Article(id=1320107639342748304, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1320107605469544753, articleNumber=null, orderNo=null, doi=10.14062/j.issn.0454-5648.20250771, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=null, receivedDate=1761148800000, receivedDateStr=2025-10-23, revisedDate=1772208000000, revisedDateStr=2026-02-28, acceptedDate=null, acceptedDateStr=null, onlineDate=1792667787633, onlineDateStr=2026-10-22, pubDate=1786982400000, pubDateStr=2026-08-18, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1792667787633, onlineIssueDateStr=2026-10-22, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1792667787633, creator=13701087609, updateTime=1792667787633, updator=13701087609, issue=Issue{id=1320107605469544753, tenantId=1146029695717560320, journalId=1263187385517883426, year='2026', volume='54', issue='9', pageStart='2949', pageEnd='3314', issueExtLink='null', onlineDate='null', pubDate='1789833600000', pubDateStr='2026-09-20', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=null, createTime=1792667779556, creator='13701087609', updateTime=1792737576818, updator='13701087609', preIssue=null, nextIssue=null, articleTotal=null, ext={EN=IssueExt(id=1320400356446687492, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1320107605469544753, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1320400356446687493, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1320107605469544753, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null, downloadFileDto=null}, startPage=3123, endPage=3136, ext={EN=ArticleExt(id=1320107639573435025, articleId=1320107639342748304, tenantId=1146029695717560320, journalId=1263187385517883426, language=EN, title=Ferroelectric and Magnetic Properties of BiFeO3-BaTiO3/SrFe12O19 Composite Multiferroic Ceramics, columnId=1263922769897599102, journalTitle=Journal of the Chinese Ceramic Society, columnName=Research Articles, runingTitle=null, highlight=null, articleAbstract=
Introduction

Multiferroic materials, which exhibit two or more primary iron orders (such as ferroelectricity and ferromagnetism), hold a significant potential in sensing and storage applications. BiFeO3 stands as the most representative room-temperature single-phase multiferroic material. Its ferroelectricity originates from lattice distortion caused by the 6s2 lone-pair electrons of Bi3+hybridizing with O 2p, while magnetism arises from Fe—O—Fe super-exchange. However, its narrow bandgap results in high leakage current and coercive field, making ferroelectric characterization challenging. Also, the periodic arrangement of G-type antiferromagnetic structures renders it macroscopically non-magnetic with a weak magnetoelectric coupling. Researchers develop some methods such as ion substitution and process optimization, among which composites with magnetic materials are effective in inducing magnetism and enhancing magnetoelectric coupling. M-type strontium ferrite (i.e., SrFe12O19, abbreviated as SrM) as a typical permanent magnet with high saturation magnetization has attracted attention due to its complex magnetic structure that can induce ferroelectric polarization, but its high leakage current limits its application in electrically controlled magnetism. To address this issue, this study was to introduce SrM into the BiFeO3 matrix to enhance magnetism and magnetoelectric coupling. To overcome the high leakage current of pure BiFeO3, we selected 0.75BiFeO3-0.25BaTiO3 (BFO-BTO) with superior iron-voltage properties as a ferroelectric matrix.We prepared a series of (1-x)(BFO-BTO)/xSrM composite multiferroic ceramics via solid-state reaction and systematically investigated the evolution of their structural, ferroelectric, magnetic, and magnetoelectric coupling properties.

Methods

In this study, (1-x)(BFO-BTO)/xSrM composite ceramics were synthesized by a solid-state reaction method. Bi2O3, Fe2O3, SrCO3, BaCO3, and TiO2 (all with purity ≥99.9%) were used as raw materials. The materials were weighed in stoichiometric proportions after drying and ground in deionized water for 24 h. The slurries were dried and sieved, then subjected to pre-sintering for BFO-BTO at 870 ℃ for 3 h and SrM at 1100 ℃ for 3 h. The resulting powders were mixed proportionally, ground again for 24 h, dried, granulated, and pressed into green bodies (10 mm diameter, 1-2 mm thickness), followed by sintering at 940 ℃ for 3 h. The sintered samples were polished and coated with silver paste, then fired at 700 ℃ for electrodes.

The crystal structure was analyzed by X-ray diffraction (XRD). The surface morphology was determined by scanning electron microscopy (SEM), and the elemental distribution was analyzed by energy dispersive spectroscopy (EDS). After 30 min polarization in a DC electric field of 40 kV/cm, the samples underwent performance testing. The dielectric properties were obtained by an impedance analyzer with a high-temperature testing system. The room-temperature ferroelectric properties were measured by a ferroelectric analyzer. The room-temperature magnetic properties before and after polarization were determined by a vibrating sample magnetometer (±20 kOe). The linear magnetoelectric coupling coefficient was determined by a magnetoelectric effect measurement system (at a test frequency of 2 kHz, DC bias magnetic fields of 0-3 kOe, and an AC excitation magnetic field of 1.07 Oe. The coupling coefficient was calculated based on αME = δV/(δHt).

Results and discussion

The structure, electrical, magnetic and magnetoelectric coupling properties of BFO-BTO/SrM composite ceramics are systematically investigated. The XRD patterns indicate that the composite consists of coexisting perovskite-type BFO-BTO and hexagonal SrM phases. The proportion of rhombohedral R3c phase in BFO-BTO gradually increases, while the tetragonal P4mm phase decreases as the SrM content increases, demonstrating that SrM addition affects the phase composition of BFO-BTO. The Rietveld refinement results are in reasonable agreement with the XRD patterns. The backscattered electron imaging reveals that the SrM phase (dark region) is uniformly distributed within the BFO-BTO matrix (bright region), exhibiting a point-like dispersion at a low doping and aggregation at a high doping. The surface scanning confirms a minor interphase element diffusion between the two phases. The average grain size of BFO-BTO increases from 0.80 μm to 1.53 μm with increasing the SrM content. The XPS spectra reveal that Fe in all the samples exists in mixed valence states of Fe2+/Fe3+, with the valence ratio showing a minimal variation upon SrM addition. The oxygen vacancy concentration has a slight increase as the SrM content increases, remaining in the range of 45%-56%.

The dielectric properties show that the dielectric constant and loss increase gradually with the increase of SrM content, which is attributed to the Maxwell-Wagner interface polarization effect. Two dielectric anomaly peaksappear in the high temperature dielectric spectra at 510 ℃ and 600 ℃, corresponding to the Curie temperature of SrM and the BFO-BTO ferroelectric phase transition temperature, respectively. The ferroelectric measurements demonstrate that a moderate content of SrM (i.e., x=0.015) optimizes the ferroelectric properties, achieving a remanent polarization of 27.33 μC·cm-2. However, the excessive content of SrM causes a sharp increase in leakage current and ferroelectric deterioration. The PFM analysis confirms that SrM addition weakens the polarization response. The results of magnetic property tests reveal that the magnetization strength of the composite material increases significantly with the increase of SrM content. As x=0.015, the saturation magnetization reaches 4.15 emu·g-1, which exceeds that of pure BFO-BTO (i.e., 0.4 emu·g-1). The sample exhibits a pronounced magnetic anisotropy, with a parallel magnetization outperforming perpendicular magnetization. After poling treatment, the remanence of the sample changes markedly, indicating the presence of stress/charge-mediated magnetoelectric coupling. The results of magnetoelectric coupling tests demonstrate that the coupling coefficient exhibits an initial increase and a subsequent decrease with increasing SrM content, reaching a maximum of 0.72 mV·cm-1·Oe-1 as x=0.035. An appropriate incorporation of SrM enhances strain-mediated magnetoelectric coupling, whereas the excessive addition degrades the piezoelectric performance and weakens the coupling effect. Compared with the similar studies, this system demonstrates a superior comprehensive performance optimization.

Conclusions

This study prepared (1-x)BFO-BTO/xSrM composite multiferroic ceramics. The results showed that the introduction of SrM could modulate the phase composition, with the optimized ferroelectric performance (i.e., Pr=27.33 μC·cm-2) as x=0.015and the maximum magnetoelectric coupling coefficient (i.e., 0.72 mV·cm-1·Oe-1) as x=0.035. The material could demonstrate potential applications in storage, sensing and related fields.

, authors=Juan LIU, Pengyu WANG, Zilong YU, Ailin XIA, authorsList=Juan LIU, Pengyu WANG, Zilong YU, Ailin XIA, authorCompany=null, correspAuthors=null, authorNote=

LIU Juan (1989-), female, Ph.D., Associate Professor. E-mail:

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铁酸铋基多铁性陶瓷由于其相对较弱的磁性,限制了其应用化进程。将其与磁性材料复合,是提升其多铁性能的有效策略之一。采用固相反应烧结工艺成功制备了复合多铁陶瓷(1-x)(0.75BiFeO3-0.25BaTiO3)/xSrFe12O19 (x=0、0.015,0.025、0.035、0.050、0.075),系统研究了该复合陶瓷的结构与磁电性能。结构精修表明,复合陶瓷的相结构为四方相P4mm、菱方相R3c以及六方相P63/mmc共存。当x = 0.015时,复合陶瓷的铁电性能得到了改善,剩余极化强度值Pr = 27.33 μC·cm-2。对块体样品进行了平行与垂直方向的磁性能测试,发现其磁性能略有差异,这与其形状各向异性有关。同时,对直流极化处理后的磁性能进行了测量,观察到显著的磁性能变化,从而证实了电控磁现象的存在。当x = 0.035时,获得最大磁电耦合系数αME = 0.72 mV·cm-1·Oe-1,说明复合M-型锶铁氧体(SrM)后材料的磁电性能得到了显著增强。

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刘娟(1989—),女,博士,副教授。

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BiFeO3-BaTiO3/SrFe12O19复合多铁陶瓷的铁电和磁性能
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刘娟 , 王鹏宇 , 余子龙 , 夏爱林
硅酸盐学报 | 研究论文 2026,54(9): 3123-3136
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硅酸盐学报 |研究论文 2026 , 54 (9) : 3123 -3136
BiFeO3-BaTiO3/SrFe12O19复合多铁陶瓷的铁电和磁性能
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刘娟 , 王鹏宇, 余子龙, 夏爱林
作者信息
  • 安徽工业大学材料科学与工程学院,安徽 马鞍山 243032
作者简介:

刘娟(1989—),女,博士,副教授。

Ferroelectric and Magnetic Properties of BiFeO3-BaTiO3/SrFe12O19 Composite Multiferroic Ceramics
Juan LIU , Pengyu WANG, Zilong YU, Ailin XIA
Affiliations
  • School of Materials Science and Engineering, Anhui University of Technology, Ma'anshan 243032, Anhui, China
  • LIU Juan (1989-), female, Ph.D., Associate Professor. E-mail:

出版时间: 2026-08-18 doi: 10.14062/j.issn.0454-5648.20250771
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铁酸铋基多铁性陶瓷由于其相对较弱的磁性,限制了其应用化进程。将其与磁性材料复合,是提升其多铁性能的有效策略之一。采用固相反应烧结工艺成功制备了复合多铁陶瓷(1-x)(0.75BiFeO3-0.25BaTiO3)/xSrFe12O19 (x=0、0.015,0.025、0.035、0.050、0.075),系统研究了该复合陶瓷的结构与磁电性能。结构精修表明,复合陶瓷的相结构为四方相P4mm、菱方相R3c以及六方相P63/mmc共存。当x = 0.015时,复合陶瓷的铁电性能得到了改善,剩余极化强度值Pr = 27.33 μC·cm-2。对块体样品进行了平行与垂直方向的磁性能测试,发现其磁性能略有差异,这与其形状各向异性有关。同时,对直流极化处理后的磁性能进行了测量,观察到显著的磁性能变化,从而证实了电控磁现象的存在。当x = 0.035时,获得最大磁电耦合系数αME = 0.72 mV·cm-1·Oe-1,说明复合M-型锶铁氧体(SrM)后材料的磁电性能得到了显著增强。

复合多铁陶瓷  /  铁电性  /  磁性  /  磁电耦合效应
Introduction

Multiferroic materials, which exhibit two or more primary iron orders (such as ferroelectricity and ferromagnetism), hold a significant potential in sensing and storage applications. BiFeO3 stands as the most representative room-temperature single-phase multiferroic material. Its ferroelectricity originates from lattice distortion caused by the 6s2 lone-pair electrons of Bi3+hybridizing with O 2p, while magnetism arises from Fe—O—Fe super-exchange. However, its narrow bandgap results in high leakage current and coercive field, making ferroelectric characterization challenging. Also, the periodic arrangement of G-type antiferromagnetic structures renders it macroscopically non-magnetic with a weak magnetoelectric coupling. Researchers develop some methods such as ion substitution and process optimization, among which composites with magnetic materials are effective in inducing magnetism and enhancing magnetoelectric coupling. M-type strontium ferrite (i.e., SrFe12O19, abbreviated as SrM) as a typical permanent magnet with high saturation magnetization has attracted attention due to its complex magnetic structure that can induce ferroelectric polarization, but its high leakage current limits its application in electrically controlled magnetism. To address this issue, this study was to introduce SrM into the BiFeO3 matrix to enhance magnetism and magnetoelectric coupling. To overcome the high leakage current of pure BiFeO3, we selected 0.75BiFeO3-0.25BaTiO3 (BFO-BTO) with superior iron-voltage properties as a ferroelectric matrix.We prepared a series of (1-x)(BFO-BTO)/xSrM composite multiferroic ceramics via solid-state reaction and systematically investigated the evolution of their structural, ferroelectric, magnetic, and magnetoelectric coupling properties.

Methods

In this study, (1-x)(BFO-BTO)/xSrM composite ceramics were synthesized by a solid-state reaction method. Bi2O3, Fe2O3, SrCO3, BaCO3, and TiO2 (all with purity ≥99.9%) were used as raw materials. The materials were weighed in stoichiometric proportions after drying and ground in deionized water for 24 h. The slurries were dried and sieved, then subjected to pre-sintering for BFO-BTO at 870 ℃ for 3 h and SrM at 1100 ℃ for 3 h. The resulting powders were mixed proportionally, ground again for 24 h, dried, granulated, and pressed into green bodies (10 mm diameter, 1-2 mm thickness), followed by sintering at 940 ℃ for 3 h. The sintered samples were polished and coated with silver paste, then fired at 700 ℃ for electrodes.

The crystal structure was analyzed by X-ray diffraction (XRD). The surface morphology was determined by scanning electron microscopy (SEM), and the elemental distribution was analyzed by energy dispersive spectroscopy (EDS). After 30 min polarization in a DC electric field of 40 kV/cm, the samples underwent performance testing. The dielectric properties were obtained by an impedance analyzer with a high-temperature testing system. The room-temperature ferroelectric properties were measured by a ferroelectric analyzer. The room-temperature magnetic properties before and after polarization were determined by a vibrating sample magnetometer (±20 kOe). The linear magnetoelectric coupling coefficient was determined by a magnetoelectric effect measurement system (at a test frequency of 2 kHz, DC bias magnetic fields of 0-3 kOe, and an AC excitation magnetic field of 1.07 Oe. The coupling coefficient was calculated based on αME = δV/(δHt).

Results and discussion

The structure, electrical, magnetic and magnetoelectric coupling properties of BFO-BTO/SrM composite ceramics are systematically investigated. The XRD patterns indicate that the composite consists of coexisting perovskite-type BFO-BTO and hexagonal SrM phases. The proportion of rhombohedral R3c phase in BFO-BTO gradually increases, while the tetragonal P4mm phase decreases as the SrM content increases, demonstrating that SrM addition affects the phase composition of BFO-BTO. The Rietveld refinement results are in reasonable agreement with the XRD patterns. The backscattered electron imaging reveals that the SrM phase (dark region) is uniformly distributed within the BFO-BTO matrix (bright region), exhibiting a point-like dispersion at a low doping and aggregation at a high doping. The surface scanning confirms a minor interphase element diffusion between the two phases. The average grain size of BFO-BTO increases from 0.80 μm to 1.53 μm with increasing the SrM content. The XPS spectra reveal that Fe in all the samples exists in mixed valence states of Fe2+/Fe3+, with the valence ratio showing a minimal variation upon SrM addition. The oxygen vacancy concentration has a slight increase as the SrM content increases, remaining in the range of 45%-56%.

The dielectric properties show that the dielectric constant and loss increase gradually with the increase of SrM content, which is attributed to the Maxwell-Wagner interface polarization effect. Two dielectric anomaly peaksappear in the high temperature dielectric spectra at 510 ℃ and 600 ℃, corresponding to the Curie temperature of SrM and the BFO-BTO ferroelectric phase transition temperature, respectively. The ferroelectric measurements demonstrate that a moderate content of SrM (i.e., x=0.015) optimizes the ferroelectric properties, achieving a remanent polarization of 27.33 μC·cm-2. However, the excessive content of SrM causes a sharp increase in leakage current and ferroelectric deterioration. The PFM analysis confirms that SrM addition weakens the polarization response. The results of magnetic property tests reveal that the magnetization strength of the composite material increases significantly with the increase of SrM content. As x=0.015, the saturation magnetization reaches 4.15 emu·g-1, which exceeds that of pure BFO-BTO (i.e., 0.4 emu·g-1). The sample exhibits a pronounced magnetic anisotropy, with a parallel magnetization outperforming perpendicular magnetization. After poling treatment, the remanence of the sample changes markedly, indicating the presence of stress/charge-mediated magnetoelectric coupling. The results of magnetoelectric coupling tests demonstrate that the coupling coefficient exhibits an initial increase and a subsequent decrease with increasing SrM content, reaching a maximum of 0.72 mV·cm-1·Oe-1 as x=0.035. An appropriate incorporation of SrM enhances strain-mediated magnetoelectric coupling, whereas the excessive addition degrades the piezoelectric performance and weakens the coupling effect. Compared with the similar studies, this system demonstrates a superior comprehensive performance optimization.

Conclusions

This study prepared (1-x)BFO-BTO/xSrM composite multiferroic ceramics. The results showed that the introduction of SrM could modulate the phase composition, with the optimized ferroelectric performance (i.e., Pr=27.33 μC·cm-2) as x=0.015and the maximum magnetoelectric coupling coefficient (i.e., 0.72 mV·cm-1·Oe-1) as x=0.035. The material could demonstrate potential applications in storage, sensing and related fields.

composite multiferroic ceramics  /  ferroelectricity  /  magnetism  /  magnetoelectric coupling effect
刘娟, 王鹏宇, 余子龙, 夏爱林. BiFeO3-BaTiO3/SrFe12O19复合多铁陶瓷的铁电和磁性能. 硅酸盐学报, 2026 , 54 (9) : 3123 -3136 . DOI: 10.14062/j.issn.0454-5648.20250771
Juan LIU, Pengyu WANG, Zilong YU, Ailin XIA. Ferroelectric and Magnetic Properties of BiFeO3-BaTiO3/SrFe12O19 Composite Multiferroic Ceramics[J]. Journal of the Chinese Ceramic Society, 2026 , 54 (9) : 3123 -3136 . DOI: 10.14062/j.issn.0454-5648.20250771
  • 国家重点研发计划(2022YFB3807602)
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doi: 10.14062/j.issn.0454-5648.20250771
  • 接收时间:2025-10-23
  • 首发时间:2026-10-22
  • 出版时间:2026-08-18
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  • 收稿日期:2025-10-23
  • 修回日期:2026-02-28
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国家重点研发计划(2022YFB3807602)
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    安徽工业大学材料科学与工程学院,安徽 马鞍山 243032
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2种不同金属材料的力学参数
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鹅膏菌科Amanitaceae 2 11 5.26 鹅膏菌属 Amanita 10 4.78
小菇科 Mycenaceae 2 12 5.74 丝盖伞属 Inocybe 5 2.39
多孔菌科 Polyporaceae 8 14 6.70 蜡蘑属 Laccaria 5 2.39
红菇科 Russulaceae 3 23 11.00 小皮伞属 Marasmius 6 2.87
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红菇属 Russula 17 8.13
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