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WO-2026096054-A1 - ANTIMONY ANODES FOR SOLID-STATE BATTERIES

WO2026096054A1WO 2026096054 A1WO2026096054 A1WO 2026096054A1WO-2026096054-A1

Abstract

The present technology relates generally to an anode for a solid-state battery, solid- state batteries including the anode, and methods of making the anode. The anode includes antimony having an average particle size of about 1 μm to about 100 μm and a sulfide-based solid-state electrolyte.

Inventors

  • WU, Xianyong
  • ULLAH, Irfan

Assignees

  • UNIVERSITY OF PUERTO RICO

Dates

Publication Date
20260507
Application Date
20250827
Priority Date
20241029

Claims (20)

  1. 1. An anode comprising: about 50 wt.% to about 90 wt.% antimony, the antimony having an average particle size of about 1 pm to about 100 pm as measured by scanning electron microscopy; and about 10 wt.% to about 50 wt.% of a first sulfide-based solid-state electrolyte.
  2. 2. The anode of claim 1, wherein the antimony has an average particle size of about 1 pm to about 50 pm as measured by scanning electron microscopy.
  3. 3. The anode of claim 1, wherein the first sulfide-based solid-state electrolyte comprises lithium phosphorus sulfur chloride, lithium phosphorus sulfur fluoride, lithium phosphorus sulfur bromide, lithium phosphorus sulfur iodide, lithium germanium phosphorus sulfide, lithium zinc germanium oxide, lithium tin phosphorus sulfide, lithium silicon phosphorus sulfide, lithium silicon aluminum sulfide, lithium sulfide, phosphorus sulfide, lithium phosphorus sulfide, silicon sulfide, lithium orthosilicate, or a combination of any two or more thereof.
  4. 4. The anode of claim 1, wherein the first sulfide-based solid-state electrolyte comprises LiePSsX, where X is F, Cl, Br, I, or a combination of two or more thereof.
  5. 5. The anode of claim 1, wherein the first sulfide-based solid-state electrolyte has an average particle size of about 1 pm to about 50 pm as measured by scanning electron microscopy.
  6. 6. The anode of claim 1, wherein an antimony mass loading is about 1 mg cm' 2 to about 2 mg cm' 2 .
  7. 7. The anode of claim 1, wherein the antimony and first sulfide-based solid-state electrolyte are present as a composite formed by grinding together antimony and the first sulfide- based solid-state electrolyte.
  8. 8. A solid-state battery comprising the anode of claim 1; a counter electrode; and Atty. Dkt. No. 118347-0138 (24-024-UPR) a solid electrolyte disposed between the anode and the counter electrode, the solid electrolyte comprising a second sulfide-based solid-state electrolyte.
  9. 9. The solid-state battery of claim 8, wherein the second sulfide-based solid-state electrolyte comprises lithium phosphorus sulfur chloride, lithium phosphorus sulfur fluoride, lithium phosphorus sulfur bromide, lithium phosphorus sulfur iodide, lithium germanium phosphorus sulfide, lithium zinc germanium oxide, lithium tin phosphorus sulfide, lithium silicon phosphorus sulfide, lithium silicon aluminum sulfide, lithium sulfide, phosphorus sulfide, lithium phosphorus sulfide, silicon sulfide, lithium orthosilicate, or a combination of any two or more thereof.
  10. 10. The solid-state battery of claim 8, wherein the second sulfide-based solid-state electrolyte comprises LiePSsX, where X is F, Cl, Br, I, or a combination of two or more thereof.
  11. 11. The solid-state battery of claim 8, wherein the second sulfide-based solid-state electrolyte is the same as the first sulfide-based solid-state electrolyte.
  12. 12. The solid-state battery of claim 8, wherein the counter electrode comprises lithium metal.
  13. 13. The solid-state battery of claim 8, wherein the counter electrode is a cathode.
  14. 14. The solid-state battery of claim 13, wherein the cathode comprises lithium cobalt oxide, lithium nickel oxide, lithium nickel cobalt oxide, lithium manganese oxide, lithium nickel manganese cobalt oxide, lithium manganese nickel oxide, lithium nickel manganese cobalt aluminum oxide, lithium iron phosphate, or a combination of any two or more thereof.
  15. 15. A process for forming an anode for a solid-state battery, the process comprising: grinding a mixture of antimony, the antimony having an average particle size of about 1 pm to about 100 pm as measured by scanning electron microscopy, and a sulfide-based solid-state electrolyte; and compressing the mixture under a pressure of about 50 MPa to about 500 MPa into a monolithic form. Atty. Dkt. No. 118347-0138 (24-024-UPR)
  16. 16. The process of claim 15, wherein the mixture comprises about 50 wt.% to about 90 wt.% antimony and about 10 wt.% to about 50 wt.% of the sulfide-based solid-state electrolyte.
  17. 17. The process of claim 15, wherein compressing the mixture comprises the pressure of about 200 MPa to about 300 MPa.
  18. 18. The process of claim 15, wherein the sulfide-based solid-state electrolyte comprises lithium phosphorus sulfur chloride, lithium phosphorus sulfur fluoride, lithium phosphorus sulfur bromide, lithium phosphorus sulfur iodide, lithium germanium phosphorus sulfide, lithium zinc germanium oxide, lithium tin phosphorus sulfide, lithium silicon phosphorus sulfide, lithium silicon aluminum sulfide, lithium sulfide, phosphorus sulfide, lithium phosphorus sulfide, silicon sulfide, lithium orthosilicate, or a combination of any two or more thereof.
  19. 19. The process of claim 15, wherein the sulfide-based solid-state electrolyte comprises LiePSsX, where X is F, Cl, Br, I, or a combination of two or more thereof.
  20. 20. The process of claim 15, wherein the sulfide-based solid-state electrolyte has an average particle size of about 1 pm to about 50 pm as measured by scanning electron microscopy.

Description

Atty. Dkt. No. 118347-0138 (24-024-UPR) ANTIMONY ANODES FOR SOLID-STATE BATTERIES CROSS-REFERENCE TO RELATED APPLICATIONS [0001] This application claims the benefit of and priority to U.S. Provisional Appl. No. 63/713,385, filed October 29, 2024, the contents of which are incorporated herein by reference in its entirety for any and all purposes. GOVERNMENT RIGHTS [0002] This invention was made with government support under OIA- 1849243 awarded by The National Science Foundation, and 80NSSC23M0189 awarded by The National Aeronautics and Space Administration. The government has certain rights in the invention. TECHNICAL FIELD [0003] The present technology relates generally to solid-state battery anodes that include antimony as an electroactive material, batteries including these anodes, and methods of making the same. SUMMARY [0004] In an aspect, which may be combined with any other aspect or embodiment, the present disclosure relates to an anode comprising about 50 wt.% to about 90 wt.% antimony, the antimony having an average particle size of about 1 pm to about 100 pm as measured by scanning electron microscopy; and about 10 wt.% to about 50 wt.% of a first sulfide-based solid-state electrolyte. [0005] In another aspect, which may be combined with any other aspect or embodiment, the present disclosure relates to a solid-state battery including the anode disclosed herein, a counter electrode, and a solid electrolyte disposed between the anode and the counter electrode, the solid electrolyte comprising a sulfide-based solid-state electrolyte. [0006] In another aspect, which may be combined with any other aspect or embodiment, the present disclosure relates to a process for forming an anode for a solid-state battery. The process comprises grinding a mixture of antimony, the antimony having an average particle size of about 1 pm to about 100 pm as measured by scanning electron microscopy, and a Atty. Dkt. No. 118347-0138 (24-024-UPR) sulfide-based solid-state electrolyte; and compressing the mixture under a pressure of about 50 MPa to about 500 mPa into a monolithic form. [0007] Further aspects and embodiments of the present technology are described herein. BRIEF DESCRIPTION OF THE DRAWINGS [0008] FIG. 1 is an illustration of a solid-state electrochemical cell with an antimony anode and a nickel manganese cobalt cathode. [0009] FIG. 2 is a graph of X-ray diffraction (XRD) characterization of microscale antimony powder used as an electroactive material in the anode. [0010] FIGS. 3A and 3B are scanning electron microscopy (SEM) images of nanoscale (FIG. 3 A) and microscale (FIG. 3B) antimony powder used as an electroactive material in the anode. [0011] FIGS. 4A and 4B are graphs of galvanostatic charge/discharge curves of electrochemical cells with antimony anodes and lithium counter electrodes in a liquid electrolyte of 1 M LiPFe in ethylene carbonate and dimethyl carbonate (EC-DMC) at 50 mA g'1. FIG. 4A includes nanoscale antimony in the anode and FIG. 4B includes microscale antimony in the anode. [0012] FIGS. 5 A and 5B are graphs of electrochemical impedance spectroscopy (EIS) results of electrochemical cells with antimony anodes and lithium counter electrodes in a liquid electrolyte of 1 M LiPFe in ethylene carbonate and dimethyl carbonate (EC-DMC) at 50 mA g'1 at the first, fifth, and tenth cycle. FIG. 5A includes nanoscale antimony in the anode and FIG. 5B includes microscale antimony in the anode. [0013] FIGS. 6 A and 6B are cross-sectional SEM images of the Antimony electrodes from electrochemical cells with antimony anodes, lithium counter electrodes, and the liquid electrolyte of 1 M LiPFe in EC-DMC after different numbers of galvanostatic cycles. FIG. 6A includes nanoscale antimony in the anode and FIG. 6B includes microscale antimony in the anode. [0014] FIG. 7 is an illustration of a reaction scheme of the formation of a solid-electrolyte interphase on antimony powder in an anode of an electrochemical cell. Atty. Dkt. No. 118347-0138 (24-024-UPR) [0015] FIGS. 8A and 8B are graphs of galvanostatic charge/discharge curves of solid-state electrochemical cells with an antimony anode and a lithium indium alloy counter electrode at 50 mA g'1. FIG. 8 A includes nanoscale antimony in the anode and FIG. 8B includes microscale antimony in the anode. [0016] FIGS. 9A and 9B are SEM images of energy dispersive spectra (EDS) analysis of antimony-solid electrolyte composites. FIG. 9A shows the nanoscale antimony mixed with the solid electrolyte. FIG. 9B shows the microscale antimony mixed with the solid electrolyte. [0017] FIGS. 10A and 10B are schemes of the antimony-solid electrolyte composite structures. FIG. 10A is an illustration of the nanoscale antimony mixed with the solid electrolyte. FIG. 10B is an illustration of the microscale antimony mixed with the solid electrolyte. [0018] FIG. 11 is a graph of EIS results of the solid-state electrochemical cell with microscale antimony anode and a lithium indi