Materials with extremely durable intercalation of lithium and manufacturing methods thereof

• US 10,784,512 B2
• Filed: 01/17/2020
• Issued: 09/22/2020
• Est. Priority Date: 08/28/2015
• Status: Active Grant

• Current Assignee: Group14 Technologies Inc.
• Original Assignee: Group14 Technologies Inc.
• Inventors: Sakshaug, Avery J., Costantino, Henry R., Feaver, Aaron M., Thompkins, Leah A., Geramita, Katharine, Kron, Benjamin E., Fredrick, Sarah, Afkhami, Farshid, Strong, Adam
• Primary Examiner(s): Kopec, Mark
• Application Number:
  US16/746,697
• Publication Number:
  US 20200152983A1
• Time in Patent Office: 249 Days
• CPC Class Codes: C04B 2111/00853 in electrochemical cells or batteries, e.g. fuel cells
• CPC Class Codes: C04B 2235/428 Silicon
• CPC Class Codes: C04B 2235/616 Liquid infiltration of green bodies or pre-forms
• CPC Class Codes: C04B 2235/6581 Total pressure below 1 atmosphere, e.g. vacuum
• CPC Class Codes: C04B 35/522 Graphite C04B35/536 takes precedence
• CPC Class Codes: C04B 35/524 obtained from polymer precursors, e.g. glass-like carbon material
• CPC Class Codes: C04B 38/0051 characterised by the pore size, pore shape or kind of porosity
• CPC Class Codes: C04B 38/0054 the pores being microsized or nanosized
• CPC Class Codes: C04B 38/0064 Multimodal pore size distribution
• CPC Class Codes: C04B 41/009 characterised by the material treated
• CPC Class Codes: C04B 41/4529 applied from the gas phase
• CPC Class Codes: C04B 41/5096 Silicon C04B35/573 takes precedence
• CPC Class Codes: C04B 41/85 with inorganic materials
• CPC Class Codes: H01B 1/04 mainly consisting of carbon-silicon compounds, carbon or silicon
• CPC Class Codes: H01M 10/0525 Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
• CPC Class Codes: H01M 2004/021 Physical characteristics, e.g. porosity, surface area
• CPC Class Codes: H01M 2220/20 Batteries in motive systems, e.g. vehicle, ship, plane
• CPC Class Codes: H01M 4/0416 involving impregnation with a solution, dispersion, paste or dry powder H01M4/0438 takes precedence
• CPC Class Codes: H01M 4/133 Electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
• CPC Class Codes: H01M 4/134 Electrodes based on metals, Si or alloys
• CPC Class Codes: H01M 4/362 : Composites
• CPC Class Codes: H01M 4/364 : as mixtures
• CPC Class Codes: H01M 4/366 : as layered products
• CPC Class Codes: H01M 4/386 : Silicon or alloys based on silicon
• CPC Class Codes: H01M 4/587 : for inserting or intercalating light metals
• CPC Class Codes: H01M 4/625 : Carbon or graphite
• CPC Class Codes: Y02E 60/10 : Energy storage using batteries

Abstract

Composites of silicon and various porous scaffold materials, such as carbon material comprising micro-, meso- and/or macropores, and methods for manufacturing the same are provided. The compositions find utility in various applications, including electrical energy storage electrodes and devices comprising the same.

Claims

1. A process for preparing silicon-carbon composite particles, the process comprising:

a. providing a porous carbon framework comprising micropores, wherein the porous carbon framework comprises particles with a Dv,50 of 1 to 1000 microns;

b. heating the porous carbon framework at an elevated temperature in the presence of a silicon-containing gas, thereby impregnating silicon within the micropores of the porous carbon framework to provide a silicon-carbon composite; and

c. performing a particle size reduction of the silicon-carbon composite to provide silicon-carbon composite particles,

wherein the silicon-carbon composite particles have a nitrogen-inaccessible volume ranging from 0.05 to 0.5 cm³/g.

2. The process according to claim 1, wherein the silicon impregnated within the micropores of the porous carbon framework is nano sized.

3. The process according to claim 1, wherein the porous carbon framework comprises pyrolyzed carbon material.

4. The process according to claim 1, wherein the porous carbon framework comprises pyrolyzed and activated carbon material.

5. The process according to claim 1, wherein the particle size reduction is performed by jet milling.

6. The process according to claim 5, wherein the jet milling is performed in the presence of nitrogen gas.

7. The process according to claim 1, wherein the elevated temperature is between 300 and 900°

C.

8. The process according to claim 1, wherein the porous carbon framework comprises a pore volume greater than 0.5 cm³/g.

9. The process according to claim 1, wherein the porous carbon framework comprises a surface area greater than 500 m²/g.

10. The process according to claim 1, wherein the porous carbon framework comprises a surface area greater than 750 m²/g.

11. The process according to claim 1, wherein the silicon-carbon composite particles comprise pores, and a majority of the pores have a diameter of 5 nm or lower.

12. The process according to claim 1, wherein the Dv,50 of the silicon-carbon composite particles ranges from 5 nm to 20 microns.

13. The process according to claim 1, wherein the Dv,50 of the silicon-carbon composite particles is greater than 20 microns.

14. The process according to claim 1, wherein a Dv,0 of the silicon-carbon composite particles ranges from 1 nm to 5 microns.

15. The process according to claim 1, wherein a Dv,0 of the silicon-carbon composite particles is greater than 5 um.

16. The process according to claim 1, wherein a Dv,100 of the silicon-carbon composite particles ranges from 8 nm to 100 microns.

17. The process according to claim 1, wherein a Dv,100 of the silicon-carbon composite particles is greater than 100 microns.

18. The process according to claim 1, wherein an silicon content of the silicon-carbon composite particles ranges from 5% to 95% by weight.

19. The process according to claim 1, wherein an oxygen content of the silicon-carbon composite particles is less than 10% by weight.

20. The process according to claim 1, wherein the porous carbon framework is heated in a fluidized bed reactor.

21. The process according to claim 1, wherein the porous carbon framework further comprises mesopores.