KR20190011132A - Lithium-nikel composite oxide for positive electrode active material of secondary batteries containing residual lithium - Google Patents

Abstract

The present invention relates to a lithium-nickel composite oxide in which a Li-O-P compound is evenly distributed in an LNO matrix. More specifically, the present invention relates to the lithium-nickel composite oxide in which the Li-O-P compound is evenly distributed in the LNO matrix, wherein the Li-O-P compound is formed in the LNO matrix by using a phosphorus compound, thereby showing an effect of reducing remaining lithium, and a method for manufacturing the same.

Description

LITHIUM-NIKE COMPOSITE OXIDE FOR POSITIVE ELECTRODE ACTIVE MATERIAL OF SECONDARY BATTERIES CONTAINING RESIDUAL LITHIUM OF LI-O-P COMPOUNDS IN A LNO MATRIX

The present invention relates to a lithium-nickel composite oxide in which a Li-OP compound is evenly distributed in an LNO matrix, and more particularly, to a lithium-nickel composite oxide having an effect of forming a Li-OP compound in an LNO matrix using a phosphorus compound, Nickel complex oxide in which the Li-OP compound in the LNO matrix is evenly distributed, and a method for producing the lithium-nickel composite oxide.

In the lithium secondary battery, the cathode active material is a main source for discharging and absorbing lithium from the crystal lattice of the cathode material during charging and discharging of the cathode as a source of lithium and storing and discharging electric energy in the battery.

The Li-rich metal oxide includes Li ₂ NiO ₂ , Li ₂ CuO ₂ , Li ₂ Co _{0 . 4} Mn _{1 . 6} O _4, etc., which have a high charging capacity because they have a Li 2 equivalent or more. However, they have a low discharge capacity due to the R-3m structure transition in the Immm structure upon charging. However, such a Li-rich metal oxide is used as a sacrificial anode concept for compensating irreversible Li of a cathode in a lithium secondary battery field.

On the other hand, Li ₂ NiO ₂ (LNO) has a high residual lithium (LiOH, Li ₂ CO ₃ ) due to the unreacted Li ₂ O on the surface.

Conventionally, in order to reduce residual lithium, it was tried to reduce residual lithium by doping Ni sites with other metals. Korean Patent Laid-Open Publication No. 10-2016-002187 attempts to reduce residual lithium by Al doping. However, Al does not enter the LNO structure in the firing process and reacts first with a lithium source (Li ₂ O) Al-O type compound (Li ₅ AlO ₄ ), and the compound of Li-Al-O type (Li ₅ AlO ₄ ) is highly reactive with H ₂ O and CO ₂ and greatly influences the residual lithium increase of LNO Rather, it may be a factor of residual lithium increase.

Korean Patent Laid-Open Publication No. 10-2010-0036896 discloses a structure in which Al is coated on the surface by wet-coating and then drying by using an Al source material as an additional process after first synthesizing LNO. However, In order to form an oxide material, a temperature of 600 or higher is suitable, and Li-Al-O synthesis is performed first in the heat treatment of about 600, so that the residual lithium reduction effect is not significant.

Korean Patent Laid-Open Publication No. 10-2015-0049829 discloses a structure in which Al ₂ O ₃ and lithium phosphorus are heat-treated to a lithium transition metal oxide, wherein residual lithium and a coating source material And the lithium transition metal compound is coated on the high Ni NCM series with lithium phosphate to reduce residual lithium and improve the electrochemical characteristics However, in order to synthesize Li ₃ PO ₄ , a heat treatment temperature of at least 600 ° C. is required, and in the case of NCM, the structure may be changed or a side reaction may occur due to a high heat treatment temperature.

The present invention has been made in order to solve the problems of the prior art as described above, and it is an object of the present invention to provide a lithium secondary battery which uses a phosphorus (P) source material in a process of synthesizing a lithium- It is an object of the present invention to provide a positive electrode active material.

In order to achieve the above object, the present invention provides a lithium-nickel composite oxide in which Li-O-P compounds in an LNO matrix are evenly distributed.

The lithium-nickel composite oxide according to the present invention is characterized in that the content of P is 3 parts by weight or less per 100 parts by weight of the lithium-nickel composite oxide.

The lithium-nickel composite oxide according to the present invention is characterized by being represented by the formula (1).

≪ Formula 1 > Li _{2 + a} Ni _x O _{2 -b} A _b

(Wherein A is an anionic P and 0 < a? 0.3, 0 < b? 0.3, a + x = 1)

In the lithium-nickel composite oxide according to the present invention, the Li-OP compound is Li ₃ PO ₄ .

The present invention also relates to

(a) preparing a lithium-nickel composite oxide;

(b) adding a phosphorus (P) compound to the lithium-nickel composite oxide to prepare a mixture; And

(c) heat-treating the mixture. The present invention also provides a method for producing a lithium-nickel composite oxide for a lithium secondary battery having a reduced lithium content.

Li accordance with the present invention a method of manufacturing a nickel complex oxide, the phosphorus (P) compounds in step (b) is _{(NH 4) 2 HPO 4,} Mg 3 (PO) 4, Ba 3 (PO 4) 2 _{, (NH 4) 3 PO 4} , Cu 3 (PO 4) 2, Fe 3 (PO 4) 2, Ni 3 (PO 4) 2, MgNH 4 PO 4 .6H 2 O, K 3 PO 4, CoPO 4, _{NaH 2 PO 4 .7H 2 O,} Mg (H 2 PO 4) 2, Co 3 (PO 4) 2, K 2 HPO 4, Na 2 HPO 4, V 3 (PO 4) 5, and Ca (H ₂ PO ₄ ) ₂ .

In the method for producing a lithium-nickel composite oxide according to the present invention, in the step (a), the lithium-nickel composite oxide is a complex of Li ₂ NiO ₂ and LNO.

In the method for producing a lithium-nickel composite oxide according to the present invention, the step (a) of producing the lithium-

(a-1) mixing a lithium (Li) compound, a nickel (Ni) compound and a phosphorus (P) compound to prepare a mixture; And

(a-2) firing the mixture under an inert atmosphere; And a control unit.

In the method for producing a lithium-nickel composite oxide according to the present invention, in the step (a-1), the lithium compound is Li ₂ O, LiOH, Li ₂ CO ₃ , Li ₂ NO ₃ , Li ₂ MnO ₃ , LiScO ₂ , Li ₂ ZrO ₃ , LiYO ₂ , Li ₂ ZrO ₃ , LiAlO ₂ , LiAl ₅ O ₈ , LiGaO ₂ , LiLaO ₂ , Li ₂ SiO ₃ , Li ₂ GeO ₃ and LiCH ₃ CO ₂ And is characterized by being either one.

Li accordance with the present invention a method of manufacturing a nickel complex oxide, the nickel (Ni) compound in the (a-1) step, _{NiO, Ni (OH) 2,} NiOOH, NiCO 3 · 2Ni (OH) 2 · 4H ₂ O, NiC ₂ O _{4 ·} and the _{2H 2 O, Ni (NO 3} ) 2 · 6H 2 O, NiSO 4 and NiSO _{4 ·} characterized in that any one selected from the group consisting of 6H ₂ O.

Li accordance with the present invention a method of manufacturing a nickel composite oxide, is the phosphorus (P) compounds in the (a-1) Step _{(NH 4) 2 HPO 4,} Mg 3 (PO) 4, Ba 3 (PO 4 ) ₂ , (NH ₄ ) ₃ PO ₄ , Cu ₃ (PO ₄ ) ₂ , Fe ₃ (PO ₄ ) ₂ , Ni ₃ (PO ₄ ) ₂ , MgNH ₄ PO ₄ .6H ₂ O, K ₃ PO ₄ , _{4, NaH 2 PO 4 · 7H} 2 O, Mg (H 2 PO 4) 2, Co 3 (PO 4) 2, K 2 HPO 4, Na 2 HPO 4, V 3 (PO 4) 5, and Ca (H ₂ PO ₄₎ and being selected from the group consisting of: _2.

The present invention also provides a lithium secondary battery using the lithium-nickel composite oxide produced by the present invention as a cathode active material.

The present invention relates to a method for producing a lithium-nickel composite oxide, which comprises calcining a phosphorus (P) source material together with a lithium compound, a nickel compound and a dry coating of a lithium-nickel composite oxide or a phosphorus (P) source material in the production of a lithium- There is an effect of providing a lithium-nickel composite oxide for a cathode active material for a secondary battery.

FIG. 1 shows the results of measurement of residual lithium in the lithium-nickel composite oxide according to Example 1 of the present invention and Comparative Example 1 and Comparative Example 2. FIG.
2 is a result of surface XPS analysis of the lithium-nickel composite oxide according to Example 1 and Comparative Example 2 of the present invention.
3 shows the results of measurement of residual lithium of the lithium-nickel composite oxide according to Example 2 and Comparative Example 2 of the present invention.
4 shows the XRD analysis results of the lithium-nickel composite oxide according to Example 2 and Comparative Example 2 of the present invention.

Hereinafter, the present invention will be described in more detail with reference to Examples. It is to be understood by those skilled in the art that these examples are for illustrative purposes only and that the scope of the present invention is not construed as being limited by these examples.

Example 1. Preparation of cathode active material

Nickel oxide NiO (OH) ₂ was sintered at 600 ° C for 10 hours under an oxygen atmosphere to prepare nickel oxide NiO. The molar ratio of Li and Ni was designed to 2.03, The prepared nickel oxide oxide and lithium oxide were mixed and fired in a nitrogen atmosphere at 685 캜 for 18 hours to prepare a lithium-nickel composite oxide (Li ₂ NiO ₂ : LNO).

The prepared LNO was pulverized and crushed again to make LNO having an average particle size of 14 μm and then mixed with 1 wt% ammonium phosphate (NH ₄ ) ₂ HPO _{4 as a} source material of phosphorus (P) Atmosphere at 685 DEG C for 6 hours to form a lithium-nickel composite oxide in which the Li-OP compound was evenly distributed in the LNO matrix.

Comparative Example 1

Nickel oxide NiO (OH) ₂ was sintered at 600 ° C for 10 hours in an oxygen atmosphere to prepare nickel oxide NiO. The molar ratio of Li to Ni and Al was designed to be 2.03 Thereafter, the prepared nickel oxide oxide, lithium oxide and aluminum hydroxide Al (OH) ₃ were mixed and fired in a nitrogen atmosphere at 685 DEG C for 18 hours to prepare a lithium-nickel composite oxide (LNO). The prepared LNO was pulverized and pulverized again to prepare LNO having an average particle diameter of 14 탆. The aluminum hydroxide used herein was a material having a purity of 98% and an average particle diameter of 1.5 to 3 탆.

Comparative Example 2

Nickel oxide NiO (OH) ₂ was sintered at 600 ° C for 10 hours under an oxygen atmosphere to prepare nickel oxide NiO. The molar ratio of Li and Ni was designed to 2.03, The prepared nickel oxide oxide and lithium oxide were mixed and fired in a nitrogen atmosphere at 685 캜 for 18 hours to prepare a lithium-nickel composite oxide (Li ₂ NiO ₂ : LNO). The prepared LNO was pulverized and pulverized again to prepare LNO having an average particle diameter of 14 탆.

Production Example 1. Preparation of Cell

In order to evaluate the electrochemical performance of the product, the mixing ratio of the final product, the denka black and the binder (KF1120) was 85: 10: 5 by weight, and the mixture was uniformly coated on the Al foil. Rolled and vacuum-dried in a vacuum oven at 120 ° C to produce a positive electrode for a coin half cell (2032). The counter electrode was made of Li-metal, and LiPF ₆ 1.0M EC: EMC 1: 2 (Vol%) was used as the electrolyte. The half-cell was manufactured and its capacity (mAh / g) was evaluated by a conventional method.

LNO sample Residual lithium
LiOH
(wt%) Residual lithium
Li ₂ CO ₃
(wt%) P content
(ppm) charge
(mAh / g) Discharge
(mAh / g) Li ₃ PO ₄
Binding
energy
(Home) Example 1
Al doping (X)
P coating / 1 wt% 1.24 0.46 2027 397.5 132.7 ~ 133.6 Comparative Example 1
Al doping (O) 4.63 0.50 - 395.3 132.2 N.D. Comparative Example 2
Al doping (X) 4.25 0.57 - 390.9 134.4 N.D. Example 2
Al doping (X)
P doping / 2.5 wt% 1.80 0.35 5107 395.6 137.4 ~ 133.6 Example 3
Al doping (X)
P doping / 2.5 wt%
(Change source) 1.97 0.41 1977 393.1 132.1 ~ 133.6 Example 4
Al doping (X)
P doping / 5 wt% 1.91 0.34 11652 398.9 126.3 ~ 133.6 Example 5
Al doping (X)
P doping / 14 wt% 1.61 0.21 30002 342.2 110.8 ~ 133.6 Example 6
Al doping (X)
P doping / 2.5 wt%
N2 + Air flow 6.74 0.98 1894 326.5 11.21 ~ 133.6

Experimental Example 1. Residual lithium measurement

A test method for measuring the residual amount of lithium-nickel complex oxide (LNO) in the prepared lithium-nickel composite oxide (LNO) was used.

Specifically, 10 g of lithium nickel composite oxide (LNO) was weighed and dispersed in 1000 ml of pure water for 5 minutes with stirring, and then the solids were removed using two filter paper with the dispersed solution. The solution from which the solid content was removed was collected and measured in an auto-titration apparatus at a concentration of 0.1 N HCl in accordance with titration conditions to calculate the amount of residual lithium.

The amount of residual lithium was measured for the cathode active material prepared in Example 1, Comparative Example 1 and Comparative Example 2, and the results are shown in FIG. 1 and summarized in Table 1.

(LiOH) on the surface of the cathode active material through dry mixing with the phosphorus (P) source material and heat treatment after the production of the lithium-nickel composite oxide (LNO) according to the embodiment of the present invention, And the phosphorus (P) source material, Li-OP was generated on the surface, thereby reducing residual lithium on the surface.

Experimental Example 2. Measurement of cell characteristics

The charge / discharge characteristics and efficiency of the coin cell fabricated from the samples of Example 1, Comparative Example 1 and Comparative Example 2 were measured, and the measurement results are summarized in Table 1 above.

Referring to the first embodiment and the second embodiment, after the phosphorus (P) source material is dry-mixed and heat-treated or the phosphorous source material is added together with the phosphorus source material, the residual lithium is reduced .

Experimental Example 3: Surface XPS analysis

The binding energy of the compound present on the surface of the cathode active material was analyzed through surface XPS analysis of the cathode active material prepared in Example 1 and Comparative Example 2, and the analysis result is shown in FIG.

XPS Analysis Equipment / Models VG Scientific / ESCALAB-250 Analytical area
Voltage / Current About Φ1.1mm
15Kv / 10Ma X-ray source Al

In FIG. 2, it can be seen that a peak was observed at ~ 133.6 eV in the case of the lithium-nickel composite oxide prepared in Example 1 above.

In the case of the binding energy of Li ₃ PO ₄ , peaks appear at ~ 133.6 eV. It is known that the reaction between Li ₃ PO ₄ and Li ₃ PO ₄ by the reaction of residual lithium and P source on the surface of the lithium- .

Example 2: Preparation of cathode active material

Nickel oxide NiO (OH) ₂ was baked at 600 ° C for 10 hours in an oxygen atmosphere to prepare nickel oxide NiO. The molar ratio of Li to Ni was designed to 2.03 (NH ₄ ) ₂ HPO ₄ of 6.8 wt% of a mixed amount of nickel oxide and lithium oxide was added to the mixed oxide of nickel oxide and lithium oxide, followed by baking at 685 ° C. for 18 hours in a nitrogen atmosphere A lithium-nickel composite oxide (Li ₂ NiO ₂ : LNO) was produced. The prepared LNO was pulverized and pulverized again to prepare LNO having an average particle diameter of 14 탆.

Example 3: Preparation of cathode active material

Nickel oxide NiO (OH) ₂ was sintered at 600 ° C for 10 hours under an oxygen atmosphere to prepare nickel oxide NiO. The molar ratio of Li and Ni was designed to 2.03, Nickel phosphate (Ni ₃ (PO ₄ ) ₂ ) in an amount of 2.5 wt% of a mixed oxide of nickel oxide and lithium oxide was further added and the mixture was calcined at 685 ° C for 18 hours in a nitrogen atmosphere A lithium-nickel composite oxide (Li ₂ NiO ₂ : LNO) was produced.

Example 4. Preparation of cathode active material

Nickel oxide NiO (OH) ₂ was sintered at 600 ° C for 10 hours in an oxygen atmosphere to prepare nickel oxide NiO. The molar ratio of Li to Ni was designed to 2.03 (NH ₄ ) ₂ HPO ₄ 5 wt% of a mixed amount of nickel oxide and lithium oxide was added to the mixed oxide of nickel oxide and lithium oxide, followed by baking at 685 ° C. for 18 hours in a nitrogen atmosphere A lithium-nickel composite oxide (Li ₂ NiO ₂ : LNO) was produced.

Example 5. Preparation of cathode active material

Nickel oxide NiO (OH) ₂ was sintered at 600 ° C for 10 hours under an oxygen atmosphere to prepare nickel oxide NiO. The molar ratio of Li and Ni was designed to 2.03, When the prepared nickel oxide oxide and lithium oxide were mixed, addition of 14 wt% ammonium phosphate (NH ₄ ) ₂ HPO ₄ of 10 wt% of a mixed amount of nickel oxide and lithium oxide was carried out and the mixture was calcined at 685 ° C. for 18 hours in a nitrogen atmosphere Thereby forming a lithium-nickel composite oxide (Li ₂ NiO ₂ : LNO).

Example 6. Preparation of cathode active material

Nickel oxide NiO (OH) ₂ was sintered at 600 ° C for 10 hours under an oxygen atmosphere to prepare nickel oxide NiO. The molar ratio of Li and Ni was designed to 2.03, When the prepared nickel oxide oxide and lithium oxide were mixed, 2.5 wt% of ammonium phosphate (NH ₄ ) ₂ HPO ₄ of 1.5 wt% of the mixed amount of nickel oxide and lithium oxide was added, and nitrogen and air gas were added sintering in a mixed atmosphere of 685 ℃, 18 hours, lithium-nickel composite oxide (Li ₂ NiO _2: LNO) made.

Preparation Example 2. Preparation of Cell

A coin cell was prepared in the same manner as in Preparation Example 1 for the positive electrode active material prepared in Example 2.

Experimental Example 4. Residual lithium measurement

Residual lithium was measured for the cathode active material prepared in Example 2, and the results are shown in FIG. 3 and Table 1 together with the results of the residual lithium measurement of the cathode active material prepared in Comparative Example 2.

Referring to FIG. 3 and Table 1, the phosphorus (P) source material is not doped in the lithium-nickel composite oxide structure, and a Li-OP compound is produced by reaction with unreacted Li ₂ O during firing, , Respectively. In addition, Li ₂ O, NiO and phosphorus (P) source materials are mixed and fired during the firing of the lithium-nickel composite oxide, not the additional coating process, to confirm that the residual lithium is removed.

Experimental Example 5. Measurement of Battery Characteristics

The charge / discharge characteristics and efficiency of the coin cell manufactured in Production Example 2 were measured, and the measurement results are summarized in Table 1 above.

Referring to Experimental Example 4 and Experimental Example 5, it can be confirmed that residual lithium was reduced without decreasing the charge-discharge capacity in the production of the lithium-nickel composite oxide by mixing the phosphorus (P) source material.

Experimental Example 6. Structural Analysis

The structure of the cathode active material prepared in Example 2 and Comparative Example 2 was analyzed by X-ray diffraction (XRD). The XRD equipment used in the analysis was Rigaku and SmartLab equipment. XRD measurement conditions were 10 ~ 80 (2 Theta), CuK 1, 45 Kv, 200 mA, and the results are shown in FIG.

Referring to FIG. 4, it can be seen that peaks are observed at the same position although there is a difference in strength, and it is confirmed that the phosphorus (P) source material in Example 2 does not affect the lithium-nickel composite oxide structure .

Having described specific portions of the present invention in detail, those skilled in the art will appreciate that these specific embodiments are merely preferred embodiments and that the scope of the present invention is not limited thereby. something to do. Accordingly, the actual scope of the present invention will be defined by the appended claims and their equivalents.

Claims (12)

Lithium-nickel composite oxide in which the Li-OP compound in the LNO matrix is evenly distributed.
The method according to claim 1,
The P content of the lithium-nickel composite oxide in which the Li-OP compound is evenly distributed is not more than 3 parts by weight per 100 parts by weight of the lithium-nickel composite oxide
Lithium-nickel composite oxide in which the Li-OP compound in the LNO matrix is evenly distributed.
The method according to claim 1,
Wherein the lithium-nickel composite oxide is represented by the following formula (1)
Lithium-nickel composite oxide in which the Li-OP compound in the LNO matrix is evenly distributed.
&Lt; Formula 1 > Li _{2 + a} Ni _x O _{2 -b} A _b
(Wherein A is an anionic P and 0 < a? 0.3, 0 < b? 0.3, a + x = 1)
The method according to claim 1,
The Li-OP compound is Li ₃ PO ₄ The
Lithium-nickel composite oxide in which the Li-OP compound in the LNO matrix is evenly distributed.
(a) preparing a lithium-nickel composite oxide;
(b) adding a phosphorus (P) compound to the lithium-nickel composite oxide to prepare a mixture; And
(c) heat treating the mixture; and
A method for producing a lithium-nickel composite oxide for a cathode active material of a secondary battery with reduced residual lithium.
6. The method of claim 5,
The phosphorus (P) compounds in step (b) is _{(NH 4) 2 HPO 4,} Mg 3 (PO) 4, Ba 3 (PO 4) 2, (NH 4) 3 PO 4, Cu 3 (PO 4) _{2, Fe 3 (PO 4)} 2, Ni 3 (PO 4) 2, MgNH 4 PO 4 .6H 2 O, K 3 PO 4, CoPO 4, NaH 2 PO 4 .7H 2 O, Mg (H 2 PO 4 ) _2, would _{Co 3 (PO 4) 2,} K 2 HPO 4, Na 2 HPO 4, V 3 (PO 4) 5, and Ca (H ₂ PO ₄₎ is selected from the group consisting of ₂
A method for producing a lithium-nickel composite oxide for a cathode active material of a secondary battery with reduced residual lithium.
6. The method of claim 5,
In the step (a), the lithium-nickel composite oxide is a complex of Li ₂ NiO ₂ and LNO
A method for producing a lithium-nickel composite oxide for a cathode active material of a secondary battery with reduced residual lithium.
6. The method of claim 5,
The step of (a) preparing the lithium-nickel composite oxide comprises
(a-1) mixing a lithium (Li) compound, a nickel (Ni) compound and a phosphorus (P) compound to prepare a mixture; And
(a-2) firing the mixture under an inert atmosphere; Containing
A method for producing a lithium-nickel composite oxide for a cathode active material of a secondary battery with reduced residual lithium.
9. The method of claim 8,
In the step (a-1), the lithium compound may be Li ₂ O, LiOH, Li ₂ CO ₃ , Li ₂ NO ₃ , Li ₂ MnO ₃ , LiScO ₂ , Li ₂ ZrO ₃ , LiYO ₂ , Li ₂ ZrO ₃ , LiAlO ₂ , LiAl ₅ O ₈ , LiGaO ₂ , LiLaO ₂ , Li ₂ SiO ₃ , Li ₂ GeO ₃ and LiCH ₃ CO ₂ .
A method for producing a lithium-nickel composite oxide for a cathode active material of a secondary battery with reduced residual lithium.
9. The method of claim 8,
The nickel (Ni) compound in the (a-1) step, _{NiO, Ni (OH) 2,} NiOOH, NiCO 3 · 2Ni (OH) 2 · 4H 2 O, NiC 2 O 4 · 2H 2 O, Ni (NO will _{3) 2 · 6H 2 O,} NiSO 4 and NiSO _{4 ·} selected from the group consisting of 6H ₂ O
A method for producing a lithium-nickel composite oxide for a cathode active material of a secondary battery with reduced residual lithium.
9. The method of claim 8,
The phosphorus (P) compounds in the (a-1) step, _{(NH 4) 2 HPO 4,} Mg 3 (PO) 4, Ba 3 (PO 4) 2, (NH 4) 3 PO 4, Cu 3 (PO _{4) 2, Fe 3 (PO} 4) 2, Ni 3 (PO 4) 2, MgNH 4 PO 4 .6H 2 O, K 3 PO 4, CoPO 4, NaH 2 PO 4 .7H 2 O, Mg (H 2 would _{PO 4) 2, Co 3 (} PO 4) 2, K 2 HPO 4, Na 2 HPO 4, V 3 (PO 4) 5, and Ca (H ₂ PO ₄₎ is selected from the group consisting of ₂
A method for producing a lithium-nickel composite oxide for a cathode active material of a secondary battery with reduced residual lithium.
A lithium secondary battery using the lithium-nickel composite oxide of claim 1 as a cathode active material.

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