Multilayer Actuator Composed of PZN–PZT and PZN–PZT/Ag Fabricated by Co-Extrusion Process

A multilayer ceramic actuator composed of piezoelectrically active Pb(Zn_1/3Nb_2/3)_0.2–Pb(Zr_0.5Ti_0.5)O_0.8 (PZN–PZT) layers and electrically conducting PZN–PZT/Ag layers was fabricated by the co-extrusion process. For the piezoelectric layers, PZN–PZT, which is sinterable at a low temperature (900°C), was used. For the conducting layers, a PZN–PZT/Ag composite, made by mixing silver particles with the PZN–PZT matrix, was employed. For the co-extrusion process, piezoelectric and conducting feedrods were made by mixing the PZN–PZT and PZN–PZT/Ag, respectively, with a thermoplastic polymer. The initial feedrods, which were composed of five 3 mm-thick PZN–PZT layers, two 1.5 mm-thick PZN–PZT layers, and six 1 mm-thick PZN–PZT/Ag layers, were co-extruded through a 24 mm × 2 mm reduction die at 105°C to produce continuous multilayered green sheets. The sheets were stacked, warm pressed, and sintered at 900°C for 4 h after binder burnout. The sintered multilayer actuator showed distinct layers without any reaction products or cracks at the interface. The thicknesses of the piezoelectric and conducting layers were about 200 and 70 μm, respectively. The displacement of the multilayer actuator, composed of 40 piezoelectric layers (with a total height of 10.8 mm), was about 10 μm at an applied voltage of 500 V.     

Piezoelectric Multilayer Ceramic/Polymer Composite Transducer with 2–2 Connectivity

A multilayer piezoelectric ceramic/polymer composite with 2–2 connectivity was fabricated by thermoplastic green machining after co-extrusion. The multilayer ceramic body was composed of piezoelectrically active lead zirconate titanate (PZN)–lead zinc niobate (PZN)-lead zirconate titanate (PZT) layers and electrically conducting PZN–PZT/Ag layers. After co-extruding the thermoplastic body, which consisted of five piezoelectric layers interspersed with four conducting layers, it was computer numeric-controlled machined to create periodic channels within it. Following binder burnout and sintering, an 18 vol% array of 190 μm thin PZT slabs with a channel size of 880 μm was fabricated. The channels were filled with epoxy in order to fabricate a PZN–PZT/epoxy composite with 2–2 connectivity. The piezoelectric coefficient (effective d ₃₃) and hydrostatic figure of merit ( d _h× g _h) of the PZN–PZT/epoxy composite were 1200 pC/N and 20 130 × 10⁻¹⁵ m²/N, respectively. These excellent piezoelectric characteristics as well as the relatively simple fabrication procedure will contribute in widening the application range of the piezoelectric transducers.     

Piezoelectric Lead Zirconate Titanate Ceramic Fiber/Polymer Composites

Piezoelectric lead zirconate titanate (PZT) ceramic fiber/polymer composites were fabricated by a novel technique referred to as "relic" processing. Basically, this involved impregnating a woven carbon-fiber template material with PZT precursor by soaking the template in a PZT stock solution. Careful heat treatment pyrolized the carbon, resulting in a PZT ceramic relic that retained the fibrous template form. After sintering, the densified relic was backfilled with polymer to form a composite. Optimized relic processing consisted of soaking activated carbon-fiber fabric twice in an intermediate concentration (405-mg PZT/(1-g solution)) alkoxide PZT solution and sintering at 1285°C for 2 h. A series of piezoelectric composites encompassing a wide range of dielectric and piezoelectric properties was prepared by varying the PZT-fiber orientation and polymer-matrix material. In PZT/Eccogel polymer composites with PZT fibers orientated parallel to the electrodes, K = 75, d ₃₃= 145 pC/N, d _h= 45 ± 5 pC/N, and d _hg_h= 3150 × 10⁻¹⁵ m²/N were measured. Furthermore, in composites with a number of PZT fibers arranged perpendicular to the electroded surfaces, K = 190, d ₃₃= 250 pC/N, d _h= 65 ± 2 pC/N, and d _h g_h= 2600 × 10⁻¹⁵ m²/N.     

Direct Measurement of Piezoelectric Strain Using a Diffraction Grating

Piezoelectric strain under a large de electric field, D ₃₃ is directly measured by using an electrically controllable diffraction (ECD) grating. The ECD grating consists of a lead lanthanum zirconate titanate piezoelectric ceramic with 65 pairs of grooves having 40-μm width and 80-μm period on its surface. The operational principle for the diffraction grating and the procedure for obtaining D ₃₃ are described. D ₃₃ is measured experimentally with a He-Ne 3.39-μm laser, yielding a value of 5.9 × 10⁻⁹ m/V under a dc electric field of 1 kV/mm. This value is discussed along with the piezoelectric constant d ₃₃ calculated from a conventional electrical resonant method.     

Continuous Poling Technique for PZT Fibers

A new technique has been developed for poling long PZT fibers by advancing the fibers along two electrical contacts maintained at the required potential difference. Two ways of maintaining the electrical contact with the ceramic are described, leading to piezoelectric d₃₃ coefficients of 400 to 450×10⁻¹² C/N in poled fibers of PZT-501A. Pre-poled fibers can be used in fabricating ceramic-polymer composites such as triple-pillar configurations with piezoelectric fibers oriented in three perpendicular directions.     

Low-Temperature Sintering of Lead Zinc Niobate–Lead Zirconate Titanate Ceramics Using Nano-Sized Powder Prepared by the Stirred Media Milling Process

Lead zinc niobate–lead zirconate titanate (PZN–PZT) nano-sized powders with a diameter of ∼35 nm were fabricated by a high-energy stirred media mill using 50 μm diameter zirconia beads as the milling media at a rotation speed of 4000 rpm for 1 h. The sintering temperature of PZN–PZT was greatly reduced, and a fully densified bulk body was obtained at only 750°C when stirred media milled nanopowder was used. The control of evaporation of lead oxide was very important to obtain high electrical properties due to the increased surface area of nano-sized powders. The ferroelectric hysteresis, piezoelectric d ₃₃ coefficient, and dielectric properties of sintered ceramics using nanopowder were measured and compared with the values obtained from a sintered specimen using conventional milled powders. Remanent polarization, d ₃₃ coefficient, and relative dielectric constant of 750°C sintered stirred media milled powders containing 2% of excess PbO and 1% of 4PbO–B₂O₃ liquid phase were 10.3 μC/cm², 277 pC/N, and 1310, respectively.     

Lead Zirconate Titanate Fiber/Polymer Composites Prepared by a Replication Process

The woven replication process was used to fabricate lead zirconate titanate (PZT)/polymer composites with 1–3, 2–3, and 3–3 connectivities by starting with novoloid-derived carbon fiber, woven fabric, and nonwoven felt templates, respectively. Activated carbon-fiber template material was impregnated with PZT by soaking it in a solution containing stoichiometric amounts of dissolved lead, zirconium, titanium, and niobium ions. Heat treatment burned out the carbon, leaving a PZT replica with the same form as the template material. Replicas were sintered in a controlled atmosphere and backfilled with an epoxy polymer to form final composites. This method, which is believed to be adaptable for mass production, is capable of producing composites with extremely fine microstructures. Woven composite samples have fiber tow diameters of 200 to 250 μm and spacings between tows of about 150 to 250 μm. Average d ₃₃= 90 pC/N, g ₃₃= 211 mV · m/N, and d_hg_h hydrophone figure of merit of 2100 × 10⁻¹⁵ m²/N values are reported for woven PZT/polymer composites.     

Fabrication and Electrical Properties of Lead Zirconate Titanate Thick Films on Si Substrate by Using Lanthanum Nickelate Buffer Layer

Lead zirconate titanate PbZr_0.53Ti_0.47O₃ (PZT) thick films have been deposited on silicon substrate by modified metallorganic decomposition process. Crack-free PZT films of 8 μm thickness can be obtained by using lanthanum nickelate LaNiO₃ (LNO) as buffer layer. The greater LNO thickness, the greater thickness of crack-free PZT can be obtained. The X-ray diffraction measurements show the films exhibit a single perovskite phase with (110) preferred orientation. SEM measurements showed the PZT thick films have a columnar structure with grain size about 60–200 nm. The thickness dependence of ferroelectric, dielectric, and piezoelectric properties of PZT thick films have been characterized over the thickness range of 1–8 μm. For PZT with thickness of 8 μm, P _r and E _c are 30 μC/cm² and 35 kV/cm, and dielectric constant and dielectric loss are 1030 and 0.031, respectively. The piezoelectric coefficient ( d ₃₃) of PZT with 8 μm thickness is obtained to be 77 pm/V. PZT thick films on LNO-coated Si substrate are potential for MEMS applications.     

Relic Processing of Fine-Scale, Large-Area Piezoelectric Ceramic Fiber/Polymer Composites

Fine-scale, large-area lead zirconate titanate (PZT) ceramic fiber/polymer composites were developed using the relic method. Carbon fabrics were used as a starting template material. These fabrics were soaked in PZT stock solution, stacked, and fired, removing the carbon and resulting in a relic structure identical to that of the original template. The relics were then sintered, backfilled with polymer, polished, and poled, resulting in a piezoelectric ceramic/polymer composite. The processing of the larger-area composites involved scaling up the procedure utilized in the fabrication of the smaller composites. The application of an optimum uniaxial pressure of 580 Pa to the stacks during firing was found to improve the piezoelectric properties and facilitate the increase in sample area. Scale-up to large area was achieved using two approaches: (1) the use of a larger template material, and (2) tiling smaller area relics together in an array configuration. The dielectric and piezoelectric properties of relic composites of 2.5 × 2.5 cm² area with ∼37 vol% PZT were K = 150 ± 8, d₃₃= 180 ± 11 pC/N, d_h= 85 ± 7 pC/N, and d _hg_h= 5525 × 10⁻¹⁵m²/N. The properties of large-area composites were comparable with those of small area.     

Sol–Gel Preparation of Thick PZN–PZT Film Using a Diol-Based Solution Containing Polyvinylpyrrolidone for Piezoelectric Applications

Dense and crack-free lead zinc niobate–lead zirconate titanate (PZN–PZT) films were deposited on silicon and glass substrates by spin coating using a sol containing propanediol and polyvinylpyrrolidone. Single-layer PZN–PZT films as thick as 0.80 μm were deposited by a single spin coating with successive heat treatments at 250° and 700°C. After heat treatment, the films were dense, crack free, and optically transparent. In addition, the crystallographic orientation of the thick film was controllable by adjusting the heat-treatment conditions. The ferroelectric properties of the (111)-oriented film were superior to those of the (100)-oriented film. On the other hand, the piezoelectric and dielectric properties of the (100)-oriented film were better than those of the (111)-oriented film. The piezoelectric coefficients ( d ₃₃) of the PZN–PZT films of 4.0-μm-thickness were 192 and 110 pC/N for the (100)-and (111)-oriented films, respectively.     

Composites of PZT and Epoxy for Hydrostatic Transducer Applications

Composites with 3–1 connectivity for transducer applications were made by embedding extruded PZT rods in an epoxy matrix. The effects of rod diameter, volume fraction of PZT, and composite thickness on the hydrostatic properties of the composites were determined. Due to decoupling of the ₃₃ and ₃₁ coefficients in a composite with 3–1 connectivity, the _n may be enhanced, even in composites of low volume fractions of PZT. Such composites alsojiave a low dielectric permittivity. The combination of high _n values and low ɛ₃₃ value results in a greatly enhanced _n. Composites with 10 vol% PZT were made with values of _h and _h which are, respectively, two times (>80×10 ⁻¹² C/N) and 25 times (>70×10⁻³ (V·m/N) the solid PZT values.     

Effect of a Transverse Tensile Stress on the Electric-Field-Induced Domain Reorientation in Soft PZT: In Situ XRD Study

The effect of a transverse tensile stress on the electric-field-induced 90°-domain reorientation in tetragonal lead zirconate titanate (PZT) near the morphotropic phase boundary was investigated in situ using X-ray diffraction (XRD). The XRD intensity ratio, I ₍₀₀₂₎/ I ₍₂₀₀₎, which represents the ratio of the volume of the c -domains to that of the a -domains on the PZT surface, was examined as a function of the electric field at various stress levels. It was found that a transverse tensile stress changes the electric-field dependence of I ₍₀₀₂₎/ I ₍₂₀₀₎, especially at higher electric fields. Without a transverse tensile stress, I ₍₀₀₂₎/ I ₍₂₀₀₎ began to saturate at E ≈ 800 kV/m. With a transverse tensile stress of 75 MPa, I ₍₀₀₂₎/ I ₍₂₀₀₎ increased with an upward curvature with the electric field, indicating that the transverse tensile stress enhanced the field-induced 90°-domain reorientation, and increased the effective piezoelectric coefficients at larger electric fields. At E = 900 kV/m, the estimated d _31,domain changed from −200 × 10⁻¹² V/m at zero stress, to −350 × 10⁻¹² V/m at 75 MPa.     

Properties of Modified Lead Zirconate Titanate Ceramics Prepared at Low Temperature (800°C) by Hot Isostatic Pressing

High-density lead zirconate titanate (PZT) ceramics were fabricated for the first time at a temperature as low as 800°C via the hot isostatic pressing (HIP) of a PZT powder with a modified composition of 0.92Pb(Zr_0.53Ti_0.47)O₃—0.05BiFeO₃—0.03Ba(Cu_0.5W_0.5)O₃ that contained 0.5 mass% MnO₂. The resultant PZT ceramics exhibited a microstructure that was denser and finer than that of PZT sintered at 935°C, which is the lowest temperature for the densification of the same composition via normal sintering. The relevant dielectric and piezoelectric properties of the HIPed PZT ceramics were as follows: coefficient of electromechanical coupling ( K ₃₁), 31.8%; mechanical quality factor ( Q _m), 1364; piezoelectric constant ( d ₃₁), −73.7 × 10⁻¹² C/N; relative dielectric constant (ɛ₃₃^T/ɛ₀), 633; dielectric loss factor (tan δ), 0.5%; Curie temperature ( T _c), 285°C; and density (ρ), 8.06 g/cm³. In addition to these reasonably good piezoelectric properties, the HIPed PZT exhibited better mechanical properties—particularly, higher fracture strength—than the normally sintered PZT.     

Oxidation Behavior of SiCN–ZrO2 Fiber Prepared from Alkoxide-Modified Silazane

The oxidation behavior of SiCN–ZrO₂ fibers and SiCN at 1350°C are compared. The as-measured parabolic rate constants for the two materials are nearly the same (15–20 × 10⁻¹⁸ m²/s). However, after implementing a correction for the difference in the compositions, the rate constant is 13.2 × 10⁻¹⁸ m²/s for the fiber, and 29.4 × 10⁻¹⁸ m²/s for SiCN. The lower oxidation rate of the fiber is ascribed to the lower carbon content in the fiber material.     

Tribological Behavior of Ti2SC at Ambient and Elevated Temperatures

The tribological properties of Ti₂SC were investigated at ambient temperatures and 550°C against Ni-based superalloys Inconel 718 (Inc718) and alumina (Al₂O₃) counterparts. The tests were performed using a tab-on-disk method at 1 m/s and 3N (≈0.08 MPa). At room temperature, against the superalloy, the coefficient of friction, μ, was ∼0.6, and at ∼8 × 10⁻⁴ mm³·(N·m)⁻¹ the specific wear rate (SWRs), was high. However, against Al₂O₃, at ∼5 × 10⁻⁵ mm³·(N·m)⁻¹ and ∼0.3, the SWRs and μ were significantly lower, which was presumably related to more intensive tribo-oxidation at the contact points. At 550°C, the Ti₂SC/Inc718 and Al₂O₃ tribocouples demonstrated comparable μ's of ∼0.35–0.5 and SWRs of ∼7–8 × 10⁻⁵ mm³·(N·m)⁻¹. At 550°C, all tribosurfaces were covered by X-ray amorphous oxide tribofilms. At present, Ti₂SC is the only member of a family of the layered ternary carbides and nitrides (MAX phases) that can be used as a tribo-partner against Al₂O₃ in the wide temperature range from ambient to 550°C.     

Extrinsic OH− Absorption in Transparent Polycrystalline Lanthana-Doped Yttria

Transparent lanthana-doped yttria fabricated by transient solid second-phase sintering under wet hydrogen typically has a broad absorption band with a peak at 3.08 μm. The absorption band shift observed in samples treated in wet deuterium indicated that the 3.08-μm absorption was due to OH⁻ ions. The diffusion rates of hydrogen defects in lanthana-doped yttria were determined in the temperature range from 1000° to 1400°C. The changes in the concentrations of OH⁻ ions upon anneals were determined by measuring infrared absorbance at 3.08 μm. The diffusion coefficient is 1.3 × 10⁻⁷, 9.9 × 10⁻⁷, and 4.1 × 10⁻⁶ cm²/s at 1000°, 1200°, and 1400°C, respectively, with an activation energy of 140 kJ/mol. Annealing in a controlled oxygen partial-pressure environment can remove the OH⁻ absorption band and bring the total absorption in the 3- to 5-μm range closer to the intrinsic values.     

Ceramic–Ceramic Actuator Composed of Two Piezoelectric Layers with Opposite Poling Directions

A ceramic–ceramic actuator composed of two piezoelectric ceramic layers with opposite poling directions was developed. One layer of the actuator had a high coercive electric field (PZT (Pb(Zr,Ti)O₃)-I; E _c=1.1 kV/mm), while the other had a relatively low coercive electric field (PZT-II; E _c=0.6 kV/mm). The actuator was fabricated by cofiring a green compact composed of the PZT-I powder on top of the PZT-II powder. When an electric field >1.1 kV/mm was applied to the sintered body, the whole specimen was poled in one direction. Subsequently, by applying a field between 0.6 and 1.1 kV/mm, only the PZT-II layer was switched to the other direction. When an electric field was applied to this oppositely poled two-layer specimen, one layer of the specimen expanded while the other layer shrank. As a result of these reverse dilations, the actuator was bent into a dome shape, yielding a large axial displacement at the center. The displacement of this actuator with dimensions of 20 mm (diameter) × 1 mm (thickness) was 16 μm at 0.9 kV/mm.     

Thermal Expansion of Silicon Carbide Monofilaments and Silicon Carbide–Borosilicate Composites

The coefficient of thermal expansion (CTE) of a 140-μm-diameter SiC monofilament was determined to be 6.5 ± 0.5 × 10⁻⁶⁰C⁻¹ in the temperature range 25°–900°C. Heat treatment of the fibers at 1400°C for 90 min resulted in both an increase in the intensities of the SiC peaks and a reduction of their width, indicating some grain growth. Furthermore, heat treatment of the fibers for 2 h at 1600°C in vacuum reduced their CTE to 5.7 × 10⁻⁶⁰C⁻¹. The anomalously high CTE and its decrease upon heat treatment were attributed to the presence of a large fraction of the atoms in the boundaries between the nanometer β-SiC grains. The thermal expansion coefficients of a series of SiC/borosilicate composites were measured as a function of fiber volume fraction in the temperature range 25°–500°C and found to follow the rule of mixtures.     

In-Plane Polarized 0.7Pb(Mg1/3Nb2/3)O3–0.3PbTiO3 Thin Films

Ferroelectric 0.7Pb(Mg_1/3Nb_2/3)O₃–0.3PbTiO₃ (PMN-PT) thin films were deposited on ZrO₂/SiO₂/silicon substrates using a chemical-solution-deposition method. Using a thin PZT film as a seed layer for the PMN-PT films, phase-pure perovskite PMN-PT could be obtained via rapid thermal annealing at 750°C for 60 s. The electrical properties of in-plane polarized thin films were characterized using interdigitated electrode arrays on the film surface. Ferroelectric hysteresis loops are observed with much larger remanent polarizations (∼24 μC/cm²) than for through-the-thickness polarized PMN-PT thin films (10–12 μC/cm²) deposited on Pt/Ti/Si substrates. For a finger spacing of 20 μm, the piezoelectric voltage sensitivity of in–plane polarized PMN-PT thin films was ∼20 times higher than that of through-the-thickness polarized PMN-PT thin films.     

Textured PMN–PT and PMN–PZT

A promising way to improve the performance of piezoelectric ceramics is grain orientation by templated grain growth. In this work lead-based piezoelectric ceramics Pb(Mg_1/3Nb_2/3)_0.68Ti_0.32O₃ (PMN–32PT) and Pb(Mg_1/3Nb_2/3)_0.42(Ti_0.638Zr_0.362)_0.58O₃ (PMN–37PT–21PZ) ceramics were textured via templated grain growth process. For texturization (001)-oriented BaTiO₃ (BT) platelets (approximately 10 μm × 10 μm × 2 μm) were utilized as templates. The texturized ceramics were accomplished by aligning the templates by tape casting. The template growth into the matrix resulted in textured ceramics with Lotgering factors between 0.94 and 0.99 for both compositions. Consequences of the texture are enhanced dielectric and piezoelectric properties. Unipolar strain-field measurements of textured ceramics showed 0.25% strain s ₃₃ at 3 kV/mm. Large signal d ₃₃^* of up to 878 pm/V were determined directly from strain measurements. Compared with randomly oriented ceramics in texturized samples unipolar strain s ₃₃ and large signal d ₃₃^* was enhanced by a factor of up to 1.8.