A large, ultra-black, efficient and cost-effective dye-sensitized solar module approaching 12% overall efficiency under 1000 lux indoor light

Article abstract of DOI:10.1039/c7ta09322e

Three novel anthracene-based organic dyes, denoted as AN-11, AN-12 and AN-14, were synthesized for outdoor and indoor dye-sensitized solar cell studies. Laboratory-fabricated small cells, as well as rigid and flexible modules, were prepared and analyzed for their photovoltaic performance under simulated outdoor and indoor conditions. Owing to the panchromatic absorption of visible light, the AN-11 module gives rise to a very black color and superior photovoltaic performance. Significantly, the AN-11 rigid module with a large active area of 26.80 cm² outperforms its Z907 counterpart under indoor conditions, reaching an overall efficiency of 11.94% under 1000 lux of T5 fluorescent light. In addition, the AN-11 module exhibits good stability during weather stress tests. Finally, the AN-11 dye is cost-effective and our studies show that the photovoltaic performance of the solar cells is not affected upon lowering the synthetic cost and increasing the synthetic scale.

Full text of DOI:10.1039/c7ta09322e

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ISSN 2050-7488
PAPER
Kun Chang, Zhaorong Chang et al.
Bubble-template-assisted synthesis of hollow fullerene-like
MoS2 nanocages as a lithium ion battery anode material
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A Large, Ultra Black, Efficient and Cost-effective Dye-sensitized
Solar Module Approaching 12% Overall Efficiency under 1000 Lux
Indoor Light
Received 00th January 20xx,
Accepted 00th January 20xx
Ming-Chi Tsai,a Chin-Li Wang,a,b Chiung-Wen Chang,a Cheng-Wei Hsu,b Yu-Hsin Hsiao,a Chia-Lin
Liu,a Chen-Chi Wang,a Shr-Yau Lin,a Ching-Yao Lin* ,a
DOI: 10.1039/x0xx00000x
www.rsc.org/
Three novel anthracene-based organic dyes, denoted as AN-11, AN-12 and AN-14, were synthesized for outdoor and
indoor dye-sensitized solar cell studies. Laboratory-fabricated small cells, as well as rigid and flexible modules were
prepared and analyzed for their photovoltaic performance under simulated outdoor and indoor conditions. Owing to the
panchromatic absorption of visible light, the AN-11 module gives rise to a very black color and superior photovoltaic
performance. Significantly, the AN-11 rigid module with a large active area of 26.80 cm2 outperforms the Z907 counterpart
under indoor conditions, reaching an overall efficiency of 11.94% under 1000 lux of T5 fluorescent light. In addition, the
AN-11 module exhibits good stability during the weather stress tests. Finally, the AN-11 dye is cost-effective and our
studies show that photovoltaic performance of the solar cells are not affected upon lowering the synthetic cost and
increasing the synthetic scale.
irradiation for outdoor applications, DSSC has the potential to
perform very efficiently under low light conditions for indoor
applications. To explore this possibility, several studies have
Introduction
Dye-sensitized solar cell (DSSC) has been widely studied in
recent decades owing to the low production costs, simple
manufacturing processes and vivid colours of the dyes.1-4
Numerous dyes have been reported to achieve high
photovoltaic performance in DSSC under 100 mW/cm2
simulated AM1.5G sunlight (or one-sun), including ruthenium
complexes,5-9 zinc porphyrins10-16 and metal-free organic
dyes.17-19 Among these dyes, organic dyes have been widely
studied owing to the advantages of possibly higher extinction
coefficients (than those of the ruthenium complexes), versatile
molecular design and low synthetic costs. For the purposes of
efficient charge transfer and electron injection, chemical
been conducted in the past few years.32-39 Among them, we
reported a cost-effective and fairly efficient anthracence-
based dye (AN-3) for DSSC under indoor conditions.34 In said
work, a large and flexible module (active area = 36.00 cm2)
sensitized with the AN-3 dye attained a power conversion
efficiency (PCE) of 5.45 % under 1000 lux of T5 fluorescent
light, slightly inferior to the 5.67% PCE of the Z907 module.
C8H17
S
N
N
C8H17
N
C8H17
O
O
N
OH
OH
C8H17
C8H17
structures of the organic dyes are often designed in a donor-
acceptor (or D- -A) fashion. In addition to the obvious roles of
the donors and acceptors, the -spacers also play an important
part of light harvesting.20,21 Many
-spacers have been
reported to be useful, including EDOT (C217),22 thiophene (JK-
46),23 fluorene (S3),24 perylene (GJ-BP)25 and arene derivatives
(LD4),26 etc. Additionally, anthracene has also been used as a
good π
-spacer in porphyrin and organic dyes.12,27-31
In addition to converting solar energy under one-sun
π-
AN-3
AN-12
π
π
S
S
N
N
NC
O
N
N
C8H17
O
π
N
OH
N
C8H17
OH
C8H17
AN-11
AN-14
Scheme 1 Chemical structures of the AN dyes.
In this work, we modified both the dyes and the solar
modules to achieve a higher PCE. For the dyes, modification of
the AN-3 dye yielded three new photo-sensitizers, denoted as
AN-11, AN-12, and AN-14. Chemical structures of the new AN
dyes are shown in Scheme 1. For AN-11, we modified the AN-3
dye34 with an additional benzothiadiazole (BTDA) group which
serves as a stronger electron-withdrawing motif. BTDA has
been a well reported as a good acceptor in the literature.18,40-42
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The benefits of using BTDA include boosting the charge parameters are listed in Table 1. For comparison, AN-3 is also
transfer processes, extending the -conjugation, and included in Fig. 2.
π
enhancing light-harvesting ability of the dyes. With BTDA, one
could expect a stronger push-pull tendency of the new AN
dyes and, hopefully, a higher PCE of the devices. For AN-12
and AN-14, an N,N-diarylamino-anthryl group is used as the
common donor, and a cyano-acrylic acid or a carboxylic acid is
employed as the anchoring groups, respectively. N,N-
diarylamino-anthryl groups are effective electron-donating
groups and they have been successfully used as the donor of
several efficient organic and porphyrin dyes.39,43,44 Cyano-
acrylic acid and carboxylic acid are widely used anchoring
groups with electron-withdrawing property.20,45-47 Based on
this design, all AN dyes should have good push-pull tendency,
and the comparison should provide insight into molecular
design of photo-sensitizers for indoor applications.
Fig. 2 (a) Absorption and (b) fluorescence emission spectra (2.0×10ꢀ6M) of
the AN dyes in THF.
For the devices, three types of solar cell/modules were
prepared, including lab-made small cells with an active area of
0.25 cm2, the R26 rigid modules with an active area of 26.80
cm2, and the F17 flexible modules with an active area of 19.80
cm2. The small cells were prepared in our laboratory and the
modules were manufactured by Taiwan DSC PV Ltd. (or TDP).
For the small cells, photovoltaic measurements were carried
out under 100 mW/cm2 simulated AM1.5G sunlight to imitate
the out-door condition, as well as under 200, 600, and 1000
lux of T5 or LED lights to represent indoor conditions of a dim
room, a common office, and a convenient store, respectively.
All AN dyes were examined in the small cells and the superior
dye was chosen to sensitize the modules for further tests. For
the modules, only indoor conditions were tested.
Table 1 Spectral and electrochemical properties of the AN dyes
Absorption, nm
(ε, 104 Mꢀ1 cmꢀ1)
528 (4.61)
433 (1.68), 515 (1.99)
438 (2.10), 517 (2.34)
Emission,a
nm
E,b V vs. SCE
E0ꢀ0
eV
2.08
2.16
2.14
,
Oxc
Redd
ꢀ1.15
ꢀ1.17
ꢀ1.09
Dye
ANꢀ11
ANꢀ12
ANꢀ14
722
644
652
+0.85
+1.07
+1.08
a2.0x10ꢀ6 M of the AN dyes in THF, excitation wavelength/nm: ANꢀ11, 528;
ANꢀ12, 515; ANꢀ14, 517. b0.5 mM of the AN dyes in THF/0.1 M TBAP/N2;
Pt working and counter electrodes; SCE reference electrode; scan rate = 100
mV sꢀ1. cPotentials were determined by differential pulse voltammetry due to
the less reversible oxidation waves. dPotentials were obtained by cyclic
voltammetry. eE0ꢀ0 values were determined by the intersection of normalized
UV−visible and fluorescent spectra.
As shown in the figure, the UV-visible spectrum of AN-11 is
consistent with that of the AN-3 parent with deviations. For
instance, AN-3 and AN-11 both give rise to one overlapped
absorption band around 500 nm with similar molar
absorptivities. However, the absorption maximum of AN-11
As such, our study showed that an R26 module sensitized
with the AN-11 dye achieved a PCE of 11.94% under 1000 lux
of T5 fluorescent light, outperforming the Z907 counterpart.
Fig. 1 collects the pictures of AN-11 in a THF solution, as
powders, and the solar devices sensitized with AN-11.
(
λmax = 528 nm) is red-shifted from that of AN-3 (λmax = 499
nm). This deviation may be attributed to more conjugated
double bonds in the chemical structure. For AN-12 and AN-14,
the spectral features are quite different from those of AN-3
and AN-11. For example, AN-12 (433 and 515 nm) and AN-14
(438 and 517 nm) exhibit two well-resolved and weaker
absorption bands. This difference may be related to the
different electron-donating groups and/or the electron-
acceptors/anchors in the chemical structures. Among the AN
dyes, absorption maxima of the lowest-energy absorption
bands show a trend of AN-11 > AN-14 > AN-12 > AN-3. These
absorption wavelengths are appropriate for indoor solar-cell
applications.
For fluorescence, the emissions are mirror images of the
corresponding lowest-energy absorptions. As expected, the
emission bands are red-shifted from the corresponding
absorption bands, centred at 722 nm for AN-11, 644 nm for
AN-12, and 652 nm for AN-14. The trend of these wavelengths
is consistent with that of the lowest-energy absorption bands,
i.e. AN-11 > AN-14 > AN-12 > AN-3. Interestingly, the
fluorescence emission of AN-11 seems very weak compared
with those of AN-12 and AN-14 at the same concentration.
This phenomenon may be related to molecular aggregation of
Fig. 1 Pictures of ANꢀ11 (a) in a THF solution (top) and as powders
(bottom), (b) the small cell, (c) the R26 rigid module, and (d) the F17 flexible
module.
Results and discussion
Absorption and fluorescence emission spectra.
The UV-Vis absorption and fluorescent emission spectra of
the AN dyes in THF are compared in Fig. 2. The related
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the AN-11 dye. More discussion is given in the photovoltaic shifted from those of AN-11 and AN-12. This further positive
section to address this possibility.
shift may be attributed to the BTDA motif and the additional,
electron-withdrawing cyano group in the chemical structure.
These assignments are consistent with the calculated MO
Electrochemistry, molecular orbitals and energy levels.
Fig. 3 shows the cyclic voltammograms (CV) of the AN dyes patterns.
in THF. The redox potentials are listed in Table 1. Due to the
To help qualitatively understand the frontier molecular
less reversible nature of the oxidation reactions, differential orbitals (MO) of the AN dyes, density-functional theory (DFT)
pulse voltammograms (DPV) were also obtained to help calculations were carried out at the B3LYP/6-31G(d,p) level of
determine the oxidation potentials.
theory.49 As shown in Fig. 4, electron densities of the highest
occupied molecular orbitals (HOMO) mainly reside at the
donors and the anthryl parts for all AN dyes. In contrast,
electron probabilities of the lowest unoccupied molecular
orbitals (LUMO) largely concentrate at the acceptor/anchoring
and the anthryl units. First of all, these MO patterns agree well
with the electrochemistry results, i.e. the oxidation reactions
are related to the electron-donating part of the molecules
whereas the reductions are related to electron-withdrawing
section of the chemical structures. Secondly, uneven
distribution of the electron densities/probabilities at the
HOMO/LUMO levels translates to a push-pull tendency of the
dyes. This tendency would result in pushing electron density
from the donors toward the anchors upon photo-excitation of
the dyes. This is a welcome merit for n-type DSSC applications.
Thirdly, the electron densities/probabilities seem to be more
localized for the HOMO and LUMO of AN-11 than those of AN-
3, suggesting a stronger push-pull tendency of the AN-11 dye
upon excitation. This suggestion is consistent with the DFT-
calculated dipole moments (AN-3: 7.96 Debyes, AN-11: 8.65
Debyes). The increased dipole moment of AN-11 may be
attributed to the presence of BTDA motif in the structure.
Fig. 3 Cyclic voltammograms (bold lines) of the AN dyes in THF/TBAP. For
the oxidation, differential pulse voltammograms were also measured (thin
lines) to help determine the potentials. Experimental conditions: [ANꢀx] = 0.5
mM in 0.1 M TBAP/THF, N2, Pt working and counter electrodes, SCE.
As shown in the figure and table, the first oxidations of AN-
11, AN-12 and AN-14 are found at +0.85, +1.07 and +1.08 V vs.
SCE, respectively. These reactions are consistent with the
formation of the cation radicals.34 The first oxidation potential
of AN-11 is very similar to that of AN-3 (+0.86 V vs. SCE).34 This
is consistent with the fact that the two dyes share a common
electron-donor in the chemical structures. For AN-12 and AN-
14, the first oxidation potentials are noticeably more positive
than those of AN-3 and AN-11. This may be due to the
different donor groups, i.e. N,N-di-octylaminophenyl-ethynyl
group vs. N,N-di-arylamino group.44 Between AN-12 and AN-14,
we observed similar oxidation potentials, consistent with their
identical electron-donating group.
Fig. 4 Frontier molecular orbitals of ANꢀ3, ANꢀ11, ANꢀ12 and ANꢀ14.
Calculation method: Gaussian 03W, DFT, B3LYP/6ꢀ31G(d,p).
Fig. 5 compares the energy levels of the HOMO/LUMO of
each dye, the conduction bands (CB) of TiO2 and the redox
For reductions, there are ill–shaped waves near -0.80 V vs.
SCE. These reactions have been established to be reduction
reactions of the anchoring groups.48 Additionally, quasi-
reversible reactions are found at -1.15, -1.17 and -1.09 V vs.
SCE for AN-11, AN-12 and AN-14, respectively. These reactions
are consistent with the formation of the anion radicals.34
These reduction potentials are all positively shifted from that
-
potential of the electrolyte (I-/I3 ).2 The HOMO/LUMO levels
are based on the corresponding redox potentials of each dye.
As clearly shown in the figure, the LUMO levels of the AN dyes
are considerably higher than the conduction bands (CB) of TiO2
and the HOMO levels are noticeably lower than the energy
level of the electrolyte. Therefore, the AN dyes should all be
capable of injecting electrons into the CB of TiO2 upon
excitation, and the resulting cations should be efficiently
regenerated by the electrolyte. A similar diagram comparing
the ground/excited states of each dye is also provided in the
ESI (Fig. S1). In short, the afore-mentioned conclusion also
applies to Fig. S1.
of AN-3 (-1.43
V vs. SCE), likely due to the electron-
withdrawing BTDA motif in the chemical structures. As shown
in Table 1, AN-11 (-1.15 V) and AN-12 (-1.17) show similar
reduction potentials possibly due to the identical electron-
acceptor/anchor group. With a different acceptor/anchor, the
reduction potential of AN-14 (-1.09 V) is further positive-
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cells under one-sun irradiation. The related parameters are
tabulated in Table 2. For comparison, data of the Z907 small
cells were also included in Table 2.
Table 2 Photovoltaic Properties of the AN and Z907 small cells under
simulated AM 1.5 Irradiation (100 mW/cm2)a
IPCE,b
Entry Jsc
Jsc
Voc
(mV)
FF
(%)
Dye loading
(nmol/cm2)
η
(%)
(mA/cm2) (mA/cm2)
ANꢀ11 12.70 13.09±0.32 680±1.0 71±1.0 6.36±0.18
300
290
370
ꢀ
ANꢀ12
ANꢀ14
Z907
6.60
6.05
7.43±0.18 680±1.0 76±1.0 3.87±0.11
6.27±0.17 600±1.0 78±1.0 2.96±0.12
13.34 16.29±0.37 763±6.0 70±1.0 8.69±0.33
aThe active area was 0.25 cm2 with a black mask of area 0.16 cm2. The
parameters are the averaged values of various number of independent devices
IPCE
(ANꢀ11 = 16 cells, ANꢀ12 = 5 cells, ANꢀ14 = 7 cells, Z907 = 5 cells). bJsc
Fig. 5 Energyꢀlevel diagram of the AN dyes, the electrolyte and TiO2.
is derived via wavelength integration of the IPCE spectra to compare with the
J
sc values obtained from the J-V measurements.
As shown in Table 2, the overall efficiencies of the small
cells exhibit a trend of AN-11 > AN-12 > AN-14 under one-sun
irradiation. The AN-11 cell outperforms the AN-12 and AN-14
cells with Jsc = 13.09 mA/cm2, Voc = 680 mV, FF = 71 %, and a
PCE of 6.36%. Upon closer inspection, we observed similar
dye-loadings of the AN cells. In addition, the Voc value of the
AN-11 cell is similar to that of the AN-12 cell but moderately
greater than that of the AN-14 cell. Therefore, these results
would suggest that a greater Jsc value may be a more
important factor contributing to the greater PCE of the AN-11
small cell. A greater Jsc value of the AN-11 cell is consistent
with the more broadened and intensified IPCE spectrum (Fig.
6b). This suggestion is supported by the integrated values of
IPCE
the IPCE responses (JscIPCE). As compared in Table 2, the Jsc
values show the same trend as in the J-V study, i.e. AN-11 >
AN-12 > AN-14. As for the fill factors (FF), FF value of the AN-
11 cell (71%) is noticeably lower than those of the AN-12 (76%)
and AN-14 (78%) cells. Given the same cell fabrication
procedure and the small deviations of the averaged values, the
lower FF value of the AN-11 cell may not be caused by defects
of the device. As such, the lower FF value of the AN-11 cell
could be related to the nature of the dye.50 As shown in Fig. 1,
the chemical structures of AN-12 and AN-14 are similar to each
other, but different from that of AN-11. As shown in Table 1,
the oxidation potentials and the absorption wavelengths of
AN-12 and AN-14 are similar to each other, but different from
those of AN-11. These differences may have impacts to the
photovoltaic parameters, such as the FF values.
Fig. 6 (a) The J–V curves (dashed lines: dark currents) and (b) IPCE spectra
under 100 mW cmꢀ2 simulated AM1.5G sunlight.
The very broad IPCE spectrum of the AN-11 cell is
consistent with the colour of the device (Fig. 1b-1d). With a
relatively simple chemical structure, it is expected to observe
an absorption band of AN-11 at 528 nm (Fig. 2a). As a result,
the AN-11 solution appears red (Fig. 1a). Much to our surprise,
the AN-11 solar devices show a very black colour. To better
understand the differences in colour, Fig. 7 collects normalized
UV-visible and IPCE spectra. Between the solution and the film
spectra, the absorption bands of the film spectra (red dotted
curves) are slightly shifted and broadened from those of the
AN solutions (black curves). These spectral changes may be
Photovoltaic properties of the small cells.
The small cells are prepared in our laboratory with an
active area of 0.25 cm2. A black mask with an aperture area of
0.16 cm2 was applied to the small cells during the photovoltaic
measurements. For the measurements, 100 mW/cm2
simulated AM 1.5G sunlight (or one-sun) was applied to
represent the outdoor environment. Fig. 6 shows the (a)
current density-voltage (J-V) curves and (b) incident photon-to-
current conversion efficiency (IPCE) spectra of the AN small
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related to intermolecular interactions of the dye molecules on contributing to the superior photovoltaic performance. This is
the surfaces of TiO2 nanocrystalline films. It has been well consistent with the J-V and IPCE measurements.
documented that the face-to-face, H-type aggregation of
π-
molecules generates a blue shift of the absorption band(s),
whereas the tilted (or head-to-tail), J-type aggregation results
in a red shift.51 Therefore, the blue-shifted film spectrum of
AN-11 suggests H-type aggregation, and the red-shifted film
spectra of AN-12 and AN-14 suggest J-type aggregation of the
dye molecules on TiO2. In addition, the broadening
phenomenon seems to be more apparent for the AN-11 film.
This implies that AN-11 may be more susceptible to
aggregation than are the AN-12 and AN-14 dyes. This
suggestion is consistent with the much weaker fluorescence
emission of the AN-11 solution shown in Fig. 2b. Note that the
afore-mentioned solutions are dilute and the films only adsorb
limited amount of the dye molecules to avoid saturation of the
absorption bands. As the amounts of the dyes increase, one
should observe further broadening of the film spectra. To
examine this possibility. Fig. 7 also includes normalized IPCE
spectra of the AN small cells (blue bold curves). Note that, in
this case, much more dye molecules were allowed to adsorb
onto the photo-anodes (Table 2). Due to the amounts of the
dyes, severe saturation was observed for the UV-visible
spectra of the photo-anodes, rendering the spectra un-usable.
Therefore, we hope to represent the region of the absorptions
of the photo-anodes by comparing the IPCE spectra. As clearly
shown in Fig. 7, the IPCE spectrum of the AN-11 small cell is
significantly more broadened than those of the AN-12 and AN-
14 counterparts, resulting in a panchromatic IPCE spectrum
covering the entire visible region from 350 to 750 nm.
Consequently, the AN-11 cell exhibits a very black colour. To
demonstrate the blackness of the AN-11 devices, large R26
modules sensitized with the AN-11, Z907, and AN-3 dyes are
compared in Fig. 8. As shown in the figure, the AN-11 module
gives rise to a very black colour whereas the Z907 and the AN-
3 modules show a brown and an orange colour, respectively.
Electrochemical impedance spectroscopy (EIS) was also
carried out in order to reveal important interfacial charge-
transfer processes. Fig. 9 compares Nyquist plots of the AN
small cells in the dark. Three semicycles are expected from 0.1
Hz to 1 MHz for each cell, including one small semicircle in the
lower frequency range (from 0.1 Hz to 2 Hz), one larger
semicircle in the middle frequency range (from 2 Hz to 1 kHz),
and another smaller semicircle in the highest frequency range
(>1 kHz). These semicircles are related to the ion diffusion in
the electrolyte, the charge-transfer processes at the
TiO2/dye/electrolyte interface, and the charge-transfer
processes at the Pt/electrolyte interface, respectively. As
expected, the semicircles in the highest frequency range (or
left side of the figure) are similar for all AN cells. For the
semicircles at the lower frequency range (right side), the
signals are obscured by the large semicircles at the middle
frequencies. Importantly, the middle semicircle of the AN-11
cell is significantly larger/broader than those of the AN-12 and
AN-14 cells. This suggests a lower charge recombination rate
thus a weaker dark current for the AN-11 cells (Fig. 6a),
Fig. 7 Comparison of the solution UVꢀvisible spectra (black solid) with the
film spectra (red dotted), and with the IPCE spectra (bold blue) of ANꢀ11
(top), ANꢀ12 (middle), and ANꢀ14 (bottom).
Fig. 8 R26 modules sensitized with (a) ANꢀ11, (b) Z907, and (c) ANꢀ3.
Fig. 9 EIS Nyquist plots of the AN cells in the dark.
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Table 3 Photovoltaic parameters of the R26 modules under T5 and LED lights
Light sourcea
Dyeb
Photon flux
(lux)
Jsc
A/cm2)
Voc
(mV)
FF
(%)
Pin
Pmax
W/cm2)
6.38 ±0.08
η
(
ꢀ
(
ꢀ
W/cm2)
(
ꢀ
(%)
T5
ANꢀ11
200
600
10.90 ±0.10
34.40 ±0.30
61.50 ±0.60
10.00 ±0.10
31.60 ±0.30
56.60 ±0.60
10.40 ±0.10
31.60 ±0.30
52.90 ±0.60
9.60 ±0.10
906.20 ±19.40
1007.80 ±24.50
1050.90 ±24.90
941.30 ±5.40
64.30 ±1.40
65.50 ±1.00
64.30 ±1.10
64.80 ±0.60
64.90 ±0.60
64.10 ±0.80
64.50 ±1.50
65.60 ±1.20
64.70 ±1.20
64.80 ±0.70
65.10 ±0.60
64.60 ±0.70
70
203
348
70
9.08 ±0.11
11.17 ±0.18
11.94 ±0.16
8.69 ±0.04
10.70 ±0.08
11.50 ±0.11
9.68 ±0.13
10.95 ±0.17
11.26 ±0.21
9.30 ±0.09
10.64 ±0.10
10.91 ±0.11
22.68 ±0.37
41.56 ±0.56
6.11 ±0.03
21.73 ±0.17
40.03 ±0.00
6.10 ±0.08
20.72 ±0.33
35.58 ±0.67
5.86 ±0.06
20.14 ±0.18
34.46 ±0.34
1000
200
Z907
ANꢀ11
Z907
600
1058.00 ±5.70
1104.40 ±5.60
908.20 ±19.90
999.20 ±21.60
1038.70 ±24.30
942.80 ±6.50
203
348
63
1000
200
LED
600
189
316
63
1000
200
600
29.40 ±0.20
48.80 ±0.50
1052.80 ±6.20
1093.50 ±5.70
189
316
1000
a T5 fluorescent light and LED were manufactured by China Electric MFG. Co. bNumber of the modules: 5.
As for the indoor performance of the AN small cells, shown in the table, a relatively similar trend as for the rigid
photovoltaic data of the small cells under 1000 lux of T5 or LED modules is also observed for the flexible modules. However,
lights were tabulated in the ESI (Table S1). In short, the same the F17 modules seem slightly less efficient than the R26
trend is observed, i.e. AN-11 > AN-12 > AN-14. Therefore, AN- counterparts. Note that active areas of the modules were used
11 is chosen to sensitize the modules for the following to calculate the PCE values in Table 3 and 4. In addition to
investigation.
active area, aperture area and total area are also important
factors when evaluating PCE of the modules.52 Therefore, we
compare PCE variation of the modules based on different area
Photovoltaic and stability tests of the modules.
For practical applications, photovoltaic measurements of dimensions in Table S2 and S3, ESI.
large modules were also evaluated. As mentioned above, AN-
Differences in the photovoltaic properties of the modules
11 was used to sensitize the modules because it outperformed may be related to the differences in the emission spectra of
other AN dyes in the small-cell tests. Two types of modules the artificial light sources. Fig. 10 compares the UV-Vis
were manufactured by Taiwan DSC PV Ltd. for the following absorption spectra of AN-11 and Z907 with the emission
tests. The R26 module is rigid with an active area of 26.80 cm2 spectra of the T5 and LED lights. As shown in the figure, the
and the F17 module is flexible with an active area of 19.80 cm2 absorption ranges of the two dyes are suitable for indoor
(Fig. 1). No masks were applied during the measurements and photovoltaic applications. Between the two dyes, AN-11
only indoor conditions were tested due to the architectural exhibits a much greater extinction coefficient and a wider
limitations of the modules. For the light sources, 200 - 1000 lux light-absorption range, possibly contributing to the superior
of T5 or LED lights were used to represent various indoor performance of the AN-11 modules under indoor irradiation.
illumination conditions, ranging from a dim room, a common
office, to that of a convenient store.
Table 3 summarizes the photovoltaic data of the R26
modules sensitized with AN-11 and Z907 under 200, 600, and
1000 lux of T5 and LED lights. For the Z907/R26 modules, the
PCE values under 200 lux T5 and LED lights are comparable
with that of the Z907 small cell under one sun irradiation. With
the illuminances increased from 200 to 1000 lux, PCE of the
Z907/R26 module also increased from 8.69% to 11.50% for T5
light and from 9.30% to 10.91% for LED light. For the AN-
11/R26 module, the PCE values under indoor conditions are
superior to that under one sun irradiation. This is consistent
with the literature reports.10,34,35 Significantly, the AN-11/R26
module outperforms the Z907/R26 module with a PCE of
11.94% under 1000 lux of T5 light. One may consider this PCE
value as highly efficient considering the large size of the R26
module. For LED light, PCE values of the AN-11/R26 modules
are also greater than those of the Z907/R26 module. As for the
F17 modules, the photovoltaic data are collected in Table 4. As
Fig. 10 Absorption spectra of ANꢀ11 and Z907 vs. the T5 and LED emission
spectrum.
6 | J. Name., 2012, 00, 1-3
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Table 4 Photovoltaic parameters of the F17 modules under T5 and LED lights
Light
sourcea
T5
Dyeb
Photon flux
(lux)
Jsc
Voc
(mV)
FF
(%)
Pin
Pmax
W/cm2)
η
(
ꢀ
A/cm2)
(
ꢀ
W/cm2)
67
(
ꢀ
(%)
ANꢀ11
200
600
7.70 ±0.20
24.40 ±0.80
41.20 ±1.20
7.40 ±0.10
23.00 ±0.60
38.40±1.60
7.30 ±0.30
23.00 ±0.60
38.10 ±1.40
7.00 ±0.20
21.90 ±0.60
36.90 ±1.10
929.40 ±4.10
1008.40 ±4.00
1039.60 ±2.60
1009.30 ±6.70
1101.00 ±6.40
1135.30 ±8.60
928.30 ±5.60
1007.90 ±3.70
1036.90 ±4.40
1007.00 ±7.70
1101.70 ±8.10
1138.50 ±6.00
76.00 ±0.90
76.30 ±0.80
75.80 ±1.30
71.10 ±1.90
73.40 ±1.80
75.00 ±1.60
75.10 ±1.40
75.70 ±0.70
76.10 ±1.20
71.60 ±1.70
73.40 ±2.00
75.20 ±1.40
5.46±0.10
18.80±0.39
32.46±0.54
5.31±0.13
18.53±0.18
32.70±1.27
5.09±0.12
17.52±0.35
30.07±0.79
5.03±0.04
17.67±0.38
31.54±0.35
8.15±0.15
9.26±0.19
9.60±0.16
7.92±0.19
9.13±0.09
9.67±0.38
8.08±0.18
9.37±0.19
9.51±0.25
7.99±0.07
9.45±0.20
9.98±0.11
203
338
67
1000
200
Z907
ANꢀ11
Z907
600
203
338
63
1000
200
LED
600
187
316
63
1000
200
600
187
316
1000
a T5 fluorescent light and LED were manufactured by China Electric MFG. Co. bNumber of the modules: 5.
To evaluate the stability of the modules under indoor
Finally, we conducted the studies of scaling-up, costing-
environments, weather-stress tests were performed. The tests down and the relationship with the photovoltaic performance.
were carried out by TDP according to the SEMI (the global So far, our study showed that the synthesis of AN-11 can be
industry association serving the manufacturing supply chain scaled up to three grams for each reaction and the cost can be
for the micro- and nano-electronics industries) standards. For cut down to about US$60/g. J-V measurements of the cost-
the rigid R26 modules, the thermal cycle test was given. In this down AN-11 small cells show no decrease in the photovoltaic
test, surrounding temperature of the AN-11/R26 modules was performance.
cycling between 60oC and -10oC at 1oC/min rate . Photovoltaic
measurements of the modules under 200 lux of T5 light
Conclusion
showed that 90.1% of the maximal out-put power of the R26
modules remained after 50 cycles of the thermal cycle test (Fig.
In this work, we report the synthesis, fundamental and
11a). For the flexible F17 modules, the damp-heat test was
photovoltaic properties of three new anthracene-based
given. In this test, the flexible modules were put under 65oC
organic dyes, denoted as AN-11, AN-12 and AN-14. Among the
and 65% of humidity. The results showed that 87.3% of the
AN dyes, AN-11 shows superior photovoltaic performance than
maximal out-put power of the AN-11/F17 modules remained
other AN dyes. Significantly, the AN-11/R26 module
after 600 hours (Fig. 11b).
outperforms the Z907 counterpart with a PCE of 11.94% under
1000 lux of T5 fluorescent light. Furthermore, our study shows
that photovoltaic performance of AN-11 is not affected upon
scaling up the synthesis and cutting down the cost. These are
the merits for industrializing AN-11 for practical applications.
Experimental
Instruments
NMR (Bruker Avance II 300 MHz), UV-visible (Agilent 8453),
fluorescence (Varian Cary Eclipse), and Mass (Microfilex
MALDI-TOF MS, Bruker Daltonics) spectra were obtained on
the indicated instruments. Elemental analyses were carried
out by the MOST Instrumentation Center at National Taiwan
University (Elementar Vario EL III). Electrochemistry was
carried out using a standard three-electrode cell (a Pt working
electrode, a Pt auxiliary electrode, and an SCE reference
electrode) on a CH Instruments Electrochemical Workstation
611A. A glove box (MBraun Uni-Lab), a vacuum line and
standard Schlenk glassware were employed to process all
materials sensitive to air. The current−voltage (J−V)
characteristics of the DSSC devices covered with a black mask
(aperture area 0.4 × 0.4 cm2) were determined with a solar
simulator (AM 1.5G, SS50 AAAEM, PET) and a source meter
Fig. 11 Photovoltaic parameters of the (a) ANꢀ11/R26 module and (b) ANꢀ
11/F17 module under the weather stress tests. Conditions: 200 lux of T5 light,
(a) the thermal cycle test: cycling between 60oC and ꢀ10oC at 1oC/min rate.;
(b) The dampꢀheat test: 65oC, and 65% of humidity.
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ARTICLE
Journal Name
(Keithley 2400). The measurement of the incident photon-to-
Syntheses of the AN dyes are based on the Sonogashira
current conversion efficiency (IPCE) was performed by the 7- cross-coupling method,53,54 and are similar to those in our
SCSpec system (Sofn Instruments Co., Ltd.) with a source previous reports.34,44 Detailed procedures and characterization
meter (Keithley 2000). The dim-light conversion efficiency data are provided in the ESI.
measurement system was purchased from Yu-Yi Enterprise
Co., Ltd., Taiwan, with a spectrophotometer (Ocean Optics
USB2000+UV−vis) and a source meter (Keithley 2401). The T5
and LED lights were manufactured by China Electric MFG. Co.
Acknowledgements
We are grateful for the financial support from the Ministry of
Science and Technology of Taiwan (MOST 105-2119-M-260-
001 and MOST-103-2119-M-260-002).
Materials
Solvents for the synthesis (ACS grade) were CH2Cl2 and
CHCl3 (Mallinckrodt Baker), hexanes (Haltermann, Hamburg,
Germany), and tetrahydrofuran (THF) (Merck, Darmstadt,
Germany). These solvents were used as received unless
otherwise stated. Other chemicals were obtained
commercially (Acros Organics). THF for cross-coupling
reactions was purified and dried with a solvent-purification
system (Asiawong SD-500, Taipei, Taiwan); about 50 ppm of
H2O was found in the resulting fluid. The Pd(PPh3)4 catalyst
(Strem, MA, USA) was used as received. For electrochemical
measurements, THF was distilled over sodium under N2. For
chromatographic purification, we used silica gel 60 (230−400
mesh, Merck).
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Graphical abstract
A large, ultra black, efficient and cost-effective dye-sensitized solar module reaches
an overall efficiency of ~12 % under 1000 lux of T5 fluorescent light.