Lithium ion battery negative electrode material and preparation method therefor

Patent metadata

Field	Value
Publication number	US-11967708-B2
Application number	US-201816760550-A
Country	US
Kind code	B2
Filing date	Nov 29, 2018
Priority date	Dec 12, 2017
Publication date	Apr 23, 2024
Grant date	Apr 23, 2024

Abstract

Disclosed are a lithium ion battery negative electrode material and a preparation method therefor. The negative electrode material comprises SiOy (0.2<y<0.9) and an M compound, wherein M is a metal. The method of the present application comprises: subjecting a raw material comprising a SiOx material and the metal M to a redox reaction, wherein the O/Si ratio, i.e. x, of the SiOx (0.5<x<1.5) material is adjusted to y (0.2<y<0.9), and at the same time, the metal M is oxidized to obtain the M compound.

First claim

What is claimed is:

1. An anode material of lithium ion battery, comprising SiO y and an M compound, with M being a metal;
wherein 0.2<y<0.9;
wherein the M compound is contained in an amount of 3%-15% by mass percentage based on the total mass of the anode material being 100%; and
wherein the anode material has a first coulombic efficiency ranging from 79.9%-86.4%.

2. The anode material according to claim 1 , wherein the anode material has a specific surface area of ≤50 m 2 /g.

3. The anode material according to claim 1 , wherein Si crystallite grains in the SiO y have a size of ≤100 nm.

4. The anode material according to claim 1 , wherein M is an active metal with a pauling electronegativity of ≤1.8.

5. The anode material according to claim 1 , wherein M includes any one selected from the group consisting of metal Na, metal K, metal Mg, metal Ca and metal Al, or M includes a combination of at least two selected from the group consisting of metal Na, metal K, metal Mg, metal Ca and metal Al.

6. The anode material according to claim 1 , wherein the anode material further comprises any one selected from the group consisting of amorphous carbon coating, graphite, carbon black, carbon nanotubes, graphene, silicon, and a metal compound, or the anode material further comprises a combination of at least two selected from the group consisting of amorphous carbon coating, graphite, carbon black, carbon nanotubes, graphene, silicon, and a metal compound.

7. The anode material according to claim 5 , wherein the metal compound comprises any one selected from the group consisting of a metal oxide, a metal silicide and a metal silicate, or the metal compound comprises a combination of at least two selected from the group consisting of a metal oxide, a metal silicide and a metal silicate.

8. The anode material according to claim 5 , wherein the metal compound comprises any one selected from the group consisting of K 2 O, Na 2 O, MgO, CaO, Al 2 O 3 , Mg 2 Si, Ca 2 Si, Al 4 Si 3 , K 2 SiO 3 , K 4 SiO 4 , K 2 Si 2 O 5 , Na 2 SiO 3 , Na 4 SiO 4 , Na 2 Si 2 O 5 , Mg 2 SiO 4 , MgSiO 3 , Ca 2 SiO 4 , CaSiO 3 , Al 4 (SiO 4 ) 3 , and Al 2 (SiO 3 ) 3 , or the metal compound comprises a combination of at least two selected from the group consisting of K 2 O, Na 2 O, MgO, CaO, Al 2 O 3 , Mg 2 Si, Ca 2 Si, Al 4 Si 3 , K 2 SiO 3 , K 4 SiO 4 , K 2 Si 2 O 5 , Na 2 SiO 3 , Na 4 SiO 4 , Na 2 Si 2 O 5 , Mg 2 SiO 4 , MgSiO 3 , Ca 2 SiO 4 , CaSiO 3 , Al 4 (SiO 4 ) 3 , and Al 2 (SiO 3 ) 3 .

9. A preparation method of the anode material of lithium ion battery according to claim 1 , comprising:
performing a redox reaction on a raw material containing SiO x material and the metal M, with the result that the O/Si ratio of the SiO x material is adjusted from x to y, while the metal M is oxidized to obtain the M compound;
wherein 0.5<x<1.5, 0.2<y<0.9, and y<x.

10. The method according to claim 9 , further comprising the following steps:
(1) mixing the raw material containing the SiO x material and the metal M uniformly, then subjecting the mixture to heat treatment and heat preservation under a non-oxidizing atmosphere to obtain SiO y as a reduction product and the M compound as an oxidation product;
wherein the metal M is contained in an amount of 3%-40% by mass percentage based on the total mass of the raw material containing the SiO x material and the metal M being 100%;
(2) subjecting the products obtained in step (1) to acid treatment by using an acid for dissolving and partially removing the M compound, and a lithium ion battery material comprising SiO y and the M compound is obtained;
wherein 0.5<x<1.5, 0.2<y<0.9, and y<x.

11. The method according to claim 9 , wherein Si crystallite grains in the raw material comprising the SiO x material in step (1) have a size of ≤100 nm.

12. The method according to claim 10 , wherein it further comprises the steps of liquid-solid separation and washing and drying the separated solid phase after the acid treatment.

13. The method according to claim 10 , wherein it further comprises using the product of step (1) and/or the product of step (2) as the raw material for step (1) and repeating the following steps: step (1), or step (1) and step (2) in sequence.

14. The method according to claim 10 , wherein the raw material containing the SiO x material in step (1) further contains an additive to form a SiO x -based composite material with the SiO x material, wherein the additive is any one selected from the group consisting of amorphous carbon coating, graphite, carbon black, carbon nanotubes, graphene, silicon, and a metal salt, or the additive is a combination of at least two selected from the group consisting of amorphous carbon coating, graphite, carbon black, carbon nanotubes, graphene, silicon, and a metal salt.

15. The method according to claim 10 , wherein the metal M in step (1) is an active metal with a pauling electronegativity of ≤1.8.

16. The method according to claim 10 , wherein the metal M in step (1) includes any one selected from the group consisting of metal Na, metal K, metal Mg, metal Ca and metal Al, or the metal M in step (1) includes a combination of at least two selected from the group consisting of metal Na, metal K, metal Mg, metal Ca and metal Al.

17. The method according to claim 10 , wherein the metal M has a particle size D50 of ≤;300 μm.

18. The method according to claim 9 , wherein a heat treatment temperature in step (1) is 550° C.-1100° C.

Assignees

• Btr New Mat Group Co Ltd

Inventors

• Liang tengyu
• Pang Chunlei
• Ren Jianguo
• Yue Min

Classifications

• H01M2004/027

  Negative electrodes · CPC title

• H01M2004/021

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

• H01M10/0525

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

• H01M4/366

  as layered products · CPC title

• H01M4/483 Primary

  for non-aqueous cells (H01M4/485 takes precedence) · CPC title