Preparation and Piezoelectric Properties of CuO-added(Ag_(0.75)Li_(0.1)Na_(0.1)K_(0.05_)NbO_3 Lead-free Ceramics

CuO-doped（Ag0.75Li0.1Na0.1K0.05）NbO3（ALNKN-xCuO, x = 0.2mol%） lead-free piezoelectric ceramics were prepared by the solid-state reaction method in air atmosphere. The effects of CuO addition on the phase structure, microstructure, and piezoelectric properties of the ceramics were investigated. The experimental results show that the ALNKN ceramics without doping CuO possess rhombohedral phase along with K2NbrO16- type phase and metallic silver phase. For all of the CuO-doped ALNKN ceramics, a pure perovskite structure with the orthorhombic phase was obtained by enclosing the samples in a corundum tube. A homogeneous microstructure with＇the grain size of about 1 ~tm was formed for the ceramics with 0.5mo1% CuO. The grain size increases with increasing amount of CuO. The temperature dependence of dielectric properties indicates that the ferroelectric phase of the ALNKN-xCuO ceramics becomes less stable with the addition of CuO. The ceramics with x = lm01% exhibit relatively good electrical properties along with a high Curie temperature. These results will provide a helpful guidance to preparing other AN-based ceramics by solid-state reaction method in air atmosphere.

Effect of Li content on the microstructure and properties of lead-free piezoelectric(K_(0.5)Na_(0.5))_(1-x)Li_xNbO_3 ceramics prepared by SPS

Lead-free piezoelectric （K0.5sNa0.5）1-xLixNbO3 （x = 0at%-20at%） ceramics were synthesized by spark plasma sintering （SPS） at low temperature and the effects of LiNbO3 addition on its crystal structure and properties were also studied. When the Li content was less than 6at%, a single proveskite phase with the similar structure of （K0.5Na0.5）NbO3 was formed; and a secondary phase with K3Li2Nb5O15 structure was observed in the 6at% 〈 x 〈 20at% compositional range. Furthermore, LiNbO3 existed as the third phase when the Li content was higher than 8at%. The grain sizes increased from 200-500 nm to 5-8 μm when the K3Li2Nb5O15 and LiNbO3 like phases were formed. With increasing Li content, the relative density of the ceramics first decreased from 97% to 93% and then kept constant. The piezoelectric coefficient d33, dielectric constant, and planner electromechanical coupling factor exhibited a decreasing tendency with increasing Li content because of the decrease in density and the formation of the secondary phase such as K3Li2Nb5O15 and LiNbO3. The formation of dense microstructure with a single phase is necessary in improving the properties of the （K0.5Na0.5）1-xLixNbO3 ceramics.

Piezoelectric and dielectric properties of Li_x(K_(0.46)Na_(0.54))_(1-x)Nb_(0.86)Ta_(0.1)Sb_(0.04)O_3 lead-free ceramics

Lead-free piezoelectric ceramics Lix(K0.46Na0.54)1-xNb0.86Ta0.1Sb0.04O3 (with x ranging from 0 to 0.1) were synthesized by conventional solid state sintering method. The effect of cationic substitution of Li for K and Na in the A sites of perovskite lattice on the structure, phase transition behavior and electrical properties were investigated. Morphotropic phase boundaries(MPB) between orthorhombic and tetragonal phase are found in the composition range of 0.06≤x≤0.08. Analogous to Pb(Zr,Ti)O3, the dielectric and piezoelectric properties are enhanced for the composition near the morphotropic phase boundary. The Li0.06(K0.46Na0.54)0.94- Nb0.86Ta0.1Sb0.04O3 ceramics show excellent electrical properties, that is, piezoelectric constant d33=215 pC/N, planar electromechanical coupling factor kp=41%, dielectric constant ε 3T3 /ε0=1 303, and dielectric loss tan δ=2.45%. The results indicate that Lix(K0.46Na0.54)1-x Nb0.86 Ta0.1Sb0.04O3 ceramic is a promising lead-free piezoelectric material.

Microstructure and electrical properties of Ti-modified (Na_(0.5)K_(0.5))(Ti_xNb_(1-x))O_3 lead-free piezoelectric ceramics

Ti-Modified (Na0.5K0.5)(TixNb1-x)O3 (NKNT) piezoelectric ceramics were fabricated by double-layer buried powder process at 1020°C for 2 h. The microstructures,and piezoelectric and dielectric properties of the lead-free NKNT ceramics were investigated. X-ray diffraction re-sults indicated that Ti4+ had diffused into the (Na0.5K0.5)NbO3 lattices to form a solid solution with a perovskite structure. The introducing of Ti into the (Na0.5K0.5)NbO3 solid solution effectively reduced the sintering temperature and...

Effect of doped Mn on piezoelectric properties of (Na_(0.5)Bi_(0.5))_ (0.92)Ba_(0.08)TiO_3 lead-free ceramics

Piezoelectric ceramics (Na0.5Bi0.5) （0.92）Ba0.08TiO3 +x%MnCO3（BNBT-Mn, x=0CD*21.6, mass fraction） were synthesized by conventional solid state reaction. The results show that when the addition of MnCO3 is 0CD*2 1.4%, BNBT-Mn ceramics exhibit a single-phase perovskite structure. With the increase of content of MnCO3, piezoelectric constant and electromechanical coupling factor increase rapidly when x is lower than 0.3. Then they both decrease when x is in the range of 0.3 and 1.6. When x=0.3, piezoelectric constant and electromechanical coupling factor reach the maximum value of 160pC/N and 58.5% respectively, which can improve the temperature stability of BNBT-Mn.

Microstructure,crystalline phase and electrical properties of Li_(0.06)(Na_(0.5)K_(0.5))_(0.94)Nb_(1-2x/5)Mg_xO_3 lead-free piezoelectric ceramics

MgO-modified Li0.06（Na0.5K0.5）0.94NbO3O3 （L6NKN） lead-free piezoelectric ceramics were synthesized by normal sintering at a rela- tively low temperature of 1000℃. The crystalline phase, microstructure, and electrical properties of the ceramics were investigated with a special emphasis on the influence of MgO content. The addition of MgO effectively improves the sintembility of the L6NKN ceramics. X-my diffr cfion analysis indicates that the morphotropic phase boundary （MPB） separating orthorhombic and tetragonal phases for the ceramics lies in the range of Mg doping content （x） from 0.3at% to 0.7at%. High electrical properties of the piezoelectric constant （d33=238 pC/N）, planar electromechanical coupling coefficient （kp=41.5%）, relative dielectric constant （εr=905）, and remanent polarization （Pr=38.3 μC/cm2） are obtained from the specimen with x=0.5at%, which suggests that the Li0.06（Na0.5K0.5）0.94Nb（1-2x/5）MgxO3 （x=0.5at%） ceramic is a promising lead-free piezoelectric material.

Synthesis and Piezoelectric Properties of Lead-free (Bi_(0.5)Na_ (0.5))_ 1-x(Ba_aSr_b)_xTiO_3 Ceramics

A new group of lead-free piezoelectric ceramics,（Bi0.5 Na0.5）1-x（BaaSrb）xTiO3（abbreviated as BNBST[100x-100a/100b],0〈x〈1,a＋b=1）,was synthesized.The ceramics were prepared by conventional ceramic sintering technique,and the ceramics with density of 95% of the theoretical one can be sintered without the atmosphere control during the sintering process.The results of the X-ray diffraction（XRD） data show that the ceramics possess a single perovskite phase.The measurements of dielectric and piezoelectric properties reveal that the ceramics provide relatively high piezoelectric charge constant d33 and high planar electromechanical coupling factor kp.For the BNBST6-95/5 ceramics,d33 is equal to 170pC/N,and kp is equal to 32.0%.The fabrication technique for these ceramics is conventional and stable.

Effects of Na/K ratio on the phase structure and electrical properties of Na_xK_(1-x)NbO_3 lead-free piezoelectric ceramics

Lead-free piezoelectric NaxK1-xNbO3（x = 0.3-0.8）（NKN） ceramics were fabricated by normal sintering at 1060°C for 2 h.Microstructures and electrical properties of the ceramics were investigated with a special emphasis on the influence of Na content.The grain size of the produced dense ceramic was decreased by increasing Na content.A discontinuous change in the space distance was found at the composition close to Na0.7K0.3NbO3 ceramic, which indicates the presence of a transitional composition between two different orthorhombic phases, which is similar to the behavior of morphotropic phase boundary（MPB） in NaxK1-xNbO3 ceramics.Such MPB-like behavior contributes to the enhanced piezoelectric coefficient d33 of 122 pC/N, planar-mode electromechanical coupling coefficient kP of 28.6%, and dielectric constant εr of 703, respectively for the Na0.7K0.3NbO3 ceramic.Cubic temperature TC and the transitional temperature TO-T from orthorhombic to tetragonal phase are observed at around 420°C and 200°C, respectively.

Microstructures and Electrical Properties of Bi_(0.5)-(Na_(1-x-y)K_xLi_y)_(0.5)TiO_3 Lead-free Piezoelectric Ceramics

The microstructures and electrical properties of Bi0.5（Na1-x-yKxLiy）0.5TiO3 lead-free piezoelectric ceramics were studied.These ceramics were prepared by conventional ceramic technique.XRD analysis reveals that the ceramics possess almost pure perovskite phase when y≤0.2.The SEM results show that,with more amounts of Li＋,the crystalline grain growing speed is accelerated,and the sintering temperature can effectively be decreased.The measurements of piezoelectric properties indicate that the ceramics with relatively low amount of Li＋ and high amount of K＋ have comparatively large piezoelectricity.The dielectric measurements show that the ceramics have properties like relaxor ferroelectrics and diffuse phase transition（DPT） at Td and Tc,respectively.The results of ferroelectric measurements reveal the system has relatively higher remanent polarization Pr（27.6 μC/cm2） and lower coercive field Ec（37.5 kV/cm）.

Effects of A-site non-stoichiometry on the structural and electrical properties of 0.96K_(0.5)Na_(0.5)NbO_3-0.04LiSbO_3 lead-free piezoelectric ceramics

Effects of A-site non-stoichiometry on the structural and electrical properties of 0.96K0.5＋xNa0.5＋xNbO3- 0.04LiSbO3 lead-free piezoelectric ceramics were examined for 0 ≤ x ≤0.02. The piezoelectric coefficients exhibited a maximum, d33 = 187 pC/N at x = 0.0075, coinciding with the maximum of the grain size and the apparent density at x = 0.0075. The apparent density and the piezoelectric coefficients decreased with increasing x at higher x which was likely due to the crystal geometrical distortion of 0.96K0.5＋xNa0.5＋xNbO3-0.04LiSbO3. In addition, super-large grains were found and this may be due to liquid phase sintering. Excess （K＋＋Na＋） attracted a sum of space charges to keep the charge neutral, resulting in charge leakage during the course of ceramic polarization, influencing the piezoelectric and ferroelectric properties. These findings are of importance for guiding the design of Ko.sNao.sNbO3-based lead-free ceramics with enhanced electrical properties.

Enhanced Ferroelectric and Converse Piezoelectric Properties of Dense Lead-Free Na_0.4K_0.1Bi_0.5TiO₃Ceramics for Actuator Applications

In this work, lead-free Na0.4Bi0.5 TiO3-K0.1Bi0.5TiO3 (NKBT) piezoelectric ceramics were prepared by the solid-state reaction method and their structural, ferroelectric and dielectric properties were systematically studied. NKBT sintered at 1150℃ for 4 h exhibited highly dense (96% - 98% of the theoretical density) and uniform grains of size 1.1 μm. The coexistence of tetragonal (P4bm) and rhombohedral (R3c) phases due to the presence of morphotrophic phase boundary for the chosen composition has been confirmed by the Rietveld refinement studies. Enhanced ferroelectric properties such as remnant polarization (Pr) and coercive field (EC) are found to be 37 μC/cm2 and 30 kV/cm, respectively. The optimized synthesis procedure for NKBT ceramics resulted in enhanced strain (%) and converse piezoelectric coefficient (d33*) of 0.3 % and 554 pm/V which is attributed to smaller grain size and switching of non 180o domains. NKBT ceramics with such excellent piezoelectric properties can be considered as a promising candidate for actuator applications.

Manufacture and Cytotoxicity of a Lead-free Piezoelectric Ceramic as a Bone Substitute—Consolidation of Porous Lithium Sodium Potassium Niobate by Cold Isostatic Pressing

Aim The piezoelectric properties and cytotoxicity of a porous lead-free piezoelectric ceramic for use as a direct bone substitute were investigated. Methodology Cold isostatic pressing （CIP） was applied to fabricate porous lithium sodium potassium niobate （Li0.06Na0.5K0.44） NbO3 specimens using a pore-forming method. The morphologies of the CIP-processed specimens were characterized and compared to those of specimens made by from conventional pressing procedures. The effects of the ceramic on the attachment and proliferation of osteoblasts isolated from the cranium of 1-day-old Sprague- Dawley rats were examined by a scanning electron microscopy （SEM） and metbylthiazol tetrazolium （MTT） assay. Results The results showed that CIP enhanced piezoelectricity and biological performance of the niobate specimen, and also promoted an extracellular matrix-like topography of it. In vitro studies showed that the CIP-enhanced material had positive effects on the attachment and proliferation of osteoblasts. Conclusion Niobate ceramic generated by CIP shows a promise for being a piezoelectric composite bone substitute.

Influence of Composition on Properties of BNT-BT Lead-Free Piezoceramics

Lead-free piezoelectric ceramics of (Bi1/2Na1/2)TiO3-BaTiO3(BNT-BT) were prepared by the conventional piezoelectric ceramic preparation technique (free air atmosphere sintering). The influence of BaTiO3 additive amount and La2O3 additive amount on the properties of BNT-BT lead-free piezoceramics were investigated. The results show that the dielectric constant(ε) and piezoelectric strain constant(d33) of materials start increasing and then decreasing while BaTiO3 additive amount increasing, the e and d33 of materials have maximum value (ε= 1650, d33 = 120 PC·N -1 ) while x (BaTiO3) =0.06 mol. Theεand d33 of materials start increasing and then decreasing while La2O3 additive amount increasing, the e and d33 of materials have maximum value (ε= 1684, d33 = 153 PC·N-1) while w(La2O3) =0.3% . The influence of La2O3 additive amount on the microstructure of BNT-BT piezoelectric ceramics was analysed by SEM( scanning electron microscope). The influence mechanism of La2O3 additive amount on the properties of BNT-BT piezoelectric ceramics was discussed. The BNT-BT ceramics with optimum comprehensive properties were obtained.

Phase Structure, Microstructure and Electrical Properties of K_xNa_((1-x))NbO_3 Piezoelectric Ceramics with Different K/Na Ratio

The K_xNa_((1-x))NbO_3(x=0.45, 0.46, 0.47, 0.48, 0.49, 0.50) lead-free piezoelectric ceramics was fabricated by conventional solid-state sintering method. It was found that the ratio of alkaline metal would affect the microstructure, bulk density, and optimum sintering temperatures of ceramics. Meanwhile, the electrical properties were also influenced by modulating the K/Na ratio, exhibiting corresponding composition-dependent properties. The optimum electrical properties of K_xNa_((1-x))NbO_3 such as piezoelectric constant d_(33) = 115 pC/N, mechanical quality factor Q_m = 20, Curie temperature Tc = 365 ~oC, ε_(33)~T/ε_0= 588.1, dielectric loss tan δ = 0.024, bulk density(ρ) = 3.08 g/cm^3, remnant polarization(P_r) = 8.87 μC/cm^2 and coercive field(Ec) = 13.79 kV/cm were obtained at x = 0.46.

Effects of Excess Barium on the Structure and Electrical Properties of(Ba,Ca)TiO_3 Piezoelectric Ceramics with High Mechanical Quality Factors

Manganese-doped Ba（0.925）Ca（0.075）TiO3 lead-free piezoelectric ceramics（abbreviated as BCT）with high mechanical quality factor were synthesized by conventional solid-state reaction method.The effects of excess Ba on the crystal structure,microstructure,and electrical properties of the ceramics were systematically investigated.X-ray diffraction and Raman spectra revealed that Ca^2＋ions were pushed from Ba sites to Ti sites of BCT when 1.5 mol%extra Ba^2＋ions were added after sintering.The grain size of the ceramics was decreased by adding extra Ba^2＋ions.The mechanical quality factor and resistivity of the ceramics decreased dramatically when the excess Ba was more than 1.5 mol%.High piezoelectric coefficients（d（33）=150-190 pC/N）and high mechanical quality factors（Qm=1 000-1 200）were obtained in the ceramics when the excess of Ba was between 0.5 mol%and 1 mol%.These results indicated that the properties of BCT ceramics could be tailored by adjusting the content of Ba.

Properties of La_2O_3-Doped PNSZT Piezoelectric Ceramics Having Tetragonal and Rhombohedral Coexistent Phases

The relationship between composition and the electric mechanical properties for La2O3-doped lead niobium stibium zirconate titanate(La2O3-doped PNSZT) piezoelectric ceramics,in which there are tetragonal and rhombohedral coexistent phases, was studied. A series of piezoelectric ceramics with good properties was obtained, having dielectric constants (ε= 1500 ~ 2500), plane electromechanical coupling factor(Kp = 0.45 ~ 0.65), mechanical quality factor( Qm = 500 ~ 1600). These materials are used for making ultrasonic sensor and filter, and marine acoustic launching and receiving device, and so on. It has been explored that the influence of composition on the lattice constant and phase composition of La2O3-doped PNSZT piezoelectric ceramics by XRD(X-ray diffraction) . The character of dielectric constant changing of La2O3-doped PNSZT piezoelectric ceramics before polarization and after polarization was studied. The affecting mechanism about composition on the electric machine properties of phase coexistent La2O3-doped PNSZT piezoelectric ceramics was analyzed and discussed.

Effect of poling condition on piezoelectric properties of (K_(0.5)Na_(0.5))NbO_3 ceramics

The lead-free piezoelectric ceramics (K0.5Na0.5)NbO3 (abbreviated as KNN) with the relative density of 97.6% were synthesized by press-less sintering owing to the careful control of processing conditions. The phase structure of KNN ceramics was analyzed. The results show that the pure perovskite phase with orthorhombic symmetry is in all ceramics specimens. The effect of poling conditions on the piezoelectric properties of KNN ceramics was investigated. The results show that the piezoelectric constant d33 and electromechanical coupling factor kp increase with poling field, poling temperature and poling time increasing, then decrease because of electric broken. Take into account of poling conditions and piezoelectric properties of pure KNN ceramics, the optimum poling conditions for pure KNN ceramics are poling field of 4 kV/mm, poling temperature of 140℃and poling time of 20-25 min.

Piezoelectric Properties of(Na0.5K0.5-xLix)NbO3 Ceramics

Lead-free piezoelectric ceramics （Na0.5K0.5-xLix）NbO3 （x=0.057-0.066） were synthesized by an ordinary sin-tering technique. Substituting Li for K can lead to structural distortion, which improves the Curie temperature （To） greatly. By adding appropriate LiNbO3 content, piezoelectric constant d33 values reach 202-212 pC/N. Electromechanical coefficients of the planar mode reach 44.4%-46.8%. The dielectric loss is below 2.6%, which is much lower than reported （about 50%）. The To of （Na0.5K0.5-xLix）NbO3 （x=0.057-0.066） is in the range of 490-510℃, at least 70℃ higher than that of pure （Na0.5K0.5）NbO3 ceramics. The results show that （Na0.5K0.5-xLix）NbO3 ceramic is a kind of good lead-free high-temperature piezoelectric material.

Influence of CeO_2 doping amount on property of BCTZ lead-free piezoelectric ceramics sintered at low temperature

Ba0.85Ca0.15Ti0.9Zr0.1O3 （BCTZ） lead-free piezoelectric ceramics co-doped with CeO2 （x=0.1 wt.%, 0.2 wt.%, 0.3 wt.%, 0.4 wt.%, 0.5 wt.%） and Li2CO3 （0.6 wt.%） were prepared by conventional solid-state reaction method. Influence of CeO2 doping amount on the piezoelectric properties, dielectric properties, phase composition and microstructure of prepared BCTZ lead-free piezoelectric ceramics doped with Li2CO3 were investigated by X-ray diffraction （XRD） and scanning electron microscopy （SEM） and other analytical methods. The results showed that the sintered temperature of BCTZ lead-free piezoelectric ceramics doped with CeO2 decreased greatly when Li2CO3 doping amount was 0.6 wt.%;a pure perovskite structure of BCTZ lead-free piezoelectric ceramics co-doped with Li2CO3 and CeO2 and sintered at 1050 ℃ could also be obtained. The piezoelectric constant （d33）, the relative permit-tivity （εr） and the planar electromechanical coupling factor （kp） of BCTZ ceramics doped with Li2CO3 increased firstly and then de-creased, the dielectric loss （tanδ） decreased firstly and then increased and decreased at last when CeO2 doping amount increased. The influence of CeO2 doping on the properties of BCTZ lead-free piezoelectric ceramics doped with Li2CO3 were caused by“soft effect”and “hard effect”piezoelectric additive and causing lattice distortion. When CeO2 doping amount （x） was 0.2 wt.%, the BCTZ ceramics doped with Li2CO3 （0.6 wt.%） and sintered at 1050 ℃ possessed the best piezoelectric property and dielectric property with d33 of 436 pC/N, kp of 48.3%,εr of 3650, tanδof 1.5%.