# US 7,608,365 B1 · Positive active material composition for rechargeable lithium battery and method of preparing positive electrode using same

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- Number: US 7,608,365 B1
- Document ID: US7608365B1
- Status: Granted
- Kind: B1
- Application number: 09/579,576
- Filed: 2000-05-25
- Granted: 2009-10-27
- Earliest claimed: 1999-05-25
- Assignees: Samsung SDI Co., Ltd.
- Inventors: Ho-Jin Kweon; Geun-Bae Kim; Hyun-Suk Jeong; Dong-Gon Park; Ki-Ho Kim
- Web page: https://patentgrep.com/patent/US7608365B1

## CPC

- H01M 4/131: Electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
- C01G 45/1228: of the type (MnO2)-, e.g. LiMnO2 or Li(MxMn1-x)O2
- C01G 45/1242: of the type (Mn2O4)-, e.g. LiMn2O4 or Li(MxMn2-x)O4
- C01G 51/42: containing alkali metals, e.g. LiCoO2
- C01G 51/50: of the type (MnO2)n-, e.g. Li(CoxMn1-x)O2 or Li(MyCoxMn1-x-y)O2
- C01G 53/42: containing alkali metals, e.g. LiNiO2
- C01G 53/502: containing lithium and cobalt
- C01G 53/504: with the molar ratio of nickel with respect to all the metals other than alkali metals higher than or equal to 0.5, e.g. Li(MzNixCoyMn1-x-y-z)O2 with x ≥ 0.5
- C01G 53/506: with the molar ratio of nickel with respect to all the metals other than alkali metals higher than or equal to 0.8, e.g. Li(MzNixCoyMn1-x-y-z)O2 with x ≥ 0.8
- H01M 4/364: {as mixtures}
- H01M 4/505: of mixed oxides or hydroxides containing manganese for inserting or intercalating light metals, e.g. LiMn2O4 or LiMn2OxFy
- H01M 4/525: of mixed oxides or hydroxides containing iron, cobalt or nickel for inserting or intercalating light metals, e.g. LiNiO2, LiCoO2 or LiCoOxFy
- H01M 4/62: Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- C01P 2002/52: containing elements as dopants
- C01P 2002/72: by d-values or two theta-values, e.g. as X-ray diagram
- C01P 2002/85: by XPS, EDX or EDAX data
- C01P 2002/88: by thermal analysis data, e.g. TGA, DTA, DSC
- C01P 2004/03: obtained by SEM
- C01P 2006/40: Electric properties
- H01M 4/0404: {by coating on electrode collectors}
- H01M 4/661: {Metal or alloys, e.g. alloy coatings (H01M4/669 take precedence)}
- H01M 10/0525: Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
- Y02E 60/10: Energy storage using batteries
- H01M: PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- C01G: COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F (metal hydrides {monoborane, diborane or addition complexes thereof} C01B6/00; salts of oxyacids of halogens C01B11/00; peroxides, salts or peroxyacids C01B15/00; thiosulfates, dithionites, polythionates C01B17/64; compounds containing selenium, or tellurium C01B19/00; binary compounds of nitrogen with metals C01B21/06; azides C01B21/08; {compounds containing nitrogen, other non-metals and metal C01B21/082}; metal amides C01B21/092; nitrites C01B21/50; {compounds of noble gases C01B23/0005}; phosphides C01B25/08; salts of oxyacids of phosphorus C01B25/16; carbides C01B32/90; compounds containing silicon C01B33/00; compounds containing boron C01B35/00; compounds having molecular sieve properties but not having base-exchange properties C01B37/00; compounds having molecular sieve and base-exchange properties, e.g. crystalline zeolites, C01B39/00; cyanides C01C3/08; salts of cyanamide C01C3/16; thiocyanates C01C3/20)
- C01P: INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- Y02E: REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION

## Abstract

A positive active material composition for a rechargeable battery includes a positive active material selected from compounds represented by formulas 1 to 13, and at least one semi-metal, metal or oxides thereof: LixMnA2 (1) LixMnO2-zAz (2) LixMn1-yM′yA2 (3) LixMn2A4 (4) LixMn2O4-zAz (5) LixMn2-yM′yA4 (6) LixBA2 (7) LIxBO2-zAz (8) LixB1-yM″yA2 (9) LixB1-yM″yO2-zAz (10) LixNiCoO2-zAz (11) LixNiCoO2-zAz (12) LixNi1-y-zCoyM″zA2 (13) where 1.0≦x≦1.1, 0.01≦y≦0.1, 0.01≦z≦0.5, M′ is at least one transition metal or lanthanide metal selected from Al, Cr, Co, Mg, La, Ce, Sr, or V, M″ is at least one transition metal or lanthanide metal selected from Al, Cr, Mn, Fe, Mg, La, Ce, Sr or V, A is selected from O, F, S or P, and B is Ni or Co.

## Claims

### Claim 1

A method of making a rechargeable lithium battery comprising:
forming a positive electrode by physically mixing a positive active material with particles of an additive to prepare a positive active material composition, the positive active material being selected from the group consisting of lithiated transition metal compounds, and the additive at least one selected from the group consisting of Si, B, Ge, Ga, Ca, Sr, Ba, and oxides thereof, coating the positive active material composition on a current collector after heat treating to place the positive active material in a uniform crystalline form, and drying the current collector coated with the positive active material composition including the particles of the additive mixed in the positive active material;
forming a negative electrode including a carbonaceous material as an active material;
preparing an electrolyte including an organic solvent including a lithium salt dissolved in the organic solvent;
wherein an amount of the additive is 1.0 to 10 wt % of the positive active material, and the lithiated transition metal compound is selected from the group consisting of formulas 1 to 13:
LixMnA2
(1)
LixMnO2-zAz
(2)
LixMn1-yM′yA2
(3)
LixMn2A4
(4)
LixMn2O4-zAz
(5)
LixMn2-yM′yA4
(6)
LixBA2
(7)
LIxBO2-zAz
(8)
LixB1-yM″yA2
(9)
LixB1-yM″yO2-zAz
(10)
LixNiCoA2
(11)
LixNiCoO2-zA2
(12)
LixNi1-y-zCoyM″zA2
(13)
wherein 1.0≦x≦1.1, 0.01≦y≦0.1, 0.01≦z≦0.5, M′ is at least one transition metal or lanthanide metal selected from the group consisting of Al, Cr, Co, Mg, La, Ce, Sr and V, M″ is at least one transition metal or lanthanide metal selected from the group consisting of Al, Cr, Mn, Fe, Mg, La, Ce, Sr and V, A is selected from O, F, S or P, and B is Ni or Co.

### Claim 2 (depends on 1)

The method of claim 1, wherein said organic solvent comprises N-methylpyrrolidone.

### Claim 3 (depends on 1)

The method of claim 1 wherein the lithiated transition metal compound is a compound represented by formula: LixBA2.
where 1.0≦x≦1.1, A is selected from O, F, S or P, and B is Ni or Co.

### Claim 4 (depends on 1)

The method of claim 1 wherein the lithiated transition metal compound is a compound represented by formula: LixB2-zAz.
where 1.0≦x≦1.1, 0.01≦z≦0.5, A is selected from O, F, S or P, and B is Ni or Co.

### Claim 5 (depends on 1)

The method of claim 1 wherein the lithiated transition metal compound is a compound represented by formula: LixB1-yM″yA2.
where 1.0≦x≦1.1, 0.01≦y≦0.1, M″ is at least one transition metal or lanthanide metal selected from the group consisting of Al, Cr, Mn, Fe, Mg, La, Ce, Sr and V, A is selected from O, F, S or P, and B is Ni or Co.

### Claim 6 (depends on 1)

The method of claim 1 wherein the lithiated transition metal compound is a compound represented by formula: LixB1-yM″yO2-zAz.
where 1.0≦x≦1.1, 0.01≦y≦0.1, 0.01≦z≦0.5, M″ is at least one transition metal or lanthanide metal selected from the group consisting of Al, Cr, Mn, Fe, Mg, La, Ce, Sr and V, A is selected from O, F, S or P, and B is Ni or Co.

### Claim 7 (depends on 1)

The method of claim 1 wherein the lithiated transition metal compound is a compound represented by formula: LixNiCoA2.
where 1.0≦x≦1.1, and A is selected from O, F, S or P.

### Claim 8 (depends on 1)

The method of claim 1 wherein the lithiated transition metal compound is a compound represented by formula: LixNiCoO2-zAz.
where 1.0≦x≦1.1, 0.01≦z≦0.5, and A is selected from O, F, S or P.

### Claim 9 (depends on 1)

The method of claim 1 wherein the lithiated transition metal compound is a compound represented by formula: LixNi1-yCoyM″zA2.
where 1.0≦x≦1.1, 0.01≦y≦0.1, 0.01≦z≦0.5, M″ is at least one transition metal or lanthanide metal selected from the group consisting of Al, Cr, Mn, Fe, Mg, La, Ce, Sr and V, and A is selected from O, F, S or P.

### Claim 10 (depends on 1)

The method of claim 1, wherein the additive comprises at least one selected from the group consisting of Ge, Ga, Ca, Ba, and oxides thereof.

### Claim 11 (depends on 1)

The method of claim 1, wherein the additive comprises at least one selected from the group consisting of Ge and oxides of Ge.

### Claim 12 (depends on 1)

The method of claim 1, wherein the additive comprises at least one selected from the group consisting of Ga and oxides of Ga.

### Claim 13 (depends on 1)

The method of claim 1, wherein the additive comprises at least one selected from the group consisting of Ca and oxides of Ca.

### Claim 14 (depends on 1)

The method of claim 1, wherein the additive comprises at least one selected from the group consisting of Ba and oxides of Ba.

### Claim 15

A method of making a lithium battery comprising:
forming a positive electrode by heat treating a positive active material to place the positive active material in a uniform crystalline form, physically mixing the positive active material with particles of an additive to prepare a positive active material composition, coating the positive active material composition on a current collector, and drying the current collector coated with the positive active material composition including the particles of the additive mixed in the positive active material, wherein the positive active material comprises at least one lithiated transition metal compound, wherein the additive comprises at least one selected from the group consisting of Si, B, Ge, Ga, Ca, Sr, Ba, and oxides thereof, and wherein an amount of the additive is 1.0 to 10 wt % of the positive active material;
forming a negative electrode including a carbonaceous material as an active material; and
preparing an electrolyte including an organic solvent including a lithium salt dissolved in the organic solvent.

### Claim 16 (depends on 15)

The method of claim 15, wherein the additive comprises at least one selected from the group consisting of Ge, Ga, Ca, Ba, and oxides thereof.

### Claim 17 (depends on 16)

The method of claim 16, wherein the additive comprises at least one selected from the group consisting of Ge, Ga, Ba, and oxides thereof.