FULL PAPER
Triboelectric Nanogenerators
Treefrog Toe Pad-Inspired Micropatterning for High-Power
Triboelectric Nanogenerator
Van-Tien Bui, Qitao Zhou, Jong-Nam Kim, Jung-Hwan Oh, Kwan-Woo Han, Ho-Suk Choi,
Sang-Woo Kim, and Il-Kwon Oh*
Inspired by treefrog’s toe pads that show superior frictional properties,
herein, an industrially compatible approach is reported to make an
efficient dielectric tribosurface design using customizable nonclose-
packed microbead arrays, mimicking the friction pads of treefrogs, in
order to significantly enhance electrification performance and reliability
of triboelectric nanogenerator (TENG). The approach involves using
an engineering polymer to prepare a highly ordered large-area concave
film, and subsequently the molding of a convex patterned triboreplica in
which the concave film is exploited as a reusable master mold. A nature-
inspired TENG based on the patterned polydimethylsiloxane (PDMS)
paired with flat aluminum (Al) can generate a relatively high power density
of 8.1 W m−2 even if a very small force of ≈6.5 N is applied. Moreover, the
convex patterned PDMS-based TENG possesses exceptional durability
and reliability over 25 000 cycles of contact–separation. Considering the
significant improvements in power generation of TENG; particularly at
very small force, together with cost-effectiveness and possibility of mass
production, the present methodology may pave the way for large-scale
blue energy harvesting and commercialization of TENGs for many practical
applications.
Dr. V.-T. Bui, Dr. Q. Zhou, J.-N. Kim, Dr. J.-H. Oh, K.-W. Han, Prof. I.-K. Oh
Creative Research Initiative Center for Functionally Antagonistic
Nano-Engineering
Department of Mechanical Engineering
Korea Advanced Institute of Science and Technology (KAIST)
291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea
E-mail: ikoh@kaist.ac.kr
Dr. V.-T. Bui
Faculty of Materials Technology
National Key Lab. of Polymer and Composite Materials
HoChiMinh University of Technology
Vietnam National University
HoChiMinh City 10288, Vietnam
Prof. H.-S. Choi
Department of Chemical Engineering and Applied Chemistry
Chungnam National University
220 Gungdong, Yuseong-gu, Daejeon 305-764, Republic of Korea
Prof. S.-W. Kim
School of Advanced Materials Science and Engineering
Sungkyunkwan University (SKKU)
Suwon 16419, Republic of Korea
The ORCID identification number(s) for the author(s) of this article
can be found under https://doi.org/10.1002/adfm.201901638.
DOI: 10.1002/adfm.201901638
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1. Introduction
Today, portable and wearable electronic
devices, smart sensors for environmental
protection and healthcare monitoring sys-
tems, and wireless sensing networks for
the Internet of Things (IoT) are becoming
indispensable in people’s modern lives.
With the technological advances of these
assisting facilities, the quality of human
life has been improved a lot, but these
devices are also simultaneously driving
an energy crisis and pollution problems
are becoming more serious due to the
use of limited lifetime rechargeable bat-
teries as a traditional power source.[1] In
addition, while the power consumption
of microelectronics is on a decreasing
trend, the amount of units has increased
dramatically, leading to an impossible task
of recharging or replacing huge number
of batteries.[2] Therefore, an innovative
kind of energy harvester, the triboelectric
nanogenerator (TENG), which can harvest
electric energy from abundant mechanical
energy in the living environment for self-
powered and autonomous integrated systems, was developed
by Zhong Lin Wang and has attracted great attention from
academic and industrial societies.[3] In general, TENGs are
constructed from two dielectric layers with different electron
affinities, assembled face-to-face with two electrodes adhering
to the backsides. TENGs generate electricity based on the
conjunction of triboelectrification and electrostatic induction
during periodic contact and separation of the dielectric layers.[4]
It has been demonstrated that TENGs have many advantages
such as light weight, robustness, simple fabrication, and high
efficiency, especially for harvesting energy from irregular, low-
frequency (<5 Hz) motions.[5] Therefore, TENGs not only are
suitable for microelectronic systems but also have potential as
a promising technology for harvesting large-scale energy from
ocean waves or wind.
Many studies investigated boosting the electrical output per-
formance of TENGs based on materials selection, new design,
and surface engineering.[3b,6] Among those studies, surface pat-
terning methods including soft lithography, block-copolymer
lithography, colloid template, and plasma treatment have been
proved to be valuable surface modifications that can produce
high-performance TENGs.[7] However, the development of such
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devices often suffers from obstacles such as high cost, low
throughput, high time consumption, complicated processes,
and difficulty in adjusting pattern features; these obstacles
definitively constrain practical applications of TENG, especially
for megascale energy harvesting, in which huge numbers of
large-area TENG devices must work together. To simplify the
fabrication procedure and realize mass production, Li and
co-workers demonstrated the use of sand paper to increase the
roughness of the tribosurface.[8] Alternatively, nature-replicated
structures were created by soft lithography using surface mor-
phologies from nature (lotus leaf, rose petal, and cicada wing)
as molds.[9] In addition, Xu and co-workers reported the fabrica-
tion of a polydimethylsiloxane (PDMS) film with a microlens
array via a combination of breath figure (BF) and micromolding
methods.[10] These approaches are valuable and possess advan-
tages for simple and large-scale fabrication; however, perfor-
mance of TENGs has still been low in the former strategy due
to random and low porous structure, and due to the difficulty of
controlling the microlens array in the latter strategy. Moreover,
the BF method requires not only an expensive block copolymer
but also a highly humid environment which, to some extent,
increases the production cost, lowers the reproducibility, and
constrains the super-large area production of TENG.[11] There-
fore, developing a new approach for producing high-perfor-
mance TENGs at low cost and with large-scale micropatterned
surfaces still remains a challenging issue.
Inspired by treefrog’s toe pads where they possess hexag-
onal micropattern structures which are able to maximize real
contact with surface profile of various substrates and thereby
enhance frictional properties. This study presents treefrog toe
pad-inspired micropatterning of dielectric tribosurfaces using
customizable nonclose-packed microbead arrays, revealing a
morphology that resembles friction pads of treefrogs in order
to significantly enhancing electrification performance and reli-
ability of TENG. The approach involves the large-scale fabrica-
tion of a concave poly(methyl methacrylate) (PMMA) film via an
improved phase separation method; then, a convex patterned
PDMS is formed using the concave film as a reusable mother
mold. The pore array features of the concave film can be pre-
cisely controlled, meaning that the surface morphology of the
corresponding convex patterned PDMS can be adjusted in term
of both pattern size and separation between the patterns. The
as-prepared convex PDMS was coupled with aluminum (Al),
which serves as both friction surface and electrode, to form a
vertical contact–separation mode TENG. The influence of sur-
face features of the convex PDMS film on the performance of
the TENG device was systematically investigated and compared.
Finally, the treefrog toe pad-inspired micropattern PDMS-based
TENG device was used to directly drive an electronic thermom-
eter and to turn on several light-emitting diodes (LEDs).
2. Results and Discussion
Mimicking natural structures has been considered a remark-
able strategy of achieving advanced multifunctional materials.
For instance, hexagonal surface micropattern that resembles
the microcosmic structure of treefrog’s toe pads (Figure  1a),
has gained significant interests in relation to controlling
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friction under both dry and wet conditions. As a part of the
efforts to create powerful friction tribosurfaces for high-perfor-
mance TENGs, we have developed a new method to produce
highly ordered hexagonally nonclose-packed micropattern
arrays on the dielectric surface. The overall fabrication process
of the convex patterned PDMS film is depicted in Figure 1b. As
can be seen, the process begins by using our improved phase
separation (IPS) method to prepare a highly ordered large-scale
concave film with a uniform thickness. Subsequently, the corre-
sponding convex patterned PDMS was fabricated via a molding
method in which the as-prepared concave film was exploited as
a reusable mother mold. Details of the experiment are provided
in the Experimental Section. Compared to the conventional
BF method, the newly developed IPS method has advantages
of fabricating an almost ordered concave film and relying on
methanol as a suitable nonsolvent that can induce the forma-
tion of a polymer layer that stabilizes droplets, enhancing the
lateral capillary force between adjacent droplets and facili-
tating the formation of an ordered structure. As a result, the
IPS method requires neither specially designed polymers nor
additional humid air, and thus large area highly ordered con-
cave films of engineering PMMA were successfully obtained.
Indeed, using the IPS method, a variety of commercial poly-
mers including polystyrene, poly(lactic acid), polyvinyl chloride,
and polyimide can be used to make highly ordered concave
films (see Figure S1 in the Supporting Information). Moreover,
it is worthwhile to note that the preparation of a concave film
by IPS just took a few minutes, while the fabrication of convex
patterned PDMS films by molding method took within 4 h.
Therefore, this strategy possesses advantages of time-saving as
well as mass production.
The convex patterned PDMS based-TENG was assembled in
a basic vertical contact–separation mode; its working principle
in single cycle operation is shown in Figure 1c. In the original
state, there is no charge generated on either the PDMS or Al
surfaces. Once two tribosurfaces are brought into physical
contact, positive charges are formed on the Al surface, while
corresponding negative charges are generated on the PDMS
surface according to the working principle of contact elec-
trification.[12] Due to charge accumulation, the triboelectric
charge density on the dielectric surface gradually increases and
reaches a saturation state after a number of contact–separation
cycles; the negative charges can be well-preserved on the PDMS
surface due to the inherent insulator-nature of PDMS. When
contacting surfaces are being separated, the electrostatic field
rising from the charges on the dielectric surface and the top Al
surface drives electrons in the attached bottom electrode to flow
through the external load to the top electrode until electrostatic
equilibrium is established. The charge density of the bottom Al
electrode is a function of the gap distance between the dielec-
tric and the top electrode. When the two surfaces become closer
again, the electrostatic field drives transferred electrons to flow
back from the top Al electrode to the attached Al electrode,
until the system goes back to the fully pressed equilibrium
state. Thereby, single cycle operation is achieved. The working
principle can be validated by current signals generated during
one cycle contact–separation of TENG (Figure 1d).
It has been thought that the enhancement of triboelectri-
fication output of the micro/nanostructured surfaces can
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Figure 1.  a) Picture illustrating a treefrog animal standing on a leaf and closed-up microstructure of its toe pads. b) Scheme representing the fabri-
cation process of the ordered concave polymer film and the convex PDMS replica. c) Sketch demonstrating the electrical generation during 1 cycle
contact–separation of TENG. d) Current signals generated during 1 cycle contact–separation of a flat PDMS based-TENG and a convex PDMS based-
TENG, respectively.

mainly be attributed to the increase in friction area. However,
in some cases, particularly in a surface structured with cylin-
drical micropatterns, the increase in contact area might not be
sufficient to explain the significant improvement of the output
electrification compared to that of the planar surface.[13]
Recently, Wu et al. proved that the amount of charge transfer is
not only determined by the friction area, but also significantly
affected by stress in the contact region.[14] In other words,
the deformation magnitude of surface patterns critically gov-
erns the output performance of the patterned surface-based

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TENGs. Otherwise, a sticky issue often associated with par-
tial contact can occur with two flat surfaces because tiny air
bubbles can be trapped inside closed regions formed by the
pressed surfaces, reducing the reliability and performance of
TENGs. Nevertheless, these issues can be overcome by pat-
terning the surface with continuously draining channels.[15]
Based on the above findings, we propose that the rational
design of an appropriate micro/nanopatterned surface that
achieves the largest contact area, maximum deformation mag-
nitude, and longest draining channel is crucial for fabricating
high-performance and reliable TENG devices. In addition,
it has been reported that porous structures can induce addi-
tional charges and also enhance final capacitance by reducing
the dielectric film thickness, resulting in enhancement of the
output performance of TENGs.[7e,16] In this case, uniformly
nonclose-packed microbead arrays with tunable separation
between patterns were prepared. Note that the uniform pat-
tern array with a special curved geometrical structure helps
to enhance the contact area,[17] while a proper separation is
favorable for achieving large deformation under a specific
pressure. Figure S2 in the Supporting Information presents
force signals obtained by a force sensor on flat and convex
patterned surfaces under the same external amplitude. It can
be observed that the impulses obtained with the flat surface
are larger than the ones obtained with the patterned surface
for both pressing and releasing states. This is because exces-
sive stress in the pressing state and a sticky phenomenon in
the releasing state should occur for the flat surface, whereas
elasticity associated with large deformation can occur in con-
tact regions of the patterned surface. This result obtained is
consistent with previous report.[17] Therefore, the tribosurface
with appropriate micropattern array prepared by this method
demonstrates dramatic enhancement of the output electric
generation compared to that of the unmodified flat surface, as
can be clearly seen in Figure 2d.
Surface morphologies of a typical as-prepared concave film
and its corresponding convex patterned PDMS are shown
in Figure 2. Figure 2a–c shows the large-area uniformity and
highly ordered honeycomb concave structures of the PMMA
film. Note that a super-large-area concave film with ordered
honeycomb structure (i.e., A4 size honeycomb film) can be
produced using this strategy (see Figure S3 in the Supporting
Information). In a typical experiment using a methanol con-
tent of 15 vol%, the size of pores is ≈2.7  µm, with separation
between pores of ≈0.8  µm (Figure 2b). From a cross-sectional
view (Figure 2c), it can be clearly observed that the monolayer
of isolated pore array formed on the surface of the polymer
film; in this monolayer, each pore has a spherical jar shape. The
inset fast Fourier transform (FFT) pattern further confirms the
long-range ordered hexagonal structure of the pore array. Sub-
sequently, convex patterned PDMS films were fabricated using
the corresponding concave films as mother molds. As shown
in Figure 2d–f, a large-area monodispersed microlens array
was observed and all figures confirm the uniformity of the con-
cave film throughout the coated surface. The microlens has a
spherical bead-shape with diameter of ≈3.7  µm and uniform
height of ≈1.6 µm, which corresponds to the pore shape of the
concave film. It is worthwhile to note that the concave PMMA
film is flexible and has sufficient mechanical strength to retain
the micropatterned structure after several iterations of the
stamping mold process (see Figure S4 in the Supporting Infor-
mation), resulting in reduced processing time and improved
reproducibility of producing the convex patterned triboelectret.
The convex patterned PDMS films with different pattern
sizes and separations between patterns (Figure  3b2–d2,b3–d3)
were fabricated using their corresponding concave films as
mother molds, which were prepared by IPS method with varied
methanol contents (Figure 3b1–d1). For comparison, another
porous PMMA film and its corresponding convex PDMS film
were also prepared using the BF method (Figure 3a1–a3). As

Figure 2.  Surface morphologies of a typical concave film prepared with a chloroform/methanol ratio of 85/15 at an ambient atmosphere (i.e., tem-
perature of 25 °C and humidity of 55%), and its corresponding convex PDMS replica. From left to right are optical microscope images, surface SEM
images, and cross-sectional SEM images, respectively, of the concave honeycomb film a–c) and the convex patterned PDMS film d–f). The inset of
(b) is the corresponding FFT pattern obtained from SEM image of the concave film.

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Figure 3.  Surface morphologies of concave polymer films and their corresponding convex patterned PDMS replicas. a1–d1) FESEM surface images
of concave porous films prepared by static BF method and IPS method with different methanol contents (10–20%). Porous polymer films with IPS were
prepared in normal ambient air with temperature of 25 °C and relative humidity level of 55%, while film with static BF was prepared under humidity
of ≈80%. a2–d2) FESEM surface images of corresponding convex patterned PDMS replicas prepared using concave porous films as mother molds.
a3–d3) FESEM cross-sectional images of PDMS replicas. Scale bars are 10 µm.

can be seen, the concave films prepared by IPS method dem-
onstrated uniformly ordered structures with methanol content
ranging from 10 to 20 vol%, whereas a nonuniform porous
film was obtained using the BF method. As a result, the
corresponding convex patterned PDMS films with uniform
microlens arrays were obtained using the IPS method, while a
nonuniform convex pattern was obtained using the BF method.
In addition, the microlens arrays obtained by IPS method pos-
sessed larger pattern size than the one prepared with the BF
method, and the size increases with increasing methanol con-
tent. Moreover, isolated microlens arrays were obtained with
IPS method at methanol content below 15%, while intercon-
nected microlens array was obtained using BF method and IPS
method at methanol content over 20%. The calculated surface
features of the convex patterned PDMS film prepared by BF
and IPS methods are provided in Figure S5 in the Supporting
Information.
It is reported that ordered honeycomb films can be pre-
pared via BF methods with special polymers such as amphi-
philic polymers, star-shape polymers, and block copolymers;
however, close-packed structures are usually obtained.[10,11,18]
Nonclose-packed patterns that can be directly obtained by the
newly developed IPS method with avoiding additional postsyn-
thetic steps thus making the process more cost-effective may
offer additional benefits over their close-packed analogues for
TENG application such as improved degree of deformation due
to increased separation between adjacent deformation sites.[19]
Therefore, well-controlled micropattern array prepared by this
method is highly desirable for the fully packed TENG where no
gap between electrodes is needed.[17]
PDMS films with different microlens arrays were prepared
and exploited as negative tribosurfaces for vertical contact–sepa-
ration mode TENGs. Three convex patterned PDMS films pre-
pared by IPS method with methanol contents of 10%, 15%, and
20% were denoted as IPS10, IPS15, and IPS20, respectively. The
effect of the film surface morphology on the electrical output
performance of the TENG devices was systematically investi-
gated and compared with the case of flat PDMS-based TENG
as a control. The open-circuit voltage and current density of the
TENG devices assembled with different PDMS films are shown
in Figure 4a,b. As can be seen, both the output voltage and cur-
rent density of the TENGs with structured PDMS films were
significantly enhanced compared to the case of using nonmodi-
fied flat PDMS film. Among the structured PDMS films, the
three films prepared with the IPS method in a methanol content
range of 10–20% demonstrated better electrical generation effi-
ciency than that of film prepared with BF method; this is because
TENGs based on IPS10, IPS15, and IPS20 films have higher
voltages and current densities than those of the TENG based
on BF film. Moreover, the TENG with PDMS film, which was
prepared via IPS method with methanol content of 10%, exhib-
ited the highest electrical output performance with a voltage of
≈490 V and current density of ≈24.4 µA cm−2 under an applied
force of ≈38 N and triggering frequency of 5 Hz. This output
voltage and current density are 2.4 and 9 times higher, respec-
tively, than those of the flat PDMS-based TENG. In addition,

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Figure 4.  Output open-circuit voltages a) and short-circuit current density b) of TENGs using flat and various-structured PDMS friction layers, respec-
tively. Dependence of output voltage and current density of TENG with IPS10 on resistance of external loads c). Variation of instantaneous power of
TENGs with flat, BF, and IPS10 on resistance of load d). Durability test of convex-TENG for 25 500 cycles e). Triggering conditions for these charac-
terizations were frequency of 5 Hz and applied force of ≈38 N.

the transfer charge densities of the TENGs using different
structured PDMS friction layers were compared as shown in
Figure S6 in the Supporting Information. It demonstrates the
similar tendency with short-circuit current densities as shown
in Figure 4b. Particularly, the TENG with IPS10 possessed the
highest transfer charge density of 41.3 µC m−2; this value is
almost 8 times higher than that of the TENG using a flat PDMS
and it is also much higher than that of the TENGs based on
other structured PDMS layers. The effect of micropatterns on
the performance enhancement of TENG device has been thor-
oughly discussed in previous studies; improvement is mainly
attributed to increase in friction area of the patterned surface
compared with the planar surface, leading to enhancement of
the triboelectric effect.[7a,20] Based on this concept, uniform pat-
tern arrays (IPS10 and IPS15), which have definitively larger
actual friction area, should possess higher electrical generation
ability than nonuniform pattern arrays (BF and IPS20). The
experimental results obtained agree well with theoretical expec-
tations. However, the increase in friction surface might not
be sufficient to explain the performance enhancement of uni-
form pattern arrays with different densities, since IPS15 has a
higher friction surface but lower electrical generation efficiency
than IPS10. As discussed above, the amount of charge transfer
not only is governed by the friction area, but also strongly
depends on the degree of deformation at the contact region.
As shown in Figure S5b in the Supporting Information, the

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separation/diameter ratio, which is closely related with the
deformation ability of patterns, was calculated and found to be
slightly higher on IPS10 than on IPS15. Therefore, IPS10 has
higher potential than IPS15 to obtain maximum deformation
and stress, resulting in output performance of IPS10-based
TENGs larger than that of IPS15-based TENGs. The highest
output obtained with IPS10 agrees with the result by Dudem
et al. They proved that the patterned surface with optimal
stress and contact area would result in the highest electrical
performance of TENG devices. Moreover, we conducted addi-
tional experiments to prove the effect of deformation degree
on performance enhancement of a convex patterned surface-
based TENG. In the first experiment, separation of IPS15-
mircrolens array was increased by stretching the film, thereby
increasing the deformation potential of the microlens array.
As expected, the TENG based on the prestretched IPS15 film
showed a considerable enhancement of both output voltage and
current compared with the case of using pristine IPS15 film
(see Figure S7 in the Supporting Information). In the second
experiment, the separation of the IPS15-microlens array was
kept at the original level, while the film was divided into several
smaller pieces and the effect of separation between the sepa-
rated pieces on the output performance was investigated. As
can be seen in Figure S8 in the Supporting Information, TENG
performance first increased with increasing separation, but
decreased with too-large separation. Based on these results, it is
clearly confirmed that TENG performance can be enhanced by
increasing the deformation degree of the electret film.
In order to determine the power generation effective-
ness of the as-prepared TENG device to external loads, the
IPS10-based TENG was connected to resistors with different
resistance values. As shown in Figure 4c, the instantaneous
voltage increased gradually while the current density decreased
with increasing external load from 103 to 109 Ω, demonstrating
a trade-off phenomenon due to ohmic loss. Based on this
result, the instantaneous output powers generated by IPS10
2
based-TENGs on the loads were calculated (Wd = I peak R); results
are depicted in Figure 4d. As can be seen, the power density
of the IPS10-based TENG first increased and then reached
a maximum value of ≈24 W m−2 at a matched resistance of
4.3 MΩ before decreasing with increase in the resistance value.
With the same characterization method, the variation of power
density of the TENG devices assembled with flat PDMS and BF
were also obtained (Figure 4d). The maximum output power
densities of the BF-based TENG and flat PDMS-based TENG
were 6.8 and 3.4 W m−2, respectively, at the same external load
of 100 MΩ. These results indicate that the IPS10 film boosts
the output power of the TENG device to 3.5 and 7 times higher
than those of the BF-PDMS film and unmodified planar PDMS
film, respectively.
Long-term durability is an important feature of TENG
devices for practical applications. The cyclic stability of the as-
prepared TENG device was evaluated by continuous testing for
25 500 cycles under the highest applied force used in this study
(≈38 N) at a frequency of 5 Hz (Figure 4e). The output voltage
signal of the as-prepared TENG device was uniform and no
obvious change after 25 500 cycles was observed. The micro-
lens array of the PDMS film was well preserved (see Figure S9
in the Supporting Information). The high durability of the
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microbead array can be attributed to its elasticity. Therefore, the
slight decrease in output voltage can be attributed to contami-
nation of the PDMS surface by dust from the air. The output
performance recovers to the initial value when dust is removed
by nitrogen blowing or a simple washing process. These results
suggest that the TENG based on the as-prepared convex pat-
terned PDMS film has exceptional structural durability and
superior performance stability.
The output performance of the TENG is strongly related to
the compressive force on the contact region; accordingly, large
force yields higher output, as shown in Figure 5a. The increase
of the output voltage and current density of the TENG can be
attributed to the increase in contact area and effectiveness of
the triboelectrification as well as reduction of the final thick-
ness of the convex patterned PDMS film with increasing com-
pressive forces. The electric output of the TENG device under a
certain triggering force has been considered as the most impor-
tant factor to determine the energy conversion efficiency of
the device. Therefore, the variation of the instantaneous power
densities of the IPS10-based TENG device corresponding to
the change of external loads under different applied forces
was investigated (see Figure S10 in the Supporting Informa-
tion). Beyond this, we conducted a comparative study of the
density of the power generated by the TENG device developed
in this study with other PDMS-based TENGs from selected
previous reports (Figure 5b).[5b,7e,16b,21] It is obviously demon-
strated that the newly developed TENG device possesses much
higher power density than those of all other selected PDMS-
based TENGs for a wide range of applied forces. Importantly,
the present TENG can yield superior power density (8.1 W m−2)
especially under small applied force (6.5 N), and this result
is believed to be highly meaningful for practical applications.
The merit of the tribomaterial produced by this method lies on
the special nonclose-packed microbead array which is inspired
by the microcosmic structure of treefrog’s toe pads showing
enlarged real contact with surface profile of various substrates,
thereby large contact area and maximized deformation magni-
tude can be propagated even if a very small compressive force
is applied. In addition, a comparison in output performance
of TENG devices based on micro/nanopatterned triboelectrets
including previously reported works and this work was con-
ducted, as shown in Table S1 in the Supporting Information.
The effect of the triggering frequency and the size of the device
on the TENG performance were also investigated and depicted
in Figure 5c,d. (Their raw data are given in Figures S12 and S13
in the Supporting Information.) The output voltage and current
density slightly increased with increase in the frequency from 1
to 10 Hz. However, the voltage increased while the current den-
sity decreased when the size of TENG device becomes larger.
In order to demonstrate the high energy harvesting effi-
ciency and high power output of the as-prepared TENG devices,
the IPS10-based TENG device was used to charge commercial
capacitors through a rectifier bridge. The charging rate curves
of capacitors charged using TENG devices with size of 3 × 3 cm2
under applied force of ≈30 N at a frequency of 20 Hz are shown
in Figure  6a. As can be seen, capacitors with small capacities
(0.1, 1, and 10 µF) can be quickly charged to over 10 V, while
a relatively large 100 µF capacitor can reach a voltage of ≈3 V
within 150 s. In addition, a 1000 µF capacitor was chosen as
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Figure 5.  Dependence of output voltage and current density of IPS10-based TENG device on applied force a), triggering frequency c), and size of device
d). b) Comparison of power densities of TENG devices obtained in present study and in previous reports. The selected references used in (b) are
provided in the Supporting Information.

a storage component to power an electronic thermometer after therefore able to successfully power the thermometer in normal
a charging process supported by the TENG under the same working condition for at least 30 s, which is long enough for
triggering conditions. The charging curve of the capacitor several right tests (see Figure 6c). An arch-shaped three-friction-
(Figure 6b) showed that it was charged to ≈2 V within 420 s; it is layered TENG device was fabricated in order to enhance the

Figure 6.  a) Charging curves of capacitors with different capacitances for IPS10-based TENG device with size of 3 × 3 cm2 applied force of ≈30 N at
frequency of 20 Hz. b) Charging and discharging process of 1000 µF capacitor by TENG device under identical triggering conditions and powering
electronic thermometer. c) Photographs illustrating experimental setup and possibility for use of TENG to charge capacitor and then to power tem-
perature sensor. d,e) TENG device with three friction layers used to instantly turn on 400 blue LEDs under simple hand pressing. f) Output voltage of
three-friction-layer TENG device under simple hand pressing.

Adv. Funct. Mater. 2019, 1901638 1901638  (8 of 10) © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
www.advancedsciencenews.com
total output power, as depicted in Figure 6d. Two convex pat-
terned PDMS films (4.5 × 4.5 cm2) were symmetrically attached
to the inside surfaces of the top and bottom Al electrodes, which
play roles of negative friction surfaces, while the center Al elec-
trode serves as the positive friction surface. 400 light-emitting
diodes can be instantaneously lit using this device to harvest
energy from simple hand pressing (see Figure 6e and Video
S1 in the Supporting Information). The output voltage of the
device was also measured to prove its high capability for pow-
ering many electronic devices, with results shown in Figure 6f.
3. Conclusion
We presented a simple, fast, scalable, and cost-effective method
to pattern a dielectric tribosurface with highly ordered and
nonclose-packed microbead arrays, mimicking the friction pads
of treefrogs. The pattern features, such as the size and separa-
tion between adjacent patterns, can be tuned by adjusting the
methanol content. The nature-inspired TENG based on the
structured PDMS film prepared with methanol content of 10%
and paired with flat Al as two friction surfaces demonstrated an
instantaneous power density of 23.9 W m−2 with output voltage
of 490 V and current density of 24.4 µA cm−2 under moderately
applied force of ≈38 N at frequency of 5 Hz, indicating a sev-
enfold power density enhancement relative to the case of a flat
PDMS-based TENG. Moreover, both the concave PMMA film
and the convex patterned PDMS film demonstrated high flex-
ibility and mechanical robustness because the concave film can
be reused many times without damage, while the convex pat-
terned PDMS based-TENG possessed an exceptional durability
and reliability for over 25 000 cycles of contact–separation. We
believe that the presented methodology can promote significant
progress in the green energy harvesting field owing to its sig-
nificant advances in facility, cost-effectiveness, efficiency, and
capability for mass production, giving this device great poten-
tial for many practical applications.
4. Experimental Section
Materials: PMMA engineering polymer (PMMA EG920) was kindly
supplied by LG Chem Co. (Seoul, Korea). PDMS and curing agent
(Sylgard 184) were purchased from Dow Corning. Copper film (thickness
of 0.1 mm) was obtained from 4Science (Seoul, Korea). The copper films
were successively cleaned with acetone, 0.1 m sulfuric acid solution,
and distilled water, followed by blow-drying in nitrogen gas prior to
use. Chloroform (anhydrous, with amylenes as stabilizers; 99.8%) and
methanol (anhydrous; 99.8%) were purchased from Sigma-Aldrich and
used as received.
Fabrication of Concave and Convex Film: Large-scale concave film
with uniform thickness was prepared by IPS method, as reported in
the previous work.[22] Briefly, a 10 wt% solution of PMMA in chloroform
was spin-coated or bar-coated onto the copper surface and dried.
Subsequently, the polymer film was exposed to the mixture of chloroform
and methanol (methanol content ranged from 10 to 20 vol%) before
drying in air (i.e., temperature of 23 °C and humidity of 55%). The
dipping conditions were dipping time of 5 s and withdrawal speed of
60 cm min−1. Ordered concave film spontaneously formed on copper
substrate after complete drying process. Note that it was possible to
obtain super-large-scale concave film with industrial coating techniques
such as doctor blade coating or “roll-to-roll” coating.
Adv. Funct. Mater. 2019, 1901638 1901638  (9 of 10)
www.afm-journal.de
For comparison, porous PMMA film was also prepared by static
BF method. Accordingly, a 10 wt% PMMA solution in chloroform was
casted onto a copper surface in a highly humid environment (humidity
of ≈80%). After drying, porous PMMA film was obtained.
The convex patterned PDMS film was fabricated by micromolding
method using the as-prepared concave PMMA film as mother mold.
The base PDMS and its crosslinker with ratio of 10:1 w/w was
thoroughly mixed and then casted onto the concave film. Note that the
casting film should be carefully degassed in vacuum to ensure liquid
PDMS completely fills the micropores. The PDMS precursor was cured
at 70 °C for 4 h, and then carefully peeled off from mold to obtain
the convex patterned PDMS film and leave the concave PMMA mold
without any damage. The concave PMMA mold can be reused many
times.
Assembly of TENG: Two polystyrene plates with aluminum adhering
to their inner surfaces were used as top and bottom mechanically
supporting substrates for TENG. The convex patterned PDMS was
then fixed onto the bottom substrate by adhering its smooth surface to
the Al while its patterned side served as friction surface. Al on the top
substrate served both as friction surface and electrode. To investigate
the influence of the surface morphology of the PDMS film on the
performance of the TENG, devices with size of (2 × 2 cm2) were used.
The separation distance of two triboelectric layers of the TENG was fixed
as about 5 mm.
Characterization: The surface morphologies of the concave PMMA
films and the convex patterned PDMS films were characterized using
field-emission scanning electron microscopy (FE-SEM, S-4800, Hitachi,
Japan). A mechanical shaker (Model No. ET-126-4, Labworks Inc.) was
used to apply vertical impulse impact to the TENG. A digital phosphor
oscilloscope (Model No. DPO 3052, Tektronix, Inc., Beaverton,
OR, USA) and a low-noise current preamplifier (Model No. SR570,
Stanford Research Systems, Inc., Sunnyvale, CA) were used for
electrical measurements. The input force applied to the TENG was
measured by a force sensor (Model No.1051V3, Dytran Instrument,
Inc.,USA) integrated with an ICP sensor signal conditioner
(Model No.480E09).[6a]
Supporting Information
Supporting Information is available from the Wiley Online Library or
from the author.
Acknowledgements
This work was supported by the Creative Research Initiative Program
(2015R1A3A2028975), funded by the National Research Foundation
of Korea (NRF). This work was supported by the Defense Acquisition
Program Administration and the Agency for Defense Development in
Korea under the contract UD170023DD.
Conflict of Interest
The authors declare no conflict of interest.
Keywords
mass fabrication, nonclose-packed, surface patterning, Treefrog toe pads,
triboelectric nanogenerators
Received: February 23, 2019
Revised: April 15, 2019
Published online:
© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
www.advancedsciencenews.com
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