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

Patent metadata

Field	Value
Publication number	US-11539043-B2
Application number	US-201514817134-A
Country	US
Kind code	B2
Filing date	Aug 3, 2015
Priority date	Aug 8, 2014
Publication date	Dec 27, 2022
Grant date	Dec 27, 2022

Abstract

A negative active material, a lithium battery including the negative active material, and a method of preparing the negative active material. The negative active material includes: a core particle including a silicon based alloy; carbon nanoparticles disposed on a surface of the core particle; and an amorphous carbonaceous coating layer disposed on at least a portion of a surface of the core particle. The negative active material may improve the lifetime characteristics of the lithium batteries.

First claim

What is claimed is:

1. A negative active material, comprising:
a plurality of core particles, each core particle comprising a silicon based alloy,
wherein the silicon based alloy comprises
an inactive matrix consisting of inactive silicon and at least one selected from the group consisting of group 2 to 14 metal elements other than silicon, and
a plurality of active silicon nanoparticles dispersed in the inactive matrix;

amorphous carbon nanoparticles on a surface of the core particle, the amorphous carbon nanoparticles having an average particle diameter of about 10 nm or more and less than 100 nm; and
an amorphous carbonaceous coating layer on at least a portion of the surface of the core particle, the amorphous carbonaceous coating layer covering the amorphous carbon nanoparticles,
wherein the amorphous carbonaceous coating layer surrounds the surface of the core particle and covers the amorphous carbon nanoparticles, and
wherein an average particle diameter of the core particle is greater than an average particle diameter of the amorphous carbon nanoparticles, the core particle being greater in amount than that of the amorphous carbon nanoparticles in combination with the amorphous carbonaceous coating layer.

2. The negative active material of claim 1 , wherein the carbon nanoparticles have an average particle diameter of about 1/10 or less of that of the core particle.

3. The negative active material of claim 1 , wherein the amorphous carbon nanoparticles have an average particle diameter ranging from about 1/1000 to about 1/10 of that of the core particle.

4. The negative active material of claim 1 , wherein the amorphous carbon nanoparticles have an average particle diameter ranging from about 1/1000 to about 1/100 of that of the core particle.

5. The negative active material of claim 1 , wherein the core particle has an average particle diameter ranging from about 1 μm to about 10 μm.

6. The negative active material of claim 1 , wherein the silicon based alloy is represented by the following Formula 1:
Si a M b   Formula 1

wherein, M comprises at least one selected from the group consisting of group 2 to 14 metal elements other than silicon, and wherein 0.5≤a≤0.9, 0.1≥b≥0.5, and a+b=1.

7. The negative active material of claim 6 , wherein M comprises at least one selected from the group consisting of iron (Fe), copper (Cu), magnesium (Mg), chromium (Cr), nickel (Ni), zinc (Zn), manganese (Mn), cobalt (Co), titanium (Ti), germanium (Ge), calcium (Ca), and aluminum (Al).

8. The negative active material of claim 1 , wherein the silicon based alloy is represented by Si a Fe b , wherein 0.5≤a≤0.9, 0.1≤b≤0.5, and a+b=1.

9. The negative active material of claim 1 , wherein an amount of the active silicon nanoparticles in the silicon based alloy is about 30 atomic % to about 50 atomic % based on a total atomic percent of the silicon based alloy.

10. The negative active material of claim 1 , wherein the active silicon nanoparticles have an average particle diameter ranging from 1 nm to about 100 nm.

11. The negative active material of claim 1 , wherein the inactive matrix comprises Si 2 Fe.

12. The negative active material of claim 1 , wherein the amorphous carbonaceous coating layer comprises a carbide of a carbon precursor selected from the group consisting of hydrocarbons, soft carbons, hard carbons, coal, coal based pitch, petroleum based pitch, mesophase pitch, coal based oil, petroleum based heavy oil, organic synthetic pitch, and combinations thereof.

13. The negative active material of claim 1 , wherein the amorphous carbonaceous coating layer has a thickness of about 0.1 μm to about 10 μm.

14. The negative active material of claim 1 , wherein an amount of the amorphous carbonaceous coating layer is about 1 part to about 30 parts based on 100 parts by weight of the core particle.

15. A lithium battery comprising the negative active material of claim 1 .

16. A method of preparing the negative active material of claim 1 , the method comprising:
mixing the amorphous carbon nanoparticles with the plurality of core particles comprising the silicon based alloy to obtain a plurality of first particles in which the amorphous carbon nanoparticles are adhered to the surface of each of the core particles;
mixing the plurality of first particles with an amorphous carbon precursor to obtain a plurality of second particles in which the amorphous carbon precursor is coated on a surface of each of the first particles; and
heat-treating the plurality of second particles at a temperature of about 500° C. to about 700° C. in an inert atmosphere.

17. The method of claim 16 , wherein the heat-treating of the second particle is performed at a temperature of about 500° C. to about 600° C. in a nitrogen atmosphere.

Assignees

• Samsung Sdi Co Ltd

Inventors

• Shin Changsu
• Park Hyunki
• Do Uisong
• Park Sangeun
• Kim Sungsu

Classifications

• H01M4/587

  for inserting or intercalating light metals · CPC title

• H01M4/386

  Silicon or alloys based on silicon · CPC title

• H01M4/366 Primary

  as layered products · CPC title

• Y02E60/10

  Energy storage using batteries · CPC title

• H01M10/0525

  Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries · CPC title