3/1/25, 8:40 PM Multiferroic triphase BFO-PZT-PVDF composite with significant magnetoelectric response for multistate device applications - Sci…
Ceramics International
Volume 47, Issue 15, 1 August 2021, Pages 21688-21697
Multiferroic triphase BFO-PZT-PVDF
composite with significant magnetoelectric
response for multistate device applications
Muhammad Mehak a 1, Muhammad Ahmed Khan a 1, Umair Ali a, Abdul Quader a,
Murtaza Saleem b, G.M. Mustafa a c, Ahmed S. Haidyrah d, Shahid Atiq a
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Abstract
Triphase multiferroic composites with higher degree of freedom, provide a new platform
for developing novel and smart technological applications. In this context, here we
present a new triphase composite, consisting of bismuth ferrite (BFO) and lead zirconate
titanate (PZT) synthesized using sol‒gel auto-combustion and solid-state routes,
respectively and then subsequently dispersed into a PVDF polymatrix, leading to a
triphase composite (BFO-PZT-PVDF). Structural analysis confirmed the composite
formation as all the intensity peaks were either matched with BFO or PZT phases.
Morphological analysis revealed that pure BFO and PZT formed well defined grains with
sharp grain boundaries. However, when they are dispersed in the polymer matrix, their
boundaries became diffused. Worth mentioning ferroelectric parameters like saturation
polarization, remanent and recoverable energy density are measured from bipolar
polarization loops. It is noticed that maximum polarization is decreased while coercivity
is increased with the increment of PZT contents in the composite. Vibrating sample
magnetometer confirmed the variation in magnetic features, exactly in accordance as
required for significant magnetoelectric coupling for practical utilization. The extent of
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3/1/25, 8:40 PM Multiferroic triphase BFO-PZT-PVDF composite with significant magnetoelectric response for multistate device applications - Sci…
magnetoelectric coupling supports the potential applications of these triphase
composites for energy storage and multistate devices.
Introduction
The sophisticated and dynamic concept of magnetoelectric coupling (ME) has attained
much more attention of research community in the recent past. The materials possessing
this feature are called multiferroic (MF) materials which have potential to play its role in
the fabrication of smart and efficient devices, for instance spintronic devices, sensors,
four stage memory devices and transducers [[1], [2], [3]]. In fact, the concurrent linear
coupling of polarization and magnetic field or magnetization and electric field in MF
materials provide an additional degree of freedom [4,5]. This triggers them further into
energy efficient behavior for portable commercial device fabrication [6]. The strong ME
coupling is a key foundation of large-scale practical applications of MF materials but
microscopic constraints limit their use at room temperature (RT) [7]. High leakage
current, which is attributed to oxygen vacancies, is one of the main drawbacks of single
and biphase MF composites [8,9]. To attain a sufficient and simultaneous polarization,
retentivity and ME coupling coefficient has been the main challenges for scientists from
past to recent decades. So, an elegant approach to [Link] peculiarities is the
formation of triphase composites i.e. ceramics-ceramic-polymers. Such composites have
ability to overcome the aforementioned shortcomings and distinctly improve the
required range of ME coupling coefficient [[10], [11], [12], [13]]. The enhanced ME
coupling response at RT is a product property of composite which is attributed to the
elastic interaction between piezoelectric and magnetostriction phases via strain [9,[14],
[15], [16]].
An extensive study has been performed on BiFeO3 (BFO) ceramics because it is the only
multiferroic material above RT. It has rhombohedrally distorted cubic perovskite crystal
structure with R3m space group. BFO possesses excellent ferroelectric behavior but weak
ME coupling at RT hinders its use in pure form for MF applications [17]. Besides BFO, the
second most important composition is lead zirconate titanate (PZT) which is a renowned
ferroelectric material. It is noted that mixing of PZT in BFO provides an additional control
on conductivity of the composite and make them viable for energy efficient applications.
In addition, this combination also helps to reduce the leakage current caused by porosity,
and mismatching of grains at interphase [18,19]. Thus, in the present work, these two
phases are embedded in chemically non-reactive polyvinylidene fluoride (PVDF) polymer
matrix. PVDF is semi-crystalline in nature that have many apparent advantages:
including (1) high volume to strength ratio, (2) easy to fabricate, (3) low cast, and (4)
easily assessable. Moreover, PVDF matrix provides support for these two constituents
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3/1/25, 8:40 PM Multiferroic triphase BFO-PZT-PVDF composite with significant magnetoelectric response for multistate device applications - Sci…
which may lead to enhance the desirable ME coupling values and reduce the
conductivity values significantly [20,21].
Recently, several studies have been devoted to triphase composites prepared in bulk and
thin film form which showed a significant improvement in ME coupling coefficient [22].
The first significant breakthrough was reported by Nan et al. where they declared a
simultaneous increase in ferroelectric and ferromagnetic behavior [23]. Another
astonishing improvement in ME coefficient of tri-phase composite films of barium
titanate (BT), cobalt ferrite (CFO) and PVDF-trifluoro ethylene (PVDF-TrFE) in polymer
form as CFO-BT-PVDF/TrFE was investigated by Xia et al. These films were synthesized by
solution spinning method and a closed look revealed that magnetic and dielectric
properties were modified [14]. In another work, Adhlakha et al. had studied the
dielectric, magnetic and ferroelectric properties of tri-phase ceramic polymer composite
films. In parallel, when (1-x)BLPFO-xPZT-0.5PVDF were prepared by solid state route, it
was observed that ferroelectric, ferromagnetic behavior and magneto-dielectric coupling
was modified by varying PZT contents in the composite [24]. Thus, these literature
survey have motivated us to explore the BFO-PZT-PVDF triphase composites at RT to
check their suitability for multifunctional devices which are based on ME coupling effect.
During literature survey, it has been observed that a lot of work has been devoted to
explore the decent behavior of BFO, PZT and PVDF separately, but no significant attention
was paid to BFO-PZT-PVDF triphase composites. Thus, to present the suitability of the
triphase composites for advanced applications like fast switching circuits and
magnetocapacitance effect-based devices, here we synthesized the triphase composites,
consisting of BFO and PZT embedded in PVDF matrix. The main aim of this research
article is to explore the structural, morphological, ferroelectric and magnetic properties
of these composites and thus check their suitability for ferroelectric energy storage and
ME coupling based multistate device applications.
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Section snippets
Samples synthesis
A well-known three step route has been adopted to synthesize the triphase composites
in a simple and convenient approach, as shown in Fig. 1. At first, to prepare pure BFO
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3/1/25, 8:40 PM Multiferroic triphase BFO-PZT-PVDF composite with significant magnetoelectric response for multistate device applications - Sci…
sample, an efficient and cost-effective sol‒gel auto-combustion method was used.
Analytical grade chemical reagents like bismuth nitrate pentahydrate [Bi(NO3)3.5H2O,
purity ≥ 98%], and iron nitrate nonahydrate [Fe(NO3)3.9H2O, purity ≥ 98%] were used as
precursors while urea (CH4N2O) and glycine (C2H5NO2) were used as fuel …
Structure analysis
The XRD patterns of pure BFO, PZT and BFO-PZT-PVDF triphase composites with different
BFO, PZT concentrations are shown in Fig. 2. The diffraction patterns were captured in 2θ
range of 10–80°, using CuKα radiations. The pattern of pure BFO exhibits intensity peaks
at 2θ values of 22.72°, 32.05°, 39.34°, 45.85°, 51.72°, 57.12°, and 67.44° which are
represented with a symbol nabla (∇). These peaks are indexed according to the analytical
treatment as described by B.D. Cullity [25]. After indexing, …
Conclusion
The triphase ceramic-polymer composite i.e. BFO-PZT-PVDF has been synthesized by
dispersing multiferroic BFO and piezoelectric PZT in PVDF polymer matrix. The XRD
analysis confirmed the cubic crystalline phases of BFO and PZT without having any
impurity peaks. FESEM images of BFO and PZT revealed their well-defined grain
boundaries. These grains were agglomerated when dispersed in PVDF polymer matrix
which is due to the hygroscopic property of Bi. Elemental profile confirmed the presence
of all …
Declaration of competing interest
The authors declare that they have no known competing financial interests or personal
relationships that could have appeared to influence the work reported in this paper. …
Acknowledgement
Ahmed S. Haidyrah would like to thank King Abdulaziz City for Science and Technology
(KACST) for supporting this work. First author also acknowledges Higher Education
Commission (HEC) of Pakistan for partial facilitation in experimental measurements
supported by NRPU-2471. …
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