density of the secondary battery is affected. In particular, when the proportion of the smaller-particle ferromanganese lithium oxide in the positive electrode sheet is relatively high, the electrolyte is easy to adsorb, so that the weight A of the electrolyte in unit capacity should be properly increased EL The method comprises the steps of carrying out a first treatment on the surface of the When the proportion of the manganese iron lithium oxide with smaller particles in the positive electrode plate is lower, the electrolyte A in unit capacity should be properly reduced EL The dosage of the electrolyte is effectively avoided, and the effect of reducing the cost can be achieved to a certain extent. However, too low an amount of electrolyte per unit volume may result in serious capacity degradation of the battery due to electrolyte drying during repeated charging. Thus, the amount of electrolyte in the secondary battery is also within a suitable range, and in some embodiments of the invention, the electrolyte weight A per unit volume EL The service performance requirement of the battery can be met within the range of 2.0-5.0 g/Ah; a is that EL The secondary battery obtained in the range of 2.5 to 4.5g/Ah has a higher energy density. The concentration of the electrolyte in the electrolyte is in the range of 0.9 to 1.1mol/L in terms of lithium element.
For A in secondary battery EL The capacity of the battery can be obtained by one-time capacity division, then the electrolyte of the battery is pumped out and weighed, the weight of the electrolyte can be calculated, and then the A of the battery can be calculated EL Is a value of (2). A of a secondary battery can be controlled in the secondary battery by controlling the amount of injected electrolyte in the secondary battery EL Values.
In the secondary battery of the present invention, a positive electrode sheet containing a positive electrode active material (the positive electrode sheet may also be referred to as a positive electrode active material layer) may be provided on one surface of the positive electrode current collector or may be provided on both surfaces of the positive electrode current collector. The positive electrode membrane can also comprise a conductive agent and a binder, wherein the types and the contents of the conductive agent and the binder are not particularly limited, and can be selected according to actual requirements. The type of the positive electrode current collector is not particularly limited, and can be selected according to actual requirements.
In the secondary battery of the invention, the positive active materials of manganese iron lithium oxide (namely manganese iron lithium phosphate) and lithium nickel cobalt manganese oxide can be doped and modified and/or coated, the type and content of doped elements are not limited, one element can be doped, multiple elements can be doped together, and doping elements commonly used in the field can be used in the invention; the kind, content and thickness of the surface coating layer are also not limited, and the coating layer may be at least one of a carbon material or a metal oxide which are commonly used in the art.
In some embodiments of the invention, the lithium iron manganese oxide includes a compound of the formula Li a Mn x Fe 1-x M 1-a PO 4 Wherein 0 is a compound of formula (I)<x<1,0.95 a is less than or equal to 1.1, and M comprises at least one of In, la, zr, ce, W, al, ti, sr, mg, sb, V, zn, cu, cr.
In some embodiments of the invention, the lithium nickel cobalt manganese oxide comprises a compound of the formula Li b (Ni y Co z Mn 1-y-z ) 1-c A c O 2 Wherein b is 0.95.ltoreq.b.ltoreq.1.1, 0<y<1，0<z<C is more than or equal to 1 and less than or equal to 0.1, and A comprises at least one of Zr, sr, W, al, ti, mg, ce, Y, B elements.
In the secondary battery of the present invention, a negative electrode sheet containing a negative electrode active material (the negative electrode sheet may also be referred to as a negative electrode active material layer) may be provided on one surface of a negative electrode current collector or may be provided on both surfaces of the negative electrode current collector. The negative electrode membrane can also comprise a conductive agent and a binder, wherein the types and the contents of the conductive agent and the binder are not particularly limited, and can be selected according to actual requirements. The type of the negative electrode current collector is not particularly limited, and can be selected according to actual requirements.
The negative electrode active material is a material common in the art, including but not limited to at least one of a carbon material, a silicon-based material; the carbon material can be at least one of graphite, hard carbon, soft carbon, carbon fiber or mesophase carbon microsphere, and the graphite can be one or more of artificial graphite and natural graphite; the silicon-based material can be one or more selected from simple substance silicon, silicon oxygen compound, silicon carbon compound and silicon alloy.
When the positive electrode membrane and the negative electrode membrane are respectively arranged on the two surfaces of the positive electrode current collector and the negative electrode current collector, the battery is considered to fall within the protection scope of the invention as long as the positive electrode membrane on any one surface of the positive electrode current collector and the negative electrode membrane on any one surface of the negative electrode current collector meet the invention. Meanwhile, the parameters of the positive and negative electrode diaphragms provided by the invention also refer to the parameters of the single-sided positive and negative electrode diaphragms.
In the secondary battery, the isolating film is arranged between the positive electrode plate and the negative electrode plate and plays a role in isolating the positive electrode from the negative electrode. The kind of the separator is not particularly limited, and may be any separator material used in existing batteries, such as polyethylene, polypropylene, polyvinylidene fluoride, and multilayer composite films thereof, but is not limited thereto.
In the secondary battery of the present invention, the kind of the electrolyte is not particularly limited either. The electrolyte comprises electrolyte salt and an organic solvent, and the specific types of the electrolyte salt and the organic solvent are not particularly limited and can be selected according to actual requirements. The electrolyte may further include an additive, the kind of which is not particularly limited, and may be a film-forming additive for a positive electrode and/or a negative electrode, or may be an additive capable of improving certain properties of a battery, such as improving high or low temperature properties of a battery.
The invention also protects electric equipment comprising the secondary battery.
The following are specific embodiments of the present invention, and the technical solutions of the present invention will be further described with reference to the embodiments, but the present invention is not limited to these embodiments. The reagents, methods and apparatus employed in the present invention, unless otherwise specified, are all conventional in the art.
Examples 1 to 32 and comparative examples 1 to 9
The secondary batteries according to the examples and comparative examples of the present invention were prepared by a method comprising the steps of:
preparation of positive electrode plate
Mixing an anode active material, a binder polyvinylidene fluoride (PVDF) and a conductive agent acetylene black according to a mass ratio of 96:3:1, and adding a solvent N-methylpyrrolidone; then transferring into a vacuum stirrer to stir until the system is uniform, thus obtaining anode slurry; uniformly coating positive electrode slurry on the two surfaces of a positive electrode current collector (carbon coated aluminum foil); and drying the coated pole piece through an oven, and then carrying out cold pressing and cutting to obtain the positive pole piece.
Preparation of negative electrode plate
Mixing a negative electrode active substance, a thickener sodium carboxymethyl cellulose, a binder styrene-butadiene rubber and a conductive agent acetylene black according to a mass ratio of 97:1:1:1, adding deionized water, and obtaining a negative electrode slurry under the action of a vacuum stirrer; uniformly coating the negative electrode slurry on a negative electrode current collector copper foil; and transferring the coated pole piece to an oven for drying, and then carrying out cold pressing and cutting to obtain the negative pole piece.
Preparation of electrolyte
The organic solvent is a mixed solution containing Ethylene Carbonate (EC), ethylmethyl carbonate (EMC) and diethyl carbonate (DEC), wherein the volume ratio of EC, EMC and DEC is 20:20:60. At the water content<In a 10ppm argon atmosphere glove box, the lithium salt LiP was dried thoroughlyF 6 Dissolving in an organic solvent, and uniformly mixing to obtain an electrolyte, wherein the concentration of lithium salt in the electrolyte is 1mol/L.
Assembly of lithium secondary battery
The positive pole piece, the isolating film (polypropylene) and the negative pole piece are sequentially stacked, so that the isolating film is positioned between the positive pole piece and the negative pole piece to play a role of isolation, the isolating film is wound into a square bare cell, the bare cell is placed into a shell, baked at 80 ℃ for water removal, injected with electrolyte and sealed, and the lithium secondary battery can be obtained after the working procedures of standing, hot and cold pressing, formation, clamping, capacity division and the like.
The specific choices of the positive electrode active material and the negative electrode active material and the parameters thereof are shown in Table 1.
For convenience of description, liMn in examples and comparative examples of the present invention 0.6 Fe 0.4 PO 4 Abbreviated as LMFP-64, liMn 0.7 Fe 0.3 PO 4 Abbreviated LMFP-73; liNi 0.6 Co 0.1 Mn 0.3 O 2 Abbreviated as NCM-613, liNi 0.8 Co 0.1 Mn 0.1 O 2 Abbreviated as NCM-811.
The particle size distribution of the positive electrode active material used in the examples and comparative examples of the present invention was tested using a malvern 3000 laser particle sizer, and the dispersant used for the test was deionized water.
Table 1 positive electrode active materials for secondary batteries and parameters thereof in examples and comparative examples
The performance of the secondary batteries obtained in the above examples and comparative examples was tested, and specific test items and test methods and results (see table 2) are as follows:
1. compacted density PD (in g/cm) 3 ): 1) Firstly, weighing the unit area of 1540.25mm 2 The mass of the empty aluminum foil is m 1 The unit is g; 2) Weighing 1540.25mm in unit area 2 The quality of the positive electrode piece with the double-sided uniformly coated positive electrode active material layer is m 2 In g, there is cw= (m 2 -m 1 ) 2, unit is g/1540.25mm 2 The method comprises the steps of carrying out a first treatment on the surface of the 3) Measuring the thickness L of the aluminum foil by a micrometer 1 The unit is mu m; the thickness of the positive electrode plate for measuring the double-sided uniform positive electrode active material is L 2 In μm, the compaction density of the pole pieces pd=2×cw/(L) 2 -L 1 ) The unit is g/cm 3 。
2. Weight of electrolyte A per unit volume EL (in g/Ah): the design capacity of the battery was b Ah, and the weight of the injected electrolyte was a g, so a EL ＝a/b(g/Ah)。
3. Discharge performance test of secondary battery:
3.1 gram Capacity at first discharge (mAh/g) test at 0.33C：
(1) Regulating the temperature of the incubator to 25 ℃, and standing for 2 hours; (2) charging to 3.65V at constant current of 0.33C, and then charging to off current of 0.05C at constant voltage; (3) standing for 5min; (4) discharging to 2.5V at constant current of 0.33C; (5) standing for 5min.
3.2 4C rate discharge performance test：
(1) Regulating the temperature of the incubator to 25 ℃, and standing for 2 hours; (2) charging to 3.65V at constant current of 0.33C, and then charging to off current of 0.05C at constant voltage; (3) standing for 5min; (4) discharging to 2.5V at constant current of 0.33C; (5) standing for 5min; (6) charging to 3.65V at constant current of 0.33C, and then charging to off current of 0.05C at constant voltage; (7) standing for 5min; (8) discharging to 2.5V at constant current of 4C; (9) standing for 5min; wherein, 4C discharge capacity retention rate (%) =4c discharge gram capacity at rate/0.33C first discharge gram capacity×100%.
3.3Cycle capacity retention test：
The circulation steps are as follows: (1) regulating the temperature of the incubator to 25 ℃, and standing for 2 hours; (2) charging to 3.65V at constant current of 0.33C, and then charging to off current of 0.05C at constant voltage; (3) standing for 5min; (4) discharging to 2.5V at constant current of 0.33C; (5) standing for 5min; (6) charging to 3.65V at a constant current of 1C, and then charging to a cut-off current of 0.05C at a constant voltage; (7) standing for 5min; (8) discharging to 2.5V at a constant current of 1C; (9) standing for 5min; repeating steps (6) - (9) until 4000 cycles. Wherein, capacity retention (%) =gram capacity after 4000 cycles/gram capacity for first cycle of 1c×100%.
4. Actual energy density of secondary battery:
the secondary batteries prepared in examples and comparative examples were fully charged at 1C rate at 25 ℃, discharged at 1C rate, and the actual discharge energy at that time was recorded; the battery was weighed using an electronic scale at 25 ℃; the ratio of the actual discharge energy of the battery 1C to the weight of the battery is the actual energy density of the battery.
Wherein 1) when the actual energy density is <80% of the target energy density, the actual energy density of the battery is considered to be very low; 2) When 80% of the target energy density is less than or equal to the actual energy density which is less than 95% of the target energy density, the actual energy density of the battery is considered to be lower; 3) When the 95% target energy density is less than or equal to the actual energy density which is less than the 105% target energy density, the actual energy density of the battery is considered to be moderate; 4) When 105% of the target energy density is less than or equal to the actual energy density and less than 120% of the target energy density, the actual energy density of the battery is considered to be higher; 5) When 120% of the target energy density is less than or equal to the actual energy density, the actual energy density of the battery is considered to be very high.
Table 2 results of performance test of secondary batteries prepared in examples and comparative examples
From the above results, it can be seen that:
from the above examples and comparative examples, the mass ratio C of lithium manganese iron phosphate in the positive electrode active material LMFP The particle size distribution width of the positive electrode active material and the compaction density of the positive electrode plateThe weight of electrolyte in the meter and unit volume can affect the electrical performance of the cell as well as the actual energy density.
The positive electrode active materials of comparative examples 1 to 4 contained only manganese iron lithium oxide or lithium nickel cobalt manganese oxide, and the discharge capacity of the secondary batteries thus prepared was low or the rate performance was significantly deteriorated. In comparative examples 5 to 9, C LMFP ·PD·[(D v90 -D v10 )/D v50 ]·[(D n90 -D n10 )/D n50 ]·A EL Less than 1 or more than 30, the discharge capacity, rate capability, cycle performance, and energy density of the resulting secondary battery are significantly inferior to those of the examples of the present invention.
Finally, it should be noted that the above embodiments are only for illustrating the technical solution of the present invention and not for limiting the scope of the present invention, and although the present invention has been described in detail with reference to the preferred embodiments, it should be understood by those skilled in the art that the technical solution of the present invention may be modified or substituted equally without departing from the spirit and scope of the technical solution of the present invention.
Claims (10)
1. The secondary battery comprises a positive electrode plate, electrolyte, a separation film and a negative electrode plate, and is characterized in that the positive electrode plate comprises a positive electrode current collector and a positive electrode film which is arranged on at least one surface of the positive electrode current collector and comprises a positive electrode active substance, the positive electrode active substance comprises ferromanganese lithium oxide and lithium nickel cobalt manganese oxide, and the secondary battery meets the following relation:
1<C LMFP ·PD·[(D v90 -D v10 )/D v50 ]·[(D n90 -D n10 )/D n50 ]·A EL ≤30；
wherein C is LMFP The weight ratio of the manganese iron lithium oxide in the positive electrode active material is as follows;
PD is the compacted density of the positive pole piece, and the unit is g/cm 3 ；
D v10 、D v50 、D v90 Particle diameters corresponding to the cumulative volume percentages of the positive electrode active materials reaching 10%, 50% and 90%, respectivelyThe unit is mu m;
D n10 、D n50 、D n90 particle sizes corresponding to the cumulative amounts of the positive electrode active materials reaching 10%, 50% and 90%, respectively, are expressed in μm;
A EL the unit is g/Ah, which is the weight of electrolyte in the unit capacity of the secondary battery.
2. The secondary battery according to claim 1, wherein the secondary battery satisfies the following relationship: c is more than or equal to 9.5 LMFP ·PD·[(D v90 -D v10 )/D v50 ]·[(D n90 -D n10 )/D n50 ]·A EL ≤14。
3. The secondary battery according to claim 1, wherein the positive electrode active material contains 10% or less by weight of lithium iron manganese oxide than C LMFP ≤90％。
4. The secondary battery according to claim 1, wherein the compacted density of the positive electrode sheet is 2.2 to 3.7g/cm 3 。
5. The secondary battery according to claim 1, wherein in the relation, (D v90 -D v10 )/D v50 1.1 to 2.5.
6. The secondary battery according to claim 1, wherein in the relation, (D n90 -D n10 )/D n50 0.5 to 2.5.
7. The secondary battery according to claim 1, wherein the electrolyte weight a per unit capacity EL 2.5-4.5 g/Ah.
8. The secondary battery according to claim 1, wherein the lithium iron manganese oxide includes a compound of the formula Li a Mn x Fe 1-x M 1-a PO 4 Wherein 0 is a compound of formula (I)<x<1,0.95 a is less than or equal to 1.1, and M comprises at least one of In, la, zr, ce, W, al, ti, sr, mg, sb, V, zn, cu, cr.
9. The secondary battery according to claim 1, wherein the lithium nickel cobalt manganese oxide comprises a compound of the formula Li b (Ni y Co z Mn 1-y-z ) 1-c A c O 2 Wherein b is 0.95.ltoreq.b.ltoreq.1.1, 0<y<1，0<z<C is more than or equal to 1 and less than or equal to 0.1, and A comprises at least one of Zr, sr, W, al, ti, mg, ce, Y, B elements.
10. An electric device comprising the secondary battery according to any one of claims 1 to 9.
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