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    PHASE FORMATION AND ELECTRICAL PROPERTIES OF BCLTS CERAMICS SYNTHESIZED VIA THE SOLID-STATE COMBUSTION TECHNIQUE
    (2025-01-01)
    Somsri, Widchaya
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    Charoenthai, Nipaphat
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    Sutthapintu, Aekkasit
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    Noisak, Jitrawan
    ;
    Lead-free Ba<inf>0.93</inf>Ca<inf>0.04</inf>La<inf>0.03</inf>Ti<inf>0.90</inf>Sn<inf>0.10</inf>O<inf>3</inf> (BCLTS) ceramics were fabricated via solid-state combustion technique. The BCLTS powders were calcined in a temperature range of 1075-1175°C for 2h and sintered in a temperature range of 1350-1450°C for 2h. The BCLTS powders exhibited a pure perovskite phase when calcined above 1150°C. All BCLTS ceramic samples displayed a perovskite structure with coexisting cubic and tetragonal phases, with a secondary phase observed only at 1450°C. The growth of grain size was increased with increasing sintering temperature (0.42 to 0.65 μm.). The highest dielectric and ferroelectric properties (ε<inf>r</inf>=3047, tan δ<inf>r</inf> = 0.029, P<inf>max</inf> = 9.52 μC/cm<sup>2</sup>, P<inf>r</inf> = 0.48 μC/cm<sup>2</sup>, E<inf>c</inf>= 1.04 kV/cm) were obtained at the sintering temperature of 1400°C. The altered phase structure in this research, compared to earlier studies, results in distinct outcomes for the dielectric and ferroelectric properties.
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    ELECTRIC AND MAGNETIC PROPERTIES OF Ba0.97Ca0.03Ti0.94Sn0.06O3-Mn0.85Ni0.15Zn0.15Fe2O4 MULTIFERROIC CERAMIC COMPOSITES FABRICATED VIA THE SOLID-STATE COMBUSTION TECHNIQUE
    (2025-01-01)
    Sonchaopria, Nutkamon
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    Meechob, Jirayut
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    Thatawong, Bhoowadol
    ;
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    Pinitsoontorn, Supree
    Multiferroic composites with the general formula (1-x)(Ba0.97Ca0.03Ti0.94Sn0.06O3)-x(Mn0.85Ni0.15Zn0.15Fe2O4) (BCTS/MNZF) (x = 0.1, 0.2, 0.3, 0.4, and 0.5) were prepared using the solid-state combustion method. The structure, morphology, dielectric, ferroelectric, magnetic, and magnetoelectric properties were analyzed. The samples were sintered at 1,300ºC for 2 h. The X-ray Diffraction (XRD) patterns revealed tetragonal perovskite, orthorhombic perovskite, and cubic spinel structures corresponding to the BCTS and MNZF phases. Secondary phases (Mn2O3 and SnO) appeared in the sintered samples with x>0.2. Increasing MNZF content enhanced ferrite grain growth in the composites. The dielectric constant showed an overall decreasing trend with increasing MNZF content, with a smaller effect at lower frequencies. At lower frequencies, the dielectric constant declined with increasing frequency before stabilizing around 10 kHz. As ferrite content increased, the density, dielectric constant, and magnetoelectric coefficient (αME) decreased from 5.66 to 5.12 g/cm³, 1388 to 862, and 7.24 to 4.05 mV/cm·Oe, respectively. While the saturation magnetization (Ms) rose substantially from 0.75 to 13.14 emu/g. These findings offer valuable insights into enhancing lead-free multiferroic composite ceramics for targeted applications in magnetoelectric devices.
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    ELECTRICAL AND MAGNETIC PROPERTIES OF MULTIFERROIC Co0.6Zn0.4Fe1.7Mn0.3O4 DOPED 0.99Bi0.47Na0.47Ba0.06TiO3-0.01Ba(Sn0.70Nb0.24)O3 CERAMICS SYNTHESIZED VIA THE SOLID-STATE COMBUSTION TECHNIQUE
    (2025-01-01)
    Luangpangai, Anupong
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    Chuai, Phomphon
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    Rittidech, Aurawan
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    Pinitsoontorn, Supree
    ;
    Jantaratana, Pongsakorn
    Multiferroic (1-x)[0.99Bi<inf>0.47</inf>Na<inf>0.47</inf>Ba<inf>0.06</inf>TiO<inf>3</inf>-<inf>0.01</inf>Ba(Sn<inf>0.70</inf>Nb<inf>0.24</inf>)O<inf>3</inf>]-xCo<inf>0.6Z</inf>n<inf>0.4</inf>Fe<inf>1.7</inf>Mn<inf>0.3</inf>O<inf>4</inf> (abbreviated as BNBT-BSN-xCZFMO) ceramics with x ranging from 0 to 0.20 were fabricated using the solid-state combustion technique. The effect of varying BNBT-BSN: CZFMO ratios on the phase structure, microstructure, electrical and magnetic properties was investigated. X-ray diffraction (XRD) analysis of pure BNBT-BSN showed a perovskite structure with rhombohedral and tetragonal phases. The doped BNBT-BSN-xCZFMO ceramics displayed coexisting rhombohedral, tetragonal, and cubic spinel phases, with the cubic spinel phase increasing when the CZFMO content increased. In addition, the XRD peaks shifted to higher angles as the CZFMO content increased, indicating a decrease in lattice parameters. The dielectric constant decreased with higher CZFMO content and higher frequencies. The pure BNBT-BSN ceramic exhibited a saturated P-E loop with a Pmax of 33.2 µC/cm<sup>2</sup>, Pr of 26.1 µC/cm<sup>2</sup>, and an Ec of 14.5 kV/cm. With increased CZFMO content, non-saturated and bloated P-E loops with lower Pmax, Pr, and Ec were observed, implying a rise in the leakage current. The addition of CZFMO induced ferromagnetic behavior in the ceramics, leading to an increase in Ms and a reduction in Hc as CZFMO content increased. The magnetoelectric coupling coefficient of BNBT-BSN-xCZFMO ceramics continuously increased with higher CZFMO content.
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    PHASE FORMATION AND ELECTRICAL PROPERTIES OF Ba0.91Ca0.09Ti0.916Sn0.084O3-0.1WT%ZnO -0.1WT%MnO2 LEAD-FREE FERROELECTRIC CERAMICS SYNTHESIZED VIA THE SOLID-STATE COMBUSTION METHOD
    (2025-01-01)
    Yimsabai, Sununta
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    Somsri, Widchaya
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    Charoenthai, Nipaphat
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    Suthapintu, Aekasit
    This work investigated the effect of firing temperatures on the phase formation, microstructure, and electrical properties of Ba0.91Ca0.09Ti0.916Sn0.084O3-0.1wt%ZnO-0.1wt%MnO2 (BCTS-ZnMn) lead-free ferroelectric ceramics synthesized via the solid-state combustion method. Glycine was used as fuel to reduce the synthesis temperature. The samples were calcined at temperatures from 1050 to 1250°C (in 50°C increments) for 3 h and sintered from 1250 to 1450°C (in 50°C increments) for 3 h. A pure perovskite phase was found in the powders calcined above 1100°C. The phase structure, microstructure, dielectric and ferroelectric properties of the ceramics were examined. The X-ray diffraction (XRD) analysis for the ceramics revealed the presence of tetragonal (T) and orthorhombic (O) phases in all the ceramics. The average particle size and average grain size increased with increasing firing temperatures. The density, dielectric constant at the Curie temperature (ɛc), Pr and Ps tended to increase with increasing sintering temperatures, up to 1400°C, and then decreased at 1450°C. The ceramic sintered at 1400°C exhibited the highest density (5.89 g/cm3), dielectric response (ɛc = 13324) and good ferroelectric behavior (Pr = 8.67 μC/cm2, Ps = 17.92 μC/cm2 and Ec = 0.99 kV/cm).
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    The role of γ-C2H5NO2 as a new transient liquid phase in cold sintering process of BaTiO3 composites
    (2024-07-01)
    Noisak, Jitrawan
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    Ieamviteevanich, Pimchanok
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    Charoonsuk, Thitirat
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    Pakawanit, Phakkhananan
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    Pinpru, Nattapong
    Dielectric materials, such as barium titanate (BT)-based materials, have excellent dielectric properties but require high temperatures (above 1300 °C) for ceramic fabrication, leading to high costs and energy loss. The cold sintering process (CSP) offers a solution to these issues and is gaining worldwide attention as an innovative fabrication route. In this work, we proposed an alternative organic ferroelectric phase, gamma-glycine (γ-GC), which acts as a transient liquid phase to fabricate high-density composites with barium titanate (BT) at low temperatures through CSP. Our findings show that the density of 15γ-GC/85BT reached 96.7%±1.6% when it was sintered at 120 °C for 6 h under 10 MPa uniaxial pressure. Scanning electron microscopy-energy dispersive X-ray spectroscopy (SEM-EDS) mappings of the composite suggested that γ-GC completely underwent the precipitation–dissolution process and, therefore, filled between BT particles. Moreover, X-ray diffraction (XRD) and Fourier-transform infrared spectroscopy (FTIR) confirmed the preservation of γ-GC without undesired phase transformation. In addition, the ferroelectric and dielectric properties of γ-GC/BT composites have been reported. The high dielectric constant (ε<inf>r</inf>) was 3600, and the low dielectric loss (tanδ) was 1.20 at 200 °C and 100 kHz for the 15γ-GC/85BT composite. The hysteresis loop showed a remanent polarization (P<inf>r</inf>) of 0.55 µC·cm<sup>-2</sup> and a coercive field (E<inf>c</inf>) of 7.25 kV·cm<sup>-1</sup>. Our findings reaffirmed that an organic ferroelectric material (γ-GC) can act as a transient liquid phase in a CSP that can successfully and sustainably fabricate γ-GC/BT composites at low temperatures while delivering outstandingly high performance.
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    Optimal Bi₀.₈Ba₀.₂FeO₃ doping in Bi₀.₅(Na₀.₇₇K₀.₂₀Li₀.₀₃)₀.₅TiO₃ multiferroic ceramics synthesized by the solid-state combustion technique
    (2025-12-01)
    Thawong, Pichittra
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    Prasertpalichat, Sasipohn
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    Suriwong, Tawat
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    Pinitsoontorn, Supree
    ;
    Jantaratana, Pongsakorn
    (1-x)Bi<inf>0.5</inf>(Na<inf>0.77</inf>K<inf>0.20</inf>Li<inf>0.03</inf>)<inf>0.5</inf>TiO<inf>3</inf>-xBi<inf>0.8</inf>Ba<inf>0.2</inf>FeO<inf>3</inf> ((1-x)BNKLT-xBBF) ceramics with x = 0-0.4 were synthesized by the solid-state combustion technique. X-ray diffraction (XRD) analysis confirmed a pure perovskite structure with coexisting rhombohedral and tetragonal phases. Rietveld refinement revealed that the unit cell volume increased with increased x due to the substitution of smaller Bi<sup>3+</sup> and Ti<sup>4+</sup> ions by larger Ba<sup>2+</sup> and Fe<sup>3+</sup> ions at the A- and B-sites, respectively. The average grain size and measured density also increased with increasing x, while the resistivity decreased. At room temperature, (1-x)BNKLT-xBBF ceramics with x = 0.2–0.4 exhibited multiferroic behavior, characterized by ferroelectric and ferromagnetic hysteresis loops. The 0.8BNKLT-0.2BBF ceramic exhibited the most favorable properties, including: the highest relative density (95.48%), the highest dielectric constant and low dielectric loss at room temperature (ε<inf>R</inf> = 1746 and tan δ<inf>R</inf> = 0.0296), good ferroelectric properties (P<inf>r</inf>=6.46 µC/cm<sup>2</sup> and E<inf>c</inf>=11.84 kV/cm) and good ferromagnetic properties (M<inf>r</inf>=0.002 emu/g, H<inf>c</inf>=110 Oe and α<inf>E</inf> = 1.092 mV/Oe·cm). These results indicate that 0.8BNKLT-0.2BBF has the potential for applications in lead-free, room temperature multiferroic applications.
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    Multifunctional properties of Mn and Fe co-doped lead-free BCT perovskite ceramics synthesized via solid-state combustion
    (2025-10-01)
    Kornphom, Chittakorn
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    Sonchaopri, Nutkamon
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    Yimsabai, Sununta
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    Jantaratana, Pongsakorn
    ;
    Pinitsoontorn, Supree
    There is a growing demand to improve the performance of multiferroic lead-free ceramics. Good ferroelectric and magnetic properties are key parameters for achieving high magnetoelectric coupling (ME). In this work, Mn and Fe were co-doped into lead-free Ba<inf>0.96</inf>Ca<inf>0.04</inf>Ti<inf>(1-x)</inf>(Mn<inf>0.5</inf>Fe<inf>0.5</inf>)<inf>x</inf>O<inf>3</inf> (BCT-xMF) ceramics with 0 ≤ x ≤ 0.030 mol%, synthesized by the solid-state combustion technique. X-ray diffraction (XRD) analysis and Rietveld refinement confirmed the formation of a pure phase with coexisting tetragonal and cubic phases in all compositions. As the Mn/Fe content increased, the percentage of the tetragonal phase decreased while the cubic phase increased, consistent with Raman spectroscopy results. Increasing Mn/Fe content also led to more oxygen vacancies and defects, and a decrease in average grain size. Analysis of the temperature-dependent dielectric constant revealed a reduction in the Curie temperature from 116 to 67 °C, corresponding to the tetragonal-to-cubic phase transformation. The ceramic with x = 0.015 showed the highest dielectric constant at the Curie temperature (ε<inf>c</inf>), maximum saturated polarization (P<inf>s</inf>), remnant polarization (P<inf>r</inf>), saturation magnetization (M<inf>s</inf>), and remnant magnetization (M<inf>r</inf>), with values of 4583, 14.09 μC/cm<sup>2</sup>, 9.31 μC/cm<sup>2</sup>, 0.0127 emu/g, and 0.006 emu/g, respectively. These results indicate that Fe/Mn co-doping into BCT ceramics enhanced both ferroelectric and ferromagnetic properties, resulting in a high magnetoelectric coefficient (α<inf>ME</inf>∼1.27 mV/cm Oe) at room temperature, making these ceramics candidates for multiferroic applications.
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    EFFECT OF (AlNb)4+ B-SITES SUBSTITUTION ON THE PHASE STRUCTURE, MICROSTRUCTURE AND ELECTRICAL PROPERTIES OF Bi0.47Na0.47Ba0.06TiO3 CERAMICS
    (2025-01-01)
    Luangpangai, Anupong
    ;
    Chongsatan, Wistsarut
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    Charoenthai, Nipaphat
    ;
    Chootin, Suphornphun
    ;
    Bi0.47Na0.47Ba0.06Ti1-x(Al0.5Nb0.5)xO3 (abbreviated as BNBT1-xANx) lead-free ceramics (x=0-0.05) were synthesized by the solid-state combustion technique. The effect of (AlNb)<sup>4+</sup> content on the phase structure, microstructure and electrical properties was investigated. A pure perovskite structure was obtained from all specimens. Rietveld refinement revealed coexisting rhombohedral and tetragonal phases in all samples and the tetragonal phase increased with increased AlNb content (x). The morphology of the BNBT1-xANx ceramics displayed nearly round grains and anisotropic grain growth. Average grain size decreased from 1.8 to 0.7 µm when x increased from 0 to 0.05 and the grain size distribution became narrower. The density, maximum dielectric constant and remnant polarization rapidly decreased with increased x. The deterioration of the electrical properties induced by (AlNb)<sup>4+</sup> substitution was due to shifting away from the morphotropic phase boundary (MPB), poor microstructure and low density.
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    Phase structure, microstructure, electrical and energy storage properties of SBNLT lead free ceramics with Zr4+ substituted into B-sites
    (2024-09-01)
    Sinkruason, Thanapon
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    Luangpangai, Anupong
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    Julphunthong, Phongthorn
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    Rittidech, Aurawan
    ;
    Pulphol, Phieraya
    Lead-free (Sr<inf>0.3</inf>Bi<inf>0.35</inf>Na<inf>0.335</inf>Li<inf>0.015</inf>) (Ti<inf>1−x</inf>Zr<inf>x</inf>) O<inf>3</inf> ceramics (SBNLT<inf>1−x</inf>Zr<inf>x</inf>) with x = 0–0.04 were prepared via the solid-state combustion technique using glycine as the fuel. The influence of Zr content on the phase structure, microstructure, electrical properties, and energy storage properties of the SBNLT<inf>1−x</inf>Zr<inf>x</inf> ceramics was examined. The presence of a pure perovskite phase was shown by X-ray diffraction (XRD) patterns, with the coexistence of rhombohedral and tetragonal phases in all samples, as certified by the Rietveld refinement method. Scanning electron microscopy (SEM) was utilized to observe the morphology of the SBNLT<inf>1−x</inf>Zr<inf>x</inf> ceramics, which revealed cube shaped grains with anisotropic growth. Average grain size increased from 2.01 to 2.49 µm when x increased from 0 to 0.01 and then reduced with further increases in Zr content. The maximum dielectric constant dropped from 4667 to 2990 when x increased from 0 to 0.04, caused by a shift from the morphotropic phase boundary (MPB). The maximum polarization (P<inf>max</inf>) of 29.18 µC/cm<sup>2</sup>, energy storage density (W<inf>total</inf>) of 0.851 J/cm<sup>3</sup> and recoverable energy storage (W<inf>rec</inf>) of 0.609 J/cm<sup>3</sup> were achieved when x = 0.02.
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    INFLUENCE OF SINTERING TEMPERATURES ON MULTIFERROIC PROPERTIES OF LEAD-FREE BNT-BT-NZF MULTIFERROIC COMPOSITE FABRICATED VIA THE SOLID-STATE COMBUSTION TECHNIQUE
    (2025-01-01)
    Chongsatan, Wistsarut
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    Boonpluk, Wiranchana
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    Pinitsoontorn, Supree
    ;
    Jantaratana, Pongsakorn
    There has been a growing interest in multiferroics, materials that combine magnetic and electric ordering, over the past few years. This research investigates the influence of sintering temperature (1075-1175°C for 2 hours) on multiferroic properties of 0.7(0.94Bi<inf>0.5</inf>Na<inf>0.5</inf>TiO<inf>3</inf>-0.06BaTiO<inf>3</inf>)-0.3(Ni<inf>0.7</inf>Zn<inf>0.3</inf>Fe<inf>2</inf>O<inf>4</inf>) (BNT-BT-NZF) multiferroic composites, fabricated using solid-state combustion with glycine as a fuel was investigated. The XRD patterns of all ceramics revealed the coexistence of a rhombohedral ferroelectric phase, a tetragonal ferroelectric phase, and a cubic ferromagnetic phase. The average grain size, dielectric constant (ε<inf>r</inf>), dielectric loss (tanδ), remnant polarization (P<inf>r</inf>), and coercive field (E<inf>c</inf>) tended to increase from 0.66 to 2.5μm, 314 to 829, 0.22 to 0.51, 0.36 to 5.82 μC/cm<sup>2</sup>, and 7.05 to 26.96 kV/cm, respectively, with increase of sintering temperature. The composite ceramics exhibited peak saturation magnetization (M<inf>s</inf> ~ 12.21 emu/g) and magnetoelectric (ME) coupling (~ 3.59 mV/cmOe) when sintered at 1150°C.