All-solid-state batteries (ASSBs) will play a crucial role in dealing with the energy crisis and removing dependence on fossil fuels. Solid-state electrolytes are a key component of ASSBs. Energy-efficient and convenient synthesis of solid-state electrolytes will be vital in the creation of ASSBs, yet different solid-state synthesis routes are rarely explored. We have probed various reaction pathways for Li-ion conductor LixLa2/3–xTiO3 (LLTO), which has a bulk ionic conductivity at 10–3 S cm–1 at room temperature. It adopts various perovskite-derivative structures. To explore the energy landscape, we used two-step syntheses to investigate the effect of using different precursors in order to determine if we can find a synthesis at lower temperatures than the single-step route using Li2CO3, La2O3 and TiO3. All of the syntheses at T &lt; 1300 °C failed, but at T = 1300 °C they all succeeded. This indicates that there is an energy barrier that needs to be overcome in order to form the perovskite structure. Furthermore, we have performed DFT calculations which elucidate the barriers that need to be overcome to form the target material. These results not only provide insight into the synthesis of LLTO, but into the solid-state synthesis technique as a whole.

Energy landscape of LixLa2/3–x/3TiO3 (LLTO) synthesis explored via various precursors

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