CN108321385A - Iron manganese phosphate lithium doping ternary positive electrode active material, lithium ion battery and preparation method thereof - Google Patents
Iron manganese phosphate lithium doping ternary positive electrode active material, lithium ion battery and preparation method thereof Download PDFInfo
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- CN108321385A CN108321385A CN201810100630.4A CN201810100630A CN108321385A CN 108321385 A CN108321385 A CN 108321385A CN 201810100630 A CN201810100630 A CN 201810100630A CN 108321385 A CN108321385 A CN 108321385A
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- positive electrode
- lithium
- manganese phosphate
- iron manganese
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- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 53
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 51
- 239000007774 positive electrode material Substances 0.000 title claims abstract description 50
- 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 title claims abstract description 35
- 238000002360 preparation method Methods 0.000 title claims abstract description 15
- 239000000463 material Substances 0.000 claims abstract description 81
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims abstract description 52
- 229910052744 lithium Inorganic materials 0.000 claims abstract description 50
- AWKHTBXFNVGFRX-UHFFFAOYSA-K iron(2+);manganese(2+);phosphate Chemical compound [Mn+2].[Fe+2].[O-]P([O-])([O-])=O AWKHTBXFNVGFRX-UHFFFAOYSA-K 0.000 claims abstract description 46
- 239000000126 substance Substances 0.000 claims abstract description 23
- 229910012748 LiNi0.5Mn0.3Co0.2O2 Inorganic materials 0.000 claims abstract description 11
- 229910014985 LiMnxFe1-xPO4 Inorganic materials 0.000 claims abstract description 4
- 229910014982 LiMnxFe1−xPO4 Inorganic materials 0.000 claims abstract description 4
- 239000006258 conductive agent Substances 0.000 claims description 32
- 239000011883 electrode binding agent Substances 0.000 claims description 31
- 239000007773 negative electrode material Substances 0.000 claims description 18
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 13
- 229910021385 hard carbon Inorganic materials 0.000 claims description 11
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims description 11
- 229910015831 LiMn0.6Fe0.4PO4 Inorganic materials 0.000 claims description 10
- 229910019142 PO4 Inorganic materials 0.000 claims description 9
- XEEYBQQBJWHFJM-UHFFFAOYSA-N iron Substances [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims description 9
- 229910021384 soft carbon Inorganic materials 0.000 claims description 9
- 229910015944 LiMn0.8Fe0.2PO4 Inorganic materials 0.000 claims description 7
- 229910021382 natural graphite Inorganic materials 0.000 claims description 7
- 229910015566 LiMn0.4Fe0.6PO4 Inorganic materials 0.000 claims description 6
- 239000002033 PVDF binder Substances 0.000 claims description 6
- 239000003792 electrolyte Substances 0.000 claims description 5
- 239000010439 graphite Substances 0.000 claims description 5
- 229920002981 polyvinylidene fluoride Polymers 0.000 claims description 5
- 229910002804 graphite Inorganic materials 0.000 claims description 4
- 229910015645 LiMn Inorganic materials 0.000 claims 1
- 239000010406 cathode material Substances 0.000 claims 1
- 230000008901 benefit Effects 0.000 abstract description 13
- 230000000052 comparative effect Effects 0.000 description 14
- 229920003048 styrene butadiene rubber Polymers 0.000 description 10
- 239000002174 Styrene-butadiene Substances 0.000 description 9
- 229920002134 Carboxymethyl cellulose Polymers 0.000 description 8
- 229910021383 artificial graphite Inorganic materials 0.000 description 8
- 229910052799 carbon Inorganic materials 0.000 description 8
- 235000010948 carboxy methyl cellulose Nutrition 0.000 description 8
- 229910016096 LiMn0.5Fe0.5PO4 Inorganic materials 0.000 description 7
- 238000000034 method Methods 0.000 description 7
- PXHVJJICTQNCMI-UHFFFAOYSA-N nickel Substances [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 7
- 239000011572 manganese Substances 0.000 description 6
- 230000008569 process Effects 0.000 description 5
- 229920006184 cellulose methylcellulose Polymers 0.000 description 4
- 238000004519 manufacturing process Methods 0.000 description 4
- MKYBYDHXWVHEJW-UHFFFAOYSA-N N-[1-oxo-1-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)propan-2-yl]-2-[[3-(trifluoromethoxy)phenyl]methylamino]pyrimidine-5-carboxamide Chemical compound O=C(C(C)NC(=O)C=1C=NC(=NC=1)NCC1=CC(=CC=C1)OC(F)(F)F)N1CC2=C(CC1)NN=N2 MKYBYDHXWVHEJW-UHFFFAOYSA-N 0.000 description 3
- QSNQXZYQEIKDPU-UHFFFAOYSA-N [Li].[Fe] Chemical compound [Li].[Fe] QSNQXZYQEIKDPU-UHFFFAOYSA-N 0.000 description 3
- 239000006182 cathode active material Substances 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- 238000005087 graphitization Methods 0.000 description 3
- CPSYWNLKRDURMG-UHFFFAOYSA-L hydron;manganese(2+);phosphate Chemical compound [Mn+2].OP([O-])([O-])=O CPSYWNLKRDURMG-UHFFFAOYSA-L 0.000 description 3
- 229910052759 nickel Inorganic materials 0.000 description 3
- 239000002994 raw material Substances 0.000 description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 3
- KAKZBPTYRLMSJV-UHFFFAOYSA-N Butadiene Chemical compound C=CC=C KAKZBPTYRLMSJV-UHFFFAOYSA-N 0.000 description 2
- 229910000616 Ferromanganese Inorganic materials 0.000 description 2
- 229910052493 LiFePO4 Inorganic materials 0.000 description 2
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 description 2
- 239000010405 anode material Substances 0.000 description 2
- 239000011230 binding agent Substances 0.000 description 2
- 230000008859 change Effects 0.000 description 2
- 239000000470 constituent Substances 0.000 description 2
- 230000007423 decrease Effects 0.000 description 2
- 230000002999 depolarising effect Effects 0.000 description 2
- 238000001035 drying Methods 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- DALUDRGQOYMVLD-UHFFFAOYSA-N iron manganese Chemical compound [Mn].[Fe] DALUDRGQOYMVLD-UHFFFAOYSA-N 0.000 description 2
- 229910052748 manganese Inorganic materials 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 229910052698 phosphorus Inorganic materials 0.000 description 2
- 239000011574 phosphorus Substances 0.000 description 2
- 239000000843 powder Substances 0.000 description 2
- 239000011347 resin Substances 0.000 description 2
- 229920005989 resin Polymers 0.000 description 2
- 239000002002 slurry Substances 0.000 description 2
- 238000012360 testing method Methods 0.000 description 2
- HIBWGGKDGCBPTA-UHFFFAOYSA-N C=CC1=CC=CC=C1.C=CC1=CC=CC=C1 Chemical compound C=CC1=CC=CC=C1.C=CC1=CC=CC=C1 HIBWGGKDGCBPTA-UHFFFAOYSA-N 0.000 description 1
- 229920000049 Carbon (fiber) Polymers 0.000 description 1
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 description 1
- 229910013421 LiNixCoyMn1-x-yO2 Inorganic materials 0.000 description 1
- 229910013427 LiNixCoyMn1−x−yO2 Inorganic materials 0.000 description 1
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 description 1
- 206010054949 Metaplasia Diseases 0.000 description 1
- 229910018095 Ni-MH Inorganic materials 0.000 description 1
- 229910018477 Ni—MH Inorganic materials 0.000 description 1
- 240000003936 Plumbago auriculata Species 0.000 description 1
- YZSKZXUDGLALTQ-UHFFFAOYSA-N [Li][C] Chemical compound [Li][C] YZSKZXUDGLALTQ-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
- 239000011149 active material Substances 0.000 description 1
- 230000001070 adhesive effect Effects 0.000 description 1
- 150000001336 alkenes Chemical class 0.000 description 1
- 239000002969 artificial stone Substances 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- MTAZNLWOLGHBHU-UHFFFAOYSA-N butadiene-styrene rubber Chemical compound C=CC=C.C=CC1=CC=CC=C1 MTAZNLWOLGHBHU-UHFFFAOYSA-N 0.000 description 1
- OJIJEKBXJYRIBZ-UHFFFAOYSA-N cadmium nickel Chemical compound [Ni].[Cd] OJIJEKBXJYRIBZ-UHFFFAOYSA-N 0.000 description 1
- 239000006229 carbon black Substances 0.000 description 1
- 239000004917 carbon fiber Substances 0.000 description 1
- 239000001768 carboxy methyl cellulose Substances 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 229910017052 cobalt Inorganic materials 0.000 description 1
- 239000010941 cobalt Substances 0.000 description 1
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 1
- 239000000571 coke Substances 0.000 description 1
- 238000005056 compaction Methods 0.000 description 1
- 238000010276 construction Methods 0.000 description 1
- 238000007334 copolymerization reaction Methods 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 235000013399 edible fruits Nutrition 0.000 description 1
- 230000005611 electricity Effects 0.000 description 1
- 239000003995 emulsifying agent Substances 0.000 description 1
- 239000000839 emulsion Substances 0.000 description 1
- 238000007720 emulsion polymerization reaction Methods 0.000 description 1
- 239000003292 glue Substances 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 239000003999 initiator Substances 0.000 description 1
- 238000010030 laminating Methods 0.000 description 1
- 238000003475 lamination Methods 0.000 description 1
- 239000004816 latex Substances 0.000 description 1
- 229920000126 latex Polymers 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 239000002931 mesocarbon microbead Substances 0.000 description 1
- 230000015689 metaplastic ossification Effects 0.000 description 1
- 239000000178 monomer Substances 0.000 description 1
- 239000011331 needle coke Substances 0.000 description 1
- 230000007935 neutral effect Effects 0.000 description 1
- 231100000252 nontoxic Toxicity 0.000 description 1
- 230000003000 nontoxic effect Effects 0.000 description 1
- 230000009965 odorless effect Effects 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 238000012536 packaging technology Methods 0.000 description 1
- 238000002161 passivation Methods 0.000 description 1
- 238000011056 performance test Methods 0.000 description 1
- 239000002006 petroleum coke Substances 0.000 description 1
- 239000006253 pitch coke Substances 0.000 description 1
- 229920000447 polyanionic polymer Polymers 0.000 description 1
- 230000009257 reactivity Effects 0.000 description 1
- 230000002441 reversible effect Effects 0.000 description 1
- 229910052708 sodium Inorganic materials 0.000 description 1
- 239000011734 sodium Substances 0.000 description 1
- 235000019812 sodium carboxymethyl cellulose Nutrition 0.000 description 1
- 229920001027 sodium carboxymethylcellulose Polymers 0.000 description 1
- 238000003860 storage Methods 0.000 description 1
- 239000011115 styrene butadiene Substances 0.000 description 1
- 230000009967 tasteless effect Effects 0.000 description 1
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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
- H01M4/36—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
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/058—Construction or manufacture
-
- 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
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
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- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Inorganic Chemistry (AREA)
- Materials Engineering (AREA)
- Battery Electrode And Active Subsutance (AREA)
Abstract
The present invention relates to field of lithium ion battery, specifically, providing a kind of iron manganese phosphate lithium doping ternary positive electrode active material, lithium ion battery and preparation method thereof.The iron manganese phosphate lithium doping ternary positive electrode active material, including 24 mass parts of 532 type ternary material, 68 mass parts and iron manganese phosphate for lithium；The chemical formula of the 532 type ternary material is LiNi0.5Mn0.3Co0.2O2；The chemical formula of the iron manganese phosphate for lithium is LiMnxFe1‑xPO4, wherein 0<x<1.The positive electrode active materials have the advantages that bulk density is high, safe and at low cost.
Description
Technical field
The present invention relates to field of lithium ion battery, in particular to a kind of iron manganese phosphate lithium doping tertiary cathode activity
Material, lithium ion battery and preparation method thereof.
Background technology
A kind of novel Green Chemistry power supply of lithium ion battery system, has compared with traditional nickel-cadmium cell, Ni-MH battery
The advantage that voltage is high, long lifespan and energy density are big.With the continuous renewal and development of lithium battery technology, light, Gao Rong, length
The advantages of service life, gradually obtains the favor of consumer.Lithium battery market expands to camera, DVD, boat film, toy etc. via mobile phone
Multiple fields.In recent years, lithium ion battery due to have many advantages, such as voltage is high, recycle often, storage time it is long, not only
It is used widely on a portable electronic device, and is widely used in electric vehicle, electric bicycle and electronic work
In terms of the large and medium-sized electrical equipment such as tool.
The performance of lithium ion battery depends primarily on positive and negative pole material, ternary anode material for lithium-ion batteries
LiNixCoyMn1-x-yO2(NCM) advantage for relying on specific capacity high, it is considered to be the lithium-ion-power cell of great application prospect is just
Pole material, however its bulk density is relatively low, cost is slightly higher, safety is slightly worse, disadvantage mentioned above not only can limiting lithium ion cell
Performance can also improve the production cost of lithium ion battery.
In view of this, special propose the present invention.
Invention content
The first object of the present invention is to provide a kind of iron manganese phosphate lithium doping ternary positive electrode active material, the positive-active
Material has the advantages that bulk density is high, safe and at low cost.
The second object of the present invention is to provide a kind of lithium ion battery, which includes above-mentioned iron manganese phosphate for lithium
Ternary positive electrode active material is adulterated, therefore has the advantages that bulk density is high, safe and at low cost.
The third object of the present invention is to provide a kind of preparation method of lithium ion battery, and this method is simple for process, science
Rationally, the lithium ion battery being prepared has the advantages that bulk density is high, safe and at low cost.
In order to realize that the above-mentioned purpose of the present invention, spy use following technical scheme：
In a first aspect, the present invention provides a kind of iron manganese phosphate lithium doping ternary positive electrode active material, including 532 type ternarys
Material 6-8 mass parts and iron manganese phosphate for lithium 2-4 mass parts；
The chemical formula of the 532 type ternary material is LiNi0.5Mn0.3Co0.2O2；The chemical formula of the iron manganese phosphate for lithium is
LiMnxFe1-xPO4, wherein 0<x<1.
As further preferred technical solution, including 532 type ternary material 6.5-8 mass parts and iron manganese phosphate for lithium 2-
3.5 mass parts.
As further preferred technical solution, including 532 type ternary material 6.5-7.5 mass parts and iron manganese phosphate for lithium
2.5-3.5 mass parts.
As further preferred technical solution, the iron manganese phosphate for lithium is LiMn0.5Fe0.5PO4, LiMn0.6Fe0.4PO4,
LiMn0.95Fe0.05PO4, LiMn0.8Fe0.2PO4Or LiMn0.4Fe0.6PO4At least one of.
Second aspect, the present invention provides a kind of lithium ion battery, including positive electrode, the positive electrode includes above-mentioned
Iron manganese phosphate lithium doping ternary positive electrode active material.
As further preferred technical solution, the positive electrode further includes positive conductive agent and positive electrode binder, institute
The mass ratio for stating positive electrode active materials, positive conductive agent and positive electrode binder is 93-97:1-2:1-2, preferably 94-96:1-2:
1-2；
Preferably, positive conductive agent includes conductive carbon black；
Preferably, positive electrode binder includes PVDF.
As further preferred technical solution, the lithium ion battery further includes negative material, the negative material packet
Include negative electrode active material, cathode conductive agent and negative electrode binder, the negative electrode active material, cathode conductive agent and negative electrode binder
Mass ratio be 94-96:0.5-2:1-4, preferably 94-95:0.5-1:1-2.
As further preferred technical solution, negative electrode active material includes natural graphite, artificial graphite, soft carbon or hard carbon
At least one of.
As further preferred technical solution, cathode conductive agent includes conductive carbon black；
Preferably, negative electrode binder includes CMC and/or SBR；
Preferably, the mass ratio of CMC and SBR is 0.5-2:0.5-2, preferably 0.8-1.5:0.8-1.5.
The third aspect, the present invention provides a kind of preparation methods of above-mentioned lithium ion battery, include the following steps：(a) divide
The positive electrode comprising the iron manganese phosphate lithium doping ternary positive electrode active material and negative material anode collection is not coated on
The both sides of body and negative current collector, are then dried and are compacted, and form positive plate and negative plate；
(b) positive plate and negative plate are assembled into battery core by required size；
(c) battery core is packed into shell, electrolyte is then injected into shell, then sealed up to the lithium ion battery.
Compared with prior art, beneficial effects of the present invention are：
Iron manganese phosphate lithium doping ternary positive electrode active material provided by the invention includes 532 type ternary materials and iron manganese phosphate
Lithium, using 532 type ternary material of iron manganese phosphate lithium doping, effectively compensate for bulk density existing for 532 type ternary materials it is low, at
The problem of this height and safety difference, improves bulk density and the safety of positive electrode active materials, while reducing cost, more
It is suitble to commercially produce and applies.
Lithium ion battery provided by the invention includes positive electrode, which includes above-mentioned iron manganese phosphate lithium doping three
First positive electrode active materials, therefore have the advantages that bulk density is high, safe and at low cost.
The preparation method of above-mentioned lithium ion battery provided by the invention is simple for process, scientific and reasonable, the lithium being prepared from
Sub- battery has the advantages that bulk density is high, safe and at low cost.
Specific implementation mode
Embodiment of the present invention is described in detail below in conjunction with embodiment, but those skilled in the art will
Understand, the following example is merely to illustrate the present invention, and is not construed as limiting the scope of the invention.It is not specified in embodiment specific
Condition person carries out according to conventional conditions or manufacturer's recommended conditions.
In a first aspect, a kind of iron manganese phosphate lithium doping ternary positive electrode active material is provided at least one embodiment,
Including 532 type ternary material 6-8 mass parts and iron manganese phosphate for lithium 2-4 mass parts；
The chemical formula of the 532 type ternary material is LiNi0.5Mn0.3Co0.2O2；The chemical formula of the iron manganese phosphate for lithium is
LiMnxFe1-xPO4, wherein 0<x<1.
Iron manganese phosphate for lithium theoretical capacity is identical as LiFePO4, is 170mAh/g, but it is relative to Li+The electrode of/Li
Current potential is 4.1V, is far above the 3.4V of LiFePO4, and the high potential of 4.1V makes iron manganese phosphate for lithium have potential high-energy density
The advantages of.Meanwhile iron manganese phosphate for lithium, there are two voltage platform, high voltage platform can improve the voltage of battery, low voltage is flat
Platform can be very good to judge the residual capacity of battery.In addition, iron manganese phosphate for lithium has high volume density, short grained iron manganese phosphate
Lithium can be filled into the gap of bulky grain ternary material, improve the bulk density of positive electrode.In addition, having benefited from iron manganese phosphate
Polyanion PO in lithium4 3-Combination so that is combined with oxygen is more preferable, low with the reactivity of electrolyte, therefore phosphorus
Phenomena such as sour ferromanganese lithium is susceptible to some bubble oxygens unlike ternary material, safety higher.Also, iron manganese phosphate for lithium
In be free of Ni, Co element, it is cheap.
In NCM ternary materials, the influence of three kinds of nickel (Ni), cobalt (Co), manganese (Mn) elements to material is different, in general,
Ni constituent contents are higher, and the gram volume of material is higher, but then the cycle performance of material and thermal stability will for Ni too high levels
Decline；Co constituent contents are higher, and entire positive electrode active materials system conductivity is higher, and the layer structure of material is better, but Co
Too high levels will increase the manufacturing cost of ternary material, while the thermal stability of material can also decline；Mn contents are higher, material
Cycle performance it is better, thermal stability is higher, but Mn elements are excessively high, and material capacity will be caused to reduce, and is eventually converted into not
The Mn of stability3+, influence the cycle performance of material.
Consider case above, present invention defines the ratios of above-mentioned Ni, Co, Mn, have especially selected 532 type ternary materials
Material, the material each element give full play to respective effect in the positive active material of mono-crystalline structures obtained, and it is living to improve anode
Property material stability, make positive electrode active materials that there is preferable cycle performance, so that final obtained lithium ion battery
With excellent chemical property.
In the present invention, according to the mass fraction, the 532 typical but non-limiting contents of type ternary material be 6 parts, 6.1 parts,
6.2 parts, 6.3 parts, 6.4 parts, 6.5 parts, 6.6 parts, 6.7 parts, 6.8 parts, 6.9 parts, 7 parts, 7.1 parts, 7.2 parts, 7.3 parts, 7.4 parts,
7.5 parts, 7.6 parts, 7.7 parts, 7.8 parts, 7.9 parts or 8 parts；According to the mass fraction, iron manganese phosphate for lithium is typical but non-limiting contains
Amount for 2 parts, 2.1 parts, 2.2 parts, 2.3 parts, 2.4 parts, 2.5 parts, 2.6 parts, 2.7 parts, 2.8 parts, 2.9 parts, 3 parts, 3.1 parts, 3.2
Part, 3.3 parts, 3.4 parts, 3.5 parts, 3.6 parts, 3.7 parts, 3.8 parts, 3.9 parts or 4 parts.Above-mentioned x is typical but non-limiting to be
0.05,0.1,0.15,0.2,0.25,0.3,0.35,0.4,0.45,0.5,0.6,0.65,0.7,0.75,0.8,0.85,0.9 or
0.95。
Above-mentioned iron manganese phosphate lithium doping ternary positive electrode active material includes 532 type ternary materials and iron manganese phosphate for lithium, is used
532 type ternary material of iron manganese phosphate lithium doping, effectively compensate for bulk density existing for 532 type ternary materials it is low, it is of high cost and
The problem of safety difference, improves bulk density and the safety of positive electrode active materials, while reducing cost, is more suitable for quotient
Industry metaplasia is produced and application.
In a preferred embodiment, including 532 type ternary material 6.5-8 mass parts and iron manganese phosphate for lithium 2-3.5
Mass parts.
In a preferred embodiment, including 532 type ternary material 6.5-7.5 mass parts and iron manganese phosphate for lithium 2.5-
3.5 mass parts.
When the quality of 532 type ternary materials and iron manganese phosphate for lithium is in above-mentioned preferred range, the property of positive electrode active materials
Can be more excellent, the balance between each performance is more preferable, it is thus possible to keep the comprehensive performance of lithium ion battery more excellent, it is practical
Application effect is more preferable.
In a preferred embodiment, the iron manganese phosphate for lithium is LiMn0.5Fe0.5PO4, LiMn0.6Fe0.4PO4,
LiMn0.95Fe0.05PO4, LiMn0.8Fe0.2PO4Or LiMn0.4Fe0.6PO4At least one of.The iron manganese phosphate for lithium is typical but non-
Restrictive is LiMn0.5Fe0.5PO4, LiMn0.6Fe0.4PO4, LiMn0.95Fe0.05PO4, LiMn0.8Fe0.2PO4,
LiMn0.4Fe0.6PO4, LiMn0.5Fe0.5PO4And LiMn0.6Fe0.4PO4Combination, LiMn0.95Fe0.05PO4And LiMn0.8Fe0.2PO4
Combination, LiMn0.8Fe0.2PO4And LiMn0.4Fe0.6PO4Combination, LiMn0.5Fe0.5PO4、LiMn0.6Fe0.4PO4With
LiMn0.95Fe0.05PO4Combination, or, LiMn0.95Fe0.05PO4、LiMn0.8Fe0.2PO4And LiMn0.4Fe0.6PO4Combination etc..
Above-mentioned iron manganese phosphate lithium doping ternary positive electrode active material mainly presses 532 type ternary materials and iron manganese phosphate for lithium
Ratio is uniformly mixed, and hybrid mode uses any one existing hybrid mode, the present invention not to make to this special
Limitation.In addition, 532 type ternary materials and iron manganese phosphate for lithium be using existing, or, voluntarily being made using existing preparation method
Standby, the present invention is not particularly limited this.
Second aspect provides a kind of lithium ion battery, including positive electrode, the anode at least one embodiment
Material includes above-mentioned iron manganese phosphate lithium doping ternary positive electrode active material.Above-mentioned lithium ion battery includes positive electrode, the anode
Material includes above-mentioned iron manganese phosphate lithium doping ternary positive electrode active material, therefore high, the safe and cost with bulk density
Low advantage.
In a preferred embodiment, the positive electrode further includes positive conductive agent and positive electrode binder, described
The mass ratio of positive electrode active materials, positive conductive agent and positive electrode binder is 93-97:1-2:1-2, preferably 94-96:1-2:1-
2.The mass ratio of positive electrode active materials, positive conductive agent and positive electrode binder is 93-97:1-2:When 1-2, the viscosity of positive electrode
It is more preferable with mobility, and the content of iron manganese phosphate lithium doping ternary positive electrode active material is moderate, the lithium ion battery being prepared
Bulk density and security performance higher.Typical but non-limiting above-mentioned mass ratio is 93:1:1、95:1:1、97:1:1、93:
2:2、95:2:2、97:2:2、94:1:1 or 96:2:2 etc..
Preferably, positive conductive agent includes conductive carbon black.Conductive carbon black (or conductive black) can improve positive electrode with
Electron-transport between plus plate current-collecting body reduces the interface contact resistance of electrode, plays the role of depolarising.
Preferably, positive electrode binder includes PVDF.PVDF (Polyvinylidene Fluoride) is polyvinyladine floride,
It is a kind of binder of function admirable, cheap, adhesive property is good, helps to improve battery performance.
In a preferred embodiment, the lithium ion battery further includes negative material, and the negative material includes
Negative electrode active material, cathode conductive agent and negative electrode binder, the negative electrode active material, cathode conductive agent and negative electrode binder
Mass ratio is 94-96:0.5-2:1-4, preferably 94-95:0.5-1:1-2.Negative electrode active material, cathode conductive agent and cathode are viscous
The mass ratio for tying agent is 94-96:0.5-2:When 1-4, the viscosity and mobility of negative material are more preferable, and negative electrode active material contains
Measure the energy density higher of moderate, to be prepared lithium ion battery.Typical but non-limiting above-mentioned mass ratio is 94:0.5:
1、95:0.5:1、96:0.5:1、94:1:2、95:1:2、96:1:2、94:2:4、95:2:4 or 96:2:4 etc..
In a preferred embodiment, negative electrode active material includes in natural graphite, artificial graphite, soft carbon or hard carbon
At least one.Above-mentioned negative electrode active material it is typical but non-limiting be natural graphite, artificial graphite, soft carbon, hard carbon, naturally
The combination of the combination of graphite and artificial graphite, soft carbon and hard carbon, the combination of natural graphite, artificial graphite and soft carbon, or, artificial stone
The combination etc. of ink, soft carbon and hard carbon.
Natural graphite cathode active material is using natural flakey Scaly graphite through crushing, nodularization, classification, passivation, table
The processes such as face handle to obtain, what high-crystallinity was naturally occurring.Natural graphite gram volume is higher, simple for process, cheap.
Artificial plumbago negative pole active material is to forge easy graphited carbon (such as petroleum coke, needle coke, pitch coke) at a certain temperature
It burns, then is made through crushing, classification, high temperature graphitization, high-crystallinity is formed by high temperature graphitization.Artificial graphite price
It is higher, but cycle and security performance are preferable.Soft carbon is after heat treatment temperature reaches graphitization temperature, and material has higher graphite
Change degree is easy graphited carbon；It common are coke, graphitized intermediate-phase carbon microballon (MCMB), carbon fiber etc..Soft carbon cathode
Active material has a low and stable charge and discharge potential platform, and charge/discharge capacity is big and efficient, good cycle.Hard carbon refers to
It is difficult to the carbon being graphitized, the crosslinked resin with special construction is thermally decomposed at 1000 DEG C or so can obtain hard carbon, and this kind of carbon exists
2500 DEG C or more of high temperature is also difficult to be graphitized, and common hard carbon has resin carbon and carbon black etc..Hard carbon cathode active material has
There are very high reversible specific capacity, generally 500-700mAh；Hard carbon stable structure and charge and discharge circulation life is long, and carbon lithium current potential
0.2V can be higher than, security performance is more preferable.
In a preferred embodiment, cathode conductive agent includes conductive carbon black.Conductive carbon black (or conductive black) energy
The electron-transport between positive electrode and plus plate current-collecting body is enough improved, the interface contact resistance of electrode is reduced, plays depolarising
Effect.
Preferably, negative electrode binder includes CMC and/or SBR.CMC (Sodium carboxymethlycellulose) is
Sodium carboxymethylcellulose, appearance are white or yellowish fibrous powder or white powder, odorless, tasteless, nontoxic；It is soluble in cold
Water or hot water form glue, and solution is neutral or alkalescence, and thickening power can be played in slurry manufacturing process.SBR
(Styrene Butadiene Rubber) is a kind of styrene-butadiene latex, and aqueous binders are by styrene (Styrene) and fourth two
Alkene (Butadiene) monomer is added emulsifier initiator etc. as medium using water and is generated by emulsion polymerization copolymerization, and state is to contain admittedly
The aqueous emulsion of amount 50% or so, mainly plays cementation in slurry manufacturing process, derives from a wealth of sources, at low cost.
Preferably, the mass ratio of CMC and SBR is 0.5-2:0.5-2, preferably 0.8-1.5:0.8-1.5.Above-mentioned CMC and
The typical but non-limiting mass ratio of SBR is 1:1、0.5:1.5、0.5:2、2:0.5、0.5:1、1:0.5、1:1.5、1.5:
0.5、1.5:1、0.8:1.5 or 1.5:0.8 etc..
The third aspect, provides a kind of preparation method of above-mentioned lithium ion battery at least one embodiment, including with
Lower step：(a) positive electrode comprising the iron manganese phosphate lithium doping ternary positive electrode active material and negative material are applied respectively
The both sides of plus plate current-collecting body and negative current collector are overlying on, is then dried and is compacted, form positive plate and negative plate；
(b) positive plate and negative plate are assembled into battery core by required size；
(c) battery core is packed into shell, electrolyte is then injected into shell, then sealed up to the lithium ion battery.
The preparation method of above-mentioned lithium ion battery is simple for process, scientific and reasonable, and the lithium ion battery being prepared has body
High, the safe and at low cost advantage of product density.
The present invention is not particularly limited the assembling mode of battery core, is assembled using conventional battery core packaging technology
, takeup type battery core or lamination type electric core are such as assembled into using conventional winding or laminating method.
Unmentioned preparation process and parameter in the present invention, such as drying temperature, drying time, compaction pressure, diaphragm and electricity
Selection of liquid etc. is solved according to the conventional selection of this field, the present invention is to this and is not particularly limited.
With reference to embodiment and comparative example, the present invention will be further described in detail.
Embodiment 1
A kind of iron manganese phosphate lithium doping ternary positive electrode active material, including 532 type ternary material, 6 mass parts and iron manganese phosphate
2 mass parts of lithium；
The chemical formula of the 532 type ternary material is LiNi0.5Mn0.3Co0.2O2；The chemical formula of the iron manganese phosphate for lithium is
LiMn0.5Fe0.5PO4。
Embodiment 2
A kind of iron manganese phosphate lithium doping ternary positive electrode active material, including 532 type ternary material, 8 mass parts and iron manganese phosphate
4 mass parts of lithium；
The chemical formula of the 532 type ternary material is LiNi0.5Mn0.3Co0.2O2；The chemical formula of the iron manganese phosphate for lithium is
LiMn0.95Fe0.05PO4。
Embodiment 3
A kind of iron manganese phosphate lithium doping ternary positive electrode active material, including 532 type ternary material, 6.2 mass parts and manganese phosphate
3.8 mass parts of iron lithium；
The chemical formula of the 532 type ternary material is LiNi0.5Mn0.3Co0.2O2；The chemical formula of the iron manganese phosphate for lithium is
LiMn0.6Fe0.4PO4。
Embodiment 4
A kind of iron manganese phosphate lithium doping ternary positive electrode active material, including 532 type ternary material, 6 mass parts and iron manganese phosphate
3.7 mass parts of lithium；
The chemical formula of the 532 type ternary material is LiNi0.5Mn0.3Co0.2O2；The chemical formula of the iron manganese phosphate for lithium is
LiMn0.6Fe0.4PO4。
Embodiment 5
A kind of iron manganese phosphate lithium doping ternary positive electrode active material, including 532 type ternary material, 6.5 mass parts and manganese phosphate
3.5 mass parts of iron lithium；
The chemical formula of the 532 type ternary material is LiNi0.5Mn0.3Co0.2O2；The chemical formula of the iron manganese phosphate for lithium is
LiMn0.6Fe0.4PO4。
Embodiment 6
A kind of iron manganese phosphate lithium doping ternary positive electrode active material, including 532 type ternary material, 7 mass parts and iron manganese phosphate
3 mass parts of lithium；
The chemical formula of the 532 type ternary material is LiNi0.5Mn0.3Co0.2O2；The chemical formula of the iron manganese phosphate for lithium is
LiMn0.6Fe0.4PO4。
Embodiment 3-6's differs only in content difference of the 532 type ternary materials with iron manganese phosphate for lithium, wherein embodiment 5
With 6 in two kinds of raw materials content in currently preferred range, the content of two kinds of raw materials is not in the present invention in embodiment 3 and 4
It is preferred that range in.
Embodiment 7-12
A kind of lithium ion battery, including positive electrode and negative material, the positive electrode respectively include embodiment 1-6 institutes
The iron manganese phosphate lithium doping ternary positive electrode active material stated further includes positive conductive agent and positive electrode binder, the positive-active
The mass ratio of material, positive conductive agent and positive electrode binder is 90:1:2, positive conductive agent is conductive carbon black, and positive electrode binder is
PVDF；
The negative material includes negative electrode active material, cathode conductive agent and negative electrode binder, the negative electrode active material,
The mass ratio of cathode conductive agent and negative electrode binder is 90:3:1, negative electrode active material is artificial graphite, and cathode conductive agent is to lead
The CMC and SBR for the quality such as electrical carbon is black, and negative electrode binder is.
Embodiment 13
A kind of lithium ion battery, including positive electrode and negative material, the positive electrode include the phosphorus described in embodiment 6
Sour ferromanganese lithium doping ternary positive electrode active material, further includes positive conductive agent and positive electrode binder, positive electrode active materials, just
The mass ratio of pole conductive agent and positive electrode binder is 95:1:2, positive conductive agent is conductive carbon black, positive electrode binder PVDF；
The negative material includes negative electrode active material, cathode conductive agent and negative electrode binder, the negative electrode active material,
The mass ratio of cathode conductive agent and negative electrode binder is 95:1:2, negative electrode active material is artificial graphite, and cathode conductive agent is to lead
The CMC and SBR for the quality such as electrical carbon is black, and negative electrode binder is.
As different from Example 12, in embodiment 13 in positive electrode and negative material the proportioning of each raw material in the present invention
It is preferred that range in.
The preparation method of the lithium ion battery of embodiment 7-13 includes the following steps：(a) it will include respectively the manganese phosphate
The positive electrode and negative material of iron lithium doping ternary positive electrode active material are coated on the two of plus plate current-collecting body and negative current collector
Then side is dried and is compacted, form positive plate and negative plate；
(b) positive plate and negative plate are assembled into battery core by required size；
(c) battery core is packed into shell, electrolyte is then injected into shell, then sealed up to the lithium ion battery.
Comparative example 1
A kind of lithium ion battery, as different from Example 7, positive electrode active materials are 532 type ternary materials in this comparative example
The chemical formula of material, the 532 type ternary material is LiNi0.5Mn0.3Co0.2O2。
Comparative example 2
A kind of lithium ion battery, as different from Example 7, positive electrode active materials are iron manganese phosphate for lithium in this comparative example,
The chemical formula of the iron manganese phosphate for lithium is LiMn0.5Fe0.5PO4。
Comparative example 3
A kind of lithium ion battery, as different from Example 7, positive electrode active materials include 532 type ternarys in this comparative example
2 mass parts of 5 mass parts of material and iron manganese phosphate for lithium.
The content of 532 type ternary materials is not in range provided by the present invention in this comparative example.
Comparative example 4
A kind of lithium ion battery, as different from Example 7, positive electrode active materials include 532 type ternarys in this comparative example
5 mass parts of 6 mass parts of material and iron manganese phosphate for lithium.
The content of iron manganese phosphate for lithium is not in range provided by the present invention in this comparative example.
The preparation method of the lithium ion battery of comparative example 1-4 is identical as the preparation method of embodiment 7.
Battery performance test
The bulk density for being measured embodiment 7-13 and the lithium ion battery in comparative example 1-4 respectively using electronic balance, is adopted
Electrochemical property test is carried out to the lithium ion battery in embodiment 7-13 and comparative example 1-4 respectively with lithium battery grading system, is tied
Fruit is as shown in table 1.
1 performance of lithium ion battery of table tests table
Although illustrate and describing the present invention with specific embodiment, it will be appreciated that without departing substantially from the present invention's
Many other change and modification can be made in the case of spirit and scope.It is, therefore, intended that in the following claims
Including belonging to all such changes and modifications in the scope of the invention.
Claims (10)
1. a kind of iron manganese phosphate lithium doping ternary positive electrode active material, which is characterized in that including 532 type ternary material 6-8 mass
Part and iron manganese phosphate for lithium 2-4 mass parts；
The chemical formula of the 532 type ternary material is LiNi0.5Mn0.3Co0.2O2；The chemical formula of the iron manganese phosphate for lithium is
LiMnxFe1-xPO4, wherein 0<x<1.
2. iron manganese phosphate lithium doping ternary positive electrode active material according to claim 1, which is characterized in that including 532 types
Ternary material 6.5-8 mass parts and iron manganese phosphate for lithium 2-3.5 mass parts.
3. iron manganese phosphate lithium doping ternary positive electrode active material according to claim 1, which is characterized in that including 532 types
Ternary material 6.5-7.5 mass parts and iron manganese phosphate for lithium 2.5-3.5 mass parts.
4. according to claim 1-3 any one of them iron manganese phosphate lithium doping ternary positive electrode active materials, which is characterized in that institute
It is LiMn to state iron manganese phosphate for lithium0.5Fe0.5PO4, LiMn0.6Fe0.4PO4, LiMn0.95Fe0.05PO4, LiMn0.8Fe0.2PO4Or
LiMn0.4Fe0.6PO4At least one of.
5. a kind of lithium ion battery, which is characterized in that including positive electrode, the positive electrode includes claim 1-4 any
Iron manganese phosphate lithium doping ternary positive electrode active material described in.
6. lithium ion battery according to claim 5, which is characterized in that the positive electrode further include positive conductive agent and
The mass ratio of positive electrode binder, the positive electrode active materials, positive conductive agent and positive electrode binder is 93-97:1-2:1-2, it is excellent
It is selected as 94-96:1-2:1-2；
Preferably, positive conductive agent includes conductive carbon black；
Preferably, positive electrode binder includes PVDF.
7. lithium ion battery according to claim 5 or 6, which is characterized in that the lithium ion battery further includes cathode material
Material, the negative material includes negative electrode active material, cathode conductive agent and negative electrode binder, the negative electrode active material, cathode
The mass ratio of conductive agent and negative electrode binder is 94-96:0.5-2:1-4, preferably 94-95:0.5-1:1-2.
8. lithium ion battery according to claim 7, which is characterized in that negative electrode active material includes natural graphite, artificial
At least one of graphite, soft carbon or hard carbon.
9. lithium ion battery according to claim 7, which is characterized in that cathode conductive agent includes conductive carbon black；
Preferably, negative electrode binder includes CMC and/or SBR；
Preferably, the mass ratio of CMC and SBR is 0.5-2:0.5-2, preferably 0.8-1.5:0.8-1.5.
10. the preparation method of claim 5-9 any one of them lithium ion batteries, which is characterized in that include the following steps：
(a) positive electrode comprising the iron manganese phosphate lithium doping ternary positive electrode active material and negative material are coated on anode respectively
The both sides of collector and negative current collector, are then dried and are compacted, and form positive plate and negative plate；
(b) positive plate and negative plate are assembled into battery core by required size；
(c) battery core is packed into shell, electrolyte is then injected into shell, then sealed up to the lithium ion battery.
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