Applied Surface Science 258 (2012) 88618866

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Applied Surface Science

journal homepage: www.elsevier.com/locate/apsusc

Antistatic modication of polypropylene by incorporating Tween/modied

Tween
Anna Zheng a, , Xiang Xu a , Huining Xiao b , Na Li a , Yong Guan a , Shuzhao Li a
a
Key Laboratory for Ultrane Materials of Ministry of Education, School of Materials Science and Engineering, East China University of Science and Technology, Shanghai 200237,
China
b
Department of Chemical Engineering, University of New Brunswick, Fredericton, New Brunswick, Canada E3B 6C1

a r t i c l e

i n f o

Article history:
Received 5 March 2012
Received in revised form 15 May 2012
Accepted 19 May 2012
Available online 28 May 2012
Keywords:
Tween
Polypropylene
Antistatic
Crosslinking
Surface treatment

a b s t r a c t
Tween, one type of non-ionic surfactants, was used as inner antistatic agent of polypropylene (PP) and the
antistatic performance of PP/Tween sheets were evaluated by surface resistivities (s ) and water contact
angles. The inuence factors including hydrophilelipophile balance (HLB) of Tween, addition amount,
process conditions and atmospheric humidity were investigated in detail and the results showed Tween
40 with HLB at 15.7 provided PP an optimum antistatic effect with surface resistivity of 1010 /sq, water
contact angle of 57 , and surface energy of 49.5 mN/m. The s of PP/Tween sheets declined approximately
1 order of magnitude with 10% increasing of relative humidity. In order to improve the washing endurance
of antistatic PP, a combination of T40 and cationic PP (CPP) were blended with PP and PP/CPP/T40 sheets
revealed improved washing durability, with s below 1011 /sq after ultrasound washing. In addition,
T40 with double bonds was synthesized and UV crosslinking of modied T40 on PP surface also presented
denite effects on water resistance.
2012 Elsevier B.V. All rights reserved.

1. Introduction
Polypropylene (PP) is one of the most widely used thermalplastics in packaging material, textile, electric appliances, and
automobile parts. However, PP products are easily accumulated
electrostatic charges due to the inherent high insulativity, causing troubles such as electric shocks and damages to the electronic
machines [13]. In particular, the biaxially oriented polypropylene
(BOPP) lms are easy to attract dusts and cling together due to the
electrostatic charges generated by friction, thus their productivity
is inuenced signicantly. In order to eliminate the static, the way
of blending antistatic agents into the PP matrix is popular under
current circumstance [2,3].
Many researchers are engaged in looking for novel antistatic
agents, such as carbon nanotubes [4,5], intrinsically conductive
polymers (ICP) [610], ionic polymers [11], and so on. Such conductive additives eliminate the electrostatic by forming a continuous
conducting network inside the plastic matrix [12]. The drawbacks
lie on large quantities of conductive additives (usually above 5%)
being needed to form transmission paths, so the reduction of the
optical transparency and alteration of the mechanical properties
often limit the application range, especially for BOPP lms.

Corresponding author. Tel.: +86 18917949223.

E-mail address: zan@ecust.edu.cn (A. Zheng).
0169-4332/$ see front matter 2012 Elsevier B.V. All rights reserved.
http://dx.doi.org/10.1016/j.apsusc.2012.05.105

Up to now, the widely used antistatic agents in industry are a

type of low molecular weight surfactants, which are the soap-like
compounds with a hydrophobic and a hydrophilic part [13], including cationic antistatic agents (e.g. dimethyl octadecyl hydroxy ethyl
ammonium nitrate), anionic antistatic agents (e.g. alkyl phosphate
diethanol amine salt), non-ionic antistatic agents (e.g. polyethylene glycol octadecyl ether) and ampholytic antistatic agents (e.g.
1-carboxyethyl-2-alkyl imidazoline sodium salt). Among them,
non-ionic antistatic agents are more popular due to their nontoxicity, good thermal stability, and high transparency. When
blended with plastics with low addition amount (usually less than
1%), such surfactants migrate to the surface and enhance the surface
conductivity by attracting a layer of water.
However, the antistatic agents with low molecular weight are
easily removed and washed out from the surface, consequently limiting their effect over time. In order to immobilize the antistatic
agents, UV crosslinking of modied surfactants on the surface is
investigated in current research. Such method has scarcely been
reported and is potential to be applied in industry due to its convenience.
to
the
previous
research
[14],
the
According
hydrophilelipophile balance (HLB) of the surfactant is of great
signicance to its antistatic performance. In order to nd antistatic
agents with proper HLB, Tween and Span surfactants, which have
different HLB values, were investigated as antistatic agents for
PP. As shown in Scheme 1, Tween and Span surfactants are nonionic surfactants with similar polysorbate structures, which are

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A. Zheng et al. / Applied Surface Science 258 (2012) 88618866

at room temperature, 10 MPa for 5 min. The sheet samples were

cut into 80 mm 90 mm 1 mm sheets for testing.
To fabricated the antistatic PP samples with immobilized antistatic agents, PP, antistatic agent combination (MT40, TPO) and
antioxygen 1010 (0.2 wt%) were made into sheet samples rstly and
then the sheets were treated under a 500 W UV light for a prescribed
time.
2.4. Characterizations of PP sheet samples

Scheme 1. Structures of Tween and Span surfactants.

nominated by the alkyl groups such as T20 (laur-), T40 (palmic-),

T60 (stearic-) and T80 (oleic-). T65 and T85 have three stearic and
oleic groups in one molecule, respectively, while Span surfactants
have no polyether in comparison to Tween. Such surfactants show
different hydrophilichydrophobic properties and are widely
used in food additives [15], cosmetics [16], detergents [17] and
self-assembly [18]. However, being used as antistatic agents for PP
is rarely reported.
In this work, Tween and Span surfactants were blended with PP
to fabricate antistatic PP sheet samples. The antistatic properties of
sheet samples were evaluated by means of surface resistivities and
water contact angle. The inuence factors of antistatic properties,
including structure, process conditions, and relative humidly (RH),
were elaborated. In order to improve the washing endurance, two
feasible methods including combination with cationic polypropylene and surface crosslinking of modied T40 were presented.
2. Experimental
2.1. Materials
PP (T36F) was purchased from China Petroleum and Chemical
Corp. Tween (T20, T40, T60, T80, T65, T85), Span (S20, S40), acryloyl chloride, and acrylic acid (AA) were supplied from Sinopharm
Chemical Reagent Co., China. Cationic polypropylene master batch
(CPP) contained 2% guanidine groups, was purchased from Shanghai Fuyuan Rubber-plastics Co. Ltd. used without further treatment.
2,4,6-Trimethyl benzoyl diphenylphosphine oxide (TPO) was used
as the photo initiator with absorption wavelength at 299, and
366 nm.
2.2. Modication of T40
A mixture of 0.1 mol T40 and 0.33 mol acryloyl chloride were
added into a 100 mL round bottom ask equipped with magnetic
stirring. After continuous stirring for 24 h at room temperature, the
product was puried by rotary evaporation to remove the unreacted acryloyl choride, denoted as MT40. Its molecular structure
was characterized by FTIR using a Nicolet 5700 infrared spectrometer (Thermo Electron Scientic Instruments Corp., USA), and 1 H
NMR using a Varian Unity 400 proton and multinuclear magnetic
resonance spectrometer.

Surface resistivities of PP/Tween sheets were measured using a

ZC-36 high resistance meter (Shanghai Precision Instruments Co.,
China) at 23 C, relative humidity 65% (65% RH), 500 V voltage,
referred to China national standard GB/T1410-1989. The reported
values are the average of the measurements of three sheets. Contact
angles were measured with an optical contact angle meter JC2000D
(Shanghai powereach Corp., China) at ambient temperature. Water
droplets were dropped carefully onto the surfaces and the average
value of ve measurements at different positions of the sample was
adopted as the contact angle.
The wash durability of sheet samples was evaluated by comparison of their s before and after washing. With respect to
washing the sheet samples suffered ultrasonic processing in water
for 30 min at the frequency of 40 kHz, and then exposed in air to be
dried at 23 C, 65% RH for 24 h.
3. Results and discussion
3.1. Inuence of hydrophilelipophile balance of surfactant on
antistatic performance
Fig. 1 shows s of PP sheets incorporated 0.5% Tween and
Span surfactants, respectively. It can be seen that the s of PP
sheets contained Tween or Span signicantly depend on the
hydrophilelipophile balance (HLB) and have decreased 14 orders
of magnitude in comparison to the neat PP sheet. According to
the military handbook DOD-HDBK-263 [19], the antistatic material has a s between 109 and 1014 /sq. The industry standards
ANSI/EIA-541-1988 (USA) and ANSI/ESD S541-200 (USA) also
dened the electrostatic dissipative (ESD) material having the s
at 105 to 1012 /sq and 104 to 1011 /sq respectively. Therefore,
the PP samples incorporated 0.5% Tween has reached the antistatic
requirement, while the Span and PEG1000 samples have limited
antistatic performance. In particular, T40 provides an optimum
antistatic effect (s = 6.3 109 /sq) measured after moulding.
It is generally accepted that the antistatic mechanism for nonionic antistatic agents is that, the low molecular weight agents
migrate to the plastic surface and improve the surface conductivity by attracting a layer of water [14]. It can be concluded that

2.3. Preparation of antistatic PP sheet samples

Prescribed percent of PP, Tween (or Span) and antioxygen 1010
(0.2 wt%) were blended in a internal mixer (SU-70, Changzhou
Suyan Science and Technology Corp., China) at 180 C, 60 rpm for
5 min. The blends were moulded into 160 mm 180 mm 1 mm
sheees rstly with a 25 t plate vulcanization machine XQLB350 350 at 200 C, 7.5 MPa for 5 min, followed by cold pressing

Fig. 1. s of PP/Tween (0.5%) sheets and PP/Span (0.5%) sheets measured in the rst
and 21st day at 23 C, 65% RH.

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Table 1
s , contact angles and surface energies of PP/T40 sheets.a
Addition of T40

s (/sq)

N/A
0.2%
0.5%
1.0%

1.22 10
5.69 1013
1.50 1010
2.41 1010

15

Contact angle ( )

Water

Diiodomethane

94.6
79.0
57.1
59.0

56.1
53.6
40.4
40.0

Surface energy
(103 N/m)

30.9
35.1
49.6
48.7

Measured at 23 C, 50% RH.

the antistatic ability of non-ionic surfactant is determined by its

mobility and hygroscopicity. The mobility depends on the compatibility with PP, and the compatibility is inuenced by the HLB of
surfactants. When the HLB value is low, the surfactant with high
hydrophobicity has a strong interaction with PP. As a result, the
mobility slows down and the s remains little changed. With the
increasing of HLB value, the interaction between surfactant and PP
decreases, leading to a faster migration of surfactant and better
antistatic performance of plastics. However, when the HLB value is
more than 16.7, the surfactant is too hydrophilic to have enough
compatibility, causing aggregation inside the PP matrix. Therefore, the antistatic performance declines. According to this analysis,
T40, with a hydrophobic tail (C15 H31 ) and four hydrophilic arms,
provides a proper hydrophilelipophile balance, so that it can be
enriched on the plastic surface rapidly and improve the surface conductivity conspicuously. While the HLB value is too low (e.g. S40)
or too high (e.g. PEG1000), the surfactants present slight antistatic
effect due to their slow migrations.
After three weeks, most sheet samples reveal a slight decrease
on the s , indicating that the antistatic agents inside the matrix
would migrate to the surface with the time prolonged. s of PP/T40
sheet remains unchanged, suggesting that T40 surfactant is saturated on the PP surface after being moulded.
3.2. Inuence of addition amount on antistatic performance
Table 1 displays s , contact angles and surface energies of
PP/T40 sheets incorporated 0.2%, 0.5% and 1% T40, respectively.
Surface energies calculated via a harmonic-mean method [20] from
water contact angles and diiodomethane contact angles can reect
the polarity of sample surface. Compared with neat PP sample,
PP/T40 (0.5%) presents excellent antistatic performance with s at
1.50 1010 /sq. When the addition amount increases to 1%, the
s as well as the surface energy reveal a slight change, indicating
that T40 surfactant is saturated on the PP surface with 0.5% additive. In other words, the outermost surface of PP is crammed with
T40 molecules, while larger addition amount cannot increase the
polarity of PP surface. With respect to PP/T40 (0.2%), T40 surfactant
is not saturated on the PP surface and the polarity declines, resulting in a lower surface energy and a higher s . In summary, with
the addition amount of T40 increasing, the antistatic performance
of PP/T40 sheet samples improves at the beginning and reaches a
plateau in the end, with the turning point of addition between 0.2%
and 0.5%.

Fig. 2. s of PP/T40 (0.5%) sheets prepared in different temperatures and hot press
times, measured at 23 C, 50% RH.

It is noted that the component with similar surface energy is

prone to be enriched on the interface, forming a transition layer
[2022]. During the process of hot press, the polar component
would be enriched on the PP surface due to the inductive effect of
the steel mould. This is one important driving force of the migration
discussed above. With the temperature increasing, the viscosity of
the melt decreases and the mobility of T40 molecules is enhanced,
thus the s decreases. In this case, the prolongation of the hot press
time would accumulate more antistatic agents on the surface, leading to an improvement of the antistatic performance. However, T40
molecules would lose antistatic ability when contacting with the
steel mould for a long time due to the decomposition.
3.4. Inuence of atmospheric humidity on antistatic performance
Fig. 3 depicts the relationship of relative humidity and the s
of PP/Tween sheets. It can be seen the s is signicantly dependent on the relative humidity. When the atmospheric humidity is
below 28% RH, s are constant at high values (above 1013 /sq).
While the relative humidity is above 28% RH, the s show almost
linear decreases with the relative humidity increasing. The average slope calculated by tting the curves is 11.52, demonstrating
that every 10% increase of RH would cause about 1 order of magnitude reduction of s . The results are well in accordance with
previous research [23]. As known, the electrostatic charges are dissipated from the water layer attracted by antistatic agents. Such
water layer has a dynamic balance with vapour in the environment. In low atmospheric humidity, the antistatic agents cannot
attract enough water from the atmosphere, resulting in poor antistatic performance. With the relative humidity increasing, more
and more water is attracted by surfactants, leading to higher surface
conductivities.

3.3. Inuence of process conditions on antistatic performance

The inuence factors of process conditions including hot press
time and temperature were investigated as shown in Fig. 2. When
the hot press time is less than 7 min, the s of PP/T40 (0.5%) sheets
decrease with temperature increasing. While the hot press time is
prolonged to 12 min, the distinction of temperature is slight, and
the antistatic performance declines in comparison to samples hot
pressed for 7 min.

Fig. 3. s of PP/Tween (0.5%) sheets measured in different relative humidities.

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Table 2
Water contact angles of PP/Tween (0.5%) sheets measured at different relative
humidities/ .

T20 0.5%
T40 0.5%
T60 0.5%
T85 0.5%

50% RH

40% RH

20% RH

61.3
57.0
64.6
58.6

73.3
55.0
54.3
53.8

69.3
56.6
62.0
59.1

Water contact angles of PP/Tween samples incorporated of 0.5%

Tween were measured in the atmospheric humidity 50% RH, 40%
RH and 20% RH. As shown in Table 2, the water contact angles reveal
slight changes with the variation of atmospheric humidity. It is not
difcult to understand that the water contact angle is dependent on
the cohesive energy density and the polarity of the material, which
are not inuenced by the humidity. This demonstrates the presence
of a layer of surfactants on the PP surface, which is not inuenced
by the atmospheric humidity.
3.5. Improvement of the washing durability by combination with
cationic polypropylene
In order to improve the washing durability of PP/T40 sheets, a
combination of T40 and cationic polypropylene (CPP) was blended
with PP, and the s of PP/T40/CPP sheets are shown in Fig. 4. CPP is
one type of functionalized polypropylene master batch contained
2% cationic guanidine groups. In comparison to the PP/CPP (5%)
sample, the introduction of T40 improved the antistatic performance, with s changed from 1014 /sq to 1010 /sq. In addition,
the introduction of CPP also reveals a slight improvement for PP/T40
(0.5%) sheets, indicating CPP and T40 display a synergistic effect in
the antistatic performance.
The washing durability of PP/Tween and PP/CPP/T40 samples was evaluated by comparison of their s before and after

Fig. 5. FTIR spectra of T40 and MT40.

Table 3
s of PP/Tween and PP/CPP/T40 sheets before and after washing.a
Antistatic agent

Before washing
(/sq)

After washing
(/sq)

T20: 0.5%
T40: 0.5%
T60: 0.5%
T85: 0.5%
CPP/T40: 10%/0.5%
CPP/T40: 10%/1%
CPP/T40: 5%/0.5%
CPP/T40: 20%/0.5%

5.05 1010
7.07 109
1.32 1010
5.88 1010
5.13 109
1.55 1010
6.03 109
4.68 109

1.39 1015
1.22 1015
1.43 1015
1.18 1015
6.92 1011
1.2 1012
1.15 1012
1.62 1011

Measured at 23 C, 50% RH.

washing. As shown in Table 3, both PP/Tween and PP/CPP/T40

samples exhibit excellent antistatic properties before washing,
with s between 109 and 1011 /sq. After ultrasonic cleaning,
PP/Tween samples lose the antistatic performance completely
while PP/CPP/T40 samples remain to be antistatic, with s between
1011 and 1012 /sq. Obviously, Tween on the surface is easily
washed off due to its low molecular weight, while CPP, whose polar
groups are grafted on the polypropylene, remains and plays a part
in electrostatic dissipation.
3.6. Immobilizing T40 by UV crosslinking
3.6.1. Synthesis of MT40
As is discussed above, PP/Tween samples have poor washing
durability since the low molecular weight surfactants are easily
washed off. In order to improve the washing durability, immobilizing the surfactants on the surface is investigated by UV crosslinking
method. As shown in Scheme 2, T40 was modied with acryloyl
chloride to obtained double bonds. The modied T40 (MT40) was

Fig. 4. s of PP/CPP/T40 sheets with variation of (a) CPP and (b) T40, measured at
23 C, 50% RH.

Fig. 6.

H NMR spectrum of MT40.

A. Zheng et al. / Applied Surface Science 258 (2012) 88618866

8865

Table 4
The variation of antistatic agent layer exposed under UV light.
Antistatic agent

Components

UV exposure

AS 0
AS 1
AS 2

MT40: 100%
MT40/TPO: 90%/10%
MT40/TPO/AA: 85%/5%/10%

5s

30 s

Uncrosslinked
Crosslinked, thin lm
Crosslinked, thin lm

Uncrosslinked
Crosslinked, thin lm
Crosslinked, thin lm

Table 5
s of UV-irradiated and untreated PP/AS sheetsa before and after washing//sq.
Antistatic agent

AS 0
AS 1

AS 2

Dosage (%)

1.0
0.5
1.0
1.5
0.5
1.0
1.5

Untreated

UV exposure 30 s

Before washing

After washing

Before washing

After washing

2.4 10
2.9 1011
3.8 1010
1.3 1010
6.5 1011
1.6 1010
1.5 1010

3.2 10
5.2 1014
4.4 1014
7.1 1013
9.8 1014
7.8 1013
2.6 1013

7.2 10
2.0 1011
2.9 1011
6.1 109
1.1 1012
2.0 1010
1.3 1010

1.5 1014
1.2 1013
5.7 1012
3.3 1011
1.8 1013
1.5 1011
1.6 1012

10

14

10

Measured at 23 C, 50% RH.

Scheme 2. Synthesis of MT40.

blended with PP to fabricate PP/MT40 sheets, and the PP/MT40

sheets were irradiated under UV light to crosslink the MT40.
The structure of MT40 is characterized by FTIR and 1 H NMR analysis as shown in Figs. 5 and 6, respectively. Compared with T40, the
new peak at 1635 cm1 corresponds to the double bond (see Fig. 5),
and the rest peaks reveal no difference with T40, indicating a successful synthesis. In the 1 H NMR spectrum, the signals appeared
in 0.81.4 ppm, 3.43.8 ppm and 5.86.5 ppm are attributed to the

alkyl protons, ethyl ether protons and vinyl protons, respectively,

which also provide the evidence of the designed structure.
3.6.2. The crosslinking effect of MT40
The crosslinking effect of MT40 was investigated by coating
MT40 or its complex on the glass slide, and then the glass slide
was exposed under UV light for 5 s or 30 s. As is shown in Table 4,
antistatic agent incorporated of TPO (AS1, AS2) can be crosslinked

Fig. 7. Proposed mechanism for antistatic PP with washing durability.

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A. Zheng et al. / Applied Surface Science 258 (2012) 88618866

within 5 s, while antistatic agent without TPO (AS0) cannot be

crosslinked even being exposed for 30 s. The results indicate that it
is possible for the MT40 layer accumulated on the PP surface to be
crosslinked in the presence of TPO.
3.6.3. Immobilizing MT40 by UV crosslinking
Table 5 shows the s of UV-irradiated and untreated PP/AS
sheets with different addition amounts before and after washing. It can be seen that before washing both UV-irradiated and
untreated sheets reveal good antistatic performance with s below
1011 /sq. After washing, the untreated samples lost the antistatic
effect, while a part of the UV-irradiated samples including PP/AS1
(1.5%) and PP/AS2 (1%) present denite antistatic effect with s at
1011 /sq. This indicates a portion of MT40 molecules were immobilized on the surface by crosslinking.
Fig. 7 depicts antistatic PP with washing durability. As shown,
the MT40 molecules enriched on the surface are easily washed off.
While the samples are irradiated with UV light, the photoinitiator
TPO decompose into free radicals, causing the crosslinking of the
double bonds. The crosslinked MT40 has high molecular weight and
plenty of alkyl anchors, preventing it to be washed off. However,
such crosslinking is inadequate and further investigation will be
carried on in future.
4. Conclusions
In summary, we demonstrate that Tween surfactants are effective antistatic agents for PP. The antistatic performance of PP/Tween
samples are inuenced by the HLB of Tween, addition amount, process conditions and atmospheric humidity. In particular, PP/T40
(0.5%) sample exhibits an optimum antistatic ability with surface
resistivity of 1010 /sq, water contact angle of 57 , and surface
energy of 49.5 mN/m. A combination of T40 and CPP has improved
the washing durability of antistatic PP samples, with s at 1011 /sq
after ultrasound clean. In addition, UV crosslinking of modied T40
on PP surface also presents denite effects on the improvement of
washing durability.

Acknowledgements
The research was supported by Shanghai Leading Academic
Discipline Project (B502) and Shanghai Key Laboratory Project
(08DZ2230500).
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