IP Library Granted Patent US 11,817,574
Granted Patent B2
US 11,817,574 · App. 17/875,611 · Granted Nov 14, 2023

Carbon-silicon three-dimensional structural composite material and preparation method thereof

Inventors: Xuelian Wu (Fujian, CN); Enqiang Zhang (Fujian, CN)
Assignee: XIAMEN HITHIUM ENERGY STORAGE TECHNOLOGY CO., LTD.
H01M4/364C01B32/184C01B32/198H01M4/386H01M4/587B82Y30/00B82Y40/00C01B2204/22
View Patent ↗
Loading inventors, assignments & file history…
Monitor This Case
Get email alerts when status or documents change.
Order Certified Copies
Most orders are placed with the USPTO same day — all within 24 business hours.
Order via The Patent Place →
Pre-filled with this patent's details
Quick Facts
Patent No.
US 11,817,574
App. No.
17/875,611
Granted
Nov 14, 2023
Kind
B2
Abstract

Provided are a carbon-silicon three-dimensional structural composite material and a preparation method thereof. The preparation method includes: dissolving graphene quantum dots in ultrapure water, dropwise adding a CuCl 2 or ZnCl 2 solution, and performing oscillation to generate a mixed emulsifier; mixing the mixed emulsifier with a graphite oxide aqueous solution and a cyclohexane solution containing nanosilicon spheres, and performing homogenization to form a uniform oil-in-water emulsion; adding hydrazine hydrate into the obtained emulsion for reduction, and performing a hydrothermal reaction to obtain a reduced emulsion; and freeze-drying the reduced emulsion, performing washing with a washing liquid, and performing vacuum drying to obtain a carbon-silicon three-dimensional structural composite material.

Claims (47)

1. A preparation method of a carbon-silicon three-dimensional structural composite material, comprising the following steps:

a first step of dissolving 0.004 g to 0.006 g of graphene quantum dots in 4 ml to 6 ml of ultrapure water, dropwise adding 0.65 ml to 0.85 ml of a CuCl 2 or ZnCl 2 solution having a concentration of 0.2 mol/ml to 0.3 mol/ml, and performing oscillation to generate a mixed emulsifier;

a second step of mixing the mixed emulsifier obtained in the first step with 10 ml to 20 ml of a graphite oxide aqueous solution having a concentration of 10 mg/ml to 20 mg/ml and 10 ml to 20 ml of a cyclohexane solution containing 0.1 g to 0.2 g of nanosilicon spheres, and performing homogenization for 20 s to 30 s to form a uniform oil-in-water emulsion;

a third step of adding 0.9 g to 1.2 g of hydrazine hydrate into the emulsion obtained in the second step for reduction, and performing a hydrothermal reaction to obtain a reduced emulsion; and

a fourth step of freeze-drying the reduced emulsion obtained in the third step, performing washing with a washing liquid, and performing vacuum drying, to obtain the carbon-silicon three-dimensional structural composite material.

2. The preparation method of the carbon-silicon three-dimensional structural composite material according to claim 1 , wherein the graphene quantum dots in the first step are prepared by:

uniformly dissolving 1 g of citric acid and 0.03 g of histidine in 20 ml of ultrapure water under a heating condition of a 40° C. to 50° C. water bath,

performing pyrolysis at 180° C. for 3 h to form a mixture,

filtering the mixture,

pouring a filtrate in a dialysis bag for dialysis treatment, and

performing freeze-drying at −40° C. after the dialysis treatment to obtain the graphene quantum dots.

3. The preparation method of the carbon-silicon three-dimensional structural composite material according to claim 1 , wherein the graphite oxide in the second step is prepared by a Hummer method.

4. The preparation method of the carbon-silicon three-dimensional structural composite material according to claim 1 , wherein the nanosilicon spheres in the second step have a particle diameter denoted by r, where r satisfies 20 mn≤r≤120 nm.

5. The preparation method of the carbon-silicon three-dimensional structural composite material according to claim 1 , wherein the cyclohexane solution containing the nanosilicon spheres in the second step is prepared by:

adding the nanosilicon spheres into a mixed solution prepared by acetone, ethanol, and water according to a ratio of 1:1:1,

performing ultrasonic treatment for 30 min,

performing washing with ethanol and ultrapure water for three times after the ultrasonic treatment, performing centrifugal separation, and taking a lower layer of solid,

performing vacuum drying at 60° C. to obtain treated silicon spheres, and

uniformly dispersing 0.1 g to 0.2 g of the treated nanosilicon spheres in 10 ml to 20 ml of a cyclohexane solution.

6. The preparation method of the carbon-silicon three-dimensional structural composite material according to claim 1 , wherein the hydrothermal reaction in the third step is performed at a temperature of 60° C. to 65° C. for 8 h to 10 h.

7. The preparation method of the carbon-silicon three-dimensional structural composite material according to claim 1 , wherein the freeze-drying in the fourth step is performed at a temperature of −40° C.

8. The preparation method of the carbon-silicon three-dimensional structural composite material according to claim 1 , wherein the washing liquid in the fourth step is ethanol.

9. The preparation method of the carbon-silicon three-dimensional structural composite material according to claim 1 , wherein the vacuum drying in the fourth step is performed at a temperature of 60° C.

10. A carbon-silicon three-dimensional structural composite material, obtained by a preparation method of the carbon-silicon three-dimensional structural composite material, the preparation method comprising the following steps:

a first step of dissolving 0.004 g to 0.006 g of graphene quantum dots in 4 ml to 6 ml of ultrapure water, dropwise adding 0.65 ml to 0.85 ml of a CuCl 2 or ZnCl 2 solution having a concentration of 0.2 mol/ml to 0.3 mol/ml, and performing oscillation to generate a mixed emulsifier;

a second step of mixing the mixed emulsifier obtained in the first step with 10 ml to 20 ml of a graphite oxide aqueous solution having a concentration of 10 mg/ml to 20 mg/ml and 10 ml to 20 ml of a cyclohexane solution containing 0.1 g to 0.2 g of nanosilicon spheres, and performing homogenization for 20 s to 30 s to form a uniform oil-in-water emulsion;

a third step of adding 0.9 g to 1.2 g of hydrazine hydrate into the emulsion obtained in the second step for reduction, and performing a hydrothermal reaction to obtain a reduced emulsion; and

a fourth step of freeze-drying the reduced emulsion obtained in the third step, performing washing with a washing liquid, and performing vacuum drying, to obtain the carbon-silicon three-dimensional structural composite material,

wherein silicon spheres are embedded between layers of graphene in the carbon-silicon three-dimensional structural composite material.

11. The carbon-silicon three-dimensional structural composite material according to claim 10 , wherein the graphene quantum dots in the first step are prepared by:

uniformly dissolving 1 g of citric acid and 0.03 g of histidine in 20 ml of ultrapure water under a heating condition of a 40° C. to 50° C. water bath,

performing pyrolysis at 180° C. for 3 h to form a mixture,

filtering the mixture,

pouring a filtrate in a dialysis bag for dialysis treatment, and

performing freeze-drying at −40° C. after the dialysis treatment to obtain the graphene quantum dots.

12. The carbon-silicon three-dimensional structural composite material according to claim 10 , wherein the graphite oxide in second step is prepared by a Hummer method.

13. The carbon-silicon three-dimensional structural composite material according to claim 10 , wherein the nanosilicon spheres in the second step have a particle diameter denoted by r, where r satisfies 20 nm≤r≤120 nm.

14. The carbon-silicon three-dimensional structural composite material according to claim 10 , wherein the cyclohexane solution containing the nanosilicon spheres in the second step is prepared by:

adding the nanosilicon spheres into a mixed solution prepared by acetone, ethanol, and water according to a ratio of 1:1:1,

performing ultrasonic treatment for 30 min,

performing washing with ethanol and ultrapure water for three times after the ultrasonic treatment, performing centrifugal separation, and taking a lower layer of solid,

performing vacuum drying at 60° C. to obtain treated silicon spheres, and

uniformly dispersing 0.1 g to 0.2 g of the treated nanosilicon spheres in 10 ml to 20 ml of a cyclohexane solution.

15. The carbon-silicon three-dimensional structural composite material according to claim 10 , wherein the hydrothermal reaction in the third step is performed at a temperature of 60° C. to 65° C. for 8 h to 10 h.

16. The carbon-silicon three-dimensional structural composite material according to claim 10 , wherein the freeze-drying in the fourth step is performed at a temperature of −40° C.

17. The carbon-silicon three-dimensional structural composite material according to claim 10 , wherein the washing liquid in the fourth step is ethanol.

18. The carbon-silicon three-dimensional structural composite material according to claim 10 , wherein the vacuum drying in the fourth step is performed at a temperature of 60° C.

Assignments (3)
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Mar 11, 2025
From: XIAMEN HITHIUM ENERGY STORAGE TECHNOLOGY CO., LTD.
To: HITHIUM TECH HK LIMITED
Reel/Frame 070462/0648 →
CHANGE OF NAME Recorded Sep 28, 2022
From: XIAMEN HITHIUM NEW ENERGY TECHNOLOGY CO., LTD.
To: XIAMEN HITHIUM ENERGY STORAGE TECHNOLOGY CO., LTD.
Reel/Frame 061554/0684 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Sep 6, 2022
From: WU, XUELIAN; ZHANG, ENQIANG
To: XIAMEN HITHIUM NEW ENERGY TECHNOLOGY CO., LTD.
Reel/Frame 061001/0817 →
Priority Claims (1)
CN 202110863229.8 · Jul 29, 2021 · national
Continuity (1)
Related Publication 20230033233A1 · Feb 2, 2023