Solid electrolyte for all solid-state lithium-ion battery and manufacturing method therefor
地域：
Cheonan-si
摘要
The method for manufacturing a solid electrolyte using an LLZ material for a lithium-ion battery comprises the steps of: providing a starting material in which lanthanum nitrate [La(NO3)3.6H2O] and zirconium nitrate [ZrO(NO3)2.6H2O] are mixed at a mole ratio of 3:2; forming an aqueous solution by dissolving the starting material; forming a precipitate by putting ammonia, which is a complex agent, and sodium hydroxide, which adjusts the pH of a reactor, into the aqueous solution, mixing the same, and then co-precipitating the mixture; forming a primary precursor powder by cleaning, drying and pulverizing the precipitate; forming a secondary precursor powder by mixing lithium powder [LiOH.H2O] with the primary precursor powder and ball-milling the mixture so as to solidify the lithium; and forming a solid electrolyte powder by heat-treating the secondary precursor powder.
說明書
The present application is a divisional application of U.S. patent application Ser. No. 14/902,488, filed on 31 Dec. 2015, and titled “Solid Electrolyte for All Solid-State Lithium-Ion Battery and Manufacturing Method Therefor”, which is a National Stage entry of International Patent Application No. PCT/KR2014/005739, filed on 27 Jun. 2014, which is specifically incorporated by reference herein for all that it discloses or teaches. The present application further claims priority to Korean Patent Application No. 10-2013-0078499 filed 4 Jul. 2013, which is also specifically incorporated by reference herein for all that it discloses or teaches.
The present invention relates to an electrolyte for an all-solid-state battery, which is a solid electrolyte for a lithium-ion battery and a method of manufacturing the same capable of synthesizing an LLZ material that is a garnet-structure nano solid electrolyte having high ion conductivity and an excellent electrochemical potential window, and a method of manufacturing the same.
As the exhaustion of fossil fuel and environment issues have been rising in prominence recently, there is a growing interest in new renewable energy and power storage systems. Accordingly, studies on secondary batteries are actively being conducted, while multiple technical problems happen.
權(quán)利要求
What is claimed is:1. A method of manufacturing a solid electrolyte for a lithium-ion battery, the method comprising:providing a starting material in which lanthanum nitrate [La(NO3)3.6H2O] and zirconium nitrate [ZrO(NO3)2.6H2O] are mixed at a molar ratio of 3:2; forming an aqueous solution by dissolving the starting material; forming a precipitate by adding a complex agent including ammonium hydroxide (NH4OH) to the aqueous solution; adding sodium hydroxide (NaOH) to the aqueous solution to adjust pH in a reactor, followed by mixing and co-precipitation of the aqueous solution; forming a primary precursor powder by washing, drying and pulverizing the precipitate; and forming a secondary precursor powder by mixing and ball-milling the primary precursor powder with lithium powder [LiOH.H2O], wherein the secondary precursor powder undergoes a heat treatment to form a heat-treated solid electrolyte powder having a composition of LixLayZrzO12, where x is 6 moles to 9 moles, y is 2 moles to 4 moles, and z is 1 mole to 3 moles. 2. The method of claim 1 , further comprising:forming the heat-treated solid electrolyte powder into a pellet sheet; and heat-treating the pellet sheet to change the heat-treated solid electrolyte powder to a crystal structure in which a cubic structure predominates. 3. The method of claim 1 ,wherein the heat-treated solid electrolyte powder is changed to a crystalline structure in which one of a cubic structure and a tetragonal structure predominates depending on a temperature of the heat treatment. 4. The method of claim 1 ,wherein a temperature of the heat treatment is 600° C. to 1200° C., and the heat-treated solid electrolyte powder has a structure in which a cubic structure coexists with a tetragonal structure or one of the cubic structure and the tetragonal structure predominates. 5. The method of claim 1 ,wherein a temperature of the heat treatment is 700° C. to 800° C., and the heat-treated solid electrolyte powder is changed into a material in which a complete cubic structure or tetragonal structure predominates by calcination at 1200° C. for 2 hours to 8 hours. 6. The method of claim 5 , wherein the heat-treated solid electrolyte powder is changed into a material having a predominating cubic structure and a fine structure with a high density of 90% or higher by calcination at 1200° C. for 5 hours. 7. The method of claim 1 ,wherein a temperature of the heat treatment is approximately 900° C., and the heat-treated solid electrolyte powder is manufactured by calcination at approximately 900° C. for 10 hours or longer. 8. The method of claim 1 ,wherein a temperature of the heat treatment is approximately 900° C., and the heat-treated solid electrolyte powder is manufactured by calcination at approximately 900° C. for 2 hours to 10 hours. 9. The method of claim 8 , wherein the heat-treated solid electrolyte powder has a predominating tetragonal structure and a high-density fine structure with a relative density of 60% or higher by calcination at approximately 900° C. for 5 hours. 10. The method of claim 1 , wherein the complex agent is a 5 N ammonium hydroxide solution, and the sodium hydroxide is added to the aqueous solution such that the aqueous solution has a pH of 10 to 11. 11. The method of claim 10 , wherein the mixing of the aqueous solution is performed by titration with the starting material added at 4 mL/min simultaneously with titration of the complex agent added at 4 mL/min. 12. The method of claim 10 , wherein the sodium hydroxide is a 1 M solution and is automatically titrated based on a pH change, wherein the reactor is a co-precipitation reactor with co-precipitation proceeding. 13. The method of claim 1 , further comprising:putting the heat-treated solid electrolyte powder into a uniaxial compression mold for molding the heat-treated solid electrolyte powder; compressing the uniaxial compression mold; and heat-treating a pellet formed in the compressed uniaxial compression mold at a temperature of the heat treatment to form a high-density fine structure. 14. The method of claim 13 , wherein the heat-treated pellet changes to a cubic structure or a tetragonal structure at a calcination temperature that is the same as or higher than the heat treatment temperature.
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