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With the aid of neutron diffraction and electrochemical impedance spectroscopy, we have demonstrated the effect of the increase in lithium concentration and distribution on Li‐ion conductivity. This has been done through the synthesis of a layered oxide Li₂(La_0.75Li_0.25)(Ta_1.5Ti_0.5)O₇, with the so‐called Ruddlesden‐Popper type structure, where bilayer stacks of (Ta/Ti)O₆octahedra are separated by lithium ions, located in inter‐stack spaces. There are also intra‐stack spaces that are occupied by a mixture of La and Li, as confirmed by neutron diffraction. The distribution of lithium over both inter‐ and intra‐stack positions leads to the enhancement of Li‐ion conductivity in Li₂(La_0.75Li_0.25)(Ta_1.5Ti_0.5)O₇compared to Li₂La(TaTi)O₇, which has a lower concentration of lithium ions, located only in inter‐stack spaces. The analyses of real and imaginary components of electrochemical impedance data confirm the enhanced mobility of ions in Li₂(La_0.75Li_0.25)(Ta_1.5Ti_0.5)O₇. While the Li‐ion conductivity needs further improvement for practical applications, the success of the strategy implemented in this work offers a useful methodology for the design of layered ionic conductors.

 

Multifunctional materials that are capable of facilitating multiple electrocatalytic processes are highly desirable. This work reports the observation of bifunctional electrocatalytic properties for water‐splitting in layered oxides, featuring 2‐dimensional layers of octahedrally coordinated transition metals separated by alkaline‐earth or rare‐earth metals. Remarkably, these materials are able to catalyze both half‐reactions of water‐splitting,i. e., oxygen‐evolution reaction (OER) and hydrogen‐evolution reaction (HER). Electrical charge‐transport studies of SrLaFe_1‐xCo_xO_4‐δin a wide range of temperatures, 25 to 800 °C, indicate semiconducting behavior for all three compounds, where there is a systematic increase in electrical conductivity as a function of temperature. The end member of the series, SrLaCoO_4‐δ, exhibits the highest electrical charge transport and best electrocatalytic activity toward both OER and HER. This catalyst also features the highest degree of polyhedral distortion as well as the presence of oxygen‐vacancies. In addition, the transition metals in this material have a favorable electronic configuration for enhanced electrocatalytic activity.

 

Materials with low thermal conductivity are essential to providing thermal insulation to many technological systems, such as electronics, thermoelectrics and aerospace devices. Here, we report ultra-low thermal conductivity of two oxide materials. Sr 2 FeCoO 6−δ has a perovskite-type structure with oxygen vacancies. It shows a thermal conductivity of 0.5 W m −1 K −1 , which is lower than those reported for perovskite oxides. The incorporation of calcium to form Ca 2 FeCoO 6−δ , leads to a structural change and the formation of different coordination geometries around the transition metals. This structural transformation results in a remarkable enhancement of the thermal insulation properties, showing the ultra-low thermal conductivity of 0.05 W m −1 K −1 , which is one of the lowest values found among solid materials to date. A comparison to previously reported perovskite oxides, which show significantly inferior thermal insulation compared to our materials, points to the effect of oxygen-vacancies and their ordering on thermal conductivity.