Sensors and Actuators B 141 (2009) 179–186

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Sensors and Actuators B: Chemical

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

Actuator properties of the complexes composed by carbon nanotube and ionic

liquid: The effects of additives
Takushi Sugino ∗ , Kenji Kiyohara, Ichiroh Takeuchi, Ken Mukai, Kinji Asaka
Research Institute for Cell Engineering, National Institute of Advanced Industrial Science and Technology (AIST), Midorigaoka 1-8-31, Ikeda, Osaka 563-8577, Japan

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

Article history: Two different types of additives were mixed into the electrode of carbon nanotube (CNT) actuators low-
Received 26 February 2009 voltage-driven in air to investigate the influence of additives on the actuator performance. The electrode
Received in revised form 27 May 2009 was composed by single-walled carbon nanotubes (SWNTs), an ionic liquid (IL), a base polymer, and
Accepted 3 June 2009
an additive. The generated strain was estimated by measuring displacement changes of the actuator
Available online 11 June 2009
element in the frequency range between 5 mHz and 200 Hz. In case of a non-conductive additive, that is,
mesoporous silica (MCM-41), the maximum strain of the actuator increased about 1.6 times as large as
Keywords:
that of the non-additive actuator. On the contrary, a conductive additive, polyaniline (poly-An), caused
Carbon nanotubes
Ionic liquid
a remarkable improvement of the strain (ca. 3 times) for the actuator. It is found that this improvement
Actuator was achieved by the effective charge storage in the actuator element. The generated stress was also
Polyaniline determined by Hooke’s law with the parameter of the maximum strain and the Young’s modulus of
Mesoporous silica actuator composite.
© 2009 Elsevier B.V. All rights reserved.

1. Introduction
In the last decade, electroactive polymers (EAP), such as conduc-
tive polymers [1–6], ionic polymer-metal composites (IPMC) [7–11],
carbon nanotube papers [12–14], have attracted much attention
as good candidates for “artificial muscles” [15] in terms of their
quick and soft actuation by low voltage like natural muscles, light
weight, and large displacement. For example, Baughman and co-
workers have reported the first bucky paper actuator that consisted
of two SWNT sheets on the both side of a double-sided Scotch
tape and showed a bending motion in aqueous electrolytes [12].
They proposed a charge injection model due to quantum chemi-
cal and double-layer electrostatic effects there. In the model, the
actuation was caused by dimensional changes of SWNTs in the
covalently bonded direction derived from the charge injection [16].
This dimensional change was free from Faradaic process that was
inevitable for conductive polymer actuators and that restricted
their lifetime and response time.
Most of EAP actuators work in electrolyte solutions. On the other
hand, smaller numbers of EAP actuators which operate in air have
been known [17–20]. Easy fabrication and operation in air bring EAP
actuators large advantages for use as “artificial muscles”. Recently,
we have reported a first dry polymer actuator consisted of SWNTs,
ionic liquid (IL), and a base polymer [21]. Our actuator can be driven
∗ Corresponding author. Tel.: +81 72 751 9191; fax: +81 72 751 9628.
E-mail address: takushi-sugino@aist.go.jp (T. Sugino).
in air with low voltages (∼±3 V) for a long time. The actuator has a
three-layered structure, that is, an electrolyte layer is sandwiched
by two electrode layers. Each layer film is easily obtained by a cast-
ing method. The actuator shows a bending motion toward the anode
side when voltage is applied which is the same bending direction as
observed for the SWNT sheet. The bending direction toward anode
side was induced by the expansion of cathode and the contraction
of anode with the ion transfer. We recently confirmed this expan-
sion and contraction mechanism by coupling a symmetry analysis,
the elasticity theory, and the experimental results [22]. The elec-
tromechanical and electrochemical properties of our actuator by
using 7 kinds of internal ILs have been investigated in order to
understand the actuation mechanism in detail [23]. We theoreti-
cally studied the structural, electrostatical, and electromechanical
properties of a three-layered composite made up of two electrodes
layers and one electrolyte layer as a separator by a method of Monte
Carlo simulation at molecular level [24,25]. From these previous
papers, we consider that steric repulsion caused by ion transfer into
the electrode, besides the charge injection to SWNTs, is an impor-
tant mechanism to induce the bending motion of our actuator. The
steric repulsion was controlled by the size-difference of cations
and anions. The ion transfer occurred non-Faradaically by simple
charge/discharge of ions. On these backgrounds, we are tempted to
improve the actuation performances such as the generated strain
and stress by tuning the electrode properties such as the conduc-
tivity or the packing density. In this paper, we study the effects
of additives in the electrode layer on the actuator performance. A
polyaniline (poly-An) and a mesoporous silica (MCM-41) were cho-

0925-4005/$ – see front matter © 2009 Elsevier B.V. All rights reserved.
doi:10.1016/j.snb.2009.06.002
180 T. Sugino et al. / Sensors and Actuators B 141 (2009) 179–186
sen as the conductive additive and the non-conductive additive,
respectively. The poly-An has a particle form (ca. 40 nm particle
size) and has a relatively high conductivity (40 S cm−1 ) compared
to the electrode conductivity (around 10 S cm−1 ) observed for our
actuator composed of SWNTs, IL, and a base polymer [23]. Mean-
while, MCM-41 is well known as a mesoporous silica that has
hexagonal packing arrays with one-dimensional channels [26]. The
channel structure can be used to capture ions [27] and molecules
[28,29]. These previous research results inspired us to use MCM-41
for the effective ion transportation into the electrode of our actu-
ator by addition of MCM-41. The MCM-41 used in this study has
2.7 nm pore size with large surface volume (∼1000 m2 g−1 BET sur-
face area). The effects of the additives on the actuator properties
were investigated and discussed by measuring the electromechan-
ical and electrochemical properties of the actuator.
2. Experimental
2.1. Materials
SWNTs (Purified HiPco® ) was purchased from Carbon
Nanotechnologies Inc. 1-Ethyl-3-methylimidazolium tetrafluoro-
borate (EMIBF4 ) (Fluka), and polyvinylidene fluoride-co-
hexafluoropropylene (PVDF-HFP: Kynar Flex® 2801) (Arkema
Chemicals Inc.) were used as received without any further purifi-
cation. Polyaniline (poly-An) (20 wt% polyaniline on carbon black),
mesoporous silica (MCM-41 type), 4-methy-2-pentanone ≥99.5%
(MP) and propylene carbonate anhydrous 99.7% (PC) were pur-
chased from Sigma–Aldrich Co. The poly-An has a ca. 40 nm particle
size, conductivity of 40 S cm−1 , and 690 m2 g−1 BET surface area.
The MCM-41 used here has a 2.7 nm pore size with ∼1000 m2 g−1
BET surface area. N,N-dimethylacetamide (DMAc) 99.0% (Kishida
Chem. Co.) was used.
2.2. Preparation of the actuator film
The typical fabrication process of three-layered actuators is
described below. The electrode layer was composed by 20 wt% of
SWNTs, 48 wt% of EMIBF4 , and 32 wt% of PVDF-HFP in the case
of CNT(50). 50.2 mg (19.9 wt%) of SWNTs, 121.7 mg (48.2 wt%) of
EMIBF4 , and 80.6 mg (31.9 wt%) of PVDF-HFP were dissolved into
9 mL of DMAc. The mixture was stirred at room temperature for
more than 1 day and furthermore was sonicated in an ultrasonic
Fig. 1. Construction of three-layered actuator strip and molecular structures of EMIBF4 and PVDF-HFP.
bath (36 kHz) for more than 24 h. As a result, a gelatinous mixture
was obtained. The electrode film was made by casting 1.6 mL of the
gelatinous mixture into a Teflon mold (the size is 2.5 cm × 2.5 cm)
and then drying the solvent (DMAc) for 3 days at 80 ◦ C in vacuo. The
same amount of poly-An (50 mg) and MCM-41 (50 mg or 25 mg) as
SWNTs (50 mg or 25 mg) were added into the DMAc solution with
SWNTs, EMIBF4 , and PVDF-HFP in cases of poly-An(50/50), MCM-
41(50/50), and MCM-41(25/25), respectively. In the abbreviation
of CNT(50), poly-An(50/50), MCM-41(50/50), and MCM-41(25/25),
the figures in the parentheses show the weight ratio of SWNTs
and additives. The thickness of the obtained electrode films was
between 45 ␮m and 80 ␮m.
The gel electrolyte layer was also prepared by a casting method
almost the same procedure as for the electrode layer. 100 mg of
EMIBF4 and 100 mg of PVDF-HFP were dissolved into the mixture
solution of MP (3 mL) and PC (250 mg) by heating at 65 ◦ C in a sand
bath. The 0.3 mL of obtained solution was casted into the Teflon
mold (2.5 cm × 2.5 cm) and dried for 3 days at 80 ◦ C in vacuo. Then,
the thickness of electrolyte films was between 15 ␮m and 20 ␮m.
A three-layered actuator film was fabricated by heat-pressing
an electrolyte film sandwiched by two electrode layers (see Fig. 1).
The total thickness of the actuator films was between 106 ␮m and
162 ␮m.
2.3. Measurement
The displacement measurements were performed by using
1 mm × 10 mm size actuator strips shown in Fig. 2a. The actuator
strip was connected to the gold electrodes. The alternating square-
wave voltages were applied to the actuator strip by a HOKUTO
DENKO Potentio/Galvanostat (HA-501G) with a waveform gener-
ator (YOKOGAWA ELECTRIC model FC200). The displacement at
5 mm away from the fixed end of gold electrodes was measured by
a laser displacement meter (KEYENCE model LC2100). The voltage,
current, and displacement were monitored simultaneously with
an oscilloscope (YOKOGAWA DL708). The actuator strip showed a
bending motion when the voltage was applied (see Fig. 2b). The
measured displacement (D) is related to the curvature (1/R) as [1]
1 2D
= 2 (1)
R L + D2
where L is the length from the fixed end of gold electrodes to the
point where the laser is irradiated on the actuator strip. From Fig. 2b,
 T. Sugino et al. / Sensors and Actuators B 141 (2009) 179–186 181

Fig. 2. Schematic representation of experimental setup for displacement measurements (a) and relationship between the curvature and the changed lengths of both electrodes
(b).

the curvature radius R is related to the changed lengths of both elec- stat mode connected with a wave generator (YOKOGAWA ELECTRIC
trode layers during the bending, L + L1 and L + L2 , respectively, FC220 model). The linear sweep of current was applied from the
as the following: outer two probe electrodes and the voltage was detected by the
inner two probe electrodes. The conductivity of the electrode film
R − (W /2) L + L2
= (2) was calculated by the slope of current–voltage curve. The Young’s
R + (W /2) L + L1
modulus of the electrode film was estimated by the stress–strain
Therefore, Eq. (2) is rewritten as curve that was measured by a thermal stress–strain measure-

L1 − L2 W
 L1 + L2
 ment instrument (SEIKO Instruments Inc. TMA/SS6000). The SEM
= 1+
L R 2L
In these two equations, it is assumed that the thickness of the
actuator strip (W) is not changed during bending. When, Eq. (1) is
substituted in Eq. (3), we obtain the following equation (Eq. (4)) to
evaluate the difference of strain (ε) because the second term of the
right hand of Eq. (3) is negligibly small.
L1 − L2 2DW
ε= = 2
L L + D2
The ionic conductivity of EMIBF4 in the gel electrolyte was
determined by an ac impedance spectroscopy. The impedance
measurement was conducted in the frequency range of 1 Hz
to 10 MHz with Solartron 1250 Impedance/Gain-phase Analyzer.
Cyclic voltammetry (CV) was carried out to study the double-layer
capacitance of the electrode by two-electrode configuration using a
HOKUTO DENKO HSV-100 model. The conductivity of the electrode
film was investigated by the four probe DC current method using a
HOKUTO DENKO Potentio/Galvanostat HA-151 model as a galvano-
(3) (scanning electron microscope) observation was performed to char-
acterize the electrode with JEOL JSM-6390.
3. Results and discussion
The displacement measurements were performed for CNT(50),
poly-An(50/50), MCM-41(50/50), and MCM-41(25/25) at the
applied square-wave voltage of ±2.0 V with different frequencies.
(4) One of the typical time profiles of the applied voltage, the current,
and the displacement for CNT(50) are shown in Fig. 3a. The cur-
rent profile showed only charging or discharging. This indicates
that the electrodes of our actuator exhibit a feature of an elec-
tric double-layer capacitor. The accumulated charge (Q) during each
half period was calculated by integrating the current. The generated
strain (ε) was calculated from Eq. (4) using the half of peak-to-
peak value in the time profile of displacement. Fig. 4 depicts the
frequency dependence of the generated strain for all the actua-
tor composites. The strains increase as the frequency becomes low.
For example, the maximum strain is more than 1000 times larger
182 T. Sugino et al. / Sensors and Actuators B 141 (2009) 179–186

Fig. 4. Frequency dependence of the generated strain (ε) for four composites.

Table 1
The generated strains at 0.005 Hz, 0.1 Hz, 1.0 Hz, and 10 Hz for all the complexes.

Complex Strain (%)

0.005 Hz 0.1 Hz 1.0 Hz 10 Hz

CNT(50) 0.69 0.49 0.22 0.047

Poly-An(50/50) 2.0 0.72 0.15 0.0048
MCM-41(50/50) 1.1 0.59 0.16 0.016
MCM-41(25/25) 0.79 0.59 0.31 0.085

Fig. 3. Time profiles of voltage, generated current, and displacement when ±2.0 V
square-wave voltage was applied (f = 0.1 Hz) (a) and the positive and negative charge
stored in the electrode (b).
than the minimum strain. Poly-An(50/50) shows the largest strain
at the lowest frequency of 5 mHz among all the composites. The
strain of poly-An(50/50) at 5 mHz is estimated to be 2.0%. This is
almost 3 times as large as that of the non-additive case (0.69% for
CNT(50)). Addition of the same amount MCM-41 to the CNT elec-
trode also induces enhancement of the strain. The strains at 5 mHz
are the following order; poly-An(50/50) > MCM-41(50/50) > MCM-
41(25/25) > CNT(50). Some of the generated strains at different
frequencies are summarized in Table 1. Poly-An(50/50) shows the
largest strains among the four different cases in the frequency
range between 5 mHz and 0.1 Hz. Even if the frequency is 0.1 Hz,
the strain of poly-An(50/50) is still ca. 1.5 times larger than that
of CNT(50). The strain of poly-An(50/50), however, decreases dras-
tically to be the smallest among the four actuator composites in
the frequency range higher than 1.0 Hz. A similar decrease of strain
was observed for MCM-41(50/50) rather than MCM-41(25/25). The
strain of MCM-41(50/50) at 5 mHz was calculated to be 1.1%, which
is 1.6 times larger compared with that of the CNT(50). Neverthe-
less, the strain of MCM-41(50/50) became smaller than that of
CNT(50) when the frequency was chosen to be higher than 1.0 Hz.
The strain of MCM-41(25/25) was as high as 0.79% at 5 mHz. It is
noteworthy that this value is quite similar to that of CNT(50) but
somehow still larger even though the amount of CNT is reduced to
half of CNT(50). Furthermore, the strain curve against frequencies
of MCM-41(25/25) is always higher than that of CNT(50).
As described above, the maximum strain and the frequency
dependence of strain were drastically changed by incorporation
of additives into the electrode layers. In order to understand
the electrochemical feature of the electrode with additives, the
double-layered capacitance (C) and the conductivity () of the
electrode were estimated. The cyclic voltammetry of the elec-
trode was measured to estimate the capacitance. Fig. 5 shows
the cyclic voltammograms of the electrodes for CNT(50), poly-
An(50/50), MCM-41(50/50), and MCM-41(25/25) with a sweep rate
at 10 mV s−1 . Peaks based on redox reaction were not observed. This
result indicates that the charge/discharge proceeds capacitively for
our actuators. This capacitive process is also supported by the cur-
rent profile as mentioned above. The conductivity of the electrode
was evaluated by the four probe DC current method. The evaluated
capacitances and conductivities are listed in Table 2. The addition of
poly-An lead to increase both capacitance and conductivity of the
electrode. This positive effect on electrical properties of both the
capacitance and the conductivity should be derived from the good
conductivity (40 S cm−1 ) of added poly-An. The improvement of
these two parameters brought the largest strain for poly-An(50/50)
Table 2
Estimated capacitance (C) and conductivity () of the electrode.
Complex C (F cm−2 )  (S cm−1 )
CNT(50) 0.0339 17
Poly-An(50/50) 0.0885 32
MCM-41(50/50) 0.0356 8.1
MCM-41(25/25) 0.0179 2.7
 T. Sugino et al. / Sensors and Actuators B 141 (2009) 179–186
Fig. 5. Cyclic voltammograms of actuator composites: sweep rate = 10 mV s−1 : (a) CNT(50), (b) poly-An(50/50), (c) MCM-41(50/50), and (d) MCM-41(25/25).
in a frequency range between 5 mHz and 0.1 Hz. On the contrary,
the conductivity became less than half although the capacitance
was not changed so much by the addition of MCM-41 (in the case of
MCM-41(50/50)). The capacitance of MCM-41(25/25) was reduced
to be almost half as large as that of CNT(50). This is caused by the
half amount of SWNTs in the case of MCM-41(25/25) compared
with CNT(50). The conductivity of the electrode for MCM-41(25/25)
was drastically decreased to be 2.7 S cm−1 . This value is less than
1/6 of that for CNT(50). These results imply that the capacitance of
the electrode was not affected so much by the addition of MCM-41
but the conductivity of the electrode was largely affected by the
addition of the MCM-41.
In our previous paper [23], we proposed a kinetic (electrome-
chanical kinetic) model of double-layer charging for our actuator
system. In the model, the generated strain in the actuator is pro-
portional to the stored charge while the voltage is applied. In order
to confirm this consideration, the stored charge in each actuator
strip was calculated from the current profile and was plotted in
Fig. 6 as a function of the frequency of applied voltage. The positive
Fig. 6. Frequency dependence of the stored charge (±Q) for four composites. Solid
lines show the positive charge and dashed–doted lines show the negative charge.
183
and the negative charges imply the accumulated current during the
applied voltage is positive and negative, respectively (see Fig. 3b).
Both the positive charge and the negative one were almost sym-
metrically stored with the periodic exchange of the anode and
cathode. The order of absolute values of the stored charges at
the lowest frequency (5 mHz) is following: poly-An(50/50) > MCM-
41(50/50) > MCM-41(25/25) ∼ = CNT(50). This order observed for
stored charge is well coincident with the order of generated strain.
This implies that larger actuation motion is caused by larger charge
stored by operating voltage. The charge–frequency curve is very
similar to the strain–frequency curve for all the actuator composites
that we studied. The stored charge of poly-An(50/50) was largest
among the four composites at 5 mHz but the charge was remarkably
reduced with increase of frequency, then it became smaller than
that of CNT(50) when the frequency became higher than 1.0 Hz.
A similar decrease of the stored charge was observed for MCM-
41(50/50), however, the difference of charge–frequency curve
between poly-An(50/50) and MCM-41(50/50) was not coincident
perfectly with that of strain–frequency curve between poly-
An(50/50) and MCM-41(50/50). The charges of MCM-41(25/25)
and CNT(50) are smaller than those of poly-An(50/50) and MCM-
41(50/50) in the frequency range of 5 mHz to 0.1 Hz. In contrast,
MCM-41(25/25) and CNT(50) can store larger amount of charge
compared with poly-An(50/50) and MCM-41(50/50) in the higher
frequency range (>1.0 Hz). It is quite interesting that almost the
same value of stored charge was observed for both MCM-41(25/25)
and CNT(50) at each frequency even though half amount of MCM-41
instead of SWNTs was used in the case of MCM-41(25/25).
These results (vide supra) can well explain the difference of
the strain–frequency curve for all the actuator composites only
when the frequency is lower than 1.0 Hz. If the frequency become
lower than 0.1 Hz, the larger amount of additive (in the cases
of poly-An(50/50) and MCM-41(50/50)) induces larger electrical
charge stored in the electrode layers then this causes larger strain
184 T. Sugino et al. / Sensors and Actuators B 141 (2009) 179–186
Table 3
The maximum strain (εmax ) at 0.005 Hz, Young’s modulus (Y), and maximum stress
() for all the complexes.
Complex εmax (%) Y (MPa)
CNT(50) 0.69 280
Poly-An(50/50) 2.0 440
MCM-41(50/50) 1.1 170
MCM-41(25/25) 0.79 120
into the electrode layers. Nevertheless, both poly-An(50/50) and
MCM-41(50/50) were charged less than the composite with no
additives (CNT(50)) when the frequency was chosen higher than
1.0 Hz, where they showed smaller strain than CNT(50). This drastic
decrease of strain observed for poly-An(50/50) and MCM-41(50/50)
is probably due to the additional packing of additives besides 50 mg
of SWNTs dispersed into the electrode. In such a densely pack-
ing condition, the penetration of ions from the electrolyte layer to
the electrode layers may be interrupted somehow. Furthermore, it
is considered that the diffusion of ions in the electrode layers is
also decelerated. This interruption of ionic transportation results in
smaller stored charge and strain when the frequency is faster than
1.0 Hz.
The mechanical stiffness of electrode is one of the parameters
to consider actuator response and power. So, the Young’s modu-
lus of electrode film was investigated by a thermal stress–strain
measurement instrument. The obtained Young’s moduli of elec-
trode films are listed in Table 3. The maximum generated stress
() during actuation motion was calculated by using two param-
eters, the maximum strain (εmax ) and the Young’s modulus (Y),
according to Hooke’s law;  = Y × εmax (see in Table 3). Interest-
ingly, the Young’s modulus was ca. 1.6 times increased by adding
poly-An compared to that of CNT(50) while it was ca. 1.6 times
decreased by the addition of same amount of MCM-41 (in the case of
MCM-41(50/50)). As a result, poly-An(50/50) exhibits highest gen-
Fig. 7. SEM images of electrode films with additives (magnification: 10,000×): (a) CNT(50), (b) poly-An(50/50), (c) MCM-41(50/50), and (d) MCM-41(25/25).
erated stress of 8.8 MPa that is more than 4 times as large as that
of CNT(50). MCM-41(50/50) shows the same stress as CNT(50). The
stress of MCM-41(25/25), however, becomes 1/2 as large as that of
 (MPa) CNT(50). From these results, the drastic decrease of strain for poly-
1.9 An(50/50) and MCM-41(50/50) in the higher frequency range may
8.8 be caused by the reduction of charge efficiency and the difference
1.9 of stiffness (Young’s modulus) of electrode.
0.94
In the previous paper [21], we reported that the actuation prop-
erties of the similar three-layered CNT polymer actuator were 0.9%
for the strain and 0.1 MPa for the generated stress, respectively. The
maximum strain of 2.0% observed for poly-An(50/50) is more than
twice as large as the previous reported value (0.9%). The maximum
generated stress is improved to be 8.8 MPa for poly-An(50/50) that
is 88 times larger than the reported value (0.1 MPa). These improved
values are comparable to those of other dry actuators such as con-
ducting polymers [17,18] and ionic polymer–metal composites [11]
including room temperature ionic liquids.
The four actuator composites studied here showed reproducible
bending displacements in the frequency range between 5 mHz and
200 Hz. There was not any degradation for all the actuator compos-
ites during the displacement measurements at the applied voltage
of ±2.0 V. This is due to the electrochemical stability of EMIBF4 as an
ionic source in the actuator composites. Fuller et al. have reported
that the electrochemical window of EMIBF4 is ca. 4.5 V [30]. Our
three-layered CNT actuators showed a stable actuation in air at least
8000 cycles at ±2.0 V with a frequency of 0.1 Hz [21]. No obvious
delamination between the electrode layers and the electrolyte layer
was observed during the long actuation.
The SEM observations were carried out to study the morphology
of the electrodes. The SEM images of electrode surfaces are shown
in Fig. 7. The morphology was dramatically changed by addition
of additives. The electrode only from CNT shows heavily entangled
bundles to form CNT fiber mesh (Fig. 7a). White particles in addition
to the CNT fiber mesh were seen in Fig. 7c and d. That indicates seg-
regation of MCM-41 from the CNT fiber mesh. The CNT fiber mesh
 T. Sugino et al. / Sensors and Actuators B 141 (2009) 179–186
was interrupted with incorporation of MCM-41. This interruption
of CNT fiber network may be the cause of lower Young’s moduli
and smaller conductivities of the electrodes by MCM-41(50/50)
and MCM-41(25/25) compared with CNT(50). On the other hand,
no segregation of poly-An was seen in the SEM image of poly-
An electrode (Fig. 7b). A structure with finer fibers and smaller
mesh was observed in the SEM image. The SEM image suggests
that the finer and intricate mesh structure makes the poly-An elec-
trode stiff and affords larger capacitance than the electrode of
CNT(50).
4. Conclusion
A poly-An and a MCM-41 were chosen as a conductive and a
non-conductive additive, respectively, in the electrode composed
of SWNTs, an IL, and a base polymer to investigate the influence of
additives on the actuator performance. The frequency dependence
of generated strain was studied for four different types of actuator
composites; CNT(50), poly-An(50/50), MCM-41(50/50), and MCM-
41(25/25). It was found that the frequency dependence curve of
strain was well coincident with the frequency dependence curve
of stored charge into the actuator elements. The electrochemical
and electromechanical properties were also investigated. Addi-
tion of poly-An increased both capacitance and conductivity of
the electrode. Furthermore, the good miscibility between SWNTs
and poly-An particles observed in SEM image should elicit advan-
tage of mechanical stiffness (Young’s modulus) for the electrode
film besides the larger capacitance and conductivity. Consequently,
the largest strain (2.0%) and stress (8.8 MPa) were observed for
poly-An(50/50) among the four actuator composites. On the con-
trary, addition of MCM-41 as a non-conductive component into the
actuator electrode induced the segregation of MCM-41 from CNT
fiber network. This diminished the conductivity and the Young’s
modulus of the electrode film. MCM-41(50/50) showed the larger
maximum strain (1.1%) than that of CNT(50) (0.69%), but it exhib-
ited the same maximum stress (1.9 MPa) as CNT(50) because of its
low Young’s modulus. MCM-41(25/25) exhibited almost the half
maximum stress (0.94 MPa) compared with CNT(50) even though it
showed the similar maximum strain (0.79%) as CNT(50). The higher
packing density of the electrode (in the cases of poly-An(50/50)
and MCM-41(50/50)) tended to increase the strain drastically with
decrease of the frequency of applied voltage. On the contrary, the
lower packing density (MCM-41(25/25)) showed a quick actuator
response. This may be caused by much faster ion transfer occurred
from the electrolyte layer to the less dense electrode layers.
Acknowledgements
This work was partially supported by New Energy and Industrial
Technology Development Organization (NEDO). The authors thank
Dr. M. Fujiwara for the SEM measurements.
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Biographies
Takushi Sugino received his PhD from Dept. of Applied Chemistry, Osaka University
in 1996. He is a senior research scientist of Artificial Cell Research Group, Research
Institute for Cell Engineering at AIST. His research background is material science
such as nonlinear optics and liquid crystals. His current interests are polymer-based
actuators and their applications as artificial muscles.
Kenji Kiyohara received his BS and MS from Kyoto University and PhD from Cornell
University. He is a senior research scientist at Research Institute for Cell Engineering
of AIST. His current research interests include analyzing nanometer-scale structures
of functional materials using molecular simulation and developing novel computa-
tional techniques.
186 T. Sugino et al. / Sensors and Actuators B 141 (2009) 179–186

Ichiroh Takeuchi received his BEng and MEng from Kyoto Institute of Technology
in 2000 and 2002, respectively. He is a staff of Artificial Cell Research Group. His
research interests are focused on investigation of relationship between equivalent
circuit model and performance of nano-carbon/ionic liquid gel actuators.
Ken Mukai received his BEng from Osaka University in 1999. He is a technical staff
of Artificial Cell Research Group. His recent research interests are electromechanical
actuators and highly conductive sheets from carbon nanotubes.
Kinji Asaka received his PhD degree in Science from Kyoto University in 1990. He is
currently a Group Leader of the Artificial Cell Research Group, Research Institute for
Cell Engineering at AIST. His current research interests include interfacial electro-
chemistry and polymer actuators. He is a member of the Society of Polymer Science,
Japan and the Society of Instrument and Control and Engineers.