Bimodal-Structured 0.9KNbO3-0.1BaTiO3 Solid Solutions with Highly Enhanced Electrocaloric Effect at Room Temperature

0.9KNbO3-0.1BaTiO3 ceramics, with a bimodal grain size distribution and typical tetragonal perovskite structure at room temperature, were prepared by using an induced abnormal grain growth (IAGG) method at a relatively low sintering temperature. In this bimodal grain size distribution structure, the extra-large grains (~10–50 μm) were evolved from the micron-sized filler powders, and the fine grains (~0.05–0.35 μm) were derived from the sol precursor matrix. The 0.9KNbO3-0.1BaTiO3 ceramics exhibit relaxor-like behavior with a diffused phase transition near room temperature, as confirmed by the presence of the polar nanodomain regions revealed through high resolution transmission electron microscope analyses. A large room-temperature electrocaloric effect (ECE) was observed, with an adiabatic temperature drop (ΔT) of 1.5 K, an isothermal entropy change (ΔS) of 2.48 J·kg−1·K−1, and high ECE strengths of |ΔT/ΔE| = 1.50 × 10−6 K·m·V−1 and ΔS/ΔE = 2.48 × 10−6 J·m·kg−1·K−1·V−1 (directly measured at E = 1.0 MV·m−1). These greatly enhanced ECEs demonstrate that our simple IAGG method is highly appreciated for synthesizing high-performance electrocaloric materials for efficient cooling devices.