In this study, we investigated the microstructure and piezoelectric properties of 0.96(K0.456Na0.536)Nb0.95Sb0.05-0.04 Bi0.5(Na0.82K0.18)0.5ZrO3 (KNNS-BNKZ) ceramics based on one-step and two-step sintering processes. One-step sintering led to significant abnormal grain (AG) growth at temperatures above 1,085 °C. With increasing sintering temperature, piezoelectric and dielectric properties were enhanced, resulting in a high d33 = 506 pC/N for one-step specimen sintered at 1,100 °C (one-step 1,100 °C specimen). However, for one-step 1,115 °C specimen, a slight decrease in d33 was observed, emphasizing the importance of a high tetragonal (T) phase fraction for superior piezoelectric properties. Achieving a relative density above 84 % for samples sintered by the one-step sintering process was challenging. Conversely, two-step sintering significantly improved the relative density of KNNS-BNKZ ceramics up to 96 %, attributed to the control of AG nucleation in the first step and grain growth rate control in the second step. The quantity of AG nucleation was affected by the duration of the first step, determining the final microstructure. Despite having a lower T phase fraction than that of the one-step 1,100 °C specimen, the two-step specimen exhibited higher piezoelectric coefficients (d33 = 574 pC/N and kp = 0.5) than those of the one-step 1,100 °C specimen due to its higher relative density. Performance evaluation of magnetoelectric composite devices composed of one-step and twostep specimens showed that despite having a higher g33, the magnetoelectric composite with the one-step 1,100 °C specimen exhibited the lowest magnetoelectric voltage coefficient, due to its lowest kp. This study highlights the essential role of phase fraction and relative density in enhancing the performance of piezoelectric materials and devices, showcasing the effectiveness of the two-step sintering process for controlling the microstructure of ceramic materials containing volatile elements.

Pb(Zr,Ti)O3 (PZT) is used for the various piezoelectric devices owing to its high piezoelectric properties. However, lead (Pb), which is contained in PZT, causes various environment contaminations. (K,Na)NbO3 (NKN) is the most well-known candidate for a lead-free composition to replace PZT. A single crystal has excellent piezoelectric-properties and its properties can be changed by changing the orientation direction. It is hard to fabricate a NKN single crystal due to the sodium and potassium. Thus, (Na,K)NbO3-Ba(Cu,Nb)O3 (NKN-BCuN) is chosen to fabricate the single crystal with relative ease. NKNBCuN pellets consist of two parts, yellow single crystals and gray poly-crystals that contain copper. The area that has a large amount of copper particles may melt at low temperature but not the other areas. The liquid phase may be responsible for the abnormal grain growth in NKN-BCuN ceramics. The dielectric constant and tan δ are measured to be 684 and 0.036 at 1 kHz in NKN-BCuN, respectively. The coercive field and remnant polarization are 14 kV/cm and 20 μC/cm2.