Chemical dismantling of permanent magnet material and battery material

Patent metadata

Field	Value
Publication number	US-11764416-B2
Application number	US-202016873846-A
Country	US
Kind code	B2
Filing date	Jul 23, 2020
Priority date	Aug 2, 2019
Publication date	Sep 19, 2023
Grant date	Sep 19, 2023

Abstract

Certain method embodiments are described and useful for recycling permanent magnet materials (e.g. permanent magnet alloys) and battery materials (e.g. battery electrode materials) to extract critical and/or valuable elements including REEs, Co and Ni. Method embodiments involve reacting such material with at least one of an ammonium salt and an iron (III) salt to achieve at least one of a liquid phase chemical reaction and a mechanochemical reaction.

First claim

We claim:

1. A method for use in recycling of a material that includes a metal content to be recovered comprising at least one of a rare earth metal, cobalt, and nickel, wherein the rare earth metal includes at least one of Sc, Y, La, Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, and Lu, comprising the step of contacting the material and a chemical reagent that includes at least one of an ammonium salt and iron (lll) salt without added oxygen reagent at a temperature up to about 100° C. to carry out at least one of a liquid phase chemical reaction and a mechanochemical reaction with the metal content to form a non-oxide and water soluble derivative of the at least one rare earth metal, cobalt and nickel.

2. The method of claim 1 wherein the contacting is carried out at a temperature from room temperature to about 100° C.

3. The method of claim 1 where the contacting is carried out by mechanical milling of the material in the presence of at least one of the ammonium salt and iron (lll) salt in the absence of water or another solvent to achieve a mechanochemical solid state reaction.

4. The method of claim 1 where the contacting is carried out by mechanical milling of the material in the presence of water and of at least one of the ammonium salt and iron (lll) salt at room temperature.

5. The method of claim 1 where the contacting is carried out in an aqueous environment or in a solution containing water as one component.

6. The method of claim 5 where the contacting is carried out in a first step by means of the mechanochemical reaction and then in a second step by means of the liquid phase chemical reaction in aqueous environment at a temperature from room temperature to about 100° C.

7. The method of claim 1 wherein the material comprises at least one of a permanent magnet alloy and a battery alloy containing at least one of the rare earth metal, cobalt and nickel.

8. The method of claim 1 that produces a water-soluble derivative of Sc, Y, La, Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, Ni or Co.

9. The method of claim 8 comprising precipitating the water soluble derivative of at least one rare earth metal in the form of a rare earth metal compound.

10. The method of claim 8 comprising precipitating the water soluble derivative of least one of cobalt and nickel in the form of at least one of a cobalt compound and nickel compound.

11. The method of claim 9 including the further step of calcining the rare earth metal compound to produce a rare earth metal oxide.

12. The method of claim 1 , wherein the ammonium salt contains at least one anion comprising a Cl − , Br − , I − , NO 3 − , HSO 4 − , and SO 4 2− .

13. The method of claim 1 , wherein the iron (lll) salt contains at least one anion comprising a Cl − , Br − , I − , NO 3 − , HSO 4 − , and SO 4 2 .

14. The method of claim 1 , wherein the contacting includes contacting the ammonium salt and a samarium-cobalt permanent magnet or magnetic alloy.

15. The method of claim 1 , wherein the contacting includes contacting the ammonium salt and a rare earth-iron-boron permanent magnet or magnetic alloy.

16. The method of claim 1 , wherein the contacting includes contacting the ammonium salt and a rare earth-containing magnet material or alloy and/or nickel-based battery material or alloy.

17. The method of claim 1 , wherein the contacting includes contacting the iron (lll) salt and a samarium-cobalt permanent magnet or magnetic alloy.

18. The method of claim 1 , wherein the contacting includes contacting the iron (lll) salt and a rare earth-iron-boron permanent magnet or magnetic alloy.

19. The method of claim 1 , wherein the contacting includes contacting the iron (lll) salt and a rare earth-containing magnet material and/or a nickel-based battery material or alloy.

20. The method of claim 1 , wherein the chemical reaction or mechanochemical reaction is carried out in an aqueous environment.

21. The method of claim 20 , wherein the aqueous environment is maintained at a temperature between 0° C. and about 100° C.

22. The method of claim 1 wherein the mechanochemical reaction is conducted by at least one of mechanical milling and grinding of the material.

23. The method of claim 22 , wherein at least one of the mechanical milling and grinding is carried out in a ball mill, a planetary mill, a shaker mill, a crusher and a grinder for time period of at least 5 minutes to 24 hours.

24. The method of claim 1 , wherein the contacting of the material dissolves rare earth metal content to form the water soluble derivative and then the water soluble derivative is precipitated as a rare earth metal oxalate, rare earth metal sulfate, rare earth metal-sodium sulfate, rare earth metal phosphate, or rare earth metal fluoride.

25. The method of claim 1 wherein the material comprises magnet scrap or battery scrap.

26. The method of claim 25 wherein the magnet scrap includes shredded non-magnet components.

27. The method of claim 1 wherein the material comprises at least one of grinding swarf, magnet scrap cuttings, polishing byproducts, magnet powders, and magnets derived from manufacturing processes including magnet manufacturing and additive manufacturing processes.

28. A method for use in recycling of a material that includes a metal content to be recovered comprising at least one of a rare earth metal, cobalt, and nickel, wherein the rare earth metal includes at least one of Sc, Y, La, Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, and Lu, comprising the step of contacting the material and a chemical reagent that includes at least one of an ammonium salt and iron (lll) salt to carry out a mechanochemical reaction in the absence of water or solvent to form a derivative of the at least one rare earth metal, cobalt and nickel.

29. The method of claim 28 wherein the mechanochemical reaction is conducted by at least one of mechanical milling and grinding of the material.

30. The method of claim 29 wherein at least one of the mechanical milling and grinding is carried out in a ball mill, a planetary mill, a shaker mill, a crusher and a grinder for time period of at least 5 minutes to 24 hours.

31. A method for use in recycling of a material that includes a metal content to be recovered, comprising at least one of a rare earth metal, cobalt, and nickel, wherein the rare earth metal includes at least one of Sc, Y, La, Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, and Lu, comprising the step of contacting the material and an iron (lll) salt reagent to carry out at least one of a liquid phase chemical reaction and a mechanochemical reaction to form a water soluble derivative of the at least one of the rare earth metal, cobalt and nickel.

32. The method of claim 31 , wherein the iron (lll) salt contains at least one anion comprising a Cl − , Br − , I − , NO 3 − , HSO 4 − , and SO 4 2− .

Assignees

• Univ Iowa State Res Found Inc
• Iowa State Univerity Res Foundation Inc

Inventors

• Balema Viktor
• Hlova Ihor
• Dolotko Oleksandr
• Pecharsky Vitalij K

Classifications

• C22B1/005 Primary

  Preliminary treatment of scrap (C22B1/02 - C22B1/26 take precedence) · CPC title

• H01M10/54 Primary

  Reclaiming serviceable parts of waste accumulators · CPC title

• Y02W30/84

  Recycling of batteries or fuel cells · CPC title

• Y02P10/20

  Recycling · CPC title

• C22B3/14

  containing ammonia or ammonium salts · CPC title