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It is a very difficult work to sinter K0.5Na0.5NbO3 (KNN)-based materials with good reduction resistance in strong reducing atmosphere. 0.945K0.48Na0.52Nb0.96Ta0.04O3-0.055BaZrO3 + 0.03ZrO2 + y mol%MnO (KNNT-0.055BZ + 0.03Zr + yMn) ceramics sintered in reducing atmosphere were prepared successfully by conventional solid-state reaction methods. MnO dopant increases grain size at y = 5-8 due to strong lattice distortion and then decreases grain size at y = 9 due to much Mn4Nb2O9 accumulated at the grain boundary. MnO dopant as an excellent sintering aid can effectively reduce volatilization of alkali metal by decreasing the sintering temperature (Tsinter). Reducing alkali metal volatilization can greatly reduce oxygen vacancies and improve piezoelectric properties. MnO dopant can improve the anti-reduction properties. The KNNT-0.055BZ + 0.03Zr + yMn ceramics at y = 6-9 show outstanding anti-fatigue of unipolar piezoelectric strain under the synergistic effect of reduced oxygen vacancies due to reduced volatilization and increased grain size. Piezoelectric properties and temperature stability of KNNT-0.055BZ + 0.03Zr ceramics sintered in reducing atmosphere are improved simultaneously by MnO dopant. Optimum inverse piezoelectric coefficient (d*33) of ceramics at y = 8 reaches up to 480 pm/V under low driving electric field E = 20 kV/cm at room temperature, and its temperature stability of d*33 reaches 158 ℃. It will be an excellent lead-free material candidate for the preparation of multilayer piezoelectric actuators co-fired with nickel electrode.
It is a very difficult work to sinter K0.5Na0.5NbO3 (KNN)-based materials with good reduction resistance in strong reducing atmosphere. 0.945K0.48Na0.52Nb0.96Ta0.04O3-0.055BaZrO3 + 0.03ZrO2 + y mol%MnO (KNNT-0.055BZ + 0.03Zr + yMn) ceramics sintered in reducing atmosphere were prepared successfully by conventional solid-state reaction methods. MnO dopant increases grain size at y = 5-8 due to strong lattice distortion and then decreases grain size at y = 9 due to much Mn4Nb2O9 accumulated at the grain boundary. MnO dopant as an excellent sintering aid can effectively reduce volatilization of alkali metal by decreasing the sintering temperature (Tsinter). Reducing alkali metal volatilization can greatly reduce oxygen vacancies and improve piezoelectric properties. MnO dopant can improve the anti-reduction properties. The KNNT-0.055BZ + 0.03Zr + yMn ceramics at y = 6-9 show outstanding anti-fatigue of unipolar piezoelectric strain under the synergistic effect of reduced oxygen vacancies due to reduced volatilization and increased grain size. Piezoelectric properties and temperature stability of KNNT-0.055BZ + 0.03Zr ceramics sintered in reducing atmosphere are improved simultaneously by MnO dopant. Optimum inverse piezoelectric coefficient (d*33) of ceramics at y = 8 reaches up to 480 pm/V under low driving electric field E = 20 kV/cm at room temperature, and its temperature stability of d*33 reaches 158 ℃. It will be an excellent lead-free material candidate for the preparation of multilayer piezoelectric actuators co-fired with nickel electrode.
The work was supported by the National Postdoctoral Program for Innovative Talents (Grant No. BX20190158), National Natural Science Foundation of China (Grant Nos. 52032005 and 51672148), and the Shuimu Tsinghua Scholar.
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