Journal of Colloid and Interface Science 512 (2018) 208–218

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Journal of Colloid and Interface Science

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

Regular Article

Preparation and cold welding of silver nanowire based transparent

electrodes with optical transmittances >90% and sheet
resistances <10 ohm/sq
Feng Xu a, Wei Xu a, Bingxin Mao a, Wenfeng Shen a, Yan Yu a, Ruiqin Tan b, Weijie Song a,⇑
a
Ningbo Institute of Material Technology and Engineering, Chinese Academy of Sciences, Ningbo 315201, PR China
b
School of Information and Computer Science, Ningbo University, Ningbo 315211, PR China

g r a p h i c a l a b s t r a c t

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

Article history: In this article, silver nanowires (AgNWs) with aspect ratios of 1000 and lengths up to 200 lm are
Received 3 July 2017 obtained by a modified polyol approach. These very long AgNWs are then utilized to prepare transparent
Revised 31 August 2017 electrodes (TEs) displaying a transmittance of 91.3% at a sheet resistance of 8.6 ohm/sq without any post-
Accepted 13 October 2017
treatment. Furthermore, we also demonstrate a process for the cold welding of Ag NWs by simply dipping
Available online 16 October 2017
the AgNWs films into CTAB solutions, resulting in a further improvement for the optoelectronic perfor-
mance. After the post-treatment, the AgNW-based TEs can achieve a transmittance of 93% at a sheet
Keywords:
resistance of 9.5 ohm/sq. In addition, the electric behaviors of AgNW-based TEs are investigated. In the
Silver nanowires
Transparent electrodes
bulk-like regime, for the as-prepared AgNW-based TEs, the Figure of merit (FOM), DC to optical conduc-
Sheet resistances tivity ratio reaches up to 566.8. After the cold welding process, the DC to optical conductivity ratio can
Optical transmittances reach even higher values (631.6). In the percolative regime, the as-prepared and welded AgNW-based
Welding TEs can achieve P (FOM with percolative-like behavior) values of 166.8 and 242.1, respectively.
Ó 2017 Elsevier Inc. All rights reserved.

1. Introduction

Electrodes with both high conductivity and high transmittance

⇑ Corresponding author. are essential for optoelectronic devices, such as solar cells, organic
E-mail address: weijiesong@nimte.ac.cn (W. Song). light emitting devices, and smart windows [1–3]. With an optical

https://doi.org/10.1016/j.jcis.2017.10.051
0021-9797/Ó 2017 Elsevier Inc. All rights reserved.
 F. Xu et al. / Journal of Colloid and Interface Science 512 (2018) 208–218
transmittance (T) > 90% and a sheet resistance (Rs) < 10 ohm/sq,
indium tin oxide (ITO) thin films currently dominate the commer-
cial transparent electrodes (TEs) market [4]. In recent years, there
have been great efforts into the development of alternative TEs,
such as conducting polymers, carbon nanotubes, graphene, metal
grids and metal nanowires [5–17], owing to the brittleness of ITO
and the scarcity of indium.
Among these materials, silver nanowire (AgNW)-based TEs are
promising due to their excellent electrical conductivity, outstand-
ing mechanical flexibility and ease of processing. Besides the Ag
nanowires, Cu nanowires are drawing attention due to much lower
cost [18,19]. Our and other studies have demonstrated the wide
applications of the AgNW-based TEs, such as the flexible transpar-
ent conductors [20,21], stretchable transparent conductors [22–
25], flexible transparent touch panels [26,27], organic photovoltaic
devices [28,29], organic light emitting diodes [30,31], flexible fuel
cell electrodes [32–35], stretchable sensors [36,37] and stretchable
piezoelectric nanogenerator [38].
Thus far, the polyol synthesis is the most popular method for
the preparation of AgNWs. Typically, a precursor (e.g., AgNO3), a
halide (e.g., NaCl, FeCl3 or CuCl2) and a capping agent, such as
poly(vinylpyrrolidone) (PVP), are added into a polyol such as ethy-
lene glycol (EG) and reacted at an elevated temperature. When
AgNWs are coated on a substrate to make a TE, one key issue is that
the insulating ligands (PVP) significantly affect the electrical per-
formance of the networks. Therefore, high-performance AgNW-
based TEs could be produced by decreasing the wire-wire junction
resistances.
The synthesis of long and thin AgNWs is therefore of key impor-
tance because increasing the length and aspect ratio (L/D)
decreases the number of high-resistance wire-wire junctions
[39]. Hu et al. obtained ultrathin AgNWs by introducing Br
into
the reaction. Accordingly, transparent films with an 8 ohm/sq sheet
resistance and 80% transmittance were obtained [13]. Lee et al.
demonstrated that AgNWs with diameters in the range of 15–30
nm and lengths up to 20 lm were prepared using the high-
pressure method in the presence of Br
[40]. A Rs of 40 ohm/sq
at T of 88% could be obtained using these AgNWs. In another inves-
tigation, Lee et al. reported the synthesis of very long AgNWs via
successive multistep growth [41]. These AgNWs generated TEs
with a Rs of 19 ohm/sq at a T of 90%. Jiu et al. synthesized AgNWs
with a diameter of 60 nm and a length of 65–75 lm by reacting at
relatively low temperatures without any agitation [42]. TEs using
these AgNWs achieved a Rs of 9.2 ohm/sq with a T of 85%. Li
et al. demonstrated a process for the synthesis and purification of
Ag NWs with diameters of 20 nm and under nitrogen atmosphere
with added Br
[43]. After purification, the Ag NWs displayed a T of
99.1% at 130.0 ohm/sq. High yield synthesis of AgNWs with a
diameter of 20 nm and an aspect ratio of 1000 were achieved in
the presence of a magnetic ionic liquid [44]. The transparent elec-
trode films exhibited the optoelectronic performance, with a trans-
mittance of 91% and sheet resistance of 15 ohm/sq. Currently, to
the best of our knowledge, despite the significant progress in the
synthesis of high aspect ratio AgNWs, the synthesis of Ag NWs
with sufficiently long lengths or high aspect ratios to make TEs
with a high T (>90%) and low Rs (<10 ohm/sq) has rarely been
reported.
The reduction of every single junction resistance using post-
treatments is another way to improve the performances of AgNWs.
To achieve this, several approaches including thermal annealing,
visible light welding, electrical current heating and mechanical
pressing were used to reduce the junction resistances [13,15,45–
51]. Among these, some research groups reported the preparation
of AgNW-based TEs with optical transmittances >90% and sheet
resistances <10 ohm/sq by effective post-treatments [50,51]. Nev-
ertheless, in these approaches, nanowires were exposed to high
209
energies, which may damage the polymer substrates and/or
devices, and may cause deformation of the nanowires, even trans-
forming nanowires into discrete nanoparticles in extreme cases. As
an alternative approach, incorporating conductive materials into
the AgNW junction, such as Ag, Au, and conductive polymers, could
sufficiently decrease the Rs under ambient conditions [13,52–56].
However, introducing extra chemicals into the AgNWs junctions
decreased the T of the TEs at the same time. The post-treatment
of AgNW-based TEs without decreasing the T under ambient con-
ditions is therefore highly desirable. Recently, chemical welding
of AgNWs were achieved at room temperature [56,57]. Laser
nanowelding of Ag nanowire is also a very promising low temper-
ature method at room temperature and ambient pressure [58–60].
Here, we developed solutions to both issues mentioned above.
First, we successfully synthesized AgNWs with an average length
of 123 lm using a modified polyol method. To the best of our
knowledge, we report for the first time the polyol synthesis of
AgNWs with enough long lengths to make TEs with a T > 90% and
Rs < 10 ohm/sq without any post-treatment. Second, without
decreasing the T, we further decrease the Rs of the AgNW-based
TEs by simply dipping the AgNW films into cetyltrimethylammo-
nium bromide (CTAB) aqueous solutions under ambient conditions.
Using a combination of these two approach, AgNW-based TEs with
a T of 93.0% at a Rs of 9.5 ohm/sq were successfully fabricated.
2. Material and methods
2.1. Material
Poly(vinylpyrrolidone) (MW = 58,000) was obtained from
Sigma-Aldrich. Ethylene glycol, poly(vinylpyrrolidone) (MW =
360,000), silver nitrate, and ferric chloride (FeCl3) were all pur-
chased from Shanghai Aladdin industrial Co., Ltd.
2.2. Synthesis of ultralong silver nanowires
In a typical synthesis, EG (100 mL) was added to the flask at
room temperature. Next, PVP (MW = 360,000, 0.32 g) and PVP
(MW = 58,000, 0.32 g) were added to the flask. Then, AgNO3
(0.72 g) was added to the previous PVP solution. After complete
dissolution, the FeCl3 solution (10 mL, 600 lM in EG) was added
to the mixture and stirred for one minute. The mixture was then
immediately transferred to an oil bath at 130 °C and stirred vigor-
ously for 10 min. Finally, the reaction was allowed to continue for
3.5 h without stirring. Afterwards, acetone and ethanol were used
to wash the precipitate with centrifugation at 1000–1500 rpm for
10 min. Finally, the AgNWs were redispersed in ethanol for use.
2.3. Preparation and cold welding of AgNW-based TEs
Typically, the AgNWs were spin-coated on a clean glass sub-
strate, designated as an as-prepared AgNW film. Then, the as-
prepared AgNWs film was dipped into a 0.01 M CTAB aqueous
solution for 5 min, rinsed with water and dried.
2.4. Characterization
SEM was performed using a FEI SIRION 200 SEM. TEM was per-
formed using a JEM2100 TEM. High resolution lattice images and
SAED patterns were recorded using a JEOL 2100/HR electron micro-
scope operating at 200 kV. The sheet resistances of the transparent
electrodes were measured using the four-probe method (Napson
Corp. Cresbox). The transmittances were collected using a UV–vis
spectrophotometer (Perkin-Elmer, Lambda 950, USA) with an inte-
grating sphere. Laser Raman spectra were acquired on a Renishaw
210 F. Xu et al. / Journal of Colloid and Interface Science 512 (2018) 208–218
inVia Reflex Raman spectrometer with a 532 nm laser. To prepare
samples for the Raman study, AgNW dispersions were evaporated
on Si wafer substrates.
3. Results and discussion
3.1. Synthesis of ultralong silver nanowires
Ultralong AgNWs were synthesized using a modified polyol
method [42,61]. Fig. 1A and B show scanning electron microscopy
(SEM) images of the ultralong AgNWs with low and high magnifi-
cations, respectively. As shown in Fig. 1C and D, the nanowires
obtained were 123 lm in length and 120 nm in diameter. The
maximum nanowire length exceeds 200 lm (see Fig. S1). The
key to the successful synthesis of ultralong AgNWs are the forma-
tion of seeds at room-temperature, the reaction at relatively low
temperature, and the use of PVP with adequate molecular weight.
In a typical synthesis, EG, PVP, AgNO3, and FeCl3 solutions were
sequentially added to the flask at room temperature. The mixture
was then immediately transferred to an oil bath preheated to
130 °C and stirred vigorously for 10 min. It is worth noting that
the AgCl seeds were formed at room temperature, not at 130 °C.
By contrast, adding AgNO3 and FeCl3 at 130 °C when other condi-
tions were fixed only gives silver nanocubes coupled with rare
nanowires (Fig. S2), which indicated that the formation of the AgCl
seeds at room temperature played a key role in the growth of
nanowires with high purities. We also verified that a low temper-
ature (130 °C) were essential to obtaining ultralong AgNWs with
high purities, which is in agreement with a previous study [42].
Polyvinyl pyrrolidone (PVP) mixtures with molecular weights of
360,000 (PVP 360,000) and 58,000 (PVP 58,000) were used in our
investigation. The molecular weight of the PVP played an impor-
tant role in the growth of the ultralong nanowires. AgNWs
obtained using a mixture of PVP 360,000 and 58,000 at a weight
ratio of 1:1 grew more rapidly in length, and thus the ultralong
Fig. 1. SEM images of the ultralong AgNWs with low (A) and high (B) magnifications, respectively; Histograms of the corresponding length (C) and diameter (D) distributions,
respectively.
nanowires were obtained in 3.5 h. By contrast, the lengths of
AgNWs using either PVP 360,000 or PVP 58,000 alone were inferior
to those of AgNWs using the mixtures of PVP 360,000 or PVP
58,000, as shown in Fig. 2 A and B. When using PVP 360,000 alone,
most of resulting nanowires were shorter than 50 lm, albeit a
small portion of them were longer than 50 lm (Fig. 2 A). In the case
of using PVP 58,000 alone, all of the nanowires were shorter than
50 lm (Fig. 2 B). Previous literature demonstrated that the use of
PVP with higher molecular weights allowed for higher AgNW
aspect ratios when the reactions were performed at 160 °C. This
can be attributed to their better capability of passivating side {1 0
0} facets or a higher viscosity of the EG solution [42,43,62]. How-
ever, our experimental results indicated that using PVP with mod-
erate molecular weights could be a better approach for the
synthesis of ultralong AgNWs at 130 °C. Compared with those per-
formed at higher temperatures, the reaction performed at 130 °C
were slower due to the low activity of EG; thus, the PVP with high
molecular weight hindered the growth of the nanowires. By con-
trast, the use of the mixtures endowed the PVP with adequate
molecular weight, leading to a tradeoff between their capability
for passivating side {1 0 0} facets and their effect on the growth
rate of the AgNWs. The AgNWs with relatively small diameters
were obtained in 3.5 h. When the reaction was extended to 5 h,
the lengths of the AgNWs remained constant but the diameters
were increased dramatically (from 120 to 156 nm, see
Fig. 2C and D). The ratio of PVP to AgNO3 was also crucial to the
length and aspect ratio of the AgNWs. When the weight ratio
was increased from 8:9 to 1:1, the average length of the AgNWs
were decreased from 123 to 70 lm (Fig. 2E and F). In addition,
AgNWs with nearly 100% morphology yields were obtained in this
work. This also plays an important role in the preparation of high-
performance AgNW-based TEs because the nanoparticles dramati-
cally degrade the optoelectronic performances of AgNW-based TEs.
Fig. 3A presents a high resolution transmission electron micro-
scope (HRTEM) image, which indicates that the {1 1 1} facets
 F. Xu et al. / Journal of Colloid and Interface Science 512 (2018) 208–218 211

Fig. 2. (A) SEM image of AgNWs obtained using PVP 360,000 alone. The scale bar = 20 lm. (B) SEM image of AgNWs obtained using PVP 58,000 alone. The scale bar = 30 lm.
(C) SEM images of the AgNWs when the reaction was extended to 5 h. The scale bar = 500 nm, and (D) Histograms of the corresponding diameter distributions. (E) SEM
images of the AgNWs when the weight ratio of PVP to AgNO3 was increased to 1:1. The Scale bar = 100 lm. (F) Histograms of the corresponding length distributions.

(d = 0.236) are parallel to the growth direction of the nanowire.

Fig. 3B shows the SAED patterns along the ½112 and [0 0 1] crystal-
lographic zone axes. Inspection of both the HRTEM image and
SAED patterns clearly shows that the nanowire grows along the
[1 1 0] axes. Therefore, the AgNWs have a penta-twined structure
and are bounded by five {1 0 0} side faces and ten {1 1 1} end faces
[63–65].
3.2. Cold welding of AgNW-based TEs
After the synthesis, AgNW dispersions in ethanol were spin-
coated on glass to produce AgNW-based TEs. To further lower
the Rs, the AgNW TE was dipped into a 0.01 M CTAB solution for
5 min, followed by washing with ultrapure water and drying at
room temperature. When the cold welding process was extended
to 10 or 15 min, the Rs remained constant, as shown in Fig. 4 A.
In general, the Rs value of the AgNW-based TEs with larger initial
Rs (R0) decreases more sharply than those of the AgNW-based
TEs with smaller R0. As shown in Fig. 4 B, the ratio of Rs reduction
to R0 generally rises sharply with increasing Rs. For instance, the Rs
of a sample with an initial Rs of 2.0 ohm/sq was decreased by
10.0%, that of a sample with a Rs of 34 ohm/sq was decreased by
27.1%, and that of a sample with a Rs of 568.2 ohm/sq was
decreased by 80.5%.
Considering that no new conductors were introduced to the
surface of the AgNWs, we propose that the decrease in Rs might
originate from the detachment of PVP adsorbed on the Ag surface.
To verify this hypothesis, we investigated the effect of the cold
212 F. Xu et al. / Journal of Colloid and Interface Science 512 (2018) 208–218

Fig. 3. (A) HRTEM image of a AgNW. (B) SAED patterns along the ½112 and [0 0 1]
crystallographic zone axes.
welding for different samples with different amount of PVP
adsorbed on the AgNW surface. The amount of ethanol used in
each round of centrifugation for sample set A are 480 mL, and
those in sample set B are 360 mL. Both sample set A and sample
set B underwent three round centrifugations. The AgNWs in sam-
ple set C were obtained after two round centrifugation using 480
mL ethanol in each round. Accordingly, the amount of PVP mole-
cules adsorbed on the Ag surface are different in sample sets A,
B, and C. After the welding, the Rs of sample set A can be decreased,
while the T remained constant. For instance, the Rs was decreased
from 13 to 11.4 ohm/sq, with T maintained at 93.8% (Fig. 5A). In the
case of sample set B, the Rs was decreased more sharply than those
of sample set A, and the transmittances simultaneously show slight
increases. For example, the Rs was decreased from 14.3 to 10.4
ohm/sq, with T rising from 93.2 to 93.4% (Fig. 5B). The welding
of sample set C not only reduced the Rs even more sharply than
that of sample set B (from 17.2 to 10 ohm/sq) but also improved
the T significantly (from 91.1 to 93.1%, see Fig. 5C). These results
showed that the samples that showed more substantial decreases
in Rs, exhibited more significant improvements in T via the cold
welding. Fig. 6 shows T versus Rs for the AgNW-based TEs before
and after the welding, respectively. As seen in Fig. 6A, the data
for the as-prepared AgNW-based TEs are discrete, which can be
attributed to the different junction resistances for different sample
sets, while those for the AgNW-based TEs after cold welding show
a smooth curve, due to the successful reduction in junction resis-
tance to a minimum level, as shown in Fig. 6B [39]. These experi-
mental results indicate that the samples with a larger amount of
PVP on the Ag surface show more substantial improvements in
the optoelectronic performances after the post-treatment. For
these AgNWs, the treatment with the CTAB aqueous solution
removes the differences in the junction resistances of the AgNWs,
and thus eliminates the deviation from the ideal electrical behavior
of AgNW-based TEs with fixed junction resistances.
Detachment of PVP from AgNW surfaces was revealed by per-
forming SERS measurements. Fig. 7 presents the SERS spectra of
Fig. 4. (A) The Rs variations of the AgNW-based TEs after the cold welding with
increasing welding time; (B) The Rs variations versus R0 (initial Rs). The Inserts are
the local enlarged plots.
PVP adsorbed on the AgNWs after and before the welding. The
strongest SERS peaks for PVP coated on the as-prepared AgNWs
are at 233 cm
1 and 1762 cm
1 in the low wavenumber region,
which can be ascribed to the mAgACO and msC@O bands, respec-
tively [66–69]. These peaks indicate that the main interaction of
PVP with the Ag surface is through the carbonyl group. The weak
peaks located at 686 cm
1 and 1409/1427 cm
1 correspond to
mNAC@O ring and mCAH bands, respectively, indicating a weak
interaction through the hydrophobic part of the PVP. After the
welding, there is residue PVP that can be detected due to the SERS
effect. The 686 cm
1 and 1409/1427 cm
1 peaks slightly move to
690 cm
1 and 1409/1428 cm
1, while the 233 cm
1 peak (mAgACO
band) disappears and a new weaker peak at 164 cm
1 appears. This
drastic change suggests that the desorption results from the
detachment of the carbonyl group from the Ag surface. The Raman
spectra of free PVP are shown in Fig. S3 for reference. Their peak
assignments in the Raman spectra are summarized in Table S1.
The CAH stretch at 2930 cm
1 is characteristic of the normal
Raman spectra of free PVP [68,70]. It shifts to a higher wavelength
located at 2938 and 2941 cm
1 for PVP/AgNW. In addition, no CAH
stretches of CTAB/AgNW are found in the Raman spectra, indicat-
ing no significant amount of CTAB molecules adsorb on the AgNW
surfaces throughout the welding (Figure S4).
As shown in Fig. 8, the TEM and SEM images show that fractal
nanoparticles are found on the nanowire surface, suggesting the
corrosion of AgNWs by CTAB molecules. It was found that
 F. Xu et al. / Journal of Colloid and Interface Science 512 (2018) 208–218 213

by the high surface energy due to the high surface-to-volume

A 100
As-prepared ratios of the nanowires [72,73]. In the case of the AgNW-based
98 After treatment TE, it is reasonable that spontaneous welding will occur automat-
ically if the residual insulating ligands are removed after deposi-
96 tion, resulting in a decrease of the junction resistance. It was
previously reported that thermal annealing [15,45] and plasmonic
94
T (%)

welding [46,47] resulted in fusing of the wires at the wire-wire

junctions. In contrast, the cold welding in this work resulted in
92 unmodified junctions that have shapes similar to those from hot
plate annealing and electroforming according to the previous liter-
90
ature [49]. This results suggest that the junction morphologies and
contact areas have little influence on the sheet resistances.
88

86 3.3. Optoelectronic performances and electric behaviors of the AgNW-

400 500 600 700 800 based TEs
Wavelength (nm)
The spectral transmittance of the AgNWs networks after the
B 100 welding were thoroughly studied at different area densities in a
As-prepared wide range, as shown in Fig. 9. After the welding, the optimized
98 After treatment AgNW-based TEs achieve a Rs of 9.5 ohm/sq with a T of 93%,
and a Rs of 6.4 ohm/sq with a T of 90.3% at 550 nm. The projec-
96 tions show that the differences between the T at different wave-
lengths decrease with increasing T. According to the experimental
94
T (%)

data, we present the 3D colormap surface plot with a projection

of T versus Wavelength and LogRs, through which the relations
92 among T, Wavelength and logRs are visualized, as shown in
Fig. 10.
90
Furthermore, the as-prepared AgNW-based TEs without any
post-treatment can achieve remarkably high performances with a
88
T of 91.3% at a Rs of 8.6 ohm/sq and a T of 90.3% at a Rs of 7.1
86 ohm/sq. to the best of our knowledge, we successfully prepared
400 500 600 700 800 the AgNW-based TEs exhibiting a T > 90% and a Rs < 10 ohm/sq
Wavelength (nm) without any post-treatment for the first time. Fig. 11 shows a plot
of T versus Rs for the as-prepared AgNW-based TEs without any
post-treatment, together with some of the best previous literature
C 100 results for the as-prepared AgNW-based TEs. Compared to previ-
As-prepared ous literature [40–44], our approach significantly improves the
98 After treatment
optoelectronic performances of the AgNW-based TEs at low sheet
resistances. On the other hand, Fig. 11 shows that the optoelec-
96
tronic performances of the ultralong AgNW-based TEs are inferior
94 to those of the ultrathin AgNW-based TEs [40,43,44] at high sheet
T (%)

resistances. Ultralong AgNWs may find applications in solar cells,

92
90
88
86
400 500 600 700
Wavelength (nm)
Fig. 5. Optical transmittance spectra of (A) Sample set 1, (B) Sample set 2, (C)
Sample set 3.
Cl
can trigger the spontaneous sintering of the Ag nanoparticles
and AgNWs at room temperature, because the halides have very
strong interactions with silver [56,66]. Similarly, in our investiga-
tion, Br
are used to trigger the welding of AgNWs. In addition,
as a surfactant, CTAB can interact with nonionic polymers through
their hydrocarbon parts [71]. The combination of these two factors
facilitates the desorption of PVP from the Ag surface at relatively
low CTAB concentration (0.01 M) in a short time (5 min). Previous
reports have stated that bare nanowires without ligands can be
welded together by simply contacting each other, which is driven
in which both the high optical transmittance and low sheet
resistance are beneficial for efficiency enhancement. On the
contrary, for display application such as touch panels, ultralow
sheet resistance is not necessary, while low haze (<1.0%) and high
transmittance is prerequisite even if the sheet resistance is up to
100 ohm/sq. Therefore, the ultrathin AgNWs are suitable for the
display application in which the haze are below 1% and even lower
800 [44].
The figures of merit (FOM) are usually used to evaluate the per-
formances of the TE materials and compare the properties of TEs
[14,74,75]. The relationship between T and Rs are described for
bulk-like TEs by:


Z0 rOp
T ¼ 1þ ð1Þ
2Rs rDC;B
where Z0 is the impedance of free space (377 X), rOp is the optical
conductivity, and rDC, B is the bulk-like DC conductivity of a TE.
Here, rDC,B/rOp can be considered an FOM, and high values of
rDC,B/rOp correspond to high T coupled with low Rs. Recently,
Coleman and coworkers [76,77] observed a discrepancy from
bulk-like behavior for thin films. Based on a previous study on other
materials [78–80], they proposed that for thin AgNW-based TEs
below a critical film thickness, tmin, the DC conductivity is no longer
214 F. Xu et al. / Journal of Colloid and Interface Science 512 (2018) 208–218

Fig. 6. The transmittance versus the sheet resistance of different sample sets (A) before and (B) after the treatments, respectively.

 1=ðnþ1Þ
A rDC;B =rOp
As-prepared P¼2 ð2bÞ
164 Z0 tmin rOp
After treatment

Here, where P is their percolative-like FOM and tmin is the thickness

1766
1409 1428 below which the DC conductivity becomes thickness dependent.
Intensity

690 Inspection of Eq. (2) shows that high values of P, but low values
of n, allow for high optoelectronic performance with a low Rs cou-
233
pled with a high T.
Fig. 12A shows a plot of T versus logRs for the AgNW-based TEs
before and after the welding. In the bulk-like regime, fitting exper-
1762
686 1409 1427 imental data to Eq. (1) gives the value of rDC, B/rOp. In the
percolation-like regime, fitting these data to Eq. (2) then gives both
P and n. Our experimental data are found to fit very well to both
regimes with Eqs. (1) and (2), respectively. The values of rDC, B/
200 600 800 1200 1400 1600 1800 2000
rOp, P and n are obtained for both AgNW-based TEs. In the case
Wavenumber (cm-1) of the as-prepared AgNW-based TEs, extremely high values of
rDC, B/rOp (566.8) and P (166.8), and low values of n (0.97) are
B achieved. These FOM values for ultralong AgNW-based TEs are
2938 As-prepared higher than those for the as-prepared AgNW-based TEs reported
After treatment previously [59,76]. After the welding, the bulk-like FOM was
increased by 11.4% (from 566.8 to 631.6); the percolative-like
FOM, P, was increased by 14.5% (from 166.8 to 242.1); and n
was decreased by 28.9% (from 0.97 to 0.69). The more dramatic
Intensity

changes in the percolative-like regime demonstrate that the junc-

2941 tion resistance has a larger influence on Rs in the percolative-like
regime than in the bulk-like regime and that the DC conductivity
follows a percolation-like thickness dependence. Fig. 12A shows
that when T > 90%, the AgNW-based TEs follow a percolation-like
electrical behavior but not a bulk-like behavior. Considering that
practical applications require T > 90% for TEs, the optoelectronic
performances of the AgNW-based TEs can be better evaluated
2000 2400 2800 3200 3600 using the percolative-like FOM (P) and exponent n, rather than
-1 the bulk-like rDC, B/rOp.
Wavenumber (cm )
Fig. 12B shows a log–log plot of (T
1/2–1) versus Rs. Linear fit-
Fig. 7. SERS spectra of PVP adsorbed on AgNWs in the low (A) and high (B) ting was applied to both bulk-like and percolative-like regime.
wavenumber regions, respectively. Inspection of Eq. (1) combined with Fig. 12B shows that the differ-
ent values of rDC, B/rOp lead to translation of the curve with bulk-
like behavior with a fixed exponent (
2) in Eq. (1). However, in Eq.
thickness independent but follows a percolation-like thickness (2), the value of n determines the slope of the curve with percola-
dependence [77]. As such, this new relationship between T and Rs tive behavior, while both n and P values determine the intercept of
for thin networks is introduced [76]: the curve. Keeping this in mind, one can deduce that a high rDC, B/
" rOp value corresponds to a high T at a certain Rs in the bulk-like

1=ðnþ1Þ #
2 regime, while the trends of the increase in T with logRs are fixed,
Z0 1
T¼ 1þ ð2aÞ as shown in Fig. 12A. In other words, the DlogRs between the dif-
P Rs
ferent curves are fixed at a particular T value. However, in the
 F. Xu et al. / Journal of Colloid and Interface Science 512 (2018) 208–218 215

Fig. 8. TEM images of (A) the as-prepared AgNWs, (B) the welded AgNWs, respectively. SEM images of the welded AgNWs in a vertical (C) and a plan view (D), respectively.

100

95

90

85

80
T (%)

75

70
T = 97.5%, Rs = 69.4 T = 91.3%, Rs = 7.1
T = 97.1%, Rs = 45.0 T = 90.3%, Rs = 6.4
65 T = 96.8%, Rs = 36.7 T = 88.8%, Rs = 5.0
T = 96.0%, Rs = 24.8 T = 87.4%, Rs = 4.6
Fig. 10. 3D colormap surface plot of transmittance spectra versus LogRs for the
T = 95.5%, Rs = 20.3 T = 85.3%, Rs = 3.7
AgNW-based TEs after cold welding. The gray lines represent the transmittance
60 T = 94.5%, Rs = 14.3 T = 82.1%, Rs = 2.8
spectra at fixed Rs.
T = 93.8%, Rs = 11.4 T = 79.6%, Rs = 2.3
T = 93.0%, Rs = 9.5 T = 72.9%, Rs = 1.8

400 500 600 700 800 the dashed line fits in Fig. 12A and B, indicating that the networks
Wavelength (nm) are very dilute at relatively low Rs (<100 ohm/sq). This is very
important to the practical applications of the AgNW-based TEs,
Fig. 9. Transmittance spectra for the AgNW-based TEs after the treatments. because a Rs value lower than 100 ohm/sq is required for most cur-
rent applications.

percolative-like regime, a lower n value corresponds to a sharper

increment of T, thereby the DlogRs between the different curves
increases with increasing T. This indicates that the junction resis-
tance accounts for a larger proportion of Rs at lower area densities
and that the post-treatment process therefore has a more signifi-
cant influence on more dilute nanowire networks with higher T
and lower Rs. The networks with the highest T and Rs deviate from
4. Conclusions
In summary, low-cost, solution-processable AgNW-based TEs
with optical transmittances > 90% and sheet resistances < 10
ohm/sq are successfully using ultralong AgNWs synthesized by a
one-pot polyol method. The synthesis of ultralong AgNWs was
216 F. Xu et al. / Journal of Colloid and Interface Science 512 (2018) 208–218

of 91.3% at a Rs of 8.6 ohm/sq and a T of 90.3% at a Rs of 7.1 ohm/sq.

100 After the post-treatment with CTAB aqueous solutions, rDC, B/rOp
and P reach 631.6 and 242.1, respectively. Furthermore, both the
conductivity and the optical transmittance of the AgNW-based
95 TEs can be improved through treatment with CTAB aqueous solu-
tions. In addition, the fits of the experimental data verify that the
T (%)

90 DC conductivity is no longer thickness independent but follows a

percolation-like thickness dependence at high T. Compared to pre-
Ref. 40 vious literature [40–44], our approach significantly improves the
85 Ref. 41 optoelectronic performances of the AgNW-based TEs at low sheet
Ref. 42 resistances. AgNW-based TEs with high optical transmittance and
Ref. 43 ultra low sheet resistance may find applications in solar cells, in
80 Ref. 44 which both the high optical transmittance and high conductivity
This work are beneficial for efficiency enhancement.
75
0 20 40 60 80 100 120 140 Acknowledgment
RS ( )
This work was supported by Ningbo Natural Science Foundation
Fig. 11. A plots of T versus Rs for the as-prepared AgNW-based TEs without any (2016A610281), Ningbo Key Laboratory of Silicon and Organic Thin
post-treatment. The literature results are shown for comparison. Film Optoelectronic Technologies, the program for Ningbo Munic-
ipal Science and Technology Innovative Research Team
(2016B10005 and 2015B11002), Jiangsu Collaborative Innovation
A 100 Center of Photovoltaic Science and Engineering, Changzhou
213164, P. R. China, International S&T Cooperation Program of
China (ISTCP) (2015DFH60240).

90 Appendix A. Supplementary material

T (%)

Supplementary data associated with this article can be found, in

the online version, at https://doi.org/10.1016/j.jcis.2017.10.051.
80
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