IP Library › Granted Patent US 11,424,442
Granted Patent B2
US 11,424,442 · App. 16/706,351 · Granted Aug 23, 2022

Methods of forming prelithiated silicon alloy electroactive materials

Inventors: Bradley R. Frieberg (Farmington Hills, MI); Xiaosong Huang (Novi, MI); Zhongyi Liu (Troy, MI); Mark W. Verbrugge (Troy, MI)
Assignee: GM GLOBAL TECHNOLOGY OPERATIONS LLC
H01M4/1395H01M4/045H01M4/0428H01M4/0471H01M10/0525H01M2004/027H01M2004/028
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Quick Facts
Patent No.
US 11,424,442
App. No.
16/706,351
Granted
Aug 23, 2022
Kind
B2
Abstract

A method of making a negative electrode material for an electrochemical cell that cycles lithium ions is provided that includes centrifugally distributing a molten precursor comprising silicon and lithium by contacting the molten precursor with a rotating surface in a centrifugal atomizing reactor. The molten precursor is solidified to form a plurality of substantially round solid electroactive particles comprising an alloy of lithium and silicon and having a D50 diameter of less than or equal to about 20 micrometers. In certain variations, the negative electroactive material particles may further have one or more coatings disposed thereon, such as a carbonaceous coating and/or an oxide-based coating.

Claims (20)

1. A method of making a negative electrode material for an electrochemical cell that cycles lithium ions, the method comprising:

centrifugally distributing a molten precursor comprising silicon and lithium by contacting the molten precursor with a rotating surface in a centrifugal atomizing reactor and solidifying the molten precursor to form a plurality of substantially round solid electroactive particles comprising an alloy of lithium and silicon and having a D50 diameter of less than or equal to about 20 micrometers.

2. The method of claim 1 , wherein the alloy is represented by a formula Li 4.4x Si, where x is greater than 0 to less than or equal to about 0.85.

3. The method of claim 1 , wherein the alloy is represented by a formula Li 4.4x Si, where x is greater than or equal to about 0.1 to less than or equal to about 0.5.

4. The method of claim 1 , wherein the alloy comprises a phase selected from the group consisting of: Li 22 Si 5 , Li 13 Si 4 , Li 7 Si 3 , Li 12 Si 7 , LiSi, Si, and combinations thereof.

5. The method of claim 1 , wherein a temperature in the centrifugal atomizing reactor is greater than or equal to 400° C. to less than or equal to about 1,000° C. during the centrifugally distributing.

6. The method of claim 1 , wherein an environment in the centrifugal atomizing reactor has less than or equal to about 0.5% by weight of any oxygen-bearing species.

7. The method of claim 1 , wherein a flow rate of the centrifugal atomizing reactor is greater than or equal to 50 kg/hour to less than or equal to about 500 kg/hour.

8. The method of claim 1 , wherein the D50 diameter is greater than or equal to about 1 μm to less than or equal to about 10 μm and the plurality of substantially round solid electroactive particles has a polydispersity index of less than or equal to about 1.2.

9. A method of making a negative electrode material for an electrochemical cell that cycles lithium ions, the method comprising:

centrifugally distributing a molten precursor comprising silicon and lithium by contacting the molten precursor with a rotating surface in a centrifugal atomizing reactor and solidifying the molten precursor to form a plurality of substantially round solid electroactive particles comprising an alloy of lithium and silicon and having a D50 diameter of greater than or equal to about 1 micrometer to less than or equal to about 20 micrometers and having a polydispersity index of less than or equal to about 1.2; and

passing the plurality of substantially round solid electroactive particles into a distinct reactor chamber in fluid communication with the centrifugal atomizing reactor and applying a coating to respective surfaces of the plurality of substantially round solid electroactive particles.

10. The method of claim 9 , wherein the coating comprises an oxide-based coating selected from the group consisting of: aluminum oxide (Al 2 O 3 ), titanium dioxide (TiO 2 ), silicon dioxide (SiO 2 ), vanadium pentoxide (V 2 O 5 ), zirconium dioxide (ZrO 2 ), hafnium dioxide (HfO 2 ), tin oxide (SnO 2 ), zinc oxide (ZnO), and combinations thereof.

11. The method of claim 10 , wherein the applying is an atomic layer deposition (ALD) process.

12. The method of claim 9 , wherein the applying is pyrolyzing a carbon-containing precursor at a temperature of greater than or equal to about 600° C. to less than or equal to about 1,400° C. and the coating comprises a carbonaceous coating comprising both graphitic carbon and amorphous carbon.

13. The method of claim 9 , wherein the distinct reactor chamber is a first reactor chamber and the coating is a first coating and the passing further comprises passing the plurality of substantially round solid electroactive particles from the first reactor chamber into a second distinct reactor chamber in fluid communication with the first reactor chamber to apply a second coating over the first coating on the plurality of substantially round solid electroactive particles.

14. The method of claim 13 , wherein (i) the first coating comprises a carbonaceous coating and the second coating comprises an oxide-based coating or (ii) the first coating comprises an oxide-based coating and the second coating comprises a carbonaceous coating.

15. The method of claim 13 , wherein the alloy is represented by a formula Li 4.4x Si, where x is greater than 0 and less than or equal to about 0.85.

16. The method of claim 13 , wherein a temperature in the centrifugal atomizing reactor is greater than or equal to 400° C. to less than or equal to about 1,000° C. during the centrifugally distributing.

17. The method of claim 13 , wherein an environment in the centrifugal atomizing reactor has less than or equal to about 0.5% by weight of any oxygen-bearing species.

Assignments (1)
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Dec 9, 2019
From: FRIEBERG, BRADLEY R.; HUANG, XIAOSONG; LIU, ZHONGYI; VERBRUGGE, MARK W.
To: GM GLOBAL TECHNOLOGY OPERATIONS LLC
Reel/Frame 051214/0837 →
Continuity (1)
Related Publication 20210175491A1 · Jun 10, 2021
Cited By (2)
US 12,573,634 US 12,725,832