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<p>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<sub>0.5</sub>Na<sub>0.5</sub>TiO<sub>3</sub>) 0.07(Ba<sub>0.945</sub>Ca<sub>0.055</sub>Ti<sub>0.91</sub>Sn<sub>0.09</sub>O<sub>3</sub>)]/xCo<sub>0.6</sub>Zn<sub>0.4</sub>Fe<sub>1.7</sub>Mn<sub>0.3</sub>O<sub>4</sub> 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 <i>x</i> = 20 exhibits the highest relative density (~ 98.14%), the highest saturation magnetization (<i>M</i><sub><i>s</i></sub> = 6.55&#xa0;emu/g), and the maximum magnetoelectric coefficient (α<sub>ME</sub> = 7.92&#xa0;mV&#xa0;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.</p>

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Structure–property correlations and magnetoelectric response of lead-free BNT–BCTS/CZFMO composite ceramics

  • 期刊论文

  • 发表日期：

    2026年6月30日

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  • Chittakorn Kornphom,
  • Nutkamon Sonchaopri,
  • Sununta Yimsabai,
  • Surirat Yotthuan,
  • Pongsakorn Jantaratana,
  • Supree Pinitsoontorn,
  • Naratip Vittayakorn,
  • Aphiwat Pankaew,
  • Theerachai Bongkarn

摘要

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(Bi0.5Na0.5TiO3) 0.07(Ba0.945Ca0.055Ti0.91Sn0.09O3)]/xCo0.6Zn0.4Fe1.7Mn0.3O4 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 (Ms = 6.55 emu/g), and the maximum magnetoelectric coefficient (αME = 7.92 mV cm−1 Oe−1), 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.