IP Library › Granted Patent US 12,633,519
Granted Patent B2
US 12,633,519 · App. 18/075,023 · Granted May 19, 2026

Cathode materials for use in lithium cells and batteries

Inventors: Michael M. Thackeray (Naperville, IL); Eungje Lee (Naperville, IL); Jason R. Croy (Plainfield, IL); Boyu Shi (Willowbrook, IL)
Assignee: UCHICAGO ARGONNE, LLC
H01M4/364H01M4/485H01M4/505H01M4/525H01M10/0525H01M2004/021H01M2004/028
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Quick Facts
Patent No.
US 12,633,519
App. No.
18/075,023
Granted
May 19, 2026
Kind
B2
Abstract

A composite electrode active material is described herein, which comprises two or more electrode active materials blended or structurally-integrated together, in one of the materials is a lithiated spinel selected from the group consisting of (a) a lithiated spinel of formula LiMn x Ni y M z O 2 ; wherein M comprises at least one metal cation other than manganese and nickel cations; x+y+z=1; 0<x<1.0; 0<y<1.0; 0≤z≤0.5; and the ratio of x:y is in the range of about 1:2 to about 2:1; and (b) a lithiated spinel of formula LiM 1 O 2 , wherein M 1 comprises a combination of Mn and Ni transition metal ions in a ratio of Mn to Ni ions of about 2:1 to about 1:1.

Claims (51)

1 . A composite electrode active material comprising a first electrode active material blended or structurally-integrated with a second electrode active material that is different from the first electrode active material;

wherein the electrode active composite material is a lithiated spinel-lithiated spinel of formula aLiM 1 O 2 •(1-a)LiM 7 O 2 in which a is about 0.9; wherein the first electrode active material is a lithiated spinel of formula LiM 1 O 2 , wherein M 1 comprises a combination of Mn and Ni transition metal ions in a ratio of Mn to Ni ions of about 2:1 to about 1:1; and the second electrode active material is a lithiated-spinel of formula LiM 7 O 2 , wherein M 7 comprises two or more cations selected from the group consisting of a Mn cation, a Ni cation, a Co cation, and a M 6 cation; wherein M 6 comprises at least one cation other than Mn, Ni, and Co cations.

2 . The electrode active material of claim 1 , wherein M 6 is at least one cation of a metal selected from the group consisting of Al, Ga, Mg, and Ti.

3 . The electrode active composite material of claim 2 , wherein the lithiated spinel-lithiated spinel is a material of formula 0.9LiMn 0.5 Ni 0.5 O 2 •0.1LiCo 0.85 Al 0.15 O 2 .

4 . The electrode active material of claim 1 , wherein a portion of the oxygen thereof is replaced by fluorine.

5 . The electrode active composite material of claim 1 , wherein the metal ions of the lithiated spinel of the first and second electroactive materials are partially disordered relative to an ideal lithiated spinel structure.

6 . An electrochemical cell comprising an anode, a cathode, and a lithium-containing electrolyte contacting the anode and cathode, wherein the cathode comprises the electrode active composite material of claim 1 .

7 . A battery comprising a plurality of the electrochemical cell of claim 6 electrically connected in series, in parallel, or in both series and parallel.

8 . A composite electrode active material comprising a first electrode active material that is structurally-integrated with a second electrode active material;

wherein:

the first electrode active material is a layered material of empirical formula Li 2 M 4 O 3 , wherein M 4 is at least one metal cation selected from the group consisting of a Mn cation, a Ti cation, and a Zr cation;

the second electrode active material is a lithiated spinel of formula LiM 1 O 2 , wherein M 1 comprises a combination of Mn and Ni transition metal ions in a ratio of Mn to Ni ions of about 2:1 to about 1:1; and

the composite electrode active material is a layered-lithiated spinel material of formula bLi 2 M 4 O 3 •(1-b)LiM 1 O 2 , in which b is about 0.1.

9 . The composite electrode active material of claim 8 , wherein the material of formula LiM 1 O 2 comprises domains of a disordered lithiated-spinel component, a disordered layered component, and a disordered rock salt component, in which the oxygen lattice of the components is cubic-close packed, and in which greater than 0 percent and less than 20 percent of lithium ions of the lithiated spinel and layered components are disordered among the octahedral sites normally occupied by the transition metal ions, and a corresponding percentage of the transition metal ions are disordered among the octahedral sites normally occupied by lithium ions, in fully-ordered, lithiated spinel and layered structures.

10 . The composite material of claim 9 , wherein greater than about 1 percent and less than 20 percent of the lithium ions of the material of formula bLi 2 M 4 O 3 •(1-b)LiM 1 O 2 are disordered among the octahedral sites normally occupied by the transition metal ions, and a corresponding percentage of the transition metal ions are disordered among the octahedral sites normally occupied by lithium ions, in fully-ordered, lithiated spinel and layered structures.

11 . The composite material of claim 9 , wherein greater than 10 percent and less than 20 percent of the lithium ions of the material of formula bLi 2 M 4 O 3 •(1-b)LiM 1 O 2 are disordered among the octahedral sites normally occupied by the transition metal ions, and a corresponding percentage of the transition metal ions are disordered among the octahedral sites normally occupied by lithium ions, in fully-ordered, lithiated spinel and layered structures.

12 . The composite electrode active material of claim 8 , wherein in M 1 is M 2 (1-w) M 3 w ; M 2 comprises a combination of Mn and Ni transition metal ions; and M 3 is at least one metal cation selected from the group consisting of an Al cation, a Ga cation, a Mg cation, a Ti cation; and a Co cation; and 0<w≤0.1.

13 . The composite electrode active material of claim 8 , wherein the composite electrode active material is a structurally integrated layered-lithiated spinel of formula 0.1Li 2 MnO 3 •0.9LiMn 0.5 Ni 0.5 O 2 .

14 . An electrode active material comprising the electrode active composite material of claim 8 , mechanically blended with or structurally integrated with a lithiated spinel of formula LiM 7 O 2 ; wherein M 7 comprises two or more cations selected from the group consisting of a Mn cation, a Ni cation, a Co cation, and a M 6 cation; and M 6 comprises at least one cation other than Mn, Ni, and Co cations.

15 . The electrode active material of claim 14 , wherein M 6 is at least one cation of a metal selected from the group consisting of Al, Ga, Mg, and Ti.

16 . An electrode active material comprising the composite electrode active material of claim 8 , mechanically blended with or structurally integrated with a layered compound of formula LiM 5 O 2 , wherein M 5 comprises at least one first row transition metal cation.

17 . The composite material of claim 16 , wherein M 5 further comprises at least one non-transition metal cation.

18 . The electrode active material of claim 8 , wherein a portion of the oxygen thereof is replaced by fluorine.

19 . The electrode active composite material of claim 8 , wherein the metal ions of the lithiated spinel of the second electroactive material are partially disordered relative to an ideal lithiated spinel structure.

20 . An electrochemical cell comprising an anode, a cathode, and a lithium-containing electrolyte contacting the anode and cathode, wherein the cathode comprises the electrode active composite material of claim 8 .

21 . A battery comprising a plurality of the electrochemical cell of claim 20 electrically connected in series, in parallel, or in both series and parallel.

22 . An electrode active composite material comprising a first electrode active material that is mechanically blended with or structurally-integrated with a second electrode active material different from the first electrode active material, and a third electrode active material different from the first and second electrode active materials;

wherein:

the first electrode active material is a layered material of formula Li 2 M 4 O 3 , wherein M 4 is at least one metal cation selected from the group consisting of a Mn cation, a Ti cation, and a Zr cation;

the second electrode active material is a lithiated spinel of formula LiM 1 O 2 , wherein M 1 comprises a combination of Mn and Ni transition metal ions in a ratio of Mn to Ni ions of about 2:1 to about 1:1; and

the third electrode active material is a lithiated spinel of formula LiM 7 O 2 , wherein M 7 comprises two or more cations selected from the group consisting of a Mn cation, a Ni cation, a Co cation, and a M 6 cation; and M 6 comprises at least one cation other than Mn, Ni, and Co cations;

wherein the composite electrode active material is a structurally integrated layered-lithiated spinel-lithiated spinel of formula cLi 2 M 4 O 3 •(1-c-d)LiM 1 O 2 •dLiM 7 O 2 in which 0<|c−d|<1; 0<c<0.2; and 0<d<0.8.

23 . The electrode active composite material of claim 22 , wherein M 6 is at least one cation of a metal selected from the group consisting of Al, Ga, Mg, and Ti.

24 . The composite material of claim 22 , wherein the composite electrode active material is a structurally integrated layered-lithiated spinel-lithiated spinel material of formula 0.1Li 2 MnO 3 •0.8LiMn 0.5 Ni 0.5 O 2 •0.1LiCo 0.85 Al 0.15 O 2 .

25 . The electrode active material of claim 22 , wherein a portion of the oxygen thereof is replaced by fluorine.

26 . The electrode active composite material of claim 22 , wherein the metal ions of the lithiated spinel of the second and third electroactive materials are partially disordered relative to an ideal lithiated spinel structure.

27 . An electrochemical cell comprising an anode, a cathode, and a lithium-containing electrolyte contacting the anode and cathode, wherein the cathode comprises the electrode active composite material of claim 22 .

28 . A battery comprising a plurality of the electrochemical cell of claim 27 electrically connected in series, in parallel, or in both series and parallel.

29 . An electrode active composite material comprising a first electrode active material that is mechanically blended with or structurally-integrated with a second electrode active material different from the first electrode active material, and a third electrode active material different from the first and second electrode active materials;

wherein:

the first electrode active material is a layered material of formula Li 2 M 4 O 3 , wherein M 4 is at least one metal cation selected from the group consisting of a Mn cation, a Ti cation, and a Zr cation;

the second electrode active material is a lithiated spinel of formula LiM 1 O 2 , wherein M 1 comprises a combination of Mn and Ni transition metal ions in a ratio of Mn to Ni ions of about 2:1 to about 1:1; and

the third electrode active material is a layered material of formula LiM 5 O 2 ; wherein M 5 comprises at least one first-row transition metal cation;

wherein the composite electrode active material is a structurally-integrated layered-lithiated spinel-layered material of formula eLi 2 M 4 O 3 •(1-e-f)LiM 1 O 2 •fLiM 5 O 2 in which 0<|e-f|<1; 0<e<0.2; and 0<f<0.8.

30 . The electrode active composite material of claim 29 , wherein M 5 additionally comprises at least one non-transition metal cation.

31 . The electrode active composite material of claim 29 , wherein M 5 is a combination of at least one first-row transition metal cation and at least one non-transition metal cation selected from the group consisting of an Al cation, a Ga cation, and a Mg cation.

32 . The electrode active composite material of claim 29 , wherein the layered-lithiated spinel-layered material is a compound of formula 0.1Li 2 MnO 3 •0.8LiMn 0.5 Ni 0.5 O 2 •0.1LiCo 0.98 Ti 0.01 Mg 0.01 O 2 .

33 . The electrode active material of claim 29 , wherein a portion of the oxygen thereof is replaced by fluorine.

34 . The electrode active composite material of claim 29 , wherein the metal ions of the lithiated spinel of the second electroactive material are partially disordered relative to an ideal lithiated spinel structure.

35 . An electrochemical cell comprising an anode, a cathode, and a lithium-containing electrolyte contacting the anode and cathode, wherein the cathode comprises the electrode active composite material of claim 29 .

36 . A battery comprising a plurality of the electrochemical cell of claim 35 electrically connected in series, in parallel, or in both series and parallel.

Assignments (2)
CONFIRMATORY LICENSE Recorded Feb 15, 2024
From: UCHICAGO ARGONNE LLC
To: U.S. DEPARTMENT OF ENERGY
Reel/Frame 066601/0140 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Nov 14, 2023
From: THACKERAY, MICHAEL M.; LEE, EUNGJE; CROY, JASON R.; SHI, BOYU
To: UCHICAGO ARGONNE, LLC
Reel/Frame 065561/0424 →
Continuity (6)
Continuation In Part 17351944 · Jun 18, 2021
Continuation In Part 17313752 · May 6, 2021
Continuation In Part 17136234 · Dec 29, 2020
Provisional Application 63286251 · Dec 6, 2021
Provisional Application 63055993 · Jul 24, 2020
Related Publication 20230108813A1 · Apr 6, 2023
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