Methods of separating metals from a lithium-ion battery leachate

Patent metadata

Field	Value
Publication number	US-2024392409-A1
Application number	US-202218689835-A
Country	US
Kind code	A1
Filing date	Sep 8, 2022
Priority date	Sep 8, 2021
Publication date	Nov 28, 2024
Grant date	—

Abstract

A method of separating metals from a lithium-ion battery leachate includes obtaining a solution with iron, aluminum, nickel, and cobalt. Ammonium phosphate is added to the solution to adjust a pH of the solution to greater than or equal to about 3.00. After adjusting the pH of the solution, at least one phosphate—including iron phosphate and aluminum phosphate—is precipitated from the solution. Then, without adding a base to the solution, a crystallized nickel-cobalt Tutton's salt is precipitated from the solution.

First claim

1 . A method of separating metals from a lithium-ion battery leachate, the method comprising:
obtaining a solution comprising iron, aluminum, nickel, and cobalt; adding ammonium phosphate to the solution to adjust a pH of the solution to greater than or equal to about 3.00; after adjusting the pH of the solution to greater than or equal to about 3.00, precipitating at least one phosphate precipitate from the solution, the at least one phosphate precipitate comprising iron phosphate and aluminum phosphate; and after precipitating the at least one phosphate precipitate from the solution and without adding a base to the solution, precipitating a crystallized nickel-cobalt Tutton's salt from the solution.

2 . The method of claim 1 , wherein during precipitating the crystallized nickel-cobalt Tutton's salt from the solution, the pH of the solution is within a range from about 2.00 to about 3.00.

3 . The method of claim 1 , further comprising, after precipitating the at least one phosphate precipitate from the solution:
filtering the solution to remove the at least one phosphate precipitate from the solution; and after the filtering, adding ammonium sulfate to the solution, wherein precipitating the crystallized nickel-cobalt Tutton's salt from the solution is substantially completed within about two days.

4 . The method of claim 1 , wherein precipitating the crystallized nickel-cobalt Tutton's salt from the solution comprises:
precipitating a first crystallized nickel-cobalt Tutton's salt from the solution; and after precipitating the first crystallized nickel-cobalt Tutton's salt from the solution, precipitating a second crystallized nickel-cobalt Tutton's salt from the solution, the first crystallized nickel-cobalt Tutton's salt comprising greater than about 50 atomic percent nickel, and the second crystallized nickel-cobalt Tutton's salt comprising greater than about 50 atomic percent cobalt.

5 . The method of claim 1 , wherein precipitating the crystallized nickel-cobalt Tutton's salt from the solution comprises:
at a temperature within a range from about 20° C. to about 25° C., precipitating a first crystallized nickel-cobalt Tutton's salt from the solution, lowering the temperature of the solution to below about 20° C.; and after lowering the temperature of the solution, precipitating a second crystallized nickel-cobalt Tutton's salt from the solution, the first crystallized nickel-cobalt Tutton's salt and the second crystallized nickel-cobalt Tutton's salt having different atomic ratios of nickel to cobalt.

6 . The method of claim 1 , wherein precipitating the crystallized nickel-cobalt Tutton's salt from the solution comprises precipitating a crystallized nickel-cobalt Tutton's salt comprising the nickel, the cobalt, and manganese.

7 . The method of claim 1 , wherein precipitating the crystallized nickel-cobalt Tutton's salt from the solution comprises precipitating a crystallized nickel-cobalt Tutton's salt comprising nickel-cobalt ammonium sulfate.

8 . The method of claim 1 , wherein obtaining a solution comprising iron, aluminum, nickel, and cobalt comprises obtaining an aqueous solution comprising iron, aluminum, nickel, and cobalt.

9 . The method of claim 8 , wherein obtaining the solution comprises obtaining a solution that is substantially free of copper.

10 . The method of claim 1 , wherein, during the precipitation of the crystallized nickel-cobalt Tutton's salt from the solution, the pH of the solution is between about 2.00 and about 4.00.

11 . The method of claim 1 , further comprising, before precipitating the at least one phosphate precipitate from the solution, adding hydrogen peroxide (H 2 O 2 ).

12 . The method of claim 1 , further comprising, before precipitating the at least one phosphate precipitate from the solution, adding ammonium hydroxide (NH 4 OH) to adjust the pH of the solution to about 4.00.

13 . The method of claim 1 , further comprising, after adjusting the pH of the solution to be greater than or equal to about 3.00, precipitating zinc phosphate from the solution.

14 . The method of claim 1 , further comprising, before precipitating the crystallized nickel-cobalt Tutton's salt from the solution, filtering the solution to remove the at least one phosphate precipitate from the solution.

15 . The method of claim 14 , wherein filtering the solution comprises removing at least about 90 weight % of the iron from the solution as originally obtained and removing at least about 90 weight % of the aluminum from the solution as originally obtained.

16 . The method claim 1 , wherein precipitating the crystallized nickel-cobalt Tutton's salt from the solution is completed within about three days of precipitating the at least one phosphate precipitate from the solution.

17 . The method of claim 1 , wherein, after obtaining the solution, all material added during a remainder of the method consists of water-soluble salts, the water-soluble salts comprising the ammonium phosphate.

18 . The method of claim 1 , further comprising, after adding the ammonium phosphate to the solution to adjust the pH of the solution to greater than or equal to about 3.00, heating and agitating the solution.

19 . The method of claim 1 , wherein throughout the method, the pH of the solution is less than about 4.00.

20 . The method of claim 1 , wherein adding ammonium phosphate to the solution comprises adding diammonium phosphate (DAP) to the solution.

Assignees

• Battelle Energy Alliance Llc

Inventors

• Klaehn John R
• Diaz Aldana Luis A
• Lister Tedd E
• Mcnally Joshua S
• Shi Meng
• Molina Montes De Oca Daniel E

Classifications

• H01M4/525

  of mixed oxides or hydroxides containing iron, cobalt or nickel for inserting or intercalating light metals, e.g. LiNiO2, LiCoO2 or LiCoOxFy · CPC title

• H01M10/54

  Reclaiming serviceable parts of waste accumulators · CPC title

• H01M10/0525

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

• C22B26/12

  Obtaining lithium · CPC title

• C22B23/0461

  by chemical methods · CPC title