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Isolation of a Ferroelectric Intermediate Phase in Antiferroelectric Dense Sodium Niobate CeramicsYang, Bin; Zhang, Hangfeng; Yan, Haixue; Abrahams, Isaac (Elsevier, 2019-08-22)Switchable ferroelectric/antiferroelectric ceramics are of significant interest for high power energy storage applications. Grain size control of this switching is an interesting approach to controlling polarization and hence dielectric properties. However, the use of this approach in technologically relevant ceramics is hindered by difficulty in fabricating dense ceramics with small grain sizes. Here an intermediate polar ferroelectric phase (P21ma) has been isolated in dense bulk sodium niobate ceramics by grain size control through spark plasma sintering methods. Our findings, supported by XRD, DSC, P-E (I-E) loops and dielectric characterization, provide evidence that the phase transition from the antiferroelectric (AFE) R-phase, in space group Pnmm, above 300 C, to the AFE P-phase, in space group Pbma, at room temperature, always involves the polar intermediate P21ma phase and that the P21ma to Pbma transition can be suppressed by reducing grain size.
Perovskite Srx(Bi1-xNa0.97-xLi0.03)0.5TiO3 ceramics with polar nano regions for high power energy storageWu, Jiyue; Mahajan, Amit; Riekehr, Lars; Zhang, Hangfeng; Yang, Bin; Meng, Nan; Zhang, Zhen; Yan, Haixue; Queen Mary University of London; Uppsala University; University of Chester (Elsevier, 2018-06-06)Dielectric capacitors are very attractive for high power energy storage. However, the low energy density of these capacitors, which is mainly limited by the dielectric materials, is still the bottleneck for their applications. In this work, lead-free single-phase perovskite Srx(Bi1-xNa0.97-xLi0.03)0.5TiO3 (x=0.30 and 0.38) bulk ceramics, prepared using solid-state reaction method, were carefully studied for the dielectric capacitor application. Polar nano regions (PNRs) were created in this material using co-substitution at A-site to enable relaxor behaviour with low remnant polarization (Pr) and high maximum polarization (Pmax). Moreover, Pmax was further increased due to reversible electric field induced phase transitions. Comprehensive structural and electrical studies were performed to confirm the PNRs and the reversible phase transitions. And finally a high energy density (1.70 J/cm3) with an excellent efficiency (87.2%) was achieved using the contribution of PNRs and field-induced transitions in this material, making it among the best performing lead-free dielectric ceramic bulk material for high energy storage.
Structure and dielectric properties of double A-site doped bismuth sodium titanate relaxor ferroelectrics for high power energy storage applicationsYang, Bin; Zhang, Hangfeng; Fortes, Dominic; Yan, Haixue; Abrahams, Isaac; University of Chester; Queen Mary University of London; Rutherford Appleton LaboratoryThe structural and dielectric properties of barium/strontium substituted Bi0.5Na0.5TiO3 were examined in compositions of general formula (Ba0.4Sr0.6TiO3)x(Bi0.5Na0.5TiO3)1-x. An average classic cubic perovskite structure is maintained from x = 0.5 to 1.0. The temperature dependence of dielectric properties of studied compositions shows relaxor-ferroelectric behaviour attributed to the existence of polar nano-regions. Ferroelectric measurements under variable temperature demonstrated two transitions from normal ferroelectric to relaxor-ferroelectric and relaxor-ferroelectric to paraelectric, at the dipole freezing temperature, Tf, and temperature of maximum permittivity, Tm, respectively. The obtained value of Tf coincides with the onset of linear thermal expansion of the cubic unit cell parameter obtained from high resolution powder neutron diffraction data. Careful analysis of the neutron diffraction data revealed no significant change in the average cubic structure from -263 to 150 C. However, changes in the Gaussian variance component of the neutron peak shape, reveal three distinct regions with transitions at about -100 and 100 C corresponding to the beginning and end of the dielectric dispersion seen in the permittivity and loss spectra. This variation in the Gaussian variance parameter is attributed to the activity of the polar nano-regions. The composition (Ba0.4Sr0.6)0.5(Bi0.5Na0.5)0.5TiO3 was found to exhibit the maximum recoverable energy storage density, with a value of 1.618 J cm-3 and 76.9% storage efficiency at a field of 17 kV mm-1.