Materials Today: Proceedings 45 (2021) 7450–7456

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Materials Today: Proceedings

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Effects of Gd-substitution on structural, and impedance spectroscopic

study of Sr2Sm1
xGdxTi2Nb3O15 tungsten bronze ceramics
Karim. Chourti a,⇑, Amine. Bendahhou a, Fath Allah. Rabie b, Mohamed. Loutou a, Soufian. El barkany a,
Mohamed. Abou-salama a
a
Laboratory of Molecular Chemistry, Materials and Environment, Department of Chemistry, Faculty Multidisciplinary Nador, University Mohamed Premier, B.P. 300 Selouane,
Nador 62700, Morocco
b
National Center for Scientific and Technical Research (CNRST)/UATRS, Morocco

a r t i c l e i n f o a b s t r a c t

Article history: In the present work, we have studied the effect of Gd-substitution on the structural, dielectric and elec-
Available online 26 February 2021 trical properties of Sr2Sm1
xGdxTi2Nb3O15 (x = 0 and 0.5) tungsten bronze ceramics prepared by a high-
temperature solid-state reaction technique. The formation of the phase of tetragonal tungsten bronze
Keywords: was verified by the Rietveld refinement using X-ray diffraction data. With increasing Gd concentration,
Tetragonal tungsten bronze the crystal structure of the Sr2Sm1
xGdxTi2Nb3O15 ceramics has slightly deformed from the tetragonal
Solid-state P4bm phase to the paraelectric P4/mbm phase. Scanning electron microscopy (SEM) of ceramics shows
X-ray diffraction
high densification and homogeneous distribution of grains of different sizes over the total surface. The
Ceramics
Impedance
crystallite size increases with Gd-substitution from 6.19 nm for Sr2SmTi2Nb3O15 to 10.83 nm for
Cole-Cole Sr2Sm0.5Gd0.5Ti2Nb3O15. The sample Sr2SmTi2Nb3O15 shows a dielectric anomaly of ferroelectric paraelec-
tric type at 332 °C, and has non-relaxor type of diffuse phase transition. In addition, the dielectric prop-
erties deteriorated and even disappeared for the sample Sr2Sm0.5Gd0.5Ti2Nb3O15, because the ceramic
presented a P4/mbm phase structure as a result of the decrease in Curie temperature (Tc) below room
temperature. The electrical property of Sr2Sm1
xGdxTi2Nb3O15 ceramic has been investigated by non-
destructive complex impedance spectroscopy (CIS) as a function of frequency at different temperatures.
Ó 2021 Elsevier Ltd. All rights reserved.
Selection and peer-review under responsibility of the scientific committee of the Fourth edition of the
International Conference on Materials & Environmental Science.

1. Introduction
Tetragonal tungsten bronze oxides (TTB) have attracted consid-
erable attention by many researchers because of their important
and advantageous electrical, magnetic, catalytic, optical or photo-
catalytic properties, with diverse applications in the electronics,
chemical and energy conversion sectors [1–5]. The chemical for-
mula of the TTB structure is (A1)2(A2)4(C)4(B1)2(B2)8O30 [6–11]
which consist of distorted BO6 octahedral linked by their summits,
forming three different interstices two square A1 sites, four pen-
tagonal A2 sites, and four trigonal C sites. The pentagonal A2 and
square A1 sites can receive large cations such as Ba2+, Sr2+, La3+
while the triangular sites C receive small cations such as Li+ [12–
14]. The octahedral sites B1 and B2 are occupied by highly charged
cations, such as Nb5+, W6+, Zn2+ [15,16]. In our study, the smallest
⇑ Corresponding author.
E-mail address: k.chourti@ump.ac.ma (Karim. Chourti).
site C is unoccupied and thus their general formula becomes (A1)2-
(A2)4(B1)2(B2)8O30. The variety of cationic sites (A1, A2, C, B1, and
B2) gives rise to a great variety of structures, allowing the improve-
ment of the characteristics of TTBs, by substitutions in A1 and A2
sites or in B1 and B2 octahedrons. The complex impedance spec-
troscopy is a very convenient and powerful experimental tech-
nique [17,18] that enables us to (i) study the physical processes
determining the electrical and dielectric properties of materials
[19], (ii) to separate the contributions of grains and grain bound-
aries to the transport properties of materials [20], and (iii) study
of conductivity, modulus spectra, relative permittivity and dielec-
tric losses as a function of frequency. The variation of impedance
parameters can be appropriately modelled with equivalent cir-
cuits, which will assist the researcher in determining the responsi-
ble physical processes [21–23]. As noted previously, much
attention has been given recently to compounds with an TTB struc-
ture and to the modulation of their properties by substitutions. A
thorough search of the literature indicates that most of the work

https://doi.org/10.1016/j.matpr.2021.02.010
2214-7853/Ó 2021 Elsevier Ltd. All rights reserved.
Selection and peer-review under responsibility of the scientific committee of the Fourth edition of the International Conference on Materials & Environmental Science.