IP Library Granted Patent US 12,068,472
Granted Patent B2
US 12,068,472 · App. 17/363,272 · Granted Aug 20, 2024

Relithiation process for direct regeneration of cathode materials from spent lithium-ion batteries

Inventors: Ilias Belharouak (Oak Ridge, TN); Yaocai Bai (Oak Ridge, TN); Rachid Essehli (Oak Ridge, TN); Jianlin Li (Oak Ridge, TN)
Assignee: UT-BATTELLE, LLC
H01M4/049H01M4/0471H01M10/0525H01M10/54H01M4/505H01M4/525Y02W30/84
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 12,068,472
App. No.
17/363,272
Granted
Aug 20, 2024
Kind
B2
Abstract

A method for the regeneration of cathode material from spent lithium-ion batteries is provided. The method includes dissolving a lithium precursor in a polyhydric alcohol to form a solution. Degraded cathode material containing lithium metal oxides are dispersed into the solution under mechanical stirring, forming a mixture. The mixture is heat treated within a reactor vessel or microwave oven. During this heat treatment, lithium is intercalated into the degraded cathode material. The relithiated electrode material is collected by filtration, washing with solvents, and drying. The relithiated electrode material is then ground with a lithium precursor and thermally treated at a relatively low temperature for a predetermined time period to obtain regenerated cathode material.

Claims (26)

1. A method comprising:

dissolving a first lithium precursor within a polyhydric alcohol to form a first solution;

combining a degraded cathode material with the first solution to form a first mixture comprising lithium ions;

heat treating the first mixture at a first temperature that is greater than room temperature and less than 200° C. to relithiate the cathode material, wherein heat treating of the first mixture is performed at atmospheric pressure, such that the lithium ions are intercalated into the degraded cathode material, producing a relithiated cathode material;

filtering and drying the relithiated cathode material from the first mixture to recover the relithiated cathode material;

combining the relithiated cathode material with a second lithium precursor to form a second mixture; and

annealing the relithiated cathode material by thermally treating the second mixture at a second temperature to produce a regenerated cathode material.

2. The method of claim 1 wherein the first lithium precursor includes lithium hydroxide, lithium chloride, lithium acetate, lithium nitrate, or lithium bromide.

3. The method of claim 1 wherein the polyhydric alcohol comprises a glycol.

4. The method of claim 1 wherein the degraded cathode material includes lithium metal oxides or lithium metal phosphates.

5. The method of claim 1 wherein the second lithium precursor includes lithium oxide, lithium hydroxide, lithium carbonate, or lithium bicarbonate.

6. The method of claim 1 wherein heat treating the first mixture includes heating the first mixture within a reactor vessel.

7. The method of claim 1 wherein heat treating the first mixture includes heat treating the first mixture within a microwave oven.

8. The method of claim 1 wherein combining the relithiated cathode material with a second lithium precursor includes grinding the relithiated cathode material into a powder.

9. The method of claim 1 wherein thermally treating the second mixture includes annealing the second mixture to the second temperature of at least 500° C.

10. The method of claim 1 wherein heat treating the first mixture includes heating the first mixture to the first temperature, and wherein thermally treating the second mixture includes heating the second mixture to the second temperature, the second temperature being greater than the first temperature.

11. The method of claim 1 wherein the filtered and dried relithiated cathode material comprises a solid.

12. A method comprising:

intermixing partially or fully degraded cathode material in a solution including a first lithium precursor and a polyhydric alcohol to form a first mixture;

heat treating the first mixture at a temperature greater than room temperature and less than 200° C. to relithiate the cathode material, wherein heat treating of the first mixture is performed at atmospheric pressure, such that the lithium ions are intercalated into the partially or fully degraded cathode material, producing a relithiated cathode material;

combining the relithiated cathode material with a second lithium precursor to form a second mixture and mechanically grinding the second mixture into a powder; and

annealing the powder to at least 500° C. to produce a regenerated cathode material for a cathode of a lithium-ion battery.

13. The method of claim 12 wherein the first lithium precursor includes lithium hydroxide, lithium chloride, lithium acetate, lithium nitrate, or lithium bromide.

14. The method of claim 12 wherein the second lithium precursor includes lithium oxide, lithium hydroxide, lithium carbonate, or lithium bicarbonate.

15. The method of claim 12 wherein the polyhydric alcohol comprises a glycol.

16. The method of claim 12 wherein the partially or fully degraded cathode material includes lithium metal oxides or lithium metal phosphates.

Assignments (2)
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Jun 17, 2022
From: BELHAROUAK, ILIAS; BAI, YAOCAI; ESSEHLI, RACHID; LI, JIANLIN
To: UT-BATTELLE, LLC
Reel/Frame 060236/0311 →
CONFIRMATORY LICENSE Recorded Dec 17, 2021
From: UT-BATTELLE, LLC
To: U. S. DEPARTMENT OF ENERGY
Reel/Frame 058420/0161 →
Continuity (2)
Provisional Application 63174082 · Apr 13, 2021
Related Publication 20220328800A1 · Oct 13, 2022