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EP-4738511-A1 - POSITIVE ELECTRODE SLURRY FOR ALL-SOLID-STATE BATTERY AND METHOD FOR PRODUCING SAME, ALL-SOLID-STATE BATTERY PRODUCED USING SAME

EP4738511A1EP 4738511 A1EP4738511 A1EP 4738511A1EP-4738511-A1

Abstract

A positive electrode slurry for an all-solid-state battery and a method for producing the positive electrode slurry, and an all-solid-state battery are provided. The positive electrode slurry includes a positive electrode active material, a conductive material, a binder, a sulfide-based solid electrolyte, a triphenylphosphine-based additive, and a solvent.

Inventors

  • OH, DAEYANG

Assignees

  • SAMSUNG SDI CO., LTD.

Dates

Publication Date
20260506
Application Date
20251103

Claims (15)

  1. A positive electrode slurry, comprising: a positive electrode active material; a conductive material; a binder; a sulfide-based solid electrolyte; a phosphine-based additive represented by Formula 1; and a solvent, wherein, in Formula 1, n 1 to n 3 are each independently 0 to 5, and R 1 to R 3 are each independently hydrogen, a halogen, a nitrile group, a nitro group, an amine group, a substituted or unsubstituted C1 to C10 alkyl group, a substituted or unsubstituted C1 to C10 alkoxy group, a substituted or unsubstituted aryl group, or a substituted or unsubstituted C5 to C14 heteroaryl group, and wherein the positive electrode slurry is a positive electrode slurry for an all-solid-state battery.
  2. The positive electrode slurry of claim 1, wherein the phosphine-based additive comprises at least one selected from the group consisting of triphenyl phosphine, tris(4-trifluoromethylphenyl)phosphine, tris(4-fluorophenyl)phosphine, tris[3,5-bis(trifluoromethyl)phenyl]phosphine, tris(4-chlorophenyl)phosphine, tris(2,4,6-trimethylphenyl)phosphine, tris(4-methoxyphenyl)phosphine, tris(pentafluorophenyl)phosphine, tris(4-methoxy-3,5-dimethylphenyl)phosphine, tris(3,5-dimethylphenyl)phosphine, tri(o-tolyl)phosphine, diphenyl(p-tolyl)phosphine, and combinations thereof.
  3. The positive electrode slurry of claim 1 or 2, wherein the phosphine-based additive is in an amount of ≥ 0.01 parts by weight to ≤ 3 parts by weight on the basis of a total 100 parts by weight of the positive electrode active material, the conductive material, and the binder.
  4. The positive electrode slurry of any of the claims 1 to 3, wherein the sulfide-based solid electrolyte is in an amount of ≥ 5 parts by weight to ≤ 25 parts by weight on the basis of a total 100 parts by weight of the positive electrode active material, the conductive material, and the binder.
  5. The positive electrode slurry of any of the claims 1 to 4, wherein the solvent is in an amount of ≥ 15 parts by weight to ≤ 50 parts by weight on the basis of a total 100 parts by weight of the positive electrode active material, the conductive material, and the binder.
  6. The positive electrode slurry of any of the claims 1 to 5, wherein a weight ratio of the phosphine-based additive to the sulfide-based solid electrolyte is ≥ 0.2 to ≤ 25.
  7. The positive electrode slurry of any of the claims 1 to 6, wherein the positive electrode active material comprises a compound represented by Formula 2: Formula 2 Li a Ni x Co y Mn z X c O 2-b , in Formula 2, 0.8≤a≤1.2, 0.8≤x≤1.0, 0≤y≤0.1, 0≤z≤0.1, 0≤c≤0.1, 0≤b≤0.05, and x + y + z + c = 1, and X being at least one element selected from the group consisting of Al, Ti, Mg, Zr, Mo, and Nb.
  8. The positive electrode slurry of any of the claims 1 to 7, wherein the binder comprises a fluoride-based binder.
  9. The positive electrode slurry of any of the claims 1 to 8, wherein the conductive material comprises at least one selected from the group consisting of natural graphite, artificial graphite, carbon black, acetylene black, Ketjen black, a carbon fiber, a carbon nanofiber, a carbon nanotube, and combinations thereof.
  10. The positive electrode slurry of any of the claims 1 to 9, wherein the sulfide-based solid electrolyte is an argyrodite-type compound comprising Li 7-a M a PS 6-c X c (0≤a≤2 and 0≤c≤2), X is F, Br, Cl, I, or a combination thereof, and M is scandium, yttrium, titanium, zirconium, hafnium, vanadium, niobium, tantalum, chromium, molybdenum, tungsten, manganese, technetium, rhenium, iron, ruthenium, osmium, cobalt, rhodium, iridium, nickel, palladium, platinum, copper, silver, gold, zinc, cadmium, mercury, aluminum, gallium, indium, thallium, silicon, germanium, tin, lead, arsenic, antimony, bismuth, or a combination thereof.
  11. A method for making a positive electrode slurry according to any of the claims 1 to 10. A method, comprising mixing a positive electrode active material, a conductive material, a binder, a sulfide-based solid electrolyte, a phosphine-based additive represented by Formula 1, and a solvent: wherein, in Formula 1, n 1 to n 3 are each independently 0 to 5, R 1 to R 3 are each independently a hydrogen atom, a halogen group, a nitrile group, a nitro group, an amine group, a substituted or unsubstituted C1 to C10 alkyl group, a substituted or unsubstituted C1 to C10 alkoxy group, a substituted or unsubstituted aryl group, or a substituted or unsubstituted C5 to C14 heteroaryl group, and wherein the method is a method for producing a positive electrode slurry for an all-solid-state battery.
  12. The method of claim 11, wherein the phosphine-based additive comprises at least one selected from the group consisting of triphenyl phosphine, tris(4-trifluoromethylphenyl)phosphine, tris(4-fluorophenyl)phosphine, tris[3,5-bis(trifluoromethyl)phenyl]phosphine, tris(4-chlorophenyl)phosphine, tris(2,4,6-trimethylphenyl)phosphine, tris(4-methoxyphenyl)phosphine, tris(pentafluorophenyl)phosphine, tris(4-methoxy-3,5-dimethylphenyl)phosphine, tris(3,5-dimethylphenyl)phosphine, tri(o-tolyl)phosphine, diphenyl(p-tolyl)phosphine, and combinations thereof.
  13. The method of claim 11 or 12, wherein the binder comprises a fluoride-based binder, and wherein the sulfide-based solid electrolyte is an argyrodite-type compound comprising Li 7-a M a PS 6-c X c (0≤a≤2 and 0≤c≤2), X is F, Br, Cl, I, or a combination thereof, and M is scandium, yttrium, titanium, zirconium, hafnium, vanadium, niobium, tantalum, chromium, molybdenum, tungsten, manganese, technetium, rhenium, iron, ruthenium, osmium, cobalt, rhodium, iridium, nickel, palladium, platinum, copper, silver, gold, zinc, cadmium, mercury, aluminum, gallium, indium, thallium, silicon, germanium, tin, lead, arsenic, antimony, bismuth, or a combination thereof.
  14. The method of any of the claims 11 to 13, wherein the phosphine-based additive is in an amount of ≥ 0.01 parts by weight to ≤ 3 parts by weight on the basis of a total 100 parts by weight of the positive electrode active material, the conductive material, and the binder.
  15. The method of any of the claims 11 to 14, wherein the sulfide-based solid electrolyte is in an amount of ≥ 5 parts by weight to ≤ 25 parts by weight on the basis of a total 100 parts by weight of the positive electrode active material, the conductive material, and the binder.

Description

CROSS-REFERENCE TO RELATED APPLICATIONS The present application claims priority to and the benefit of Korean Patent Application No. 10-2024-0154225, filed on November 04, 2024, in the Korean Intellectual Property Office. BACKGROUND 1. Field One or more embodiments of the present disclosure relate to a positive electrode slurry for an all-solid-state battery and a method for producing the same, and an all-solid-state battery produced using the same. 2. Description of the Related Art In response to increasing industrial demand, the development of batteries with high energy density and enhanced safety has been actively pursued. For example, lithium-ion batteries have been commercialized not only in the fields of information related devices and communication devices, but also in the field of the automotive industry (e.g., automobiles). Given that user safety and/or wellbeing is a top concern in the automotive industry, battery safety is of particular importance. Recently, all-solid-state batteries, in which the liquid electrolyte (solution) is replaced (substituted) with a solid electrolyte, have been proposed. Because these batteries do not use flammable organic solvents as dispersion media, the risk of fire or explosion is significantly reduced, even in the event of a short circuit. Accordingly, all-solid-state batteries offer substantially improved safety compared to related art lithium-ion batteries that utilize liquid electrolytes. SUMMARY One or more aspects of the present disclosure are directed toward a positive electrode slurry with improved adhesion characteristics and a method for producing the same. One or more aspects of the present disclosure are directed toward a positive electrode for an all-solid-state battery with excellent or suitable performance, and an all-solid-state battery including the same. Additional aspects will be set forth in part in the description which follows and, in part, will be apparent from the description, or may be learned by practice of the presented embodiments of the disclosure. According to one or more embodiments of the present disclosure, a positive electrode slurry for an all-solid-state battery includes a positive electrode active material, a conductive material, a binder, a sulfide-based solid electrolyte, a phosphine-based additive represented by Formula 1, and a solvent. In Formula 1, n1 to n3 may each independently be 0 to 5, andR1 to R3 may each independently be hydrogen, a halogen, a nitrile group, a nitro group, an amine group, a substituted or unsubstituted C1 to C10 alkyl group, a substituted or unsubstituted C1 to C10 alkoxy group, a substituted or unsubstituted aryl group, or a substituted or unsubstituted C5 to C14 heteroaryl group. According to one or more embodiments of the present disclosure, a method for producing a positive electrode slurry for an all-solid-state battery includes mixing a positive electrode active material, a conductive material, a binder, a sulfide-based solid electrolyte, a phosphine-based additive represented by Formula 1, and a solvent. In Formula 1, n1 to n3 may each independently be 0 to 5, andR1 to R3 may each independently be hydrogen, a halogen, a nitrile group, a nitro group, an amine group, a substituted or unsubstituted C1 to C10 alkyl group, a substituted or unsubstituted C1 to C10 alkoxy group, a substituted or unsubstituted aryl group, or a substituted or unsubstituted C5 to C14 heteroaryl group. According to one or more embodiments of the present disclosure, an all-solid-state battery includes a positive electrode, a negative electrode, and a solid electrolyte layer between the positive electrode and the negative electrode, and the positive electrode may include a positive electrode current collector and a positive electrode active material layer on the positive electrode current collector. The positive electrode active material layer may be formed by using the positive electrode slurry produced according to the method of the present disclosure. BRIEF DESCRIPTION OF THE DRAWINGS The accompanying drawings are included to provide a further understanding of the present disclosure, and are incorporated in and constitute a part of this disclosure. The drawings illustrate embodiments of the present disclosure and, together with the description, serve to explain principles of the present disclosure. The above and other aspects, features, and advantages of certain embodiments of the present disclosure will be more apparent from the following description taken in conjunction with the accompanying drawings. In the drawings: FIG. 1 is a cross-sectional view of an all-solid-state battery according to one or more embodiments of the present disclosure;FIG. 2 is a cross-sectional view of an all-solid-state battery according to one or more embodiments of the present disclosure;FIGS. 3 and 4 are respectively a plan view and a cross-sectional view of an all-solid-state battery according to one or more embodiments of the present disc