Nano Energy 34 (2017) 69–75

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High-power triboelectric nanogenerator prepared from electrospun mats MARK

with spongy parenchyma-like structure
⁎
Bin Yua,b, Hao Yua,b, , Hongzhi Wanga,b, Qinghong Zhanga,b, Meifang Zhua,b
a
College of Material Science & Engineering, Donghua University, Shanghai, China
b
State Key Lab for Modification of Chemical Fibers & Polymer Materials, No. 2999 North Renmin Road, Songjiang District, Shanghai 201620, China

A R T I C L E I N F O A BS T RAC T

Keywords: A triboelectric nanogenerator was prepared from electrospun polymer mats with a spongy parenchyma-like
Triboelectric nanogenerator structure. The spongy parenchyma-like structure was imparted on the electrospun mats via cold-compacting
Energy harvesting post treatment. The optimized triboelectric nanogenerator attained a maximum electrical output, short circuit
Electrospinning current, and load power of 695 V, 58 μA, and 3.1 W m−2, respectively. Energy harvesting from human slapping
Spongy parenchyma-like structure
motion was used by the triboelectric nanogenerator to power an everyday scientific calculator. The mechanism
of how the triboelectric power was enhanced by the spongy parenchyma-like structure is discussed, and is
similar to the effect of an electret. The surface potential of the triboelectric nanogenerator based on an
electrospun mat with a spongy parenchyma-like structure was higher than that based on an untreated
electrospun mat. This triboelectric nanogenerator and its technology may have potential in portable electronics
and flexible sensors.

1. Introduction ning parameters [45]. This variety of nanostructures gives electrospin-

Triboelectric nanogenerators (TENGs) are a promising approach to
energy scavenging [1–14]. The output of TENGs is based on the
coupling of triboelectrification and electrostatic induction [15–18], but
TENGs suffer from low power density, require complex preparation
[5,7–9,19,20]. So the practical application of TENGs is currently
limited by their low output performance. Several strategies have
recently been reported to overcome these problems, and include
surface optimization [21–28], material hybridization [29–36], and
output management [37–41].
There has been much effort to prepare hybrid materials or/and
rough surfaces for frictional materials because of their increased
surface potential [22,24–26]. The surfaces of materials have been
modified by various methods, which inevitably increase technological
and manufacturing costs, and sometimes degrade the materials proper-
ties. A simple, cost-effective, and efficient process for manufacturing
triboelectric materials is therefore of interest. Electrospinning is a
straightforward, economical, and versatile approach to prepare nanos-
tructured mats from various materials [42–44]. The advantages of
electrospun nanofiber mats include their high specific surface area,
very high surface roughness, and good flexibility. Nanofiber mats with
complex structures such as nonwoven, aligned, and patterned can be
manufactured in a controllable manner, by controlling the electrospin-
ning great potential for preparing triboelectric materials for TENGs
[25,26,31].
However, electrospun mats do have a significant drawback. As the
three-dimensional (3D) structure mats (Fig. 1), the open porous
structure distributing inside mats could cause the segmental dissipa-
tion of charge [26,31], when the frictional materials contact each other.
On the other hand, in the 3D structure, only nanofibers near the
contacting surface are able to collect and deliver charge between the
two contacting layers, which act as triboelectric layers. Large amounts
of nanofibers between the nanofibers of the superficial frictional layer
and the adjacent electrode negatively affect the power output of
TENGs. TENGs can break down from their unsealed structure, and
from nanofiber abrasion on the triboelectric layers. The latter is of
particular concern if the thickness of the nanofiber layer with negative
role nanofibers decreases, or if this nanofiber layer is lost altogether.
Therefore it needs an effective method to make fully use of the
nanofiber layer. The electret [46–49], particularly the porous spongy
electret, has been used to enhance the power performance of TENG,
due to its outstanding effect on surface charge density
[23,34,38,50,51]. The large amounts of useless, even disadvantageous
nanofibers in mats can become useful if they are transfer into porous
spongy-structure electret. Moreover, the porous structure will be
polarized in-situ, owe to the strong electric field during electrospinning.

⁎
Corresponding author at: College of Material Science & Engineering, Donghua University, Shanghai, China.
E-mail address: yuhao@dhu.edu.cn (H. Yu).

http://dx.doi.org/10.1016/j.nanoen.2017.02.010
Received 22 December 2016; Received in revised form 24 January 2017; Accepted 7 February 2017
Available online 08 February 2017
2211-2855/ © 2017 Elsevier Ltd. All rights reserved.
B. Yu et al.
Fig. 1. Schematic diagram of electrospun nanofibers mat with different effects on TENG. The green nanofibers located at the surface of mat act as triboelectric layer, which can collect
and deliver charges so as to enhance the output power of TENG. However, as the open porous structure, the red nanofibers are negative for output enhancement because they are so far
to collect and deliver charges, moreover they will dissipate charges to the external environment.
In this study, electrospun polymer mats with a spongy parenchyma-
like structure were prepared. These electrospun mats were then applied
in a triboelectric nanogenerator (denoted SP-TENG), which exhibited
good power performance. The spongy parenchyma-like structure of the
polymer mats was obtained by subjecting them to cold-compacting
post treatment. The majority of the nanostructure on the surface of the
contact layers was retained upon post treatment. Post treatment also
caused the negative-effect nanofiber to transfer into the spongy
parenchyma-like structure. The resulting structure could be polarized
by an electric field, similarly to the effect of an electret. These findings
may promote to practical application of TENGs in smart portable
electronic equipment.
2. Materials and methods
2.1. Materials
Polyvinylidene fluoride (PVDF) powder (FR904, weight average
molecular weight Mw=6×105) was purchased from Shanghai 3 F New
Material Co., Ltd., P. R. China. Poly(3-hydroxybutyrate-co-3-hydro-
xyvalerate) (PHBV) (Y1000P, weight average molecular weight
Mw=2.67×105, ratio of Poly(3-hydroxyvalerate) HV=1.10 mol%) was
purchased from Zhengjiang Tianan Biological Co., Ltd. Analytical
reagent grade N,N-dimethylformamide (DMF), trichloromethane, and
acetone were obtained from the Shanghai Chemical Reagent Plant, P.R.
China.
2.2. Electrospinning and cold-compacting post treatment of polymer
mats
PVDF was dissolved in 6: 4 DMF: acetone (w/w) at 80 °C for 30 min
to prepare PVDF solution (10%, w/w). PHBV was dissolved in
trichloromethane at 60 °C for 1 h to prepare PHBV solution (8%, w/
w). The purpose built electrospinning equipment is shown in Fig. S1 ().
Using this equipment, homogeneous polymer solutions were charged
into plastic syringes and were subjected to a direct-current (DC)
voltage of up to 18 kV, using a DC power supply (JG50-1, Shanghai
Shenfa Detection Instruments, P. R. China). Spinning solutions were
delivered from a stainless needle tip at a flow rate of 1 ml h−1, using a
micro-syringe pump (KDS101, USA). The distance between the needle
tip and roller collector was 15 cm. The relative humidity and tempera-
ture were controlled at ~20% and 25 ± 2 °C, respectively.
After electrospinning, electrospun polymer mats were treated by
cold-compacting at different pressures by a sheeter (HY-12, Tianjin
Tianguang Instruments Co., Ltd., P. R. China) between two metallic all-
polishing pressing surfaces. The dwell time was controlled at 60 s, after
which the pressure was withdrawn rapidly.
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Nano Energy 34 (2017) 69–75
2.3. Fabrication of SP-TENGs
After post treatment, PVDF and PHBV mats of size of 40×55 mm
were adhered to the top and bottom of a rectangular flexible poly-
ethylene terephthalate (PET) film of size of 100×60×0.1 mm. The PET
film had previously been folded in half along the length direction.
Aluminum foil used to collect the polymer nanofibers during electro-
spinning then acted as the electrodes for the SP-TENG.
2.4. Characterization
A Hitachi S-4800 field-emission scanning electron microscope (FE-
SEM) was used to investigate the morphologies of the polymer
electrospun fibers and closed-nanopore structures. A thin platinum
layer was sputtered on the surface of samples before examination, to
prevent charging. The electrical output generated by the SP-TENGs
(including voltage and current) was measured using a high-power
source meter instrument (Model 2657A, Keithley, USA).
Measurements were carried out under the force of the bending stage
produced by a custom-made apparatus at a frequency of 2 Hz, as
shown in Fig. S2 (Supporting information). The densities of the mats
were determined using a solid density instrument (Ultrapycnometer
1000, Quantachrome USA). Each sample (40×55 mm) without electro-
des was tested five times at room temperature, and reported results are
the averages of these five measurements. The surface potentials of the
polymers mats were determined using an electrostatic voltmeter (Trek
541A, USA), at relative humidity of ~20% and room temperature. First,
two sides of the polymers mats assembled in the TENG were rubbed
together for 10 min, to ensure even charge delivery. Second, one side of
the mat was tested with the electrostatic voltmeter. The TENG was then
reassembled to allow rubbing for a further 10 min, after which the
other side was tested.
3. Results and discussion
Schematic diagrams of the fabrication of the SP-TENG are shown in
Fig. 2a. The substrate was a flexible rectangular PET film that had been
folded in half. This provided flexibility for friction, and separation
between the positive and negative triboelectric materials. The alumi-
num foil used to collect the polymer nanofibers during electrospinning
also acted as electrodes, and was connected to an external circuit.
Fig. 2a (iv) shows a digital photograph of the SP-TENG. Fig. 2f and g
show the output voltages of TENGs based on electrospun polymer mats
before and after post treatment on both PVDF and PHBV mats,
respectively. These output voltages were obtained when connected
with a resistance of 100 MΩ, at a frequency of 2 Hz. Post treatment of
the polymer mats resulted in the voltage increasing by approximately
three times, from 240 V before post treatment to 695 V after post
treatment. Schematic diagrams of the formation of the electrospun
polymer mats (Fig. 2b and c), and FE-SEM images of their micro-
B. Yu et al. Nano Energy 34 (2017) 69–75

Fig. 2. (a). Schematic diagrams of the fabrication of the SP-TENG based on a closed-nanopore electrospun mat.(i), (ii) and (iii) show the process of fabrication of the TENG; (iv) shows a
digital photograph of the SP-TENG. (b), (c) Schematic diagrams of electrospun polymer mats with different quantity of surface charges before and after the post treatment on both PVDF
and PHBV mats. (d), (e) FE-SEM images of electrospun polymer mats before and after the post treatment on both PVDF and PHBV mats. Scale bars indicate 500 nm. (f), (g) Optimal
output voltages of SP-TENGs before and after post treatment on both PVDF and PHBV mats, connecting with a resistance of 100 MΩ.

structures (Fig. 2d and e), are shown, respectively. Comparing the FE-
SEM images shows that the fluffy 3D microstructure on the electrospun
mat transferred into the structure of the spongy parenchyma, upon
post treatment on both PVDF and PHBV mats. This occurred because
the glass transition temperature was lower than room temperature. The
polymer nanofibers readily cemented with each other, to form spongy
parenchyma-like closed nanopores. This greatly increased the output of
the TENG.
The pressure used in the post treatment was systematically varied
to determine the optimal formation conditions of the PVDF and PHBV
electrospun mats. The post treatment pressure was found to affect the
output voltages of TENGs based on PVDF mats, when the PHBV mats
were not subjected to post treatment. The triboelectric performance
resulting from treating a single side (i.e. PVDF side) of the SP-TENG
did not continuously increase with increasing pressure. Fig. 3a shows
that there was a maximum voltage of about 585 V (resistance of
100 MΩ, which was used in all subsequent measurements) at a post
treatment pressure of 25 MPa. Further increasing the pressure led to a
decrease in the triboelectric output voltage. The effect of closed
nanopores in the electrospun polymer mats enhanced the TENG
output, as discussed in more detail. Fig. 3b shows the short circuit
currents of SP-TENGs containing electrospun PVDF mats subjected to
different post treatment pressures. Similar to the output voltage, the
maximum short circuit current occurred at a post treatment pressure of
25 MPa. Average triboelectric voltages and short circuit currents at
each pressure are shown in Fig. 3c.
Electrospun PHBV mats pressed at different pressures were used to
assemble SP-TENGs with post treated PVDF mats (the optimized
PVDF pressure was held constant at 25 MPa). The test results showed
similar trends, as shown in Fig. 3d, e, and f. The maximum triboelectric
voltage and short circuit current were obtained upon pressing the
PHBV mat at 6 MPa.
The maximum output voltage and short circuit current of the
optimized SP-TENG were 695 V and 58 μA, respectively, which were
316% and 363% higher than those prior to post treatment, respectively
(Fig. 3f).
Electrical measurements of the optimized SP-TENG are shown in
Fig. 4 and S4 (Supporting information). Fig. 4a shows output current
densities and voltages measured under various external loads, at a
frequency of 2 Hz. Fig. 4b shows maximum output powers measured
under external loads of 0.1–1000 MΩ. The output power is determined
by the following equation:
U2
P=
R (1)
where the U and R stand for output voltage of TENG and loading
resistance. The efficiency of the SP-TENG is defined as the ratio
between the input mechanical energy and the generated electric energy
that is delivered to the load, determined by the following equation:
Eele ∫ P dt
η= =
WF WF (2)
where Eele and WF stand for the electric energy and the input
mechanical energy. The WF was calculated to be about 1.10 mJ for
one cycle by the custom-made apparatus. The output current density
decreased with increasing resistance. The output voltage increased with
increasing resistance until it reached saturation. Consequently, the
output power and efficiency of SP-TENG reached a maximum of about

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B. Yu et al.
Fig. 3. Electrical measurements of various SP-TENGs, at a frequency of 2 Hz. (a) Output voltages and (b) short circuit currents of SP-TENGs containing electrospun PVDF mats
subjected to different post treatment pressures on only PVDF electrospun mats (PHBV mats not post treated), and (c) statistical results. (d) Output voltages and (e) short circuit currents
of SP-TENGs containing electrospun PHBV mats subjected to different post treatment pressures on PHBV electrospun mats (when the treated pressure on PVDF mats kept on 25 MPa),
and (f) statistical results.
3.1 W m−2 and 47.6%, at an external load of 10 MΩ (Fig. 4b and c).
Fig. 4d shows that the SP-TENG was connected to the calculator by
means of transition of a bridge rectifier circuit. The calculator operated
as normal, upon subjecting the SP-TENG to continuous patting motion.
A video showing the powering of the scientific calculator is available in
the Supporting information.
Fig. 5 shows a schematic of the proposed mechanism for the
enhanced surface potential of the electrospun polymer mats subjected
to post treatment in the SP-TENG. In the initial state, the ‘fluffy’
polymer mat composed of nanofibers contains many interspaces
between nanofibers (Fig. 5a and b). These interspaces connect to form
the 3D network structure. Charge exchange causes the electric charge
to dissipate into the external environment, through the inner paths of
interspaces within the mat. This reduces the surface potential of the
overall TENG upon operation. The surface potential can be described
by the following formula:
φ,s=φs −φd
where φ,s is the surface potential of the nanopore-based mat, φs is the
total surface potential formed by the surface nanostructure of the
PVDF mat, and φd is the quantity of dissipation surface potential by the
inner paths. The interspaces gradually disappear as pressure is applied.
The spongy parenchyma-like structure forms, because nanofibers are
extruded when pressure is exerted on the mat. This significantly
reduces the size of the inner paths formed by the interspaces, and
Nano Energy 34 (2017) 69–75
mitigates charge dissipation (decreasing φd ). On the other hand, the
charges are stored into these formed inner nanopores. Thus, the
nanoporse can induce charges to be kept on surface of mat, like as a
charge trap. However, there are limited charges stored in one nano-
pore. So the quantity of pores is the key to enhance surface potential of
mat. The electric quantity in one polarized pores is defined as q, so the
surface potential increased by induced charges can be calculated by the
following formula:
φi=n
1
4πεp
∫ drqq (4)
where n is the quantity of nanopores, εp is the dielectric constant of
polymer, and rq is the distance between the given nanopore and mat
surface. In the formula (4),
1
4πεp
∫ drqq is almost invariable for one
nanopore. Thus the φi is subject to the change of the pore quantity n .
In the case of Fig. 5c and d, the surface potential can be calculated
(3) by the following formula:
φ,s=φi +φs −φd (5)
Subjecting the polymer mat to the stronger pressure results in
spaces no longer being interconnected, the more closed nanopores
occur throughout the entire mat, as shown in Fig. 5e and f. This
increases φi and decreases φd in Eq. (5). Accordingly, the TENG output
performance is improved because of the enhanced surface potential φ,s .
Closed nanopores are gradually destroyed upon subjecting the
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B. Yu et al. Nano Energy 34 (2017) 69–75

Fig. 4. Electric measurements of the optimized SP-TENG. (a) Output current densities and voltages of the SP-TENG under various external loads, at a frequency of 2 Hz. (b) (c) Output
powers and efficiency of the SP-TENG under external loads of 0.1–1000 MΩ. (d) Digital photograph of the scientific calculator operating normally, while subjecting the SP-TENG to
continuous patting motion.

Fig. 5. Surface potential enhancing mechanisms of polymer electrospun mats. (a) FE-SEM image and (b) schematic diagram of the initial PVDF electrospun mat. The exchanged charges
are dissipated because of the fluffy 3D network structure, so as to lower surface potential. (c) FE-SEM image and (d) schematic diagram of the PVDF mat subjected to a given pressure.
Corresponding results for (e) (f) optimum and (g) (h) excessive pressures. SEM scale bars indicate 1 µm. The suitable treated pressure can make mats form amount of spongy
parenchyma-like structures, which are polarized to make it helpful to hold charges on surface of triboelectric layer. However excessive pressure decreases the quantity of spongy
parenchyma-like structures.

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B. Yu et al.
Fig. 6. (a) Relative densities and (b) surface potentials of electrospun PVDF mats, upon subjecting to different post treatment pressures. (c) Relative densities and (d) surface potentials
of electrospun PHBV mats, upon subjecting to different post treatment pressures.
electrospun mat to excess pressure, as shown schematically in Fig. 5g
and h. The electrospun nanofiber mat tends to form a solid thin film,
and its surface nanostructure is destroyed. This is detrimental to the
surface potential of the working materials in the TENG.
The relative densities of the mats were measured to further
investigate the mechanism of the formation of the spongy parenchy-
ma-like structure in the mat upon post treatment. The results are
shown in Fig. 6. The surface potentials of the mats were also tested, to
confirm the validity of this mechanism. Fig. 6a shows the densities of
untreated and post treated electrospun mats. The relative density of the
electrospun PVDF mat decreased with increasing post treatment
pressure until 25 MPa, because of nanopores continued to form within
the mat. The relative density then increased with further increasing
pressure, because the nanopores collapsed. Corresponding with the
above mechanism, the maximum number of closed nanopores occurred
at 25 MPa, along with the highest open circuit current (Fig. 6a). The
surface potential of the PVDF mat in Fig. 6b also indicated that the
formation of more closed nanopores led to a higher potential. Results
for the PHBV mats exhibited similar trends to those for the PVDF mats,
as shown in Fig. 6c and d. The optimum pressure was 6 MPa, at which
the initial surface potential of the PHBV mat reached 850 V.
4. Conclusions
We report electrospun mats with a spongy parenchyma-like struc-
ture, and their application in a high-power triboelectric nanogenerator.
A cost-effective cold-compacting post treatment is used to form
complex microstructures in the friction materials. The optimized SP-
TENG fabricated with PVDF and PHBV mats can effectively scavenge
mechanical energy from the external environment. The optimized SP-
TENG produces a maximum output voltage, short circuit current, and
load power of 695 V, 58 μA and 3.1 W m−2, respectively. The perfor-
mance of the SP-TENG is enhanced by over three times compared with
that of the TENG containing untreated electrospun mats. The working
principle is verified by measuring the relative densities and surface
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Nano Energy 34 (2017) 69–75
potentials of mats subjected to various post treatment conditions. The
SP-TENG can directly power an everyday scientific calculator. The
advantages of the SP-TENG include its simple fabrication, low cost, and
high performance. It may have potential in energy supplies for portable
electronics.
Acknowledgement
We gratefully acknowledge the financial support by Natural Science
Foundation of China (No.51473034), The Shanghai Natural Science
Foundation (15ZR1401200), the Program for Professor of Special
Appointment (Eastern Scholar) at Shanghai Institutions of Higher
Learning, Program of Shanghai Academic Research Leader
(16XD1400100), the Program of Introducing Talents of Discipline to
Universities (No.111-2-04), and the Fundamental Research Funds for
the Central Universities (2232014A3-06).
Appendix A. Supplementary material
Supplementary data associated with this article can be found in the
online version at doi:10.1016/j.nanoen.2017.02.010.
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