Piezoelectric Properties and Microstructure of (K,Na)NbO3– KTiNbO5 Composite Lead-Free Piezoelectric Ceramic

We developed a (K,Na)NbO3-based lead-free piezoelectric ceramic with a KTiNbO5 system, (K1−xNax)0.86Ca0.04Li0.02Nb0.85O3−δ–KTiNbO5–BaZrO3–Co3O4–Fe2O3–ZnO (KNN–NTK composite). This KNN–NTK composite exhibits a very dense microstructure, and kp = 0.52, ε33T/ε0 = 1600, and d33 = 252 pC/N. We found that a portion of the KTiNbO5 converted into K2(Ti,Nb,Co,Zn)6O13 and/or CoZnTiO4. We were able to reproducibly prepare granulated powder of KNN–NTK in batches of 100 kg using a spray-dryer. In addition, we performed a detailed investigation of the microstructure of KNN–NTK composite. The results show that a tetragonal and an orthorhombic phase coexist in a main KNN phase over a wide range of 0.56 ≤ x ≤ 0.75. The granular nanodomains of the orthorhombic phase dispersed within the tetragonal matrix in the KNN phase. A maximum value of kp = 0.56 occurred for x = 0.56. The Na fraction x corresponding to maximum kp was also the minimum x required to generate the orthorhombic phase. We conclude that the KNN–NTK composite exhibits excellent piezoelectric properties because of the two-phase coexisting state. This gentle phase transition of KNN–NTK composite seems to be a relaxor, but the diffuseness degree γ = 1.07 suggests otherwise