Negative active material, method of preparing the same, and lithium battery including negative active material

Patent metadata

Field	Value
Publication number	US-9966594-B2
Application number	US-201213464404-A
Country	US
Kind code	B2
Filing date	May 4, 2012
Priority date	Jun 30, 2011
Publication date	May 8, 2018
Grant date	May 8, 2018

Abstract

A negative active material, a method of preparing the same, and a lithium battery including the negative active material are disclosed. The negative active material includes a silicon-based nanocore and a first amorphous carbonaceous coating layer that is formed of carbonized organic material and that is uniformly and continuously formed on a surface of the silicon-based nanocore, whereby irreversible capacity losses due to volumetric expansion/contraction caused when a lithium battery is charged and discharged are compensated and cycle lifetime characteristics are enhanced.

First claim

What is claimed is:

1. A negative active material, comprising:
a secondary particle comprising agglomerated primary nanoparticles, wherein the primary nanoparticles comprise:
a silicon-based nanocore; and
a first amorphous carbonaceous coating layer that is a continuous layer and is disposed on a surface of the silicon-based nanocore, wherein the secondary particle further comprises a crystalline carbonaceous material mixed with the primary nanoparticles within the secondary particle, wherein the secondary particle further comprises pores therein, the pores being arranged between the primary nanoparticles.

2. The negative active material of claim 1 , wherein the primary nanoparticles have an average diameter in a range of about 100 to about 300 nm.

3. The negative active material of claim 1 , wherein the silicon-based nanocore comprises one selected from the group consisting of Si, SiO x where 0<x ≤2, and a Si—Z alloy, wherein Z is an alkali metal, an alkali earth metal, a Group XIII element, a Group XIV element, a transition metal, a rare earth element, or a combination thereof, wherein Z is not Si.

4. The negative active material of claim 1 , wherein the first amorphous carbonaceous coating layer comprises a carbide of an organic material selected from the group consisting of sucrose, glucose, galactose, fructose, lactose, starch, mannose, ribose, aldohexose, ketohexose, and combinations thereof.

5. The negative active material of claim 1 , wherein an amount of the first amorphous carbonaceous coating layer is in a range of about 1 to about 10 parts by weight based on 100 parts by weight of the silicon-based nanocore.

6. The negative active material of claim 1 , wherein a thickness of the first amorphous carbonaceous coating layer is in a range of about 1 nm to about 100 nm.

7. The negative active material of claim 1 , wherein the crystalline carbonaceous material comprises a carbonaceous material having a crystalline flake structure.

8. The negative active material of claim 1 , wherein the crystalline carbonaceous material comprises one selected from the group consisting of a polycyclic nano-sheet, a lamination of polycyclic nano-sheets, and a combination thereof.

9. The negative active material of claim 1 , wherein the secondary particle further comprises, on a surface thereof, a secondary carbonaceous coating layer comprising a material selected from the group consisting of soft carbon, hard carbon, a meso-phase pitch carbide, sintered coke, and combinations thereof.

10. The negative active material of claim 1 , wherein the secondary particles have an average diameter in a range of about 5 μm to about 30 μm.

11. A lithium battery comprising:
a negative electrode comprising the negative active material according to claim 1 ;
a positive electrode comprising a positive active material and facing the negative electrode; and
an electrolyte interposed between the negative electrode and the positive electrode.

12. The negative active material of claim 1 , wherein an amount of the first amorphous carbonaceous coating layer is in a range of about 4 to about 6 parts by weight based on 100 parts by weight of the silicon-based nanocore.

13. The negative active material of claim 1 , the negative active material being absent of any conductive material selected from a group consisting of natural graphite, artificial graphite, carbon blacks, acetylene black, Ketjen black, and carbon fibers; metallic powders such as copper powder, nickel powder, aluminum powder, and silver powder; conductive polymers such as polyphenylene derivatives and mixtures thereof.

14. A negative active material comprising a secondary particle comprising agglomerated primary nanoparticles, wherein each of the primary nanoparticles comprise:
a silicon-based nanocore, wherein the silicon-based nanocore comprises one selected from the group consisting of Si, SiO x where 0<x≤2, and a Si—Z alloy, wherein Z is an alkali metal, an alkali earth metal, a Group XIII element, a Group XIV element, a transition metal, a rare earth element, or a combination thereof, wherein Z is not Si; and
a first amorphous carbonaceous coating layer that is a continuous layer and is disposed on a surface of the silicon-based nanocore, wherein the first amorphous carbonaceous coating layer comprises a carbide produced by carbonizing an organic material selected from a group consisting of sucrose, glucose, galactose, fructose, lactose, starch, mannose, ribose, aldohexose, ketohexose, and combinations thereof,
wherein the secondary particle further comprises a crystalline carbonaceous material, wherein the crystalline carbonaceous material comprises a carbonaceous material having a crystalline flake structure, wherein the crystalline carbonaceous material comprises one selected from the group consisting of a polycyclic nano-sheet, a lamination of polycyclic nano-sheets and combinations thereof, wherein the secondary particle further comprises, on a surface thereof, a secondary carbonaceous coating layer comprising a material selected from the group consisting of soft carbon, hard carbon, a meso-phase pitch carbide, sintered coke, and combinations thereof, wherein the secondary particle further comprises pores therein, the pores being arranged between the primary nanoparticles.

15. The negative active material of claim 14 , wherein the primary nanoparticles have an average diameter in a range of about 100 to about 300 nm, wherein an amount of the first amorphous carbonaceous coating layer is in a range of about 4 to about 6 parts by weight based on 100 parts by weight of the silicon-based nanocore, wherein a thickness of the first amorphous carbonaceous coating layer is in a range of about 1 nm to about 100 nm, wherein the secondary particles have an average diameter in a range of about 10 μm to about 20 μm.

16. The negative active material of claim 1 , wherein an amount of the crystalline carbonaceous material is in the range of about 75 to about 95 parts by weight based on 100 parts by weight of the primary nanoparticles.

17. The negative active material of claim 14 , wherein an amount of the crystalline carbonaceous material is in the range of about 75 to about 95 parts by weight based on 100 parts by weight of the primary nanoparticles.

18. The negative active material of claim 1 , wherein the first amorphous carbonaceous coating layer is produced by subjecting an organic material coated on the silicon based nanocore to a heat treatment process at a temperature in a range of about 700 to about 1000° C.

19. The negative active material of claim 14 , wherein the primary nanoparticles have an average diameter in a range of about 100 to about 300 nm.

Assignees

• Kim Beom Kwon
• Kim Jae Myung
• Lee So Ra
• Shin Chang Su
• Do Ui Song
• Samsung Sdi Co Ltd

Inventors

• Kim Beom-Kwon
• Kim Jae-Myung
• Lee So-Ra
• Shin Chang-Su
• Do Ui-Song

Classifications

• H01M4/134

  Electrodes based on metals, Si or alloys · CPC title

• H01M4/1395

  of electrodes based on metals, Si or alloys · CPC title

• H01M2004/021

  Physical characteristics, e.g. porosity, surface area · CPC title

• H01M2004/027

  Negative electrodes · CPC title

• H01M4/364

  as mixtures · CPC title