CN104201374A - High-capacity lithium ion battery cathode material and preparation method thereof - Google Patents
High-capacity lithium ion battery cathode material and preparation method thereof Download PDFInfo
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- CN104201374A CN104201374A CN201410461935.XA CN201410461935A CN104201374A CN 104201374 A CN104201374 A CN 104201374A CN 201410461935 A CN201410461935 A CN 201410461935A CN 104201374 A CN104201374 A CN 104201374A
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- 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
- H01M4/362—Composites
- H01M4/364—Composites as mixtures
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- 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
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- 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
- H01M4/485—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of mixed oxides or hydroxides for inserting or intercalating light metals, e.g. LiTi2O4 or LiTi2OxFy
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- 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
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- 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
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M4/628—Inhibitors, e.g. gassing inhibitors, corrosion inhibitors
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
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Abstract
The invention relates to a high-capacity lithium ion battery cathode material and a preparation method thereof. The material consists of two active substances, namely LiNi<1-a-b>CoaAlbO2 and lithium cobalt oxide, as well as Al2O3 coating layers coating the surfaces of the active substances, wherein a is larger than 0.1 and smaller than 0.3, b is larger than 0.01 and smaller than 0.2, and 1-a-b is larger than 0 and smaller than 1; a lithium nickel and cobalt aluminate material accounts for 10-90 percent of the mass sum of the lithium nickel and cobalt aluminate material and the lithium cobalt oxide; the mass ratio of the Al2O3 coating layers to the active substances is (0.001-0.05):1. The preparation method comprises the following steps: uniformly mixing the two active substances, namely the LiNi1-a-bCoaAlbO2 and the lithium cobalt oxide according to the certain proportion; adding the mixture into a trivalent aluminum source solution and stirring to form a solid-liquid mixture; enabling the trivalent aluminum source solution to uniformly coat the surfaces of active substance particles; drying and calcining to obtain the high-capacity lithium ion battery cathode material. The specific capacity of the material disclosed by the invention is greatly improved compared with that of the lithium cobalt oxide; the compaction density, the conductivity and a voltage platform of the material are greatly improved compared with those of the lithium nickel and cobalt aluminate material; the material has better rate performance and cycle performance.
Description
Technical field
The present invention relates to a kind of lithium ion battery, particularly relate to anode material for lithium-ion batteries of a kind of high power capacity and preparation method thereof.
Technical background
Lithium ion battery has been widely used in the mobile digital product scopes such as mobile phone, camera, notebook computer, along with scientific and technological progress, the application of lithium ion battery will be more and more wider, requirement to its size, weight, useful life etc. is also more and more higher, and the positive electrodes such as the lithium of the cobalt of application acid in the market, LiFePO4, LiMn2O4 have been difficult to meet the demand of market to lithium ion battery high-energy-density.
Under the condition of performance same capability, improve the volume energy density of battery, just need to improve the loading of active material unit volume, the compacted density of material is larger, and volume loading is also just larger, and its volume energy density is just higher.And cobalt acid lithium has the high feature of compacting, electric conductivity and cycle performance are better simultaneously, but the specific capacity of cobalt acid lithium is lower, and can cause other electrical properties to reduce when improving compacted density, and the space of further improving energy density is less.Therefore the positive electrode of developing height ratio capacity is imperative, it is high that nickel cobalt lithium aluminate positive electrode has specific capacity, good cycle, the advantage such as raw material is cheap, but its low conductivity and low compacted density have limited the application of this material on lithium ion battery with high energy density.Bi-material is mixed to use, can be that bi-material obtains complementation in performance, and capacity, compacted density, the conductivity of composite material are all increased, simultaneously cycle performance and be doubly forthrightly also improved.
Summary of the invention
The object of the present invention is to provide a kind of high power capacity, forthright good low-cost positive electrode doubly, overcome the deficiency of existing positive electrode, adopt coated modification simultaneously, improve the cycle performance of material.
To achieve these goals, the present invention has adopted following technical scheme:
First aspect, a kind of anode material for lithium-ion batteries of high power capacity, described composite positive pole is by LiNi
1-a-bco
aal
bo
2, cobalt acid two kinds of active materials of lithium and be coated on the Al on active material surface
2o
3coating layer forms, 0.1<a<0.3 wherein, 0.01<b<0.2,0<1-a-b<1.
As preferably, described nickel cobalt lithium aluminate material accounts for 10%～90% of nickel cobalt lithium aluminate material and cobalt acid lithium quality summation.
As preferably, described Al
2o
3the mass ratio of coating layer and active material is 0.001～0.05:1.
As further preferred, described Al
2o
3the mass ratio of coating layer and active material is 0.005～0.02:1.
Second aspect, a kind of preparation method of anode material for lithium-ion batteries of the high power capacity as described in first aspect, is characterized in that, comprises the following steps:
(1) by a certain amount of LiNi
1-a-bco
aal
bo
2mix according to a certain percentage with two kinds of active materials of cobalt acid lithium;
(2) mixed active material is joined in the solution of trivalent aluminium source and stir and form solidliquid mixture, make aluminium source solution evenly be coated on active material particle surface;
(3) by step, the solidliquid mixture in is (2) dried, and dried solid material is calcined after a period of time at a certain temperature, cooling, pulverize, sieving obtains positive electrode
As preferably, described LiNi
1-a-bco
aal
bo
2d50 be 5～25 μ m, the D50 of cobalt acid lithium is 5～25 μ m.
As further optimization, described LiNi
1-a-bco
aal
bo
2for the second particle that primary particle is reunited and formed, D50 is 10～20 μ m, D10>=5 μ m, and D90≤30 μ m, the D50 of described cobalt acid lithium is 10～20 μ m, D10>=5 μ m, D90≤30 μ m.
As preferably, trivalent aluminium source solution is aluminum nitrate aqueous solution.
As preferably, described calcining heat is 500～800 ℃, and calcination time is 3～10h.
Compared with prior art, great advantage of the present invention and beneficial effect are as follows:
(1) bi-material is mixed according to a certain percentage, make the specific capacity of the composite material of gained have more significantly and improve with respect to the sour lithium of cobalt, compacted density, conductivity and voltage platform are enhanced with respect to nickel cobalt lithium aluminate material.
(2) nickel cobalt lithium aluminate positive electrode very easily absorbs appearance " jelly " phenomenon, adopt aluminum nitrate as the raw material of clad material, aluminum nitrate aqueous solution is faintly acid, can carry out pickling to composite material, reduce the pH value of material, material is carried out to K cryogenic treatment simultaneously, can improve drawing abillity, guarantee the consistency of pole piece.
(3) mixed material being carried out to surface is coated, make coating layer in isolated electrolyte and positive electrode, lithium ion freely be passed through, thereby avoid the decomposition of electrolyte under high voltage completing when discharging and recharging, improved cycle life and the stability of ion battery.
Documents:
CN102544474B discloses the preparation method of high energy energy density positive composite material of lithium battery, by LiCoO
2with LiNi
xco
ym
(1-x-y)o
2bi-material proportionally mixes, after mixing, process to reduce lithium carbonate, the lithia impurity of composite material remained on surface, improve energy density, processing characteristics and the cycle performance of material, difference of the present invention is that mixed material is coated, aluminum nitrate aqueous solution is faintly acid simultaneously, can reduce the pH value of composite material.
Accompanying drawing explanation
Fig. 1 is the first charge-discharge curve chart of the composite positive pole of embodiment 1.
Fig. 2 is the cycle charge-discharge curve chart of the composite positive pole of embodiment 1.
Embodiment
For the present invention being had to darker understanding; below in conjunction with embodiment, technical scheme is clearly and completely described; but embodiments of the invention are only used to explain the present invention; and unrestricted the present invention; the every other case study on implementation that those skilled in the art obtain under the prerequisite of not making creative work, all belongs to protection scope of the present invention.
Embodiment 1:
By LiNi
0.8co
0.15al
0.05o
2be dry mixed in the ratio of 5:5 with two kinds of active materials of cobalt acid lithium, mixing time is 2h.
Aluminum nitrate is at room temperature mixed with respectively to aluminum nitrate solution, above-mentioned mixed active material is joined in aluminum nitrate solution and stirs and form solidliquid mixture, make aluminum nitrate solution evenly be coated on active material particle surface; By forming Al after aluminum nitrate calcining
2o
3quality account for mix after active material quality 1%.
Above-mentioned solidliquid mixture is dried, dried solid material is put into stove and carry out roasting, with the heating rate of 4 ℃/min, rise to 500 ℃, and at 500 ℃ of insulation 7h, cooling, obtain composite positive pole after pulverizing, sieving.
The electrochemical property test of material adopts blue electric battery test system to test at 25 ℃, and test voltage scope is 3V～4.3V; High rate performance test condition: 0.2C discharges and recharges once, and 0.2C charging 1C electric discharge once; Cycle performance test condition: discharge and recharge with 1C multiplying power, circulate 100 weeks, investigate capability retention.The specific discharge capacity of material under 0.2C multiplying power is 181.2mAh/g, and the specific discharge capacity under 1C multiplying power is 172mAh/g, and 1C/0.2C electric discharge ratio is 94.9%, and high rate performance is better.100 weeks capability retentions of 1C charge and discharge cycles are greater than 97%, and cycle performance is better.
Embodiment 2:
By LiNi
0.8co
0.15al
0.05o
2be dry mixed in the ratio of 6:4 with two kinds of active materials of cobalt acid lithium, mixing time is 2h.
Aluminum nitrate is at room temperature mixed with respectively to aluminum nitrate solution, above-mentioned mixed active material is joined in aluminum nitrate solution and stirs and form solidliquid mixture, make aluminum nitrate solution evenly be coated on active material particle surface; By forming Al after aluminum nitrate calcining
2o
3quality account for mix after active material quality 0.5%.
Above-mentioned solidliquid mixture is dried, dried solid material is put into stove and carry out roasting, with the heating rate of 4 ℃/min, rise to 600 ℃, and at 600 ℃ of insulation 6h, cooling, obtain composite positive pole after pulverizing, sieving.
Embodiment 3:
By LiNi
0.8co
0.1al
0.1o
2be dry mixed in the ratio of 4:6 with two kinds of active materials of cobalt acid lithium, mixing time is 2h.
Aluminum nitrate is at room temperature mixed with respectively to aluminum nitrate solution, above-mentioned mixed active material is joined in aluminum nitrate solution and stirs and form solidliquid mixture, make aluminum nitrate solution evenly be coated on active material particle surface; By forming Al after aluminum nitrate calcining
2o
3quality account for mix after active material quality 2%.
Above-mentioned solidliquid mixture is dried, dried solid material is put into stove and carry out roasting, with the heating rate of 4 ℃/min, rise to 700 ℃, and at 700 ℃ of insulation 5h, cooling, obtain composite positive pole after pulverizing, sieving.
Embodiment 4:
By LiNi
0.8co
0.18al
0.02o
2be dry mixed in the ratio of 3:7 with two kinds of active materials of cobalt acid lithium, mixing time is 2h.
Aluminum nitrate is at room temperature mixed with respectively to aluminum nitrate solution, above-mentioned mixed active material is joined in aluminum nitrate solution and stirs and form solidliquid mixture, make aluminum nitrate solution evenly be coated on active material particle surface; By forming Al after aluminum nitrate calcining
2o
3quality account for mix after active material quality 2%.
Above-mentioned solidliquid mixture is dried, dried solid material is put into stove and carry out roasting, with the heating rate of 4 ℃/min, rise to 600 ℃, and at 600 ℃ of insulation 5h, cooling, obtain composite positive pole after pulverizing, sieving.
Claims (9)
1. an anode material for lithium-ion batteries for high power capacity, is characterized in that, by LiNi
1-a-bco
aal
bo
2, cobalt acid two kinds of active materials of lithium and be coated on the Al on active material surface
2o
3coating layer forms, 0.1<a<0.3 wherein, 0.01<b<0.2,0<1-a-b<1.
2. the anode material for lithium-ion batteries of high power capacity according to claim 1, is characterized in that, described nickel cobalt lithium aluminate ternary material accounts for 10%～90% of nickel cobalt lithium aluminate ternary material and cobalt acid lithium quality summation.
3. the anode material for lithium-ion batteries of high power capacity according to claim 1, is characterized in that, described Al
2o
3the mass ratio of coating layer and active material is 0.001～0.05:1.
4. the anode material for lithium-ion batteries of high power capacity according to claim 1, is characterized in that, described Al
2o
3the mass ratio of coating layer and active material is 0.005～0.02:1.
5. a preparation method for the anode material for lithium-ion batteries of high power capacity according to claim 1, is characterized in that, comprises the following steps:
(1) by a certain amount of LiNi
1-a-bco
aal
bo
2mix according to a certain percentage with two kinds of active materials of cobalt acid lithium;
(2) mixed active material is joined in the solution of trivalent aluminium source and stir and form solidliquid mixture, make aluminium source solution evenly be coated on active material particle surface;
(3) by step, the solidliquid mixture in is (2) dried, and dried solid material is calcined after a period of time at a certain temperature, cooling, pulverize, sieving obtains positive electrode.
6. the preparation method of the anode material for lithium-ion batteries of high power capacity according to claim 5, is characterized in that, described LiNi
1-a-bco
aal
bo
2d50 be 5～25 μ m, the D50 of cobalt acid lithium is 5～25 μ m.
7. the preparation method of the anode material for lithium-ion batteries of high power capacity according to claim 5, is characterized in that, described LiNi
1-a-bco
aal
bo
2for the second particle that primary particle is reunited and formed, D50 is 10～20 μ m, D10>=5 μ m, and D90≤30 μ m, the D50 of described cobalt acid lithium is 10～20 μ m, D10>=5 μ m, D90≤30 μ m.
8. the preparation method of the anode material for lithium-ion batteries of high power capacity according to claim 5, is characterized in that, described trivalent aluminium source solution is aluminum nitrate aqueous solution.
9. the preparation method of the anode material for lithium-ion batteries of high power capacity according to claim 5, is characterized in that, described calcining heat is 500～800 ℃, and calcination time is 3～10h.
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Cited By (6)
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| CN104577093A (en) * | 2015-01-13 | 2015-04-29 | 海宁美达瑞新材料科技有限公司 | Surface coating modified lithium ion battery cathode material and preparation method thereof |
| CN104900881A (en) * | 2015-06-09 | 2015-09-09 | 海宁美达瑞新材料科技有限公司 | Lead-doped modified lithium ion battery composite positive electrode material and preparation method thereof |
| CN105428625A (en) * | 2015-12-09 | 2016-03-23 | 山东齐星新材料科技有限公司 | Method for preparing alumina coated lithium cobalt oxide lithium ion battery material by aluminum salt solution aftertreatment |
| CN106450202A (en) * | 2016-11-01 | 2017-02-22 | 江苏海四达电源股份有限公司 | Positive and negative electrode materials and electrode system of high-compaction high-capacity lithium ion battery |
| CN108886146A (en) * | 2016-03-30 | 2018-11-23 | 松下知识产权经营株式会社 | Positive electrode active material for nonaqueous electrolyte secondary battery, the manufacturing method of positive electrode active material for nonaqueous electrolyte secondary battery and non-aqueous electrolyte secondary battery |
| CN113921891A (en) * | 2021-09-07 | 2022-01-11 | 山东派智新能源科技有限公司 | Low-temperature large-magnification cylindrical lithium ion battery and manufacturing method thereof |
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Cited By (7)
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| CN104577093A (en) * | 2015-01-13 | 2015-04-29 | 海宁美达瑞新材料科技有限公司 | Surface coating modified lithium ion battery cathode material and preparation method thereof |
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| CN108886146A (en) * | 2016-03-30 | 2018-11-23 | 松下知识产权经营株式会社 | Positive electrode active material for nonaqueous electrolyte secondary battery, the manufacturing method of positive electrode active material for nonaqueous electrolyte secondary battery and non-aqueous electrolyte secondary battery |
| CN108886146B (en) * | 2016-03-30 | 2023-02-17 | 松下知识产权经营株式会社 | Positive electrode active material for nonaqueous electrolyte secondary battery, method for producing same, and nonaqueous electrolyte secondary battery |
| CN106450202A (en) * | 2016-11-01 | 2017-02-22 | 江苏海四达电源股份有限公司 | Positive and negative electrode materials and electrode system of high-compaction high-capacity lithium ion battery |
| CN113921891A (en) * | 2021-09-07 | 2022-01-11 | 山东派智新能源科技有限公司 | Low-temperature large-magnification cylindrical lithium ion battery and manufacturing method thereof |
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