Heat Resistance and Electrophysical Characteristics of Polyheteroarylenes and Ferroelectric–Polymer Film Composites Based on Them

Article abstract of DOI:10.1134/S1070427220020056

Abstract: Structurally related poly(amido-o-hydroxy amides) derived from 5,5-methylenebis(2-aminophenol) with tetramethylsiloxane and heteroaromatic (benzoxazole and benzotriazole) fragments incorporated in the second amine component or formed by polyheterocyclization of the corresponding prepolymers were prepared. The effect of modifying fragments introduced into the base poly(o-hydroxy amide) on the heat resistance of powders and films and of films of photosensitive compounds based on the synthesized polymers with the naphthoquinone diazide component was analyzed. The electrophysical parameters of the polymer films and film composites with a nanodispersed ferroelectric filler, (PZT: ceramic powder with the composition Pb_0.81Sr_0.04Na_0.075Bi_0.075(Zr_0.58 Ti_0.42)O₃, Russian brand PZT-1), prepared on the basis of modified polymer binders, were determined. Introduction of 20 mol % sulfur-containing fragments into the polymer binder ensures a 50–65?C increase in the heat resistance for all types of films without increasing the level of the dielectric loss for the composite coatings.

Full text of DOI:10.1134/S1070427220020056

ISSN 1070-4272, Russian Journal of Applied Chemistry, 2020, Vol. 93, No. 2, pp. 188−196. © Pleiades Publishing, Ltd., 2020.
Russian Text © The Author(s), 2020, published in Zhurnal Prikladnoi Khimii, 2020, Vol. 93, No. 2, pp. 187−196.
MACROMOLECULAR COMPOUNDS
AND POLYMERIC MATERIALS
Heat Resistance and Electrophysical Characteristics
of Polyheteroarylenes and Ferroelectric–Polymer
Film Composites Based on Them
a
b
b
b
c
D. A. Chigirev , M. N. Bol’shakov , G. K. Lebedeva , A. Yu. Marfichev , Yu. V. Shagaiko ,
c,
a
L. I. Rudaya *, and I. M. Sokolova
a
Ulyanov (Lenin) St. Petersburg State Electrotechnical University LETI, St. Petersburg, 197376 Russia
Institute of Macromolecular Compounds, Russian Academy of Sciences, St. Petersburg, 199004 Russia
b
c
St. Petersburg State Institute of Technology (Technical University), St. Petersburg, 190013 Russia
*
e-mail: 9241890@mail.ru
Received January 31, 2019; revised September 28, 2019; accepted December 3, 2019
Abstract—Structurally related poly(amido-o-hydroxy amides) derived from 5,5-methylenebis(2-aminophenol)
with tetramethylsiloxane and heteroaromatic (benzoxazole and benzotriazole) fragments incorporated in the second
amine component or formed by polyheterocyclization of the corresponding prepolymers were prepared. The effect
of modifying fragments introduced into the base poly(o-hydroxy amide) on the heat resistance of powders and films
and of films of photosensitive compounds based on the synthesized polymers with the naphthoquinone diazide
component was analyzed. The electrophysical parameters of the polymer films and film composites with a nano-
dispersed ferroelectric filler, (PZT: ceramic powder with the composition Pb0.81Sr0.04Na0.075Bi0.075(Zr0.58 Ti0.42
)
O , Russian brand PZT-1), prepared on the basis of modified polymer binders, were determined. Introduction of
3
2
0 mol % sulfur-containing fragments into the polymer binder ensures a 50–65°C increase in the heat resistance
for all types of films without increasing the level of the dielectric loss for the composite coatings.
Keywords: poly(o-hydroxy amide), poly(benzoxazole), poly(benzothiazole), nanocomposite, ferroelectric, heat
resistance, dielectric permittivity, dielectric loss tangent
DOI: 10.1134/S1070427220020056
Searching for new polymer composites with fer-
roelectric fillers and studying their properties remain
topical, because such materials are demanded in such
branches of engineering as radio-, opto-, and acousto-
electronics and nonlinear optics [1–4].
ing the composite with the filler to 40–45 vol % allows ε′
to be increased to 430, but in so doing, as expected, tan δ
increases to 0.1 and higher values. So, there is some in-
ner contradiction in the practice to manufacture the com-
posites with low dielectric losses and enlarged dielectric
permittivity by increasing the filler loading degree.
In the development of film capacitor structures, the
main goal is preparation of a heat-resistant composite
One of the ways to reduce the dielectric loss in the
ferroelectric/polymer composite is using a dielectric
polymer matrix with high insulation properties: low die-
lectric permittivity and low dielectric loss, e.g., polyam-
ido acid (PAA) or poly(o-hydroxy amide) (POA), with
POA being preferable because of its lower tendency to
hydrolysis [11–14].
(ferroelectric/polymer) film dielectric with increased
values of the dielectric permittivity and electric strength
and decreased dielectric loss tangent (tan δ). Depend-
ing on the production technology and concentration of
the ferroelectric filler, the reached values of the dielec-
tric permittivity ε′ in ferroelectric/polymer composites
range from 40 to 200, and those of tan δ, from 0.04 to
It is important that the parameters and functional
destination of heterophase nanocomposites being devel-
oped can be varied in a wide range by varying the struc-
0
.08, with no more than 30 vol % loading of the polymer
with the filler [5–10]. An increase in the degree of load-
188

HEAT RESISTANCE AND ELECTROPHYSICAL CHARACTERISTICS
189
Scheme 1.
HO
CH2
OH
+
Cl
Cl
H N
NH2
2
NH
OH
NH
(
CH ) NCOCH
3 2
3
–2HCl
HO
N
CH2
n
N
O
O
–
2nH O
2
CH2
n
ture and properties of the polymer matrix. Specifically
the polymer matrix is responsible for the heat resistance
of the composite coating, adhesion to supports of differ-
ent chemical nature, and formation of the polymer ma-
trix–filler grain interface.
prepared by introducing silicon- and sulfur-containing
fragments into the macromolecule of base POA I; de-
velopment of photosensitive formulations and ferroelec-
tric/polymer dielectric composites based on them; and
analysis of the influence of the polymer matrix compo-
sition on the properties of the formed films (heat resist-
ance, adhesion, and electrophysical parameters).
This paper continues the studies on modification of
the base polymer matrix, POA I [15], and deals with
synthesis of structurally related poly(о-hydroxy amides)
and poly(amido-о-hydroxy amides) and comprehensive
study of the properties of polymer matrices and poly-
mer/ferroelectric composites based on them.
The presence of –(CH ) SiOSi(CH ) – fragments
3
2
3 2
in the polymer molecule should enhance the adhesion
to silicon-containing supports, and benzothiazole rings
formed by thermal cyclodehydration of o-mercapto
amides should enhance the heat resistance compared to
POA I [18].
POA I is formed by polycondensation of 5,5-meth-
ylenebis-(2-aminophenol) with isophthaloyl dichlo-
ride (IPC) [16], followed by heat treatment leading to
cyclodehydration with the formation of hydrophobic
poly(benzoxazole) (PBO), which exhibits high heat re-
sistance (up to 400°С), high chemical durability, and
low moisture capacity. This fact predetermined its use
as a material for protective layers in various multilev-
el electronic circuits [17], humidity sensors, and other
electronic devices (Scheme 1).
One of the most important conditions in preparation
of copolymers is the choice of the ratio of diamines in-
troduced into the reaction. The macromolecules should
contain a sufficient amount of alkali-soluble fragments
with hydroxy groups, which would allow the develop-
ment of photosensitive formulations with a naphthoqui-
none diazide component, Posylux 2402, based on them,
ensuring the formation of a highly heat-resistant micro-
relief in films using photolithographic operations with
alkaline development.
To bring these results to the process practice, it was
necessary to find polymer binders exhibiting, compared
to POAI, increased levels of adhesion to supports of dif-
ferent chemical nature and of heat resistance.
EXPERIMENTAL
The goals of this work were synthesis and study of a
series of new polymers, poly(amido-o-hydroxy amides)
Isophthaloyl dichloride (IPC) (Sigma–Aldrich, CAS
99-63-8) and 3,3′-(1,1,3,3-tetramethyldisiloxane-1,3-
RUSSIAN JOURNAL OF APPLIED CHEMISTRY Vol. 93 No. 2 2020

190
CHIGIREV et al.
–
1
diyl)bis(propan-1-amine) were used without preliminary
purification. 2-(Chloromethyl)oxirane (EPC) (Sigma–
Aldrich, 99%, CAS 106-89-8) was distilled before use.
Posylux 2402 (LLC FRAST-M, Moscow, Russia) was
used without preliminary purification.
2,4-Diaminobenzenethiol: ν, cm : 3461 and 3433
(NH ), 1692 (NH ); δ, ppm: 4.02 (H, SH), 5,30 (4H,
2
2
2NH ), 6.01, 6.07, 7,04 (3Н, C H ).
2
6
3
Synthesis of POA I. 46 g of 5,5-methylenebis(2-ami-
nophenol) was dissolved in 180 mL of DMAA contain-
ing no more than 0.035% moisture at room temperature.
The solution was cooled to –5...0°С, and a solution of
40.6 g of IPC in 30 mL of DMAA was added to the
cooled solution with stirring at a rate allowing self-
heating of the reaction mixture over 40°C to be avoided.
After adding the whole amount of IPC, the cooling was
stopped, and the reaction mixture was allowed to stand
at room temperature for 2 h and again was cooled to
Devices and measurement methods. The IR spectra
of solid substances were taken from KBr pellets with
a Shimadzu FTIR-8400 S spectrometer in the interval
–1
1
6
00–4000cm .The НNMRspectrawererecordedwith
a Bruker AC-400 spectrometer using tetramethylsilane
TMS) as internal reference. The chemical shifts are
(
given in the δ scale relative to TMS.
The kinematic viscosity of polymers was measured
with a VPZh-1 glass capillary viscometer.
–
5...0°С. Then, 31.5 mL of freshly distilled EPC was
added dropwise over a period of 15–20 min, after which
the solution was stirred at room temperature for 60 min.
Copolymers II–IV were prepared by analogy with POA
I by the reaction of IPC with a mixture of diamines
taken in a definite molar ratio: 5,5-methylenebis(2-ami-
nophenol) : 3,3′-(1,1,3,3-tetramethyldisiloxane-1,3-di-
yl)bis(propan-1-amine) = 3 : 2 (II), 5,5-methylenebis(2-
The heat resistance of powdered polymer samples
was evaluated by thermal gravimetric analysis (TGA),
performed with a DTG-60 combined thermal analysis
installation (Shimadzu, Japan) using 10-mg samples.
The samples were placed in open corundum crucibles
and heated in the self-generated air atmosphere at a
–
1
rate of 5 deg min . From the experiment results, we
determined the heat resistance parameters τ and τ :
aminophenol)
methyl)benzo[d]thiazol-2-amine = 4 : 1 (III), and
,5-methylebebis(2-aminophenol) : 2,4-diaminoben-
:
6-((2-aminobenzo[d]thiazol-5-yl)
5
10
temperatures corresponding to the polymer weight loss
of 5 and 10% after the removal of residual solvents,
low-volatile components, and water due to thermal
cyclodehydration of POA to PBO and poly(o-mercapto
amide) (PMA) to poly(benzothiazole) (PBT).
5
zenethiol = 4 : 1 (IV).
Preparation of powdered samples of POA I–IV. A
1
0-mL portion of the reaction solution of the polymer
was diluted with 20 mL of DMAA and added dropwise
to 500 mL of an isopropanol : chloroform mixture (1 :
5
,5-Methylenebis(2-aminophenol) was synthesized
by condensation of о-aminophenol with formalin in the
presence of sulfuric acid and sodium sulfite [19]. The
sulfur-containing diamine, 6-((2-aminobenzo[d]thiazol-
5
by volume) cooled to –5÷0°С. The precipitate was
filtered off, washed with two portions of the precipitating
mixture and then with isopropanol and acetone, and
dried at 70°С for 5 h and then at 40°С in a vacuum oven
for 3 h. Yield 80–90%.
5
-yl)methyl)benzo[d]thiazol-2-amine, was prepared by
thiocyanation of 4,4’-diphenylmethane in the presence
of bromine [20], and 2,4-diaminobenzenethiol, by
reduction of 2,4-dinitrochlorobenzene with Na S·9H O
–
1
The reduced viscosity (η, dL g ) for polymer I
2
2
–1
was 0.89 (0.5% solution in H SO ), and for 0.5 g dL
2
4
by analogy with [21]. The above-described compounds
were prepared by these procedures for the first time.
The structure of the diamines was confirmed by
solutions in DMAA it was 0.359 for II, 0.178 for III, and
0
.162 for IV.
1
Preparation of I–IV:Posylux 2402 photosensitive
IR (KBr) and Н NMR (DMSO-d ) spectroscopy.
6
–
1
formulations. Photosensitive formulations based on I–
IV were prepared by mixing the reaction solution of
the polymer binder with a solution of Posylux 2402 in
DMAA at the component weight ratio of 5 : 1 (in terms
of the dry polymer weight).
5
3
2
3
,5-Methylenebis(2-aminophenol): ν, cm : 3378.09,
305.76 (NH ), (OH), 3024.18 (СН ), 2910.38,
924.56 (СН ), 1598.88 (NH ), 1213.14 (OH); δ, ppm:
.49 (2H, CH ), 4.29 (4H, 2NH ), 6.36, 6.38, 6.47 (6H,
2
Ar
2
2
2
2
C H ), 8.85 (2Н, ОН). 6-((2-Aminobenzo[d]thazol-5-
6
4
–
1
yl)methyl)benzo[d]thazol-2-amine: ν, cm : 3430 and
376 (NH ), 1621 (NH ), 2932 (CH ), 1535 (C=N);
Procedure for forming the microphotorelief in pho-
toresist films. Films on silicon supports were formed
by centrifugation followed by drying in a thermostat at
95 ± 5°С. The coating thickness after drying was deter-
3
2
2
2
δ, ppm: 3.92 (2H, CH ), 7.06, 7.08 (2H, C H ), 7.19,
2
6
4
7
.21 (2H, C H ), 7.35 (4H, 2NH ), 7,45 (2H, C H ).
6 4 2 6 4
RUSSIAN JOURNAL OF APPLIED CHEMISTRY Vol. 93 No. 2 2020

HEAT RESISTANCE AND ELECTROPHYSICAL CHARACTERISTICS
191
mined with an MII-4 interference microscope. The mi-
a frequency of 200 kHz at room temperature.
crorelief in films was created by photolithography using
an EM 576 exposure installation, followed by the devel-
opment in an aqueous KOH solution. The solution con-
centration and time of the latent image development were
chosen experimentally for each photoresist. The film de-
velopment time for the photoresists based on polymers I–
IV was 45 s (0.3% KОН), 40 s (0.6% KOH), 25 s (0.45%
KOH), and 2 min (0.2% KOH), respectively. The heat
treatment of photoresist films with the relief image was
performed by stepwise heating at 150–350°С (heating
step 50°C with keeping at each temperature for 15 min).
The polymer and composite coatings deposited
on supports were heat-treated in air in an SUOL-
0
.25.1/12.5-I1 muffle furnace in the stepwise mode:
polymer coatings, at temperatures from 150 to 350°С
with 50°C step and keeping for 15 min at each
temperature; composite coatings, at temperatures from
1
50 to 350°С with 50°C step and keeping for 30 min
at each temperature. The furnace temperature was
monitored with a chromel–alumel thermocouple. The
heat treatment of the coatings consisted of the following
–
1
steps: heating at a rate of 10 deg min , keeping for
the preset time at preset temperature, and, after the
annealing completion, slow cooling of the specimens
with the furnace.
Procedure for preparing polymer/ferroelectric film
composites. Polymer/ferroelectric film composites were
prepared by the procedure described in [16, 22], except
the operation of ultrasonic dispersion of the ferroelectric
filler in a polymer solution. In this study, to obtain a
more homogeneous suspension, coarse particles of the
ferroelectric filler powder were allowed to sediment
from the solvent (DMAA), after which the remaining
suspension was used for forming coatings.
The capacitance and dielectric loss tangent of the
capacitor structures were measured at room temperature
at a frequency of 200 kHz with an E7-20 LCR meter.
RESULTS AND DISCUSSION
Sample preparation for electrophysical studies. Film
coatings of polymers I–IV and based on them compos-
The synthesized polymers can be described by
Scheme 2.
ites were formed on two types of supports: Si–SiO –Pt
2
The fragment ratio m/k in the copolymer structure
was chosen taking into account the fact that the films
formed should exhibit high adhesion to various kinds
of supports and ensure the formation of a highly heat-
resistant microrelief using photolithographic operations.
andAl foil of А99 grade, GOST (State Standard) 11069–
2
001, 80 ± 5 μm thick. To form capacitor structures on
plates of single-crystalline silicon of (100) orientation,
lower platinum electrodes 80 nm thick were deposited
onto the whole surface of the Si support by ion-plas-
ma sputtering. A three-electrode ion-plasma sputtering
installation was used; the support temperature in the
course of the film deposition was 450°С. After forming
a dielectric coating on the support surface, drying, and
heat treatment, a system of upper electrodes was depos-
ited onto this coating by ion-plasma sputtering through
a shadow mask. The composite coating thickness was
varied from 3 to 100 μm. The thickness of the upper
platinum electrodes was 100 nm and the size varied
Previously [23] we studied the adhesion of films of
photoresists based on silicon-containing poly(amido-
о-hydroxy amides) with different content of
–(CH ) SiOSi(CH ) – fragments to supports of different
3
2
3 2
chemical nature. The POA-Si copolymer II with the
fragment ratio m : k = 0.6 : 0.4 showed the best properties.
Data on the adhesion of films of photoresists based on
POA I and POA-Si II, formed on different supports, are
given in Table 1. The adhesion of photoresist films was
evaluated by the number of squares with the microrelief,
peeled of onto SP 3007 adhesive tape, in accordance
with ISO 2409 standard (GOST 31149–2014: Paint-
and-Varnish Materials. Determination of the Adhesion
by Cross-Cut Test).
2
from 1 to 6.75 mm . To increase the degree of filler
loading in preparation of a composite coating, we chose
the method of filler sedimentation in a suspension of the
ferroelectric nanodispersed filler in the polymer solu-
tion. The composite coating thickness was varied from
3
to 100 μm.
For the photoresist based on copolymer II, we
observed virtually no peel-off of fragments of the
formed photorelief onto the adhesive tape from all
types of supports; therefore, such polymer can be
recommended for making microrelief layers both on
Procedureformeasuringelectrophysicalparameters.
To evaluate the electrophysical properties of film
coatings, we measured the capacitance (С) and dielectric
loss tangent (tan δ) of the formed capacitor structures at
RUSSIAN JOURNAL OF APPLIED CHEMISTRY Vol. 93 No. 2 2020

192
CHIGIREV et al.
Scheme 1.
Table 1. Adhesion of films of photoresists based on POA I and POA-Si II, formed on supports of different chemical nature
Number of peeled-off squares of the photorelief formed in
Polymer binder of photoresist
Support type
the filma
I
I
Si
28/100
46/100
40/100
5/100
0/100
0/100
2/100
5/100
SiO2
Si N
I
3
4
I
Al
II
II
II
II
Si
SiO2
Si N
3
4
Al
a
Developer: 0.3% aqueous KOH for the photoresist based on polymer binder I and 0.6% aqueous KOH for the photoresist based on polymer
binder II.
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HEAT RESISTANCE AND ELECTROPHYSICAL CHARACTERISTICS
193
Fig. 2. Weight loss of films of polymers I–IV, formed
from reaction solutions on a Si substrate under the
conditions of stepwise heating to 500°С with a step of
50°C and keeping for 15 min at each temperature.
Fig. 1. Curves of thermal gravimetric analysis of
powdered samples of POA I–IV.
the above-mentioned types of supports and on silicon
substrates with metal routing.
residual low-molecular-mass fractions, and it is higher
than that for the corresponding powdered samples
(Figs. 1, 2). The polyheterocyclization of POAand PMA
with the formation of benzoxazole and benzothiazole
rings occurs at 300–350°С and is accompanied by
~20% weight loss. The lowest weight loss is observed
for copolymer II, and this result, as for the powdered
samples, correlates with the content of units capable of
cyclodehydration.
We studied the heat resistance of powders prepared by
precipitation of the synthesized polymers from reaction
lacquers; of films formed from reaction solutions of
polymers I–IV on Si supports; and of photoresist films
based on them (Figs. 1–3).
The lowest weight loss in the course of heating up
to the onset of degradation is observed for copolymers
II–IV, and the highest weight loss, for base polymer I
(Fig. 1), in agreement with the content of units capable
of cyclodehydration. The temperatures τ and τ ,
5
10
corresponding to the 5 and 10% weight loss, respectively,
relative to the initial polymer weight after the removal
of water, solvents, and low-volatile components are,
respectively, 366 and 385°C for I, 327 and 360°C for II,
3
97 and 437°C for III, and 406 and 450°С for IV. Lower
values of these temperatures for copolymer II can be
attributed to thermal instability of the –Si–C– bond
[24]. According to [18], the presence of benzothiazole
fragments should enhance the heat resistance of the
copolymers. Our studies confirmed this assumption.
The presence of even 20% benzothiazole fragments,
along with benzoxazole units, in the base matrix I after
the cyclodehydration enhances the heat resistance of the
polymers formed by 50–65°C (copolymers III and IV).
In the course of stepwise heating to 250°С, the weight
loss of the films formed from the reaction solutions of
polymers I–IV is associated with the degradation of the
Fig. 3. Weight loss of films of photoresists I–IV, formed
on a Si substrate under the conditions of stepwise
heating to 500°С with a step of 50°C and keeping for
1
5 min at each temperature.
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194
CHIGIREV et al.
Table 2. Dielectric parameters of polymer and composite coatings
Polymer binder/support
Filler
ε′
tan δ
0.02
(I)/Si/Pt
3.4
–
–
(
(
(
(
(
(
(
II)/Si/Pt
3.5
3.7
0.01
III)/Si/Pt
IV)/Si/Pt
I)/Si/Pt
–
0.03
–
8.0
0.02
0.04–0.08a
PZT-1-1
PZT-1-1
PZT-1-1
PZT-1-1
23–185a
10.0
15.0
38.0
II)/Si/Pt
0.04
III)/Al foil
IV)/Al foil
0.03
0.1
a
Data for a series of specimens with different film thickness, range 3–15 μm.
It should be noted that the thermal curing of the
polymer films was not accompanied by their peel-off,
and there were no flaws and cracks in the films.
the degree of loading with the ferroelectric filler, are in
the range 10–185, and the maximal values of tan δ do not
exceed 0.1. Such value of tan δ in the composite based
on copolymer IV is most likely due to an increase in the
degree of loading with the ferroelectric filler, rather than
to parameters of the polymer matrix.
Data on the heat resistance show that introduction
of 40% Si-containing units as modifying fragments into
the base polymer molecule (copolymer II) leads to an
approximately 30°C decrease in the heat resistance,
whereas introduction of even 20% sulfur-containing
fragments considerably enhances the heat resistance:
For films of IV, it is higher by 40–60°C.
The minimal value of tan δ = 0.03 was observed for
composite coatings based on polymer matrix III. As
shown in [22], owing to specific process features of pre-
paring composite coatings, ε increases with the coating
thickness, because the degree of filling of the composite
with the ferroelectric filler increases also. The corre-
sponding dependences for the POA I/PZT-1 composite
are given in [22]. The maximal value of ε = 185 in the
experimental samples of the composite coatings corre-
sponds to no more than 35 vol % filling with the fer-
roelectric filler. It should be noted that the structure and
hence the dielectric parameters of the composite coating
can depend on the material and on the state of the sur-
face of the support used. However, in this case for the
coatings of equal thickness prepared on Si/Pt supports
and Al foil we observed no differences in the dielectric
parameters exceeding the uncertainty of their determi-
nation (±10% for ε and ±0.01 for tan δ).
The characteristic features of the curves and the rela-
tionships of the thermal degradation of photoresist films
are similar to the relationships of the weight loss of the
films formed from reaction polymer solutions (Fig. 3).
The results of measuring the electrophysical
parameters of the polymer and composite coatings
are given in Table 2. For all the polymer matrices, the
values of tan δ were in the interval 0.01–0.03. The
lowest value of tan δ was observed for polymer II.
Modification of the initial polymer I with benzothiazole
rings did not lead to a noticeable increase in tan δ, but
for the most heat-resistant copolymer IV the dielectric
permittivity ε′ considerably exceeded that of the initial
polymer I (Table 2). Such an increase in the dielectric
permittivity can be attributed to increased polarity of
the structure of copolymer IV, caused by the asymmetric
structure of the polymer unit. In combination with the
resistance to temperatures of up to 480°С, this fact
allows copolymer IV to be recommended as the most
promising for the use as a polymer matrix for dielectric
composites with increased dielectric permittivity.
As shown in [22], the composite coatings
consisting of polymer matrix I and PZT-1 as a filler
are characterized by the stability of ε′ (temperature
stability up to 300°С and frequency stability up to
7
1
0 Hz) and, correspondingly, of the capacitance of the
capacitor structures. Because the temperature stability
ε΄ of the composite with a ceramic ferroelectric filler
is largely ensured by the characteristics of the polymer
matrix, enhanced (up to 480°C) heat resistance of
sulfur-containing polymer matrices allows us to expect
Introduction of PZT-1 filler, as expected, increases
both ε′ and tan δ. The reached values of ε′, depending on
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HEAT RESISTANCE AND ELECTROPHYSICAL CHARACTERISTICS
195
wider range of the temperature stability of ε′ for the
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