Abstract
The ionic conductivity of Li6Y(BO3)3 (LYBO) was enhanced by the substitution of tetravalent ions (Zr4+ and Ce4+) for Y3+ sites through the formation of vacancies at the Li sites, an increase in compact densification, and an increase in the Li+-ion conduction pathways in the LYBO phase. As a result, the ionic conductivity of Li5.875Y0.875Zr0.1Ce0.025(BO3)3 (ZC-LYBO) reached 1.7 × 10−5 S cm−1 at 27 °C, which was about 5 orders of magnitude higher than that of undoped Li6Y(BO3)3. ZC-LYBO possessed a large electrochemical window and was thermally stable after cosintering with a LiNi1/3Mn1/3Co1/3O2 (NMC) positive electrode. These characteristics facilitated good reversible capacities in all-solid-state batteries for both NMC positive electrodes and graphite negative electrodes via a simple cosintering process.
Highlights
The steady evolution of new crystal systems with high ionic conductivities has recently heightened expectations for the realisation of all-solid-state batteries (ASSBs).[1]
The lattice distortion by doping the tetravalent ion is supressed; the lattice distortion in Ce-doped Li5.975Y0.975Ce0.025(BO3)[3] (U 1⁄4 0.02354 deg2) is closer to that in undoped Li6Y(BO3)[3] (U 1⁄4 0.01488 deg2) than that in Zr-doped Li5.975Y0.975Zr0.025(BO3)[3] (U 1⁄4 0.119 deg2), as can be con rmed in Table S1.† Considering the conductivities shown in Table S3,† that of the LYBO-type structure is drastically enhanced by 0.025 Ce4+ doping (Li5.975Y0.975Ce0.025(BO3)[3]; s 1⁄4 6.9 Â 10À7 S cmÀ1 at 27 C), which is due to the formation of vacancies at Li sites in the structure and the increase in compact densi cation, as discussed above
Zr4+-ion doping exerts three types of effects that enhance the conductivity of the LYBO-type structure: (1) the formation of vacancies at Li sites, (2) an increase in compact densi cation, and (3) an increase in the Li+-ion conduction pathways in the LYBO phase associated with structural distortion
Summary
The steady evolution of new crystal systems with high ionic conductivities has recently heightened expectations for the realisation of all-solid-state batteries (ASSBs).[1]. We prepared tetravalent ion (Zr4+ and Ce4+)-doped LYBO-type materials and con rmed an ionic conductivity enhancement to z10À5 S cmÀ1 at 27 C.
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