Solid-state electrolyte and method of manufacture thereof

Abstract

A method of manufacturing a solid-state electrolyte including: providing a solvent; dissolving a precursor compound including lithium, a precursor compound including lanthanum, and a precursor compound including zirconium in the solvent to provide a precursor composition, wherein a content of lithium in the precursor composition is greater than a stoichiometric amount; spraying the precursor composition onto a heated substrate to form a film; and heat-treating the film at 300° C. to 800° C. to manufacture the solid state electrolyte, wherein the solid-state electrolyte includes Li (7-x) Al x/3 La 3 Zr 2 O 12 wherein 0≤x≤1, and wherein the solid state electrolyte is in a form a film having a thickness of 5 nanometers to 1000 micrometers.

1 .- 20 . (canceled) 
     
     
         21 . A solid state electrolyte film, comprising:
 cubic Li (7-x) Al x/3 La 3 Zr 2 O 12  wherein 0≤x≤1, and   wherein a thickness of the film is 5 nanometers to 1000 micrometers.   
     
     
         22 . The solid state electrolyte film of  claim 21 , wherein the film has a thickness of 0.1 to 10 micrometers. 
     
     
         23 . The solid state electrolyte film of  claim 21 , wherein a content of the cubic Li (7-x) Al x/3 La 3 Zr 2 O 12  is 50 to 100 weight percent, based on a total weight of the solid state electrolyte film. 
     
     
         24 . The solid state electrolyte film of  claim 21 , wherein a content of the cubic Li (7-x) Al x/3 La 3 Zr 2 O 12  is 80 to 100 wt %, based on a total weight of the solid state electrolyte film. 
     
     
         25 . The solid state electrolyte film of  claim 23 , further comprising tetragonal Li (7-x) Al x/3 La 3 Zr 2 O 12 , and
 wherein a content of the tetragonal Li (7-x) Al x/3 La 3 Zr 2 O 12  is greater than 0 weight percent to 50 weight percent, based on a total weight of the solid state electrolyte film.   
     
     
         26 . The solid state electrolyte film of  claim 23 , further comprising amorphous Li (7-x) Al x/3 La 3 Zr 2 O 12 . 
     
     
         27 . The solid state electrolyte film of  claim 26 , wherein
 a content of the cubic Li (7-x) Al x/3 La 3 Zr 2 O 12  is 70 to 95 weight percent, and   a content of the amorphous Li (7-x) Al x/3 La 3 Zr 2 O 12  is 10 to 30 weight percent, each based on a total content of the solid state electrolyte film.   
     
     
         28 . The solid state electrolyte film of  claim 23 , further comprising tetragonal Li (7-x) Al x/3 La 3 Zr 2 O 12  and amorphous Li (7-x) Al x/3 La 3 Zr 2 O 12 . 
     
     
         29 . The solid state electrolyte film of  claim 28 , wherein
 a content of the cubic Li (7-x) Al x/3 La 3 Zr 2 O 12  is 70 to 95 weight percent,   a content of the tetragonal Li (7-x) Al x/3 La 3 Zr 2 O 12  is greater than 0 weight percent to 50 weight percent, and   a content of the amorphous Li (7-x) Al x/3 La 3 Zr 2 O 12  is 10 to 30 weight percent, each based on a total content of the solid state electrolyte film.   
     
     
         30 . The solid state electrolyte film of  claim 21 , wherein the film has a porosity of 0 to 10%, when determined by scanning electron microscopy. 
     
     
         31 . The solid state electrolyte film of  claim 21 , wherein the film has a surface roughness of 0.1 to 50 micrometers. 
     
     
         32 . The solid state electrolyte film of  claim 21 , wherein a defect content of the film is 0 to 5 percent, based on a total area of the film. 
     
     
         33 . A lithium battery comprising the solid state electrolyte film of  claim 21  in at least one of a positive electrode, a separator, or a negative electrode. 
     
     
         34 . The lithium battery of  claim 33 , wherein the separator is between the positive electrode and the negative electrode. 
     
     
         35 . The lithium battery of  claim 34 , wherein the separator comprises a microporous polymeric film and the solid state electrolyte film on the microporous polymeric film. 
     
     
         36 . The lithium battery of  claim 33 , wherein the positive electrode comprises a positive electrode active material and a liquid electrolyte.