Open Journal of Organic Polymer Materials, 2011, 3, 1-7
doi:10.4236/ojopm.2011.11001 Published Online October 2011 (http://www.SciRP.org/journal/ojopm)
The Effect of Interfacial Interactions on a Structure and
Properties of Polyurethane Elastomer/Poly(Vinyl Chloride)
Blends
T. L. Malysheva1, S. V. Golovan1, D. L. Starokadomsky1,2
1Institute of Macromolecular Chemistry of the NAS of Ukraine
2O.O. Chuiko Institute of Surface Chemistry of the NAS of Ukraine, Ukraine
Received August 10, 2011; revised September 12, 2011; accepted September 25, 2011
Abstract
The effect of chemical structure of segmented poly(urethane-urea)s on its interfacial interactions with
poly(vinyl chloride) as well as supramolecular structure and the properties of prepared composites has been
studied. A direct influence of flexible and rigid segments of elastomers on a compatibility, structure and the
physical-mechanical properties of poly(urethane-urea)/poly(vinyl chloride) blends was investigated. A for-
mation of intermolecular hydrogen bonds network in the poly(urethane-urea)/poly(vinyl chloride) systems
was evaluated by FTIR analysis. Morphology studies have shown the effect of interfacial interactions on a
size of thermoplastic phase dispersed within elastomer matrix. Obtained poly(urethane-urea)/poly(vinyl
chloride) micro- and nanocomposites have improved tensile properties.
Keywords: Polymer Composites, Compatibility, Microphase Separation, Glass Transition, Hard Domains,
Crystallites, Associates, H-Bonds, Urethane-Urea Groups, Interfacial Interactions
1. Introduction
Recently, interfacial non-covalent interactions in poly-
mer-polymer systems have attracted the attention be-
cause of possibilities to control physical-mechanical
characteristics of the polymer materials in accordance to
requirements. It could be achieved by a formation of
stable supramolecular structure of the blends with en-
hanced interface adhesion and optimal dispersity of the
components. Strong interfacial interactions, which di-
rectly depend on chemical, thermodynamic and morpho-
logical features of the systems, increase contact surface
area, and improve dispersability of the components, and
simultaneously decrease the sizes of dispersed phase to
nano-level, leading to the formation of nanocomposites.
Among polymer blends, thermoplastic/elastomer
blends are particularly interesting due to simplified
control of physical-mechanical characteristics of the
blends over a wide range by varying their composition
and preparation conditions. Polyurethaba elastomers are
commonly modified by introducing poly(vinyl chloride)
(PVC) to produce flexible materials with enhanced
chemical, hydrolytic and environmental stability, and
improved fire resistance [1].
Overview of literature sources has shown that hetero-
geneous structure of binary polyurethane-based systems
greatly depends on the chemical structure of immiscible
flexible and rigid segments of polyurethane elastomers
[2-10]. Presence of chlorine- and oxygen-containing polar
functional groups, which could form strong intermolecu-
lar physical bonds network, significantly affect the inter-
actions of the components, structurization processes and
physical-mechanical properties of the polymer compos-
ites. Due to intermolecular hydrogen bonding between
ester carbonyl groups of polyurethane and active
α-hydrogen of PVC chains the ester-based polyurethanes
are more compatible with PVC component compared to
polyurethanes that contain ether segments in the main
chain [8].
Poly(ether-urethane)s synthesized from oligooxypro-
pylene glycol (OPG) are immiscible with PVC and its
blends are characterized by poor mechanical properties
in all compositional range. Oligooxytetraethylene glycol
(OTMG) segments of poly(ether-urethane)s are partially
compatible with PVC resulting in increased glass transi-
tion temperature of corresponding flexible segments.

T. L. MALYSHEVA ET AL. 2
Poly(ester-urethane)s with adipic acid/glycol based flexi-
ble oligoester segments form fully heterogeneous blends
with poly(vinyl chloride) component independently from
preparation techniques [9,10]. Increasing polar urethane
groups content in elastomer main chain reduces compati-
bility of the components of corresponding polymer sys-
tems [11]. There are only few works related to influence
of rigid segments of polyurethanes on its compatibility
with PVC polymer. Even though PVC suppresses the seg-
regation of rigid segments in polyurethane elastomers,
Xiao et al [8] show that polyurethane based on consider
polyurethane based on 4, 4’-diphenylmethane diisocyanate
(MDI)/1, 4-butanediol segments are immiscible with PVC.
Enhanced compatibility of the components could be de-
tected when highly polar 4, 4’-diaminodiphenylmethane
based rigid segments are introduced into poly-(urethane-
urea) elastomer macromolecules [12].
This paper investigates the influence of chemical
structure of segments of poly(urethane-urea)s on the
compatibility with poly(vinyl chloride) and the structure-
properties relationships in these polymer blends.
2. Experimental
2.1. Materials
For synthesis of poly(urethane-urea)s (PUU), oligomeric
diols such as oligooxypropylene glycol (OPG; Mw =
1000), oligooxytetramethylene glycol (OTMG; Mw =
1000) and poly(ethylene-butylene)adipate (PEBA; Mw =
2000) were used. As urethane constituent a pure
2,4-toluene diisocyanate (2,4-TDI) or mixture of isomers
2,4- and 2,6-toluene diisocyanates (2,4-TDI/2,6-TDI;
65/35 by weight) were selected. N,N-dimethylformamide
(DMF) was distilled under reduced pressure and deion-
ized water was used. Other initial components were
purified by widely used conventional methods.
Poly(vinyl chloride) (PVC) with molecular weight of
8.0×104 (by viscosimetry) and chlorine content of 56.3
wt.% was taken for preparation of the polymer compos-
ites.
2.2. Characterization
Thermophysical properties of the samples were studied
using differential scanning calorimeter DSC-2M (Kievp-
ribor, Ukraine) in the temperature range from 173 to 473
K with a programmed heating rate of 2 K/min. Following
parameters of the samples were determined: glass
transition temperatures (Tg, K), heat of fusion (Qf, J/g),
degree of crystallinity (Хcr, %) and melting point (Тm, К).
Chemical structure of the components and physical
bonds network formed in the prepared polymer blends
were evaluated via FTIR analysis using Bruker Tensor®
37 FTIR spectrometer in the spectral region of 400-4000
cm-1.
In order to characterize micro- and nano-scale hetero-
geneity of PUU/PVC, samples were characterized by
examining samples sputter-coated with gold film of 5-10
nm thickness in a scanning Electron Microscope (JEOL
JSM 6060 LA) Scanning Electron Microscope at an ac-
celerating voltage of 30 kV.
Tensile tests were performed on dumbbell-shape
specimens at ambient temperature at a crosshead speed
of 35 mm/min using an FU-1000 universal testing ma-
chine (Kazan’, Russia). The average data from five tests
are given in this work. Tensile strength at break, σb,
modulus at 100% elongation, E100, elongation at break, εb,
and residual elongation, εres, were measured.
2.3. Synthesis of Prepolymers
Prepolymers for synthesis poly(urethane-urea)s were
synthesized from olygomeric diols (OPG, OTMG or
PEBA) and aromatic diisocyanates (2,4-TDI or 2,
4-TDI/2, 6-TDI) by a conventional diisocyanate/diol
method.
2.4. Synthesis of Poly(Urethane-Urea)s
PUUs have been synthesized in DMF solution from
as-prepared prepolymers and water as typical chain
extender according to two-step method described
elsewhere [13]. Compositions of prepared poly(urethane-
urea)s was summarized in Table 1.
Poly(urethane-urea) samples with thickness of 10-15
and 200-300 μm were prepared by film casting technique
on a Teflon substrate from DMF polymer solutions. The
composite films were dried at 323 K in an oven to a
constant weight.
3. Results and Discussion
In Table 2 the basic thermophysical parameters of initial
poly(urethane-urea)s as well as prepared PUU/PVC
blends are presented.
Microphase separation between flexible and rigid
segments of pure PUU-1 leads to appearance of two
glass transition temperatures: (i) glass transition
temperature of amorphous oligoether phase (Tg1) and (ii)
relaxation of rigid domains (Tg2). PVC component has
glass transition temperature (Tg3) at 343 K. PUU-1 based
polymer blends containing 30 and 70 wt.% PVC are
characterized by presence of two relaxations due to
typical biphasic structure of the compositions.
For PUU-1/30PVC blend with 30 wt.% of PVC

T. L. MALYSHEVA ET AL. 3
Table 1. Compositional characteristics of synthesized poly(urethane-urea)s.
Sample Oligomeric
ether/ester Diisocyanate Rigid segments content [%] Intrinsic viscosity (η) [cm3/g]
PUU-1 OPG 2,4-TDI/2,6-TDI 26.8 0.08
PUU-2 OTMG 2,4-TDI 26.8 0.061
PUU-3 PEBA 2,4-TDI/2,6-TDI 8.0 0.120
Table 2. DSCa) characteristics of pure PUUs and PUU/PVC blends.
Composition
PVC
content
[wt.%]
Tg1
[К]
Tg2
[К]
Tg3
[К]
Tg4
[К]
Qf
[J/g]
Хcr
[%]
Тm
[К]
PUU-1 - 248 343 - - - - -
PUU-1/30PVC 30 258 - 356 - - - -
PUU-1/70PVC 70 248 - 328 - - - -
PUU-2 - 224 - - - - - -
PUU-2/30PVC 30 245 - 350 312 - - -
PUU-3 - 238 - - - 20,7 5,8 328
PUU-3/30PVC 30 254 - - - 5,3 1,5 323
PUU-3/40PVC 40 278 - - - - - -
PUU-3/70PVC 70 303 - 362 - - - -
a) the data from a second scan was analyzed t o eliminate thermal prehistory of the samples
content the Tg1 of elastomer matrix increases from 248 to
258 K. Relaxation transition at higher temperatures (Tg3)
related to combined transformation (degradation) of
domain structure of PUU-1 elastomer and dispersed PVC
phase. The increase in Tg3 is due to the restriction of
segmental mobility of PVC polymer chains as a result of
their intermolecular interactions with rigid segments of
the elastomer at the interface. For PUU-1/70PVC blend,
Tg3 decreases to 328 K, whereas Tg1 (relaxation of
oligoether segments) of dispersed elastomer phase is
essentially same as in the initial PUU-1. Enhancing
mutual diffusion of macromolecules of both polymers
because of its interactions at the interface should increase
Tg1, while a degradation of domain structure of elastomer
phase may initiate increasing a segmental mobility of
oligoether segments and decreasing Tg1. Probably, a
basic reason of the lower Tg1 is partial degradation of a
structure of associated hard domains in dispersed PUU-1
phase. The changes observed for glass transition tempe-
ratures may lead to improvement of interface adhesion in
studied biphasic polymer systems.
PUU-2 elastomer is characterized by single glass
transition temperature of oligoether segments. This
suggests reduced segregation of asymmetric 2,4-TDI
based rigid segments into hard domains and a formation
of smaller aggregates, which form fluctuated structure of
physical bonds network. It is clearly seen that enhancing
compatibility of PUU-2 with PVC component (at 30
wt.% of PVC) induces an appearance of new relaxation
of mixed phase (Tg4). Abnormal decreases in the density
of the blends with 15 - 50 wt.% of PVC is attributed to a
decrease in the macromolecular packing density that
results from the poor mixing of the components at the
interface and a formation of disarranged interface region
(Figure 1). A density of typically biphasic PUU-1/PVC
composites has an additive behavior that suggests poor
compatibility of the components in the heterogeneous
systems.
It is known that PEBA oligoester is immiscible with
PVC [14] and the blends of PVC with polyurethane
based on PEBA and MDI/1, 4-butanediol rigid segments
are typically biphasic systems [9]. Studies on
thermophysical properties of PEBA based pure PUU-3
elastomer and PUU-3 containing composites have shown
0 255075100
1,1
1,2
1,3
1,4
PVC content [wt.%]
Density [g/cm3]
1
2
Figure 1. Density versus PVC content plots for PUU-1/PVC
(1) and PUU-2/PVC (2) composites.
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T. L. MALYSHEVA ET AL. 4
that introducing PVC into PUU-3 elastomer matrix
decreases the heat of fusion (Qf), the degree of
crystallinity (Xcr) and crystallites size, and restricts the
segmental mobility of PEBA oligoester segments. The
composites with PVC content below 40 wt% are
characterized by suppressed crystallization of flexible
segments and the blends have only single broad glass
transition temperature. This suggests the formation of
strong physical bonds network resulted in enhancing
compatibility between components of PUU-3/PVC
blends. In other words, highly polar urethane-urea rigid
segments of PUU-3 elastomer substantially enhance a
compatibility between the components of the blends.
When the PVC content reaches 70 wt.%, phase
separation occurs as indicated by the appearance of
relaxation transition of PVC constituent were clearly
identified.
The interfacial interactions in the pure PUUs and PUU
based polymer blends were found and thoroughly studied
by FTIR spectroscopy analysis. Participation of
urethane-urea functional groups in hydrogen bonding
(H-bonding) processes was estimated by comparative
analysis of NH stretching vibrations band (sNH) in the
spectral region of 3500-3200 cm-1. The involvement of C
= O groups in hydrogen bonds network was determined
by analysis of amide I band in the region of 1800-1600
cm-1. The presence of urea groups in PUUs mainchain
changed the polarity of rigid and flexible segments of
polymer and hydrogen bonding between C = O of urea
and NH groups of rigid segments. As an internal
standard the reference aromatic C = C stretching
vibration band (C = C) at about 1600 cm-1 was selected.
Basic FTIR characteristics of the functional groups,
which participate in H-bonding, have been summarized
in Table 3. Wavenumber band position (ν), optical
density (D), a quantity of self-associated C = O of urea
(α) and the integrated intensity of the hydrogen bonded
NHb-groups (ANH) were determined and analyzed.
In FTIR spectrum of PUU-1 sample (Figure 2) the
characteristic bands of self-associated H-bonded C = O
of urea (referred as C = Ocb) and urethane (referred as C
= Oub) functional units of rigid segments of the PUU
macromolecules are identified. Additionally, the
presence of non-bonded (“free”) carbonyls of urethane
and NH of urethane H-bonded with ether fragments were
also determined.
The quantity of self-associated C = Ocb groups of urea
(α value) was calculated from spectral data as a ratio of
band areas of C = Ocb and all C = O groups of
poly(urethane-urea). The α value for pure PUU-1 was
calculated as 0.104. Addition of 30 wt.% PVC to PUU-1
decreases α value by 15 % increases the absorbance of C
= Of by 5.8 %, while the intensity of C = Oub at ν = 1693
cm-1 remains unchanged. Despite of the destruction of
NHδ+…δ–O = C type hydrogen bonds network the
integrated intensity of the ANH decreases by only 5 %.
Thus, the changes in FTIR spectra are indicative of
partial destruction of domain structure of elastomer
matrix due to interfacial interactions of urethane-urea
NH groups with chlorine function of the PVC
thermoplastic. Similar intermolecular hydrogen bonding
of NHδ+…Clδ– type in PUU/PVC systems was earlier
reported earlier[12]. Intermolecular interactions between
PVC and rigid segments of PUU increase the Tg3 in the
blends. Decrease in the intensity of C = Ocb band by 52
% and large increase in the optical density of C = Of
band (see Figure 3, curve 2) with increasing PVC
content up to 70 wt.% could be due to fewer associated
rigid segments. Aforementioned data confirm the DSC
results on the effect of partial destruction of associated
rigid segments on Tg1 in PUU-1/70PVC system.
A much greater influence of dispersed PVC
thermoplastic phase has been found on the
supramolecular structure of PUU-2 elastomer matrix
(Figure 3). The level of association of the urea groups
association in OTMG-based PUU-2 is higher than in
OPG-based PUU-1. For the PUU-2/30PVC blend, the C
= Ocb content decreases by 80% and ANH value decreases
by 12%. C = Ocb content reaches 80% and ANH value
reduces by 12%. Stretching vibrations band of NH
groups shifts from 3302 to 3298 cm-1 and a shoulder
appears in the region of 3420-3380 cm-1 due to stretching
vibrations of “free” (non-bonded) NH groups. These
changes provide evidence for extensive
Table 3. FTIR spectral characteristics of PUUs and PUU based polymer blends.
С = Ocb C = Of NHb
Sample ν
[сm-1]
Di
[a.u.] α ν [сm-1]
Di
[a.u.]
ν
[сm-1] АNH
PUU-1 1638 1,46 0,104 1730 3,36 3290 8,1
PUU-1/30PVC 1638 1,16 0,088 1728 3,57 3288 7,8
PUU-1/70PVC 1639 0,84 0,050 1730 8,05 3290 6,8
PUU-2 1643 1,05 0,150 1730 1,73 3302 4,1
PUU-2/30PVC 1644 0,22 0,015 1728 1,92 3298 3,6
PUU-2/70PVC 1652 0,36 - 1729 1,95 3303 3,2

T. L. MALYSHEVA ET AL. 5
1600 1800
Wavenumber [cm-1]
Absorbance [a.u.]
1638
1730
1693
Figure 2. FTIR spectra of PUU-1 (1) and PUU-1/PVC
composites with 30 wt.% (2) and 70 wt.% (3) of PVC.
1600 1700
Wavenumber [cm-1]
Absorbance [a.u.]
1643
1730
1717
3300
1
2
3
3302
3298
3303
Figure 3. FTIR spectra of pure PUU-2 (1), PUU-2/30PVC (2)
and PUU-2/70PVC (3) compositions.
destruction of intramolecular hydrogen bonds network in
elastomer matrix as a result of stronger interface of
NHδ+…Clδ– interactions at the interfacial layer.
Introducing PUU elastomer in PVC thermoplastic
matrix (PUU-2/70PVC sample) gives rise to a broad
band of weakly associated and “free” urea groups in the
FTIR spectrum (Figure 3, curve 3). The decrease in ANH
and a shift of stretching vibrations band of NH groups to
high wavenumbers confirm a reduction in both the
interfacial interactions and the compatibility between the
blend components.
FTIR spectra of initial PUU-3, which was synthesized
using oligoester constituent (in contrast to both
oligoether based PUU-1 and PUU-2), and PUU-3
containing composites are shown in Figure 4.
In the spectrum of pure PUU-3, there is an intense C =
Of band at ν = 1727 cm-1 and a weak NHb band at ν =
3340 cm-1. This shows that a major part of carbonyls are
“free”, indicating a low level of participation of C = O in
H-bonding processes. In FTIR the spectrum of
PUU-3/40PVC, an intense band due tostretching
vibrations of H-bonded carbonyls appears at 1723 cm-1 as
a result of interfacial interactions between C = O of ester
groups of PUU-3 and active α-hydrogen of PVC chains.
Increase in the integrated intensity of NHb band by 68 %
is due to interactions between NH of urea and chlorine of
PVC. Thus, hydrogen bonds are formed in the blend
mainly via NHδ+…δ–O = C bonds and partially, from
NHδ+…Clδ– bonds (due to small content of urea groups).
DSC data show that the prepared blend is a single phase
system. Increasing PVC content to 70 wt.% increases the
fraction of “free” C = О and decreases ANH value as a
result of the reduced compatibility between the blend
components and the formation of heterogeneous
structure of the blends occurs.
The FTIR spectrum of thermoplastic/elastomer blends
at 30 wt.% of elastomer content in the spectral region of
C-Cl stretching vibrations is presented in Figure 5. The
relative intensities of the bands at 615 and 638 cm-1 are
routinely used for the estimation of the degree of
crystallinity, stereoregularity and conformation re-
arrangements in PVC polymer. The ratio of the optical
densities of the C1 stretching bands at 638 cm-1 (D638)
from the crystalline region of syndiotactic polymer and
at 615 cm-1 (D615 ) from the atactic polymer is generally
used for evaluation of an index of crystallinity (K) of
PVC using Equation 1.
638
315
D
KD  (1)
The degree of crystallinity (globular crystallites) of
PVC, is 10% from wide angle X-ray diffraction analysis,
and the K value is 1.04 from FTIR data. Introducing 30
wt.% of poly(urethane-urea) elastomer into PVC matrix
reduces K value to 0.95, 0.92 and 0.88 for PUU-1,
PUU-2 and PUU-3, respectively. This large effect on the
conformation and the crystallinity of PVC matrix su-
ggests that has dispersed PUU-3 phase is dispersed in the
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opyright © 2011 SciRes. OJOPM

T. L. MALYSHEVA ET AL. 6
1600 1800
Wavenumber [cm-1]
Absorbance [a.u.]
1727
1723
1730
3300
1
2
3
3340
Figure 4. FTIR spectra of PUU-3 (1), PUU-3/40PVC (2) and
PUU-3/70PVC (3) samples.
600 700
Absorbance [a.u.]
Wavenumber [cm-1]
2
3
4
1
615
638
Figure 5. FTIR spectra of PVC (1), PVС/30PUU-1 (2),
PVС/30PUU-2 (3) and PVС/30PUU-3 composites (4).
PVC matrix.
Finally, based on FTIR spectral analysis, it can be de-
duced that the chemical structure of poly(urethane-urea)
significant influence on interfacial interactions (hydrogen
H-bonds network), which in turn affects to str-
ucturization processes and the final properties of the
polymer blends.
Influence of interfacial interactions on morphology of
the composites were evaluated by analyzing the samples
in a scanning electron microscope. SEM micrographs of
heterogeneous PUU-1/30PVC composition showed an
average particle size of 1-2 μm (Figure 6(a)). The
stronger interfacial interactions in PUU-2/30PVC system
substantially reduce an average particles size of
dispersed PVC phase to 80 - 200 nm (Figure 6(b)).
PUU-3/30PVC sample was characterized by fine
dispersion of the components at molecular level and the
blend could be referred as typical nanocomposite
(Figure 6(c)).
Mechanical properties of poly(urethane-urea)/poly
(vinyl chloride) composites are presented in Figure 7.
Tensile strength at break (σb) values for PUU-1/PVC
composites is higher than that due to additivity alone
because of the enhanced interfacial adhesion between the
components. σb in PUU-2/PVC and PUU-3/PVC co-
mpositions containing 30 - 50 wt.% of thermoplastic
show large compositional dependence. Elasticity mo-n
dulus at 100 % elongation (E100) for PUU-3 based
composition decreases at low (~30 wt.%) PVC content as
a result of decreasing in a crystallinity Elasticity modulus
at 100 % elongation (E100) for PUU-3 based composition
decreases at low (~30 wt.%) PVC content as a result of a
decrease in the crystallinity of oligoester segments. In
contrast, E100 grows at higher thermoplastic co-
ncentrations. From the data presented in Figure 7 it
could be seen that basic physical-mechanical properties
of the micro- and nano-structurized poly-(urethane-urea)
Figure 6. SEM images of PUU-1/30PVC (a), PUU-2/30PVC
(b) and PUU-3/30PVC (c) compositions.

T. L. MALYSHEVA ET AL. 7
00
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4. Conclusions
The chemical structure of flexible and rigid segments of
poly(urethane-urea)s have a large influence on the inte-
rfacial interactions and compatibility of poly (ure-
thane-urea) elastomer and poly(vinyl chloride) therm-
oplastic. An increase in the energetic characteristics of
hydrogen bonds networks dramatically reduces the size
of dispersed PVC thermoplastic phase in elastomer
matrix. This micro- and nano-structurized poly(uret-
hane-urea)/poly(vinyl chloride) thermoplastic elasto-
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