COMPOSITE NEGATIVE ACTIVE MATERIAL, NEGATIVE ELECTRODE INCLUDING COMPOSITE NEGATIVE ACTIVE MATERIAL, AND LITHIUM SECONDARY BATTERY INCLUDING NEGATIVE ELECTRODE

• US 20170092940A1
• Filed: 03/17/2016
• Published: 03/30/2017
• Est. Priority Date: 09/25/2015
• Status: Active Grant

• Current Assignee: Samsung Electronics Co. Ltd., Samsung SDI Company Limited
• Original Assignee: Samsung Electronics Co. Ltd., Samsung SDI Company Limited
• Inventors: Kim, Guesung, Mun, Jinsoo, Jung, Heechul
• Granted Patent: US 10,249,874 B2
• Time in Patent Office: Days
• US Class Current: 1/1
• CPC Class Codes: H01M 10/052 Li-accumulators
• CPC Class Codes: H01M 10/0525 Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
• CPC Class Codes: H01M 10/0568 characterised by the solutes
• CPC Class Codes: H01M 10/0569 characterised by the solvents
• CPC Class Codes: H01M 10/0587 of accumulators having only wound construction elements, i.e. wound positive electrodes, wound negative electrodes and wound separators
• CPC Class Codes: H01M 2004/027 Negative electrodes
• CPC Class Codes: H01M 2220/20 Batteries in motive systems, e.g. vehicle, ship, plane
• CPC Class Codes: H01M 2220/30 Batteries in portable systems, e.g. mobile phone, laptop
• CPC Class Codes: H01M 2300/0034 Fluorinated solvents
• CPC Class Codes: H01M 2300/004 Three solvents
• CPC Class Codes: H01M 4/0402 Methods of deposition of the material
• CPC Class Codes: H01M 4/0404 by coating on electrode collectors
• CPC Class Codes: H01M 4/0435 Rolling or calendering
• CPC Class Codes: H01M 4/0471 involving thermal treatment, e.g. firing, sintering, backing particulate active material, thermal decomposition, pyrolysis
• CPC Class Codes: H01M 4/134 Electrodes based on metals, Si or alloys
• CPC Class Codes: H01M 4/1395 of electrodes based on metals, Si or alloys
• CPC Class Codes: H01M 4/364 as mixtures
• CPC Class Codes: H01M 4/366 as layered products
• CPC Class Codes: H01M 4/38 of elements or alloys
• CPC Class Codes: H01M 4/382 Lithium H01M4/405 takes precedence
• CPC Class Codes: H01M 4/386 : Silicon or alloys based on silicon
• CPC Class Codes: H01M 4/582 : Halogenides
• CPC Class Codes: H01M 4/5825 : Oxygenated metallic salts or polyanionic structures, e.g. borates, phosphates, silicates, olivines
• CPC Class Codes: H01M 4/587 : for inserting or intercalating light metals
• CPC Class Codes: H01M 4/622 : being polymers
• CPC Class Codes: H01M 4/625 : Carbon or graphite
• CPC Class Codes: H01M 4/661 : Metal or alloys, e.g. alloy coatings H01M4/669 take precedence
• CPC Class Codes: Y02E 60/10 : Energy storage using batteries
• CPC Class Codes: Y02P 70/50 : Manufacturing or production processes characterised by the final manufactured product

Abstract

A composite negative active material including: a silicon-containing negative active material; and a non-metal doped metal phosphate, wherein the non-metal doped metal phosphate includes two or more metals. Also a negative electrode including the composite negative active material, and a lithium secondary battery including the negative electrode

Claims

1. A composite negative active material comprising:

a silicon-containing negative active material; and

a non-metal doped metal phosphate, wherein the non-metal doped metal phosphate comprises two or more metals.

2. The composite negative active material of claim 1, wherein the silicon-containing negative active material comprises at least one selected from elemental silicon, SiO_x wherein 0<

x<

2, a Si—

C composite, and a Si alloy.

3. The composite negative active material of claim 2, wherein the Si alloy comprises at least one selected from Fe₃Si, Fe₂Si, Fe₅Si₃, FeSi, FeSi₂, FeSi₃, AlSi₂, Cu₅Si, Mg₂Si, NiSi, TiSi₂, and Si₇T₄Ni₄.

4. The composite negative active material of claim 1, wherein a non-metal dopant in the non-metal doped metal phosphate comprises at least one selected from fluorine, sulfur, nitrogen, and boron.

5. The composite negative active material of claim 4, wherein the non-metal doped metal phosphate is represented by Formula 1:

M_xMePO₄E_y  

 

Formula 1

wherein, in Formula 1,

M is at least one selected from lithium, sodium, rubidium, lanthanum, strontium, and radium,

Me is at least one selected from aluminum, titanium, magnesium, zinc, vanadium, manganese, gallium, chromium, iron, rhodium, nickel, indium, and cobalt,

E is a non-metal dopant and is at least one selected from F, S, N, and B,

M is different from Me, and

0.01≦

x<

2 and 0.01≦

y<

2.

6. The composite negative active material of claim 1, wherein an amount of the non-metal doped metal phosphate is less than 10 parts by weight, based on 100 parts by weight of the silicon-containing negative active material.

7. A negative electrode comprising a composite negative active material according to claim 1.

8. The negative electrode of claim 7, further comprising an additional negative active material.

9. A lithium secondary battery comprising the negative electrode according to claim 1.

10. A composite negative active material comprising:

a core comprising silicon; and

a coating layer on the core, wherein the coating layer comprises a non-metal doped metal phosphate represented by Formula 1

M_xMePO₄E_y  

 

Formula 1

wherein, in Formula 1,

M is at least one selected from lithium, sodium, rubidium, lanthanum, strontium, and radium,

Me is at least one selected from aluminum, titanium, magnesium, zinc, vanadium, manganese, gallium, chromium, iron, rhodium, nickel, indium, and cobalt,

E is a non-metal dopant and is at least one selected from F, S, N, and B,

M is different from Me, and

0.01≦

x<

2 and 0.01≦

y<

2.

11. The composite negative active material of claim 10, wherein the composite negative active material comprises at least one selected from elemental silicon, SiO_x wherein 0<

x<

2, a Si—

C composite, and a Si alloy.

12. A method of preparing a composite negative active material, the method comprising:

providing a silicon-containing negative active material;

contacting the silicon-containing negative active material with a solution of a non-metal doped phosphate to form a coated negative active material;

drying the coated negative active material to form a dried negative active material; and

heat-treating the dried negative active material to prepare the composite negative active material.

13. The method of claim 12, wherein the silicon-containing negative active material comprises at least one selected from elemental silicon, SiO_x wherein 0<

x<

2, a Si—

C composite, and a Si alloy.

14. The method of claim 12, wherein the heat-treating comprises heat-treating in a nitrogen atmosphere.

15. A composite negative active material comprising:

a silicon-containing negative active material comprising silicon; and

a non-metal doped metal phosphate represented by the formula

Li_xAlPO₄F_y

wherein 0.01≦

x<

2 and 0.01≦

y<

2.

16. The composite negative active material of claim 15, wherein the composite negative active material comprises at least one selected from elemental silicon, SiO_x wherein 0<

x<

2, a Si—

C composite, and a Si alloy.