Interconnected silicon porous structure for anode active material

Patent metadata

Field	Value
Publication number	US-11223036-B2
Application number	US-201916686889-A
Country	US
Kind code	B2
Filing date	Nov 18, 2019
Priority date	Nov 19, 2018
Publication date	Jan 11, 2022
Grant date	Jan 11, 2022

Abstract

An anode active material comprises a silicon-carbon secondary particle comprising a composite having an exterior conformal carbon coating and formed of type I primary particles. Each type I primary particle comprises a core particle of interconnected silicon, the interconnected silicon formed of nano-sized silicon particles each connected to at least one other particle, inner pores internal to the core particle and defined by the interconnected silicon, an internal carbon coating on internal wall surfaces of the inner pores and a conformal carbon coating on the core particle.

First claim

What is claimed is:

1. An anode active material comprising:
a silicon-carbon secondary particle comprising a composite having an exterior conformal carbon coating, the composite comprising:
type I primary particles each comprising:
a core particle of interconnected silicon, the interconnected silicon formed of nano-sized silicon particles each connected to at least one other particle;
inner pores internal to the core particle and defined by the interconnected silicon;
an internal carbon coating on internal wall surfaces of the inner pores; and
a conformal carbon coating on the core particle.

2. The anode active material of claim 1 , wherein the composite further comprises:
type II primary particles each comprising a single nano-sized silicon particle having a conformal carbon coating, wherein the type I primary particles and the type II primary particles are loosely bonded, allowing for movement of individual primary particles.

3. The anode active material of claim 2 , wherein the composite further comprises:
type III primary particles each comprising multiple nano-sized silicon particles chemically bonded together and conformally coated with carbon, wherein the type I primary particles, the type II primary particles and the type III primary particles are loosely bonded, allowing for movement of individual primary particles.

4. The anode active material of claim 1 , wherein the composite further comprises:
type III primary particles each comprising multiple nano-sized silicon particles chemically bonded together and conformally coated with carbon, wherein the type I primary particles and the type III primary particles are loosely bonded, allowing for movement of individual primary particles.

5. The anode active material of claim 1 , wherein the inner pores provide each type I primary particle with an inner porosity of between 20% and 30%, inclusive.

6. The anode active material of claim 1 , wherein the inner pores have a mean dimension of between 2 nm to 5 nm, inclusive.

7. The anode active material of claim 1 , wherein the silicon-carbon secondary particle has a D50 diameter of between 1 μm and 10 μm, inclusive.

8. The anode active material of claim 1 , wherein the nano-sized silicon particles each have a longest dimension of 10 nm or less.

9. The anode active material of claim 1 , wherein the nano-sized silicon particles have a D50 particle diameter between 3 nm and 6 nm, inclusive.

10. The anode active material of claim 1 , wherein the exterior conformal carbon coating of the silicon-carbon secondary particle has a thickness of between 2 nm and 5 nm, inclusive.

11. The anode active material of claim 1 , wherein the composite has an internal porosity of between 10% and 40%, inclusive.

12. The anode active material of claim 1 , wherein the exterior conformal carbon coating is a graphene coating.

13. The anode active material of claim 1 , further comprising an artificial solid electrolyte interphase layer on the exterior conformal carbon coating.

14. The anode active material of claim 1 , further comprising a silicon-carbide layer between the internal wall surfaces of the inner pores and the internal carbon coating and between the core particle and the conformal carbon coating, wherein the silicon-carbide layer is amorphous.

15. The anode active material of claim 14 , wherein a thickness of the silicon-carbide layer is less than 5 nm.

16. The anode active material of claim 14 , wherein a composition of the silicon-carbide layer includes a gradually decreasing amount of silicon towards the internal carbon coating and the conformal carbon coating, and a gradually decreasing amount of carbon towards the core particle.

17. A lithium ion battery, comprising:
an anode having a layer of the anode active material as claimed in claim 1 ;
a cathode having a layer of cathode active material; and
an electrolyte.

18. Silicon-carbon secondary particles for use as anode active material, each silicon-carbon secondary particle comprising:
type I primary particles each comprising:
a core particle of interconnected silicon, the interconnected silicon formed of nano-sized silicon particles each fused to at least one other nano-sized silicon particle;
inner pores internal to the core particle and defined by the interconnected silicon;
an internal carbon coating on internal wall surfaces of the inner pores; and
a conformal carbon coating on the core particle and sealing the core particle; and

an exterior conformal carbon coating on each type secondary particle, wherein the inner pores provide the type I primary particle with an inner porosity between 20% and 30%, inclusive, and a D50 diameter of the nano-sized silicon particles is between 2 nm and 6 nm, inclusive.

19. The silicon-carbon secondary particles of claim 18 , wherein the inner pores have a mean dimension of between 2 nm to 5 nm, inclusive.

20. The silicon-carbon secondary particles of claim 18 , wherein a D50 diameter of each silicon-carbon secondary particle is between 1 μm and 10 μm, inclusive.

21. The silicon-carbon secondary particles of claim 18 , wherein each silicon-carbon secondary particle has a porosity of between 10% and 40%, inclusive.

22. The silicon-carbon secondary particles of claim 18 , further comprising:
type II primary particles each comprising a single nano-sized silicon particle having a conformal carbon coating, wherein the type I primary particles and the type II primary particles are loosely bonded, allowing for movement of individual primary particles.

23. The silicon-carbon secondary particles of claim 22 , further comprising:
type III primary particles each comprising multiple nano-sized silicon particles chemically bonded together and conformally coated with carbon, wherein the type I primary particles, the type II primary particles and the type III primary particles are loosely bonded, allowing for movement of individual primary particles.

Assignees

• Apple Inc

Inventors

• Liu Zuqin
• Mank Richard M
• Kim Hyea
• Dai Hongli
• Kang Sunho
• Zhang Ji-Guang
• Yi Ran
• Li Qiuyan
• Li Xiaolin
• Xu Wu
• Patel Rajankumar L
• Lim Hyung-Seok
• Wang Chongmin
• Luo Langli
• He Yang

Classifications

• H01M4/133

  Electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx · CPC title

• H01M4/386

  Silicon or alloys based on silicon · CPC title

• H01M4/134 Primary

  Electrodes based on metals, Si or alloys · CPC title

• H01M4/625

  Carbon or graphite · CPC title

• H01M2004/027

  Negative electrodes · CPC title