NR/EPDM elastomeric rubber blend

miscibility evaluation by two-level fractional

factorial design of experiment
Cite as: AIP Conference Proceedings 1614, 82 (2014); https://doi.org/10.1063/1.4895176
Published Online: 17 February 2015

Jeefferie Abd Razak, Sahrim Haji Ahmad, Chantara Thevy Ratnam, et al.

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 NR/EPDM Elastomeric Rubber Blend Miscibility
Evaluation by Two-Level Fractional Factorial
Design of Experiment

Jeefferie Abd Razaka,c, Sahrim Haji Ahmada, Chantara Thevy Ratnamb,

Mazlin Aida Mahamoodc, Juliana Yaakubc and Noraiham Mohamadc
a
School of Applied Physics, Faculty of Science and Technology, Universiti Kebangsaan Malaysia,
43600, UKM Bangi, Selangor, Malaysia
b
Composites and Polymer Blends Group, Radiation Processing Technology Division,
Malaysian Nuclear Agency, Bangi, 43000, Kajang, Malaysia
c
Carbon Research Technology Group, Advanced Manufacturing Centre of Excellence, Universiti Teknikal Malaysia
Melaka, Hang Tuah Jaya, 76100, Durian Tunggal, Melaka, Malaysia

Abstract. Fractional 25 two-level factorial design of experiment (DOE) was applied to systematically prepare the
NR/EPDM blend using Haake internal mixer set-up. The process model of rubber blend preparation that correlates the
relationships between the mixer process input parameters and the output response of blend compatibility was developed.
Model analysis of variance (ANOVA) and model fitting through curve evaluation finalized the R 2 of 99.60% with
proposed parametric combination of A = 30/70 NR/EPDM blend ratio; B = 70°C mixing temperature; C = 70 rpm of
rotor speed; D = 5 minutes of mixing period and E = 1.30 phr EPDM-g-MAH compatibilizer addition, with overall 0.966
desirability. Model validation with small deviation at +2.09% confirmed the repeatability of the mixing strategy with
valid maximum tensile strength output representing the blend miscibility. Theoretical calculation of NR/EPDM blend
compatibility is also included and compared. In short, this study provides a brief insight on the utilization of DOE for
experimental simplification and parameter inter-correlation studies, especially when dealing with multiple variables
during elastomeric rubber blend preparation.
Keywords: NR/EPDM blend; parametric combination; desirability; output response; miscibility; inter-correlation; two-
level factorial design
PACS: 81.05.Lg 81.05.Ue

INTRODUCTION
Polymer blending can be developed more rapidly with tailored outstanding properties and cost saving than the
development of new polymer compound [1-2]. Currently, various researches on elastomeric rubber blend has been
conducted and reported by many authors [1-4]. Most of the blend like NR/EPDM, NR/NBR, NR/SBR, NR/EVA,
SBR/NBR [4], NBR/EVA [1], NBR/HNBR [2] and NR/CR were incompatible and need to be improved accordingly
to suit their specific targeted applications. For the past few years, many researchers have employed natural rubber
(NR) and ethylene-propylene-diene-monomer EPDM synthetic rubber for the preparation of elastomeric blends [5-
14]. Vulcanized NR/EPDM blend systems have been extensively studied because of their superior performance in
tire application, as well as significant improvement in heat and ozone resistance [9]. In addition, the presence of
various functional fillers in NR/EPDM blends enhances the engineering properties and its functionalities.
The processing condition like mixing speed, blending period and temperature provide a strong influence on the
resulted properties of the blend [2]. Parametric testing of blend preparation has been studied and reported previously
by many authors through conventional one parameter at time approach without considering the inter-correlation
effects between involving processing factors [5, 8, 15-19]. However, limited or no works deals with rubber or
polymer blend using Design of Experiment (DOE) strategy in their study has been highlighted. This study is mainly
to develop a process model of NR/EPDM blend preparation which correlates the relationship between the internal
mixer process input parameters and the resultant blend compatibility. Tensile strength as output response was
evaluated by using a systematic fractional two level factorial design of experiment and later, the best parametric
combination of NR/EPDM blend processing attributes is suggested. The theoretical calculation using Schneier’s

The 2014 UKM FST Postgraduate Colloquium

AIP Conf. Proc. 1614, 82-89 (2014); doi: 10.1063/1.4895176
© 2014 AIP Publishing LLC 978-0-7354-1250-7/$30.00

82
equation was also included as to evaluate the compatibility between NR and EPDM and to compare with the
experimental findings.

MATERIALS AND METHODS

The commercial grade SMR 20 supplied by Mentari Equipment and Project Sdn. Bhd. has 0.16 max. %wt. dirty
retained on 44 apertures, 1.00 max. % wt. ash content, 0.60 max. %wt. nitrogen, 0.80 max. %wt. volatile matter, 30
min Wallace rapid plasticity (Po) and 40 min. % of plasticity retention index (PFU). Ethylene propylene diene rubber
(EPDM) grade BUNA EP T 9650 was supplied by LANXESS, Pittsburgh, USA. The Mooney viscosity UML (1+8)
at 150°C is 60±6 MU, ethylene content 53±4 wt%, ENB content 6.5±1.1 wt% with volatile matter ≤ 0.75 wt%,
specific gravity 0.86 and total ash ≤ 0.50 wt% with non-staining stabilizer. Both rubber were masticated with two-
roll mill prior of their use. Other compounding ingredients such as sulphur, zinc oxide and stearic acid were
purchased from Systerm/Classic Chemical Sdn. Bhd., and tetramethylthiuram disulfide (TMTD) from Aldrich
Chemistry; N-cyclohexylbenthiazyl sulphenimide (CBS) and N-(1,3-Dimethylbutyl)-N’-phenyl-p-phenylenediamine
(6PPD) were supplied by Flexyx America, USA and all are used as received. The compounding process was
performed in accordance to ASTM D-3192. The formulations recipes were summarized in the TABLE (1) for all
NR/EPDM blend.

TABLE (1). Compounding formulation used in NR/EPDM blend preparation .

NR/EPDM system EPDM-g-MAH ZnO Stearic acid 6-PPD CBS TMTD Sulphur

30 - 50 phr of EPDM 1.00 - 5.00 5.00 2.00 2.00 1.00 0.30 1.50

The cure characteristic testing was conducted in accordance to ISO 3417 for maximum cure time tc90. The
compounded NR/EPDM nanocomposites blend were vulcanized using a semi EV system in a hot press on a three
pieces preheated die placed on 46 cm x 46 cm platen using an electrically heated press maintained at the temperature
of 150°C with 150 kgf of the molding pressure. The experimental design was generated by using the Design Expert
6.0.10 software implementing the fractional two-level factorial design of 25.Three center points with one replication
and no blocks were selected to increase the reliability and the acceptance level of the resulted outcomes. The design
generates overall 19 set of sample preparation with parametric combination as per listed in TABLE (2). The real
values for each factor coded are listed in the TABLE (3). The compounding process for NR/EPDM blend and the
testing of the fabricated samples were done in a random order following to the generated experimental design as per
suggested by the software. The analysis was conducted based on the step-by-step approach started with the
meaningful effects selection, model selection, and model analysis by using the analysis of variance (ANOVA) and
then ended by the model fitting through the model curve evaluation.
Tensile test as output response was carried out according to ASTM D1822 on a testometric tensometer Toyoseiki
Strograph-R1. Dumb-bell shaped specimens of ~2 mm thickness were cut from the molded sheet with a Wallace die
cutter. The specimens were tested at a crosshead speed of 500 mm/min and the tests were performed at 23±2°C of at
least 7 samples. The averaged tensile strength in MPa unit was then input to the DOE software for statistical analysis
and data validation. To support the discussion, the fracture surface micrographs viewed by SEM are also included.

RESULTS AND DISCUSSION

Compatibility Evaluation using Heat of Mixing Calculation

Khalf et al. [20] used the theoretical calculations heat of mixing to investigate the compatibility of NBR/SBR
blends according to Schneier’s Equation which is:

83
 ª X2 º 1
'Hm { X 1M 1U1(G 1  G 2) 2 «  (1  X 1) M 1U1) 2 »} 2 (1)
¬ (1  X 2) M 2 U 2 ¼

X, ρ dan M are the weight fraction of the polymer, density, and monomer unit molecular weight respectively, δ
(cal/cc)½ is the solubility parameter of the polymers. The heat of mixing plots over the entire range of compositions
and weight percent in NR/EPDM blend is plotted (FIGURE 1). Polymer pairs of calculated heat of mixing under the
value 41.85x10-3 J/mole are considered to be compatible and on the other hand blends with heat of mixing upper
than this limit are considered to be incompatible, thermodynamically [20]. For the incompatible case, the
macromolecules in this blend mixture are in a disordered state [21]. The range at 0.30 to 0.50 weight fraction of NR
falls within the limit line of the theoretical compatibility. Thus, 30 to 50 phr of EPDM component was blended with
NR for the best processing parametric decision.

TABLE (2). Parametric combination for NR/EPDM blends preparation using 2 5 fractional factorial design strategies.

Experiment NR/EPDM Ratio Mixing Temperature Rotor Speed Mixing Period EPDM-g-MAH
[A], phr [B], °C [C], rpm [D], minutes Content [E], phr
1 -1 -1 -1 -1 +1
2 +1 -1 -1 -1 -1
3 -1 +1 -1 -1 -1
4 +1 +1 -1 -1 +1
5 -1 -1 +1 -1 -1
6 +1 -1 +1 -1 +1
7 -1 +1 +1 -1 +1
8 +1 +1 +1 -1 -1
9 -1 -1 -1 +1 -1
10 +1 -1 -1 +1 +1
11 -1 +1 -1 +1 +1
12 +1 +1 -1 +1 -1
13 -1 -1 +1 +1 +1
14 +1 -1 +1 +1 -1
15 -1 +1 +1 +1 -1
16 +1 +1 +1 +1 +1
17 0 0 0 0 0
18 0 0 0 0 0
19 0 0 0 0 0

TABLE (3). Selected level of variables for NR/EPDM blends preparation.

NR/EPDM Ratio Mixing Temperature Rotor Speed Mixing Period EPDM-g-MAH Content
(phr) (°C) (phr) (minutes) (phr)
30 (-1) 70 (-1) 50 (-1) 5.0 (-1) 1.0 (-1)
40 (0) 90 (0) 60 (0) 7.0 (0) 3.0 (0)
50 (+1) 110 (+1) 70 (+1) 9.0 (+1) 5.0 (+1)

Regression Analysis for Output Response of NR/EPDM Blend Tensile Strength [Y]
Using fractional 25 factorial designs in DOE generates half normal plot as shown in the FIGURE 2 (a). It can be
seen that variable A, B, D and E as well as the interaction term of AD, CD, DE, AE, BE, BC and AC were
positioned away from the straight line (significance terms) and about four variable and interaction point were plotted
in line (non-significance terms). From the effect list, the variable D (mixing period) is listed as the most significance
factor with percent contribution of 26.20% and sum of square (SS) of 2.88. The variable C (rotor speed) contributed
very less to the response with only 0.038% contribution and can be neglected. The effects of every model terms
were given in Table 4. All single variables effects are negative suggesting that decreasing A, B, C, D and E from the
high level to the low level will increase the tensile strength response. The interaction effect between variable AB,
BD and CE are extremely small and not significance. Positive interaction between AD, BE and DE indicates good
dependent between both independent variable in effecting the miscibility response of NR/EPDM blend in terms of
their tensile strength attribute. FIGURE 2 (b) is a plot of the residuals versus the predicted values of the tensile
strength. This plot appears satisfactory and there are no reasons in suspecting problems with the validity of

84
experimental conclusions whereby the residuals plot appears approximately along a straight line and then the
normality assumptions is satisfied.
For NR/EPDM blend processing parameter testing, the analysis of variance (ANOVA) stated that the model F-
value of 104.33 implies the model is significant and there is only a 0.01% chance that a “Model F-Value” this large
could occur due to noise. It is also analyzed that variable and interaction terms A, B, D, E, AC, AD, AE, BC, BE,
CD and DE are significant model terms since all of them were selected as model terms with P value are less than
0.0500. The curvature F-value of 345.61 implies there is significant curvature as measured by difference between
the average of the center points and the average of the factorial points in the design space. There is only a 0.01%
chance that a curvature F-value this large could occur due to noise. This model is accurate and can be used to
navigate the design space since it show a high coefficient of determination of R 2 value. The R2 implies that the
sample variation of 0.9960 for tensile strength is attributed to the independent variables tested. The R 2 value also
indicates that only 0.083% of the total variation was not explained by the model.

FIGURE 1. Heat of mixing plot for NR/EPDM blend at various weight fraction of NR.

FIGURE 2. (a) Half normal plot of NR/EPDM blend tensile strength; (b) Plot of residuals versus predicted tensile strength
response for NR/EPDM blend.

TABLE (4). The effect list of every model terms for NR/EPDM blending process
using Haake internal mixer.
Term Studentised Effects Sum of Squares % Contribution
A -0.19 0.14 1.32
B -0.58 1.34 12.21
C -0.032 4.128E-003 0.038
D -0.85 2.88 26.20
E -0.32 0.40 3.61
AC -0.52 1.10 9.95
AD 0.17 0.12 1.06
AE -0.27 0.29 2.61
BC -0.49 0.97 8.80
BE 0.48 0.93 8.47

85
 CD -0.21 0.17 1.54
DE 0.25 0.25 2.31

The regression model that used to predict the tensile strength response at any point in the space spanned by the
factor is given as follows:

Y = +5.39 – 0.095*A – 0.29*B – 0.016*C – 0.42*D – 0.16E – 0.26*AC + 0.085*AD – 0.13*AE – 0.25*BC +
0.24*BE – 0.10*CD +0.13*DE (2)

TABLE (5). Analysis of Variance for experimental data of NR/EPDM blend preparation/
Source of Sum of squares Degrees of Mean square Fo P-Value
variation freedom
Model 8.60 12 0.72 104.33 < 0.0001
A 0.14 1 0.14 21.11 0.0059
B 1.34 1 1.34 195.67 < 0.0001
C 4.128e-003 1 4.128E-003 0.60 0.4732
D 2.88 1 2.88 419.92 < 0.0001
E 0.40 1 0.40 57.93 0.0006
AC 1.10 1 1.10 159.53 < 0.0001
AD 0.12 1 0.12 16.96 0.0092
AE 0.29 1 0.29 41.87 0.0013
BC 0.97 1 0.97 141.05 < 0.0001
BE 0.93 1 0.93 135.66 < 0.0001
CD 0.17 1 0.17 24.63 0.0042
DE 0.25 1 0.25 37.02 0.0017
Curvature 2.37 1 2.37 345.61 < 0.0001
Error 0.033 2 0.017
Total 11.01 18

Equation (2) indicates the first order regression model with negative (-ve) notation for all single variables
indicates all parameter are at high level of their range. The intercept is the grand average of all 19 observations, and
the regression coefficient of -0.095, -0.29, -0.016, -0.42 and -0.16 are one-half the corresponding factor effect
estimates based on a two-unit change (from -1 to +1). Three-dimensional response surface plot of tensile strength is
depicted as in the Figure 3a. The response surface plot is based on the fitted first order model from the regressors B
and E which contributing higher effect to the output response. Based on the examination of the fitted surface, it is
clear that the tensile strength is maximum at 7.281 MPa as lower mixing temperature (B) and lower amount of
EPDM-g-MAH compatibilizer (E) is used. For instance, addition of EPDM-g-MAH creates access EPDM content in
the formulation recipes. EPDM had lower mechanical properties as compared than NR. Thus, the negative constant
value of E in the regression equation clearly indicates the contribution of EPDM-g-MAH compatibilizer in reducing
the response yield. However, the negative effects of D could be improved in the interaction terms of BE and DE
whereby the interaction with B and D factor are benefited for the response properties enhancement. The negative
constant value of A and E are well correlated between each other to support the finding by previous author that
found the decreased in the tensile strength could occurred with the increasing weight ratio of EPDM in the blend
[10]. This also agreed and confirmed by another author on their work of NR/EPDM blend with varied blending ratio
which the output response is reduced as the EPDM content increase [7]. This reduction in tensile strength is due to
the incompatibility and poor interfacial adhesion between the NR and the EPDM or R-EPDM rubber which resulted
from the difference in unsaturation level between NR and EPDM results in a maldistribution in the blend system [7],
[22]. NR rich blend exhibits higher TS due to the NR crystallinity exhibited upon stretching [7]. The interaction
term of D with E shows the highest effect of tensile strength with positive coefficient value of 0.13. This indicates
that the mechanical shearing effect introduced by a Banbury rotor rotation provides a significant contribution to the
Y response. Thus, the higher the rotor speed could possibly results the higher performance of blend tensile strength
properties. This may due to an increase interaction generated between NR and EPDM phase through high shearing
of rotor in the confined mixer space which later improve the compatibility between them. The interaction of this
factor with E, the EPDM-g-MAH compatibilizer provides positive effects in enhancing the tensile strength response.
This clearly tells the capability of a rotor speed in assisting the dispersion of EPDM-g-MAH within the blend phases

86
to provide chemically good interaction between the NR and EPDM that improves the mechanical behavior of the
tensile strength. This also applies to the interaction term AD. EPDM and R-EPDM are highly saturated elastomers
due to their saturated backbones and low diene content. The blending of EPDM with highly unsaturated NR resulted
in a cure rate mismatch in the rubber phases. The difference in the molar concentrations of double bonds in each
elastomer resulted in differences in the polarity, number of allylic sites for sulphur vulcanization and reactivity of
the crosslink sites [22]. Curatives, which are considered to be polar molecules, generally exhibit greater diffusion
into NR, resulting in differences in the reactant concentrations and thus an uneven crosslink distribution and inferior
tensile strength [22]. However, through this study, it is believed that the rotor speed could perform its role in
improving the incompatibility between both rubber phases.
However, as to predict the best parametric combination of NR/EPDM blend preparation using Haake internal
mixer with good reproducibility of the tensile strength result that representing the miscibility of the blend, the
optimization menu is utilized. All the variables were limit in range and the output response is targeted into a
maximum goal creates the final solution of parametric combination with predicted value of maximum tensile
strength at 7.17237 Mpa that is suggested in the ramps mode as depicted in the Figure 3(b). With higher desirability
of about 0.966, the best parameter of each variable is proposed as A = 30/70 NR/EPM; B = 70°C, C = 70 rpm; D = 5
minutes and E = 1.30 phr.
The proposed parameter by Design Expert software was then validated by repeating the experiment using the
parameter given. It is found that the suggested experiment is repeatable with lower deviation of only +2.09% with
maximum tensile strength obtained at 7.322 Mpa. The fracture morphology of NR/EPDM blend compounded with
this parameter of processing is depicted as in the FIGURE 4 as to support the discussion on blend miscibility. It is
assumed that the higher the tensile strength, the better the miscibility of produced NR/EPDM blend. Selection of
accurate and reliable combination of processing parameters with the best value of each is required to improve the
processability and miscibility of the rubber blend. The SEM tensile fractured micrographs for NR/EPDM blend
prepared by using the selected parameters obtained from this study are presented in FIGURE 3. Uncompatibilized
NR/EPDM blend clearly shows the phase separation and segregation of EPDM phase within NR phase (FIGURE 3
(a)), while compatibilized NR/EPDM blend shows minor phase of EPDM seems embedded within a major phase of
NR. Addition of EPDM-g-MAH at a suggested amount by the DOE software, successful in improving the chemical
and physical interaction between NR and EPDM phases where the wettability and dispersion of non-polar and
saturated EPDM within the double-bond polar and non-saturated NR rubber phase component is better than
uncompatibilized blend.

FIGURE 3. (a) Response surface plot of tensile strength of NR/EPDM blend; (b) Ramp mode suggestion of parametric
combination for the best NR/EPDM blend tensile strength.

CONCLUSION
Systematic blending of NR/EPDM rubber blend using DOE two-level fractional factorial approach is applied in
this study. Low level (-1) for all single variable except high level (+1) for D factor gives increase value to the output

87
 response. Furthermore, B and D variable play a dominant role in influencing the response with contribution of 12.21
and 26.20%, respectively. At the end, parametric combination for each variable is proposed as A = 30/70 NR/EPM;
B = 70°C, C = 70 rpm; D = 5 minutes and E = 1.30 phr; which provides small deviation at +2.09% for maximum
tensile strength at 7.17237 MPa and higher desirability at 0.966 and R 2 of 99.60%. The ratio of NR/EPDM
suggested by the process model also is well correlated with the theoretical calculation using heat of mixing
understanding. In overall, improved miscibility for incompatible NR/EPDM blend could be obtained through correct
manipulation of combinatorial effects of the processing variables and this could be best to carried out by using the
process model method with tensile strength as an output response.

FIGURE 4. (a) NR/EPDM blend without EPDM-g-MAH compatibilizer addition (3000x Magnification); (b) NR/EPDM blend
with 1.30 phr EPDM-g-MAH compatibilizer additions (3000x Magnification).

ACKNOWLEDGEMENT
We are greatly acknowledged research funding of FRGS/2012/FKP/TK04/02/1/F00132 – Universiti Teknikal
Malaysia Melaka (UTeM). Special thanks to Carbon Research Technology (CRT), UTeM and Mr. Mohd Iqbal
Shueb (MNA – Polymer Division, MNA) for the continuous mutual support and knowledge transfer. Corresponding
author would like to express his special gratitude to Ministry of Education, Malaysia (MOE), Universiti Kebangsaan
Malaysia (UKM), Universiti Teknikal Malaysia Melaka and Malaysian Nuclear Agency (MNA) for special financial
and technical supports which made this work possible.

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