Lithium-stuffed garnet electrolytes with secondary phase inclusions

A composition comprising:

• a primary cubic phase lithium-stuffed garnet characterized by the chemical formula LiALaBAlCM″DZrEOF, wherein 5<A<8, 1.5<B<4, 0.1<C<2, 0≤D<2;
• 1<E<3, 10<F<13, and M″ is selected from the group consisting of Mo, W, Nb, Y, Ta, Ga, Sb, Ca, Ba, Sr, Ce, Hf, and Rb;
• a secondary phase inclusion in the primary cubic phase lithium-stuffed garnet;
• wherein:
• the primary cubic phase lithium-stuffed garnet is present at about 70-99.9 vol % with respect to the volume of the composition;
• and
• the secondary phase inclusion is present at about 30-0.1 vol % with respect to the volume of the composition.

A process of making a composition, wherein the compositions comprises:

• a primary cubic phase lithium-stuffed garnet characterized by the chemical formula LiALaBAlCM″DZrEOF, wherein 5<A<8, 1.5<B<4, 0.1<C<2, 0≤D<2;
• 1<E<3, 10<F<13, and M″ is selected from the group consisting of Mo, W, Nb, Y, Ta, Ga, Sb, Ca, Ba, Sr, Ce, Hf, and Rb;
• a secondary phase inclusion in the primary cubic phase lithium-stuffed garnet;
• wherein:
• the primary cubic phase lithium-stuffed garnet is present at about 70-99.9 vol % with respect to the volume of the composition;
• and
• the secondary phase inclusion is present at about 30-0.1 vol % with respect to the volume of the composition;
• the process comprising the following steps:
• (a) providing a mixture of chemical precursors to the mixture, wherein the amount of Al in the mixture exceeds the solubility limit of Al in LLZO;
• and
• (b) calcining the mixture by heating it to at least 800° C.

A green film comprising a primary cubic phase lithium-stuffed garnet characterized by the chemical formula LiALaBAlCM″DZrEOF, wherein 5<A<8, 1.5<B<4, 0.1<C<2, 0≤D<2;

• 1<E<3, 10<F<13, and M″ is selected from the group consisting of Mo, W, Nb, Y, Ta, Ga, Sb, Ca, Ba, Sr, Ce, Hf, and Rb;
• a secondary phase inclusion in the primary cubic phase lithium-stuffed garnet;
• wherein:
• the primary cubic phase lithium-stuffed garnet is present in the multiphase thin film solid-state electrolyte at about 70-99.9 vol % with respect to the volume of the multiphase thin film electrolyte;
• and
• the secondary phase inclusion is present in the multiphase thin film solid-state electrolyte at about 30-0.1 vol % with respect to the volume of the multiphase thin film electrolyte.