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    Structure–property correlations and magnetoelectric response of lead-free BNT–BCTS/CZFMO composite ceramics
    (2026-06-01)
    Kornphom, Chittakorn
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    Sonchaopri, Nutkamon
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    Yimsabai, Sununta
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    Yotthuan, Surirat
    ;
    Jantaratana, Pongsakorn
    Lead-free multiferroic composite ceramics have garnered increasing attention as an eco-friendly alternative for magnetoelectric (ME) devices. In this work, (100-x) [0.93(Bi<inf>0.5</inf>Na<inf>0.5</inf>TiO<inf>3</inf>) 0.07(Ba<inf>0.945</inf>Ca<inf>0.055</inf>Ti<inf>0.91</inf>Sn<inf>0.09</inf>O<inf>3</inf>)]/xCo<inf>0.6</inf>Zn<inf>0.4</inf>Fe<inf>1.7</inf>Mn<inf>0.3</inf>O<inf>4</inf> composite ceramics, abbreviated as (100-x) BNT-BCTS/xCZFMO were synthesized via a solid-state combustion route. Analysis of XRD data using the Rietveld method confirmed the coexistence of rhombohedral and tetragonal perovskite (BNT–BCTS) phases and a cubic spinel (CZFMO) phase without additional impurity phases. The 0–3 connectivity was verified using SEM/EDS, PFM, and MFM measurements, confirming discrete CZFMO magnetic grains are embedded within a continuous BNT–BCTS piezoelectric matrix. Williamson–Hall (W–H) analysis, treated as a semi-quantitative approach due to fitting limitations in the multiphase composite system, suggested a composition-dependent microstrain trend. The reduced microstrain at intermediate CZFMO contents was consistent with enhanced crystallite growth, improved densification, and the maximum magnetoelectric response. The composition with x = 20 exhibits the highest relative density (~ 98.14%), the highest saturation magnetization (M<inf>s</inf> = 6.55 emu/g), and the maximum magnetoelectric coefficient (α<inf>ME</inf> = 7.92 mV cm<sup>−1</sup> Oe<sup>−1</sup>), showing higher ME coefficients than many previously reported lead-free composites. This work demonstrates the potential of BNT–BCTS/CZFMO composites for multifunctional electronic devices, including magnetic sensors, energy harvesters, and magnetoelectric transducers.
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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
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    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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    High-performance triboelectric and piezoelectric nanogenerator enabled by BF-BT-NZN multifunctional ceramic filler
    (2025-10-01)
    Sumang, Rattiphorn
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    Jantaratana, Pongsakorn
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    Charoonsuk, Thitirat
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    Vittayakorn, Naratip
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    Bongkarn, Theerachai
    The development of efficient and flexible energy-harvesting materials is essential for advancing self-powered electronic devices. In this study, we report the fabrication of flexible composite films by incorporating (1-x)(0.75BiFeO<inf>3</inf>-0.25BaTiO<inf>3</inf>)-xNd(Zn<inf>0.67</inf>Nb<inf>0.33</inf>)O<inf>3</inf>,abbreviated as (BF-BT-NZN), ceramic powder into a PDMS matrix, with filler contents ranging from 5 to 25 wt%. The optimized 10 wt% composite film demonstrated a maximum output voltage of 112.24 V and a current of 5.69 µA approximately 11 and 18 times higher than pure PDMS, respectively. Following a poling treatment, the output further increased to 149.54 V and 10.71 µA. The film exhibited excellent flexibility and durability, enabling practical applications such as powering LEDs, a digital watch, and charging capacitors. These results highlight the potential of BF-BT-NZN/PDMS composites as high-performance materials for wearable energy-harvesting applications.
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    Electric and magnetic properties of multiferroic CZFMO doped BNLTBKTBaT composite ceramics prepared via the solid-state combustion method
    (2025-07-01)
    Klinbanmor, Metarsit
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    Thatawong, Bhoowadol
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    Somsri, Widchaya
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    Prasertpalichat, Sasiphon
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    Vittayakorn, Naratip
    The present research work describes in detail investigations of the multiferroic properties of (1-x) (0.85Bi<inf>0.5</inf>Na<inf>0.475</inf>Li<inf>0.025</inf>TiO<inf>3</inf>-0.11Bi<inf>0.5</inf>K<inf>0.5</inf>TiO<inf>3</inf>-0.04BaTiO<inf>3</inf>)-xCo<inf>0.6</inf>Zn<inf>0.4</inf>Fe<inf>1.7</inf>Mn<inf>0.3</inf>O<inf>4</inf> [(1-x)BNLTBKTBaT-xCZFMO]; x = 0, 0.05, 0.10, 0.15 and 0.20 composite ceramics, synthesized by the solid-state combustion technique. The effect of increasing x content on the phase structure, microstructure, electrical and magnetic properties of (1-x)BNLTBKTBaT-xCZFMO composite ceramics was investigated. X-ray diffraction patterns of the BNLTBKTBaT sample showed a pure perovskite phase (rhombohedral and tetragonal structures). When CZFMO was added, the XRD patterns showed a co-structure between perovskite and cubic spinel ferrite structures. The composite grains were composed of large and small sizes, which were composed of mainly the elements of BNLTBKTBaT and CZFMO, respectively. As x increased, the average grain size of the larger grains increased, and the smaller grains got smaller. The density decreased from 5.54 to 4.61 g/cm<sup>3</sup> as x increased. Increasing the amount of CZFMO in BNLTBKTBaT also resulted in a decrease in the dielectric constant (ε<inf>r</inf>) and the remnant polarization (P<inf>r</inf>), with the leakage current observed at x = 0.20. The saturation magnetization (M<inf>s</inf>) and the magnetoelectric coupling coefficient (α<inf>E</inf>) increased with increased x. It was found that x = 0.15 gave the optimal electric, magnetic, and magnetoelectric properties (ε<inf>r</inf> = 425, P<inf>r</inf> = 1.64 μC/cm, M<inf>s</inf> = 1.1948 emu/g and α<inf>E</inf> = 4.88 mV/cm-Oe), which makes the composite potentially more applicable for information technology and spintronics devices.
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    Improved Dielectric, Magnetic, and Multiferroic Properties of (Bi0.5Na0.5)0.7La0.3(Ti0.7Fe0.3)O3 Ceramics Synthesis by the Solid-State Combustion Technique
    (2025-06-01)
    Kornphom, Chittakorn
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    Somsri, Widchaya
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    Prasertpalichat, Sasipohn
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    Thatawong, Bhoowadol
    ;
    Kruea-In, Chatchai
    Lead-free (Bi<inf>0.5</inf>Na<inf>0.5</inf>)<inf>0.7</inf>La<inf>0.3</inf>(Ti<inf>0.7</inf>Fe<inf>0.3</inf>)O<inf>3</inf> ceramics (abbreviated as BNLTF) are synthesized by the solid-state combustion technique using glycine as fuel. The effect of the firing temperature (calcined between 700 and 800 °C for 2 h and sintered between at 800 and 900 °C for 2 h) on the phase structure, microstructure, electrical, and magnetic properties is investigated. Pure BNLTF powders are obtained with a calcination temperature of 750 °C for 2 h and the crystal size increases from 47 to 62 nm when the calcination temperature increases from 700 to 800 °C. All sintered BNLTF ceramics show a pure perovskite structure with a rhombohedral phase. The average grain size increases with increasing sintering temperatures. A well-packed microstructure with the highest density (5.98 g cm<sup>−3</sup>), good dielectric properties at room temperature (ε<inf>r</inf> ≈ 589 and tanδ ≈ 0.572), soft ferroelectric behavior, and excellent magnetic properties (M<inf>s</inf> ≈ 0.091 emu g<sup>−1</sup>, M<inf>r</inf> ≈ 0.0026 emu g<sup>−1</sup>) is obtained from the ceramic sintered at 875 °C for 2 h. The multiferroic BNLTF ceramic sintered at 875 °C has a maximum magnetoelectric coupling coefficient (α<inf>E</inf> ≈ 2.08 mV cm<sup>−1</sup> Oe<sup>−1</sup>) when the magnetic field is near 4500 Oe.
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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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    Vittayakorn, Naratip
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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.
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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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    Vittayakorn, Naratip
    ;
    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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    ELECTRIC AND MAGNETIC PROPERTIES OF Ni0.475Zn0.475Li0.025Al0.025Fe2O4 DOPED (Bi0.5Na0.5)0.94Ba0.06TiO3 CERAMICS PREPARED BY THE SOLID-STATE COMBUSTION METHOD
    (2025-01-01)
    Pattanakasem, Wiwat
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    Sookboon, Chirarat
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    Somsri, Widchaya
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    Vittayakorn, Naratip
    ;
    Pinitsoontorn, Supree
    In this study, we synthesized (1-x)((Bi<inf>0.5</inf>Na<inf>0.5</inf>)<inf>0.94</inf>Ba<inf>0.06</inf>TiO<inf>3</inf>)-x Ni<inf>0.475</inf>Zn<inf>0.475</inf>Li<inf>0.025</inf>Al<inf>0.025</inf>Fe<inf>2</inf>O<inf>4</inf> [(1-x)BNBT-xNZLAF] ceramics with x= 0, 0.05, 0.10, 0.15, and 0.20 using the solid-state combustion method. The phase formation, microstructure, and dielectric, ferroelectric, ferromagnetic, and magnetoelectric properties were investigated. BNBT and NZLAF powders were calcined at 750°C and 900°C for 2 h., respectively. The calcined powders were then mixed in various ratios to produce (1-x)BNBT-xNZLAF composites, which were sintered at 1125°C for 2 h. X-ray diffraction analysis indicated that undoped BNBT ceramics exhibited a typical perovskite structure with coexisting rhombohedral (R) and tetragonal (T) phases. With increasing NZLAF content, the cubic spinel (C) phase emerged with the R and T perovskite phases. Rietveld refinement indicated a higher percentage of the C phase as x increased. When x increased from 0 to 0.10, the average grain size and density increased (from 1.0 to 9.8 m and 5.45 to 5.61 g/cm3, respectively) followed by a drop at higher NZLAF levels. Doping BNBT ceramics with NZLAF resulted in a reduction in the dielectric constant (εr), dielectric loss (tan δ), and remnant polarization (Pr). The undoped BNBT ceramic showed a saturated P-E hysteresis loop, while NZLAF doped ceramics exhibited unsaturated P-E loops and increased leakage current. Magnetic measurements showed a transition from diamagnetic to ferromagnetic behavior with NZLAF doping. As x increased, the remnant magnetization (Mr), saturation magnetization (Ms), and magnetoelectric coefficient also increased (Mr0.058 emu/g, Ms3.594 emu/g, and MEcoefficient 2.64 mV/cm•Oe at x=0.25). These results suggest that NZLAF-doped BNBT ceramics hold potential for multiferroic material applications.