Research Article

Cite This: ACS Appl. Mater. Interfaces XXXX, XXX, XXX−XXX www.acsami.org

Highly Transparent and Flexible All-Solid-State Supercapacitors

Based on Ultralong Silver Nanowire Conductive Networks
Xing Liu,†,§ Dongdong Li,†,§ Xin Chen,† Wen-Yong Lai,*,†,‡ and Wei Huang†,‡
†
Key Laboratory for Organic Electronics and Information Displays, Institute of Advanced Materials (IAM), Jiangsu National
Synergetic Innovation Center for Advanced Materials (SICAM), Nanjing University of Posts and Telecommunications, 9 Wenyuan
Road, Nanjing 210023, China
‡
Shaanxi Institute of Flexible Electronics (SIFE), Northwestern Polytechnical University (NPU), 127 West Youyi Road, Xi’an
710072, Shaanxi, China
*
S Supporting Information
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ABSTRACT: Ultralong silver nanowires (Ag NWs) are preferred for enabling
transparent conductive networks with low sheet resistance, high transparency, and
excellent mechanical flexibility, which offer great merits in achieving high-
performance and flexible energy storage devices. Herein, a new type of polyol
process was proposed for the synthesis of ultralong Ag NWs. Uniform Ag NWs with
the average length of 75 μm were obtained. Transparent conductive films (TCFs)
based on the as-prepared Ag NWs exhibited low sheet resistance of 15.2 Ω/sq at
84% transmittance with a negligible change in sheet resistance after bending.
Flexible all-solid-state supercapacitors based on the resulting Ag NW TCFs showed
high transparency (>50%), good mechanical flexibility, and high cyclic stability with
only slight areal capacitance decays after 100 times of bending (∼25%) and 5000
charge−discharge cycles (∼15%). The results manifest great potentials of the
resulting TCFs based on ultralong Ag NWs for flexible and wearable energy-storage
applications.
KEYWORDS: flexible supercapacitors, transparent supercapacitors, silver nanowires, ultralong, all-solid-state

1. INTRODUCTION highly transparent and flexible supercapacitors, ultralong Ag

Electrochemical energy storage in the form of supercapacitors
have been widely considered as the promising power supply
source for future flexible and portable electronic devices due to
their high power capability and long cycling stability.1−6 The
latest progress of next-generation flexible electronics may also
require the ultimate form of power source with high flexibility
and transparency for both functional and aesthetic reasons,
especially for wearable electronics, smart windows, etc.7−9 As
the core component, transparent conductive films (TCFs) and
their structures undoubtedly play critical roles in controlling
their performances.10,11 Among various TCFs, indium tin
oxide (ITO) has been widely employed in various optoelec-
tronic devices (e.g., organic light-emitting diodes (OLEDs),
solar cells, touch screen displays, etc.) due to its high optical
transmittance (>90%) and low sheet resistance (<25 Ω/
sq).12,13 However, the limited reserves of the element indium
and high vacuum deposition technique lead to high material
and processing cost.14 Meanwhile, the inherent brittleness of
ITO also limits its further applications in flexible elec-
tronics.15,16 Therefore, the development of new transparent
conductive materials is urgently needed to fulfill the low-cost,
flexible, and wearable requirements.
Of the existing various alternatives, silver nanowires (Ag
NWs) are rather promising to offer comparable performance to
ITO with low cost and high mechanical flexibility.17−23 For
NWs are preferred to construct flexible TCFs with high optical
transmittance, low sheet resistance, and superior flexibility.
This is because long nanowires can offer both longer
percolation paths and higher flexural resistance with less
material usage.24 Therefore, the development of ultralong Ag
NWs is critical. However, due to the difficulty in controlling
the length and uniformity of Ag NWs, it is still largely
challenging to achieve ultralong silver nanowire conductive
networks for constructing high-performance transparent and
flexible supercapacitors.
The polyol method has been considered as the most
promising process for preparing ultralong Ag NWs by using
poly(vinylpyrrolidone) (PVP) as the capping agent and
ethylene glycol (EG) as the reducing agent and solvent.
However, various factors in this process including additive
agents, stirring speed, ratio of chemicals, and injection speed of
chemicals could affect the nucleation and growth of Ag NWs,25
and thus relatively short nanowires 1−20 μm in length were
usually obtained for a common preparation.26−28 The ability to
regulate the number of seed crystals and simultaneously
improve its growth process is considered critical for the
Received: June 18, 2018
Accepted: August 24, 2018
Published: August 24, 2018

© XXXX American Chemical Society A DOI: 10.1021/acsami.8b10138

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ACS Applied Materials & Interfaces
Figure 1. (a, b) SEM and high resolution SEM (HRSEM) images of the as-prepared Ag NWs (inset: Ag NW suspensions in alcohol). (c) XRD
spectrum and (d) the length distribution of Ag NWs.
synthesis of ultralong Ag NWs with uniform sizes. Based on
the considerations mentioned above, we proposed a simple
and straightforward methodology to synthesize Ag NWs with
high length and uniformity. The nucleation and growth process
were effectively controlled by adjusting the stirring process and
the injection rate of AgNO3. Flexible TCFs based on long Ag
NWs showed a low sheet resistance and a high mechanical
flexibility. Furthermore, flexible all-solid-state supercapacitors
with high transparency, good flexibility, and superior electro-
chemical performance were prepared, manifesting their great
potential applications in flexible and wearable energy-storage
devices.
2. EXPERIMENTAL DETAILS
2.1. Preparation of Ag NWs. In a typical synthetic route, 30 mL
EG solution containing 0.26 g PVP (Mw = 1 300 000) and 0.493 mL
CuCl2 solution (7.4 mM) was added into a three-necked flask and
stirred at 180 °C for 1 h before cooling down to 160 °C. Then, 10 mL
AgNO3 solution (1 mM) in EG was injected at the rate of 0.17 mL/s
and stirred for 5 min. After that, the stirring was stopped and the
solution was heated for another 85 min at 160 °C. The nanowires
were precipitated by the addition of ethanol and isolated via
centrifugation.
2.2. Fabrication of Transparent Electrodes. Ag NWs in
ethanol solution (0.36 wt %) was spin-coated onto the poly(ethylene
terephthalate) (PET) substrates at 1500 rpm for 1 min before
annealing at 120 °C for 15 min. The poly(3,4-
ethyelenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS)
layer was obtained by spin-coating the preprocessed PEDOT:PSS
solution (1.20 wt %) on top of the Ag NW films at 500 rpm for 5 s
and 1500 rpm for 55 s successively, followed by annealing at 120 °C
for 15 min. The preprocessing of PEDOT:PSS solution consisting of
filtering with 0.22 μm syringe filters, mixing with 2 vol % surfactant
(Triton-X 100) and 6 vol % EG, and sonicating gave a uniform
formulation.
2.3. Preparation of Supercapacitors. Supercapacitors were
constructed with the structure of PET/Ag NWs/PEDOT:PSS/
H3PO4/poly(vinyl alcohol) (PVA)/PEDOT:PSS/Ag NWs/PET, in
which the middle H3PO4/PVA layer served as the electrolyte and the
Ag NWs/PEDOT:PSS films on both sides were used as the
electrodes. The H3PO4/PVA electrolyte was prepared by mixing 1.0
B DOI: 10.1021/acsami.8b10138
Research Article
g H3PO4 and 1.0 g PVA with 10.0 mL deionized water at 120 °C
before drop-coating on top of the PEDOT:PSS layer. The two Ag
NWs/PEDOT:PSS electrodes were then pressed together to form a
symmetrical supercapacitor. The amount of PEDOT:PSS (0.019 mg/
cm2) and Ag NWs remained invariant for preparing different
electrodes.
2.4. Characterization. The morphologies of Ag NWs were
recorded by a Hitachi S-4800 field-emission scanning electron
microscope (FE-SEM). Powder X-ray diffraction (XRD) was
performed on a Rigaku-Ultima III X-ray diffractometer equipped
with a Cu Kα radiation (λ = 0.1541 nm). The photographic images
were taken by a digital camera (Canon 600D, Japan). The optical
transmittances of the samples were measured by an UV−vis
spectrophotometer (Shimadzu UV-3600). The sheet resistances of
films were obtained by a four-point probe system (FP-001). The
electrochemical properties of the supercapacitors including cyclic
voltammetry (CV), galvanostatic charge−discharge (GCD), and
impedance spectroscopy were measured with a CHI660 electro-
chemical workstation.
3. RESULTS AND DISCUSSION
SEM images of the Ag NWs are shown in Figure 1a,b, which
clearly manifest that the as-prepared nanowires are mono-
disperse with uniform sizes. The average dimension of the Ag
NWs was determined to be 75 μm in length and 120 nm in
diameter, respectively, through random measurements of more
than 200 nanowires. The resulting ultralong Ag NWs are
favorable for preparing TCFs with high transparency, high
electrical conductivity, and excellent flexibility due to their
extremely high aspect ratio (>600). XRD spectra (Figure 1c)
show four typical diffraction peaks at 38.2, 44.5, 64.5, and
77.4° corresponding to the (111), (200), (220), and (311)
crystalline planes of the face-centered cubic lattice. The
statistics of the length distribution given in Figure 1d shows
that the as-prepared nanowires are mainly in the range of 70−
90 μm, exhibiting a narrow size distribution. The results
demonstrate superior advantages of a shorter and simpler
synthesis process as compared with those grown by previous
one-step/multistep methods,24,29 which are much more
favorable for further large-scale production.
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Figure 2. SEM images of Ag NWs synthesized at different injection rates of AgNO3: (a) 0.03 mL/s, (b) 0.06 mL/s, (c) 1.00 mL/s, and (d) 3.30
mL/s (inset: the average length of Ag NWs synthesized at different injection rates of AgNO3).

Figure 3. SEM images of Ag NWs synthesized at different stirring times: (a) 15 min, (b) 30 min, (c) 60 min, and (d) 90 min (inset: the average
length of Ag NWs synthesized at different stirring times).

To understand the possible mechanism, a series of
experiments were conducted to investigate the role of the
stirring process and the injection rate of AgNO3 solution in the
synthesis of Ag NWs. As shown in Figure 2a, un-uniform Ag
NWs with the average length of 30 μm were obtained when a
low injection rate of 0.03 mL/s was adopted for AgNO3
solution. As the injection rate of AgNO3 solution increases to
0.06 mL/s (Figure 2b), the average length of Ag NWs
increases to 50 μm, and the size distribution tends to be
homogeneous. When the injection rate of AgNO3 solution
increases to 0.17 mL/s, uniform and ultralong Ag NWs with
the average length of 75 μm can be prepared (Figure 1).
Further increase in the injection rate of AgNO3 solution to
1.00 and 3.30 mL/s (Figure 2c,d) reduces the average length
of Ag NWs reduces, and a large number of nanoparticles are
observed in their final products. This indicates that the
C DOI: 10.1021/acsami.8b10138
injection rate of AgNO3 is a critical factor that affects the
morphology of Ag NWs (inset, Figure 2d), and excessive and
low injection rates are both unfavorable for the formation of
seed crystals and their subsequent growth process. Figure 3a−d
shows the SEM image of Ag NWs synthesized at different
stirring times before statics. It can be seen that the Ag NWs
become shorter and thicker when longer stirring time were
used (inset, Figure 3d). This suggests that the absence of
stirring for a certain time (Figure 1) is essential for growing Ag
NWs with desirable length and uniformity.
According to the above analysis, it is believed that an
appropriate injection rate of AgNO3 and a specific static
process both play the key role in controlling the length and
uniformity of Ag NWs, and the corresponding mechanism can
be surmised as follows. When the reaction was performed at
low injection rates of AgNO3 solution (such as 0.03 mL/s), the
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Figure 4. Photograph of (a) Ag NW TCFs and (b) a lighted LED with the Ag NW TCFs as the circuits. Optical transmittance and sheet resistance
(c) and flexible tests (d) of the Ag NW TCFs.
nucleation would occur in an intermittent mode due to the
slow accumulation of the monomer, and thus short and un-
uniform Ag NWs were obtained during the subsequent growth
process (Figure 2a). In contrast, when high injection rates
(such as 3.3 mL/s) were adopted, massive seed crystals were
formed instantly, but their subsequent random growth led to
irregular length and large diameter of Ag NWs (Figure 2d).
Based on the above analysis, a relatively moderate injection
rate of AgNO3 solution (∼0.17 mL/s) was thus explored to
improve the nucleation and growth processes of Ag NWs.
Through this adjustment, the monomer accumulation was
accelerated, which improved the crystallization process of Ag
NWs. Simultaneously, the growth of Ag NWs based on the
existing nuclei was also effectively regulated by a long-time
static. As a result, uniform Ag NWs with the average length of
75 μm were obtained (Figure 1).
The as-prepared Ag NWs shown in Figure 1 were
subsequently spin coated on PET substrates for fabricating
the flexible TCFs. As a comparison, the Ag NWs with average
length and diameter of 30 μm and 120 nm were also employed.
It can be seen in Figure 4a,b that the Ag NW TCFs are highly
transparent and can offer high conductivity as demonstrated by
a lighted light-emitting diode (LED). Figure 4c shows the
optical transmittance and sheet resistance of the Ag NW TCFs
before and after PEDOT:PSS deposition. A sheet resistance as
low as 15.2 Ω/sq at 84% transmittance was obtained for the
long Ag NWs, which is superior to the shorter Ag NWs with a
higher sheet resistance of 19.7 Ω/sq at 78% transmittance. The
sheet resistance versus transmittance of long Ag NWs also
represents fairly excellent properties among different metal
nanowire-based TCFs (Figure S1). After coating a PE-
DOT:PSS layer, both reduced transmittance (62%) and
surface roughness can be observed (Figures S2−S4), but the
sheet resistance was improved to 10 Ω/sq. To test the
mechanical flexibility of the as-prepared TCFs, the changes in
sheet resistance with bending times (at the bending angle of
180°) were investigated. As shown in Figure 4d, the sheet
resistances of the TCFs based on the long Ag NWs only
D DOI: 10.1021/acsami.8b10138
Research Article
slightly increase (less than 15%) even after 100 times bending,
manifesting high mechanical flexibility. As compared, TCFs
based on the short Ag NWs show 21% increasement in sheet
resistance under identical conditions.
To demonstrate the as-prepared Ag NW TCFs for potential
application in wearable energy-storage devices, flexible and
transparent all-solid-state supercapacitors with a symmetrical
structure of PET/Ag NWs/PEDOT:PSS/H3PO4/PVA/PE-
DOT:PSS/Ag NWs/ PET were fabricated. As shown in Figure
5a, the supercapacitors utilized H3PO4/PVA as the electrolytes
and Ag NW/PEDOT:PSS films as the electrodes. A high
transmittance of ∼51% was obtained for the resulting
supercapacitors (Figure S5), demonstrating great potential
applications in wearable electronics. Figure 5b,c shows nearly
rectangular CV curves even at a high scan rate of 400 mV/s
and symmetrical triangular GCD curves at various current
densities, demonstrating excellent capacitive behaviors of the
supercapacitors (Figure S6). The CV and GCD curves of the
supercapacitors with various device areas are shown in Figure
5d,e. It can be seen that the current density and the
discharging time gradually decreased with increasing device
areas from 1 to 4 cm2, indicating a slight attenuation of the
supercapacitor performance with increasing device areas.
Figure 6a,b shows the decreased areal capacitance of the
supercapacitors with increasing device areas at various scan
rates and current density, attributed to the higher internal
resistance of the supercapacitors with larger device areas
(Figures S7 and S8).
Cycling stability and flexibility are important parameters for
the practical application of supercapacitors, especially in
wearable electronic devices. As shown in Figure 7a, an
ignorable change in the CV curves was observed when the
supercapacitors were highly bent (the areal capacitances were
0.273 and 0.271 mF/cm2 for the supercapacitors with and
without bending, respectively). It retained over 75% of the
original areal capacitance after 100 times of bending (Figures
7b and S9), which suggests a high flexibility of the resulting
supercapacitors. In addition, 5000 charge−discharge cycles
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ACS Applied Materials & Interfaces Research Article

Figure 5. (a) Schematic diagram of flexible all-solid-state supercapacitor. (b) CV curves of the supercapacitor with device area of 2.25 cm2 at
various scan rates. (c) GCD curves of the supercapacitor with device area of 2.25 cm2 at various current densities. (d) CV curves of the
supercapacitor with various device areas at a scan rate of 100 mV/s. (e) GCD curves of the supercapacitor with various device areas at a current
density of 0.025 mA/cm.

Figure 6. (a) Areal capacitance calculated from CV data of the supercapacitors with various device areas. (b) Areal capacitance calculated from
GCD data of the supercapacitors with various device areas.

were performed for the supercapacitors (Figure 7c,d), which 4. CONCLUSIONS

In summary, we have presented a facile methodology for the
demonstrated only slight areal capacitance decays (less than synthesis of ultralong Ag NWs (∼75 μm in length) with
uniform sizes. The nucleation and growth processes can be
15%) and thus a high cyclic stability of the resulting effectively controlled by adjusting the stirring process and the
injection rate of AgNO3. At a moderate injection rate of ∼0.17
supercapacitors. mL/s of AgNO3 solution, the crystallization process of Ag
E DOI: 10.1021/acsami.8b10138
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ACS Applied Materials & Interfaces
Figure 7. (a) CV curves of the supercapacitor with and without bending at a scan rate of 300 mV/s (inset: photograph of the supercapacitor under
bending). (b) Capacitance retention after different bending times at the angle of 60°. (c, d) Cyclic stability tests of the supercapacitors.
NWs was improved, and simultaneously the growth of the
existing nuclei was effectively regulated by a specific static
process. Flexible TCFs based on the ultralong Ag NWs showed
low sheet resistance of 15.2 Ω/sq at 84% transmittance and
high mechanical flexibility with a negligible change in sheet
resistance after bending. Flexible all-solid-state supercapacitors
based on the resulting Ag NW TCFs showed high transparency
(>50%), good mechanical flexibility, and high cyclic stability
with only slight areal capacitance decays after 100 times of
bending (∼25%) and 5000 charge−discharge cycles (∼15%).
The results manifest the great potentials of the resulting TCFs
based on ultralong Ag NWs for flexible and wearable energy-
storage applications.
■
ASSOCIATED CONTENT
*
S Supporting Information
The Supporting Information is available free of charge on the
ACS Publications website at DOI: 10.1021/acsami.8b10138.
AFM images, SEM images, optical transmittance,
specific capacitance, areal capacitance, impedance spec-
troscopy, GCD curves of the supercapacitors (PDF)
■
AUTHOR INFORMATION
Corresponding Author
*E-mail: iamwylai@njupt.edu.cn.
ORCID
Wen-Yong Lai: 0000-0003-2381-1570
Wei Huang: 0000-0001-7004-6408
Author Contributions
§ 15458.
X.L. and D.L. contributed equally to this work.
Notes
The authors declare no competing financial interest.
■
ACKNOWLEDGMENTS
The authors acknowledge financial support from the National
Key Basic Research Program of China (973 Program,
F DOI: 10.1021/acsami.8b10138
Research Article
2014CB648300, 2017YFB0404501), the National Natural
Science Foundation of China (21835003, 21422402,
21674050, and 61704085), the Natural Science Foundation
of Jiangsu Province (BK20140060), Program for Jiangsu
Specially-Appointed Professors (RK030STP15001), the Lead-
ing Talent of Technological Innovation of National Ten-
Thousands Talents Program of China, the Excellent Scientific
and Technological Innovative Teams of Jiangsu Higher
Education Institutions (TJ217038), the Synergetic Innovation
Center for Organic Electronics and Information Displays, the
Priority Academic Program Development of Jiangsu Higher
Education Institutions (PAPD), the NUPT “1311 Project”, the
333 Project of Jiangsu Province (BRA2017402), the Natural
Science Foundation of Universities from Jiangsu Province
(17KJD510004), and NUPTSF (NY216025 and NY217073).
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G DOI: 10.1021/acsami.8b10138
ACS Appl. Mater. Interfaces XXXX, XXX, XXX−XXX