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CN-122000354-A - Positive electrode slurry for all-solid battery, method for manufacturing the same, and all-solid battery manufactured using the same

CN122000354ACN 122000354 ACN122000354 ACN 122000354ACN-122000354-A

Abstract

Provided are a positive electrode slurry for an all-solid battery, a method for manufacturing the positive electrode slurry, and an all-solid battery. 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

  • WU DAYANG

Assignees

  • 三星SDI株式会社

Dates

Publication Date
20260508
Application Date
20251103
Priority Date
20241104

Claims (20)

  1. 1. A positive electrode slurry, the positive electrode slurry comprising: A positive electrode active material; A conductive material; A binder; sulfide-based solid electrolytes; phosphine-based additive represented by formula 1, and The solvent is used for the preparation of the aqueous solution, 1 (1) , Wherein, in the formula 1, N 1 to n 3 are each independently 0 to 5, and R 1 to R 3 are each independently hydrogen, halogen, nitrile, nitro, amine, substituted or unsubstituted C1 to C10 alkyl, substituted or unsubstituted C1 to C10 alkoxy, substituted or unsubstituted aryl or substituted or unsubstituted C5 to C14 heteroaryl, and Wherein the positive electrode slurry is a positive electrode slurry for an all-solid battery.
  2. 2. The positive electrode slurry of claim 1, wherein the phosphine-based additive comprises at least one selected from the group consisting of triphenylphosphine, 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 (o-tolyl) phosphine, diphenyl (p-tolyl) phosphine, and combinations thereof.
  3. 3. The positive electrode slurry according to claim 1, wherein the amount of the phosphine-based additive is 0.01 to 3 parts by weight based on 100 parts by weight in total of the positive electrode active material, the conductive material, and the binder.
  4. 4. The positive electrode slurry according to claim 1, wherein the amount of the sulfide-based solid electrolyte is 5 parts by weight to 25 parts by weight based on 100 parts by weight in total of the positive electrode active material, the conductive material, and the binder.
  5. 5. The positive electrode slurry according to claim 1, wherein the amount of the solvent is 15 parts by weight to 50 parts by weight based on 100 parts by weight in total of the positive electrode active material, the conductive material, and the binder.
  6. 6. The positive electrode slurry according to claim 1, wherein a weight ratio of the phosphine-based additive to the sulfide-based solid electrolyte is 0.2% to 25%.
  7. 7. The positive electrode slurry according to claim 1, wherein the positive electrode active material comprises a compound represented by formula 2: 2, 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 is at least one element selected from the group consisting of Al, ti, mg, zr, mo and Nb.
  8. 8. The positive electrode slurry of claim 1, wherein the binder comprises a fluoride-based binder.
  9. 9. The positive electrode slurry of claim 1, wherein the conductive material comprises at least one selected from the group consisting of natural graphite, artificial graphite, carbon black, acetylene black, ketjen black, carbon fibers, carbon nanofibers, carbon nanotubes, and combinations thereof.
  10. 10. The positive electrode slurry according to claim 1, wherein the sulfide-based solid electrolyte is a sulfur silver germanium ore-type compound including Li 7- a M a PS 6-c X c , wherein 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. 11. A method, the 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: 1 (1) , Wherein, in the 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 manufacturing a positive electrode slurry for an all-solid battery.
  12. 12. The method of claim 11, wherein the phosphine-based additive comprises at least one selected from the group consisting of triphenylphosphine, 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 (o-tolyl) phosphine, diphenyl (p-tolyl) phosphine, and combinations thereof.
  13. 13. The method of claim 11, wherein the binder comprises a fluoride-based binder, and Wherein the sulfide solid electrolyte is a sulfur silver germanium ore type compound comprising Li 7-a M a PS 6-c X c , wherein a is more than or equal to 0 and less than or equal to 2, c is more than or equal to 0 and less than or equal to 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. 14. The method according to claim 11, wherein the amount of the phosphine-based additive is 0.01 to 3 parts by weight based on 100 parts by weight in total of the positive electrode active material, the conductive material, and the binder.
  15. 15. The method according to claim 11, wherein the amount of the sulfide-based solid electrolyte is 5 parts by weight to 25 parts by weight based on 100 parts by weight in total of the positive electrode active material, the conductive material, and the binder.
  16. 16. The method of claim 11, wherein the weight ratio of the phosphine-based additive to the sulfide-based solid electrolyte is 0.2 to 25.
  17. 17. An all-solid battery, the all-solid battery comprising: a positive electrode, a negative electrode, and a solid electrolyte layer between the positive electrode and the negative electrode, Wherein the positive electrode comprises a positive electrode current collector and a positive electrode active material layer on the positive electrode current collector, and Wherein the positive electrode active material layer is formed by using the positive electrode slurry according to any one of claims 1 to 10.
  18. 18. The all-solid battery according to claim 17, wherein the positive electrode active material layer includes a binder-modified material generated by a reaction between an eluting material of the sulfide-based solid electrolyte and the phosphine-based additive.
  19. 19. The all-solid battery of claim 18, wherein the binder-modifying material comprises at least one selected from the group consisting of substituted or unsubstituted triphenylphosphine sulfide, phosphorus sulfide, lithium sulfide, and combinations thereof.
  20. 20. The all-solid battery according to claim 18, wherein the amount of the binder-modifying material is 0.0001 parts by weight to 1 part by weight based on 100 parts by weight in total of the positive electrode active material, the conductive material, and the binder.

Description

Positive electrode slurry for all-solid battery, method for manufacturing the same, and all-solid battery manufactured using the same The present application claims priority and rights of korean patent application No. 10-2024-0154225 filed at the korean intellectual property office on 4/11/2024, the entire contents of which are incorporated herein by reference. Technical Field One or more embodiments of the present disclosure relate to a positive electrode slurry for an all-solid battery, a method of manufacturing the same, and an all-solid battery manufactured using the same. Background In response to increasing industrial demands, development of batteries having high energy density and enhanced safety has been actively pursued. For example, lithium ion batteries are commercialized not only in the fields of information-related devices and communication devices, but also in the field of automobile industry (e.g., automobiles). Battery safety is particularly important in view of the fact that user safety and/or well-being are important concerns in the automotive industry. Recently, all solid-state batteries in which a liquid electrolyte (solution) is replaced (substituted) with a solid electrolyte have been proposed. Because these batteries do not use flammable organic solvents as a dispersion medium, the risk of fire or explosion is significantly reduced even in the event of a short circuit. Thus, the all-solid-state battery provides significantly improved safety as compared to the related-art lithium ion battery using a liquid electrolyte. Disclosure of Invention One or more aspects of the present disclosure relate to a positive electrode slurry having improved adhesion characteristics and a method for manufacturing the positive electrode slurry. One or more aspects of the present disclosure relate to a positive electrode for an all-solid battery having excellent or suitable performance and an all-solid battery including the positive electrode. Additional aspects will be set forth in part in the description which follows and, in part, will be obvious from the description, or may be learned by practice of the disclosed embodiments as presented. According to one or more embodiments of the present disclosure, a positive electrode slurry for an all-solid 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. 1 (1) In the formula (1) of the present invention, N 1 to n 3 may each independently be 0 to 5, and R 1 to R 3 may each independently be hydrogen, halogen, nitrile, nitro, amine, substituted or unsubstituted C1 to C10 alkyl, substituted or unsubstituted C1 to C10 alkoxy, substituted or unsubstituted aryl or substituted or unsubstituted C5 to C14 heteroaryl. According to one or more embodiments of the present disclosure, a method for manufacturing a positive electrode slurry for an all-solid 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. 1 (1) In the formula (1) of the present invention, N 1 to n 3 may each independently be 0 to 5, and R 1 to R 3 may each independently be hydrogen, halogen, nitrile, nitro, amine, substituted or unsubstituted C1 to C10 alkyl, substituted or unsubstituted C1 to C10 alkoxy, substituted or unsubstituted aryl or substituted or unsubstituted C5 to C14 heteroaryl. According to one or more embodiments of the present disclosure, an all-solid 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 manufactured according to the method of the present disclosure. Drawings The accompanying drawings are included to provide a further understanding of the disclosure, and are incorporated in and constitute a part of this disclosure. The accompanying drawings illustrate embodiments of the present disclosure and, together with the description, serve to explain the principles of the present disclosure. The above and other aspects, features and advantages of certain embodiments of the present disclosure will become more apparent from the following description 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; fig. 3 and 4 are a plan view and a cross-sectional view, respectively, of an all-solid st