Li et al.

Nanoscale Research Letters 2013, 8:67

http://www.nanoscalereslett.com/content/8/1/67

NANO EXPRESS

Open Access

Efficient PbS/CdS co-sensitized solar cells based

on TiO2 nanorod arrays
Yitan Li1, Lin Wei2, Xiya Chen1, Ruizi Zhang1, Xing Sui1, Yanxue Chen1*, Jun Jiao3,4 and Liangmo Mei1

Abstract
Narrow bandgap PbS nanoparticles, which may expand the light absorption range to the near-infrared region, were
deposited on TiO2 nanorod arrays by successive ionic layer adsorption and reaction method to make a photoanode
for quantum dot-sensitized solar cells (QDSCs). The thicknesses of PbS nanoparticles were optimized to enhance
the photovoltaic performance of PbS QDSCs. A uniform CdS layer was directly coated on previously grown PbSTiO2 photoanode to protect the PbS from the chemical attack of polysulfide electrolytes. A remarkable short-circuit
photocurrent density (approximately 10.4 mA/cm2) for PbS/CdS co-sensitized solar cell was recorded while the
photocurrent density of only PbS-sensitized solar cells was lower than 3 mA/cm2. The power conversion efficiency
of the PbS/CdS co-sensitized solar cell reached 1.3%, which was beyond the arithmetic addition of the efficiencies
of single constituents (PbS and CdS). These results indicate that the synergistic combination of PbS with CdS may
provide a stable and effective sensitizer for practical solar cell applications.
Keywords: TiO2, PbS, CdS, Nanorod, Solar cells

Background
Quantum dot-sensitized solar cells can be regarded as a
derivative of dye-sensitized solar cells, which have
attracted worldwide scientific and technological interest
since the breakthrough work pioneered by ORegan and
Grtzel [1-5]. Although the light-to-electric conversion
efficiency of 12% [6] reported recently was very impressive, the use of expensive dye to sensitize the solar cell is
still not feasible for practical applications. Therefore, it
is critical to tailor the materials to be not only costeffective but also long lasting. Inorganic semiconductors
have several advantages over conventional dyes: (1) The
bandgap of semiconductor nanoparticles can be tuned
by size to match the solar spectrum. (2) Their large intrinsic dipole moments can lead to rapid charge separation and large extinction coefficient, which is known to
reduce the dark current and increase the overall efficiency. (3) In addition, semiconductor sensitizers provide
new chances to utilize hot electrons to generate multiple
charge carriers with a single photon. Hence, nanosized
narrow bandgap semiconductors are ideal candidates
* Correspondence: cyx@sdu.edu.cn
1
School of Physics, State Key Laboratory of Crystal Materials, Shandong
University, Jinan 250100, Peoples Republic of China
Full list of author information is available at the end of the article

for the optimization of a solar cell to achieve improved

performance.
Recently, various nanosized semiconductors including
CdS [7], CdSe [8], CuInS2 [9], Sb2S3 [10,11], PbS [12], as
well as III-VI quantum ring [13,14] have been studied
for solar cell applications. Among these nanomaterials,
lead sulfide (PbS) has shown much promise as an impressive sensitizer due to its reasonable bandgap of
about 0.8 eV in the bulk material, which can allow extension of the absorption band toward the near infrared
(NIR) part of the solar spectrum. Recently, Sambur et al.
experimentally demonstrated the collection of photocurrents with quantum yields greater than one electron per
photon in the PbS QD-sensitized planar TiO2 single
crystal utilizing polysulfide electrolyte, which is undoubtedly encouraging to the future photovoltaic development
[15]. Furthermore, PbS has a large exciton Bohr radius
of about 20 nm, which can lead to extensive quantum
size effects. It has been reported that its absorption
range can be tuned by adjusting the particle size of the
quantum dots [16,17]. Until now, as one of the most impressive alternative semiconductors, PbS-sensitized solar
cells have been studied by many groups [18-22]. In most
of the reported works, PbS quantum dots were grown
on TiO2 nanotubes [20], ZnO nanorod arrays [21], and

2013 Li et al.; licensee Springer. This is an Open Access article distributed under the terms of the Creative Commons
Attribution License (http://creativecommons.org/licenses/by/2.0), which permits unrestricted use, distribution, and reproduction
in any medium, provided the original work is properly cited.

Li et al. Nanoscale Research Letters 2013, 8:67

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TiO2 photoanode with hierarchical pore distribution

[22]. Little work has been carried out on large-area single-crystalline TiO2 nanorod array photoanode. Compared to the polycrystal TiO2 nanostructures such as
nanotubes [23] and nanoparticles [24], single-crystalline
TiO2 nanorods grown directly on transparent conductive
oxide electrodes provide a perfect solution by avoiding
the particle-to-particle hopping that occurs in polycrystalline films, thereby increasing the photocurrent efficiency. In addition to the potential of improving electron
transport, they enhance light harvesting by scattering the
incident light.
In this paper, narrow bandgap PbS nanoparticles and
single-crystalline rutile TiO2 nanorod arrays were combined to produce a practical semiconductor-sensitized
solar cell. Several sensitizing configurations have been
studied, which include the deposition of only PbS or
only CdS and the hybrid system PbS/CdS. Optimized
PbS SILAR cycle was obtained, and the uniformly coated
CdS layer can effectively minimize the chemical attack
of polysulfide electrolytes on PbS layer. Therefore, the
performance of sensitized solar cells was stabilized and
long lasting. The power conversion efficiency of PbS/
CdS co-sensitized solar cell showed an increase of approximately 500% compared with that sensitized by only
PbS nanoparticles.

Methods
Growth of TiO2 nanorod arrays by hydrothermal process

The TiO2 nanorod arrays were grown directly on fluorinedoped tin oxide (FTO)-coated glass using the following
hydrothermal methods: 50 mL of deionized water was
mixed with 40 mL of concentrated hydrochloric acid.
After stirring at ambient temperature for 5 min, 400 L of
titanium tetrachloride was added to the mixture. The mixture was injected into a stainless steel autoclave with a
Teflon container cartridge. The FTO substrates were
ultrasonically cleaned for 10 min in a mixed solution of
deionized water, acetone, and 2-propanol with volume
ratios of 1:1:1 and were placed at an angle against the
Teflon container wall with the conducting side facing
down. The hydrothermal synthesis was conducted at
180C for 2 h.After synthesis, the autoclave was cooled
to room temperature under flowing water, and the FTO
substrates were taken out, rinsed thoroughly with
deionized water, and dried in the open air.
Deposition of PbS and CdS layers with successive ionic
layer adsorption and reaction method

In a typical SILAR cycle for the deposition of PbS nanparticles, the FTO conductive glass, pre-grown with TiO2
nanorod arrays, was dipped into the 0.02 M Pb(NO3)2
methanol solution for 2 min then dipped into 0.02 M
Na2S solution (obtained by dissolving Na2S in methanol/

Page 2 of 7

water with volume ratios of 1:1) for another 5 min. This

entire SILAR process was repeated from 1 to 10 cycles to
achieve the desired thickness of PbS nanoparticle layer.
Similarly, for the CdS nanoparticle layer, Cd2+ ions were
deposited from a 0.05 M Cd(NO3)2 ethanol solution, and
the sulfide sources were 0.05 M Na2S in methanol/water
(50/50 v/v). For the hybrid PbS/CdS co-sensitized samples, the CdS deposition was carried out immediately after
PbS deposition. The samples are labeled as PbS(X)/CdS
(Y)-TiO2, where X and Y refer to the number of PbS and
CdS SILAR cycles, respectively.
Characterization

The crystal structure of the CdS-TiO2 and PbS-TiO2 samples were examined by X-ray diffraction (XRD; XD-3, PG
Instruments Ltd., Beijing, China) with Cu K radiation
( = 0.154 nm) at a scan rate of 2/min. X-ray tube voltage
and current were set at 40 kV and 30 mA, respectively.
The surface morphology and the cross section of the
CdS-TiO2, PbS-TiO2, and PbS/CdS-TiO2 nanostructures
were examined by a field-emission scanning electron microscopy (FESEM; FEI Sirion, FEI Company, Hillsboro,
OR, USA).
Solar cell assembly and performance measurement

The solar cells were assembled using the CdS-TiO2,

PbS-TiO2, and PbS/CdS-TiO2 nanostructures as the
photoanodes, respectively. Pt counter electrodes were prepared by depositing 20-nm Pt film on FTO glass using a
magnetron sputtering. A 60-m-thick sealing material
(SX-1170-60, Solaronix SA, Aubonne, Switzerland) was
pasted onto the Pt counter electrodes. The Pt counter
electrode and a nanostructure photoanode were sandwiched and sealed with the conductive sides facing inward.
A polysulfide electrolyte was injected into the space between two electrodes. The polysulfide electrolyte was composed of 0.1 M sulfur, 1 M Na2S, and 0.1 M NaOH, which
were dissolved in methanol/water (7:3 v/v) and stirred at
60C for 1 h.
A solar simulator (model 94022A, Newport, OH, USA)
with an AM1.5 filter was used to illuminate the working
solar cell at light intensity of 1 sun (100 mW/cm2). A
sourcemeter (2400, Keithley Instruments Inc., Cleveland,
OH, USA) was used for electrical characterization during
the measurements. The measurements were carried out
with respect to a calibrated OSI standard silicon solar
photodiode.

Results and discussion

Morphology and crystal structure of the nanostructured
photoanodes

Figure 1a shows the typical FESEM images of TiO2

nanorod arrays on an FTO-coated glass substrate, confirming that the FTO-coated glass substrate was uniformly

Li et al. Nanoscale Research Letters 2013, 8:67

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Figure 1 Typical FESEM images of the bare TiO2 nanorod array and PbS-TiO2 nanostructures. (a) FESEM image (40 tilted) of the bare TiO2
nanorod array grown on FTO glass by hydrothermal method. (b) FESEM images of PbS-TiO2 nanostructures after 1, (c) 3, and (d) 5 SILAR cycles.

covered with ordered TiO2 nanorods. The density of

nanorods was approximately 20 nanorods/m2 with suitable space for deposition of PbS and CdS nanoparticles.
Figure 1b,c,d shows TiO2 nanorods coated by PbS nanoparticles after 1, 3, 5 SILAR cycles, respectively. With the
increase of SILAR cycles, the thickness of the PbS nanoparticles increased correspondingly. For the sample coated
with 5 SILAR cycles, the space between the TiO2 nanorods was filled with PbS nanoparticles, and a porous PbS
nanoparticle layer was formed on the surface of the TiO2
nanorods. As discussed later, this porous PbS layer can
cause a dramatic decrease in photocurrent and efficiency
for the solar cells.

Figure 2 shows the cross-sectional SEM images of PbS

(3)/CdS(0)-TiO2 and PbS(3)/CdS(10)-TiO2 nanostructures.
Compared with Figure 2a, a uniform protective layer of
CdS was successfully deposited on the top of PbS nanoparticles. As we will discuss later, after the CdS coating, a remarkable enhancement of the cell performance and the
photochemical stabilization of PbS sensitizer was observed.
XRD patterns of the bare TiO2 nanorod array, the PbS(3)/
CdS(0)-TiO2 nanostructure, and PbS(0)/CdS(10)-TiO2
nanostructure were shown in Figure 3. As shown in
Figure 3a, besides the diffraction peaks from cassiterite on
structured SnO2, all the other peaks could be indexed as
the (101), (211), (002), (310), and (112) planes of tetragonal

Figure 2 Cross-sectional SEM images of PbS-TiO2 nanostructures without (a) and with (b) CdS capping layer.

Intensity/(a.u.)

Page 4 of 7

(b)

TiO2 (301)
TiO2 (112)

TiO2 (002)

SnO2 (301)

TiO2 (211)

SnO2 (211)

SnO2 (310)

FTO/TiO2

SnO2 (200)

SnO2 (110)

(a)

SnO2 (101)
TiO2 (101)

Li et al. Nanoscale Research Letters 2013, 8:67

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CdS-TiO

(111)
(220)

(222)

(331)

(c)
PbS-TiO
(200)
(111)

(220)
(222)

20

30

40

50

(400)

60

(331)
(420)

70

(422)

80

2/Degree
Figure 3 XRD patterns of bare TiO2 nanorod array (a), CdS-TiO2 nanostructure (b), and PbS-TiO2 nanostructure (c).

rutile structure TiO2 (JCPDS no.02-0494). The formation

of rutile TiO2 nanorod arrays could be attributed to the
small lattice mismatch between FTO and rutile TiO2 [25].
Both rutile and SnO2 have near identical lattice parameters with a = 0.4594, c = 0.2958, and a = 0.4737,
c = 0.3185 nm for TiO2 and SnO2, respectively, making
the epitaxial growth of rutile TiO2 on FTO film possible.
On the other hand, anatase and brookite have lattice parameters of a = 0.3784, c = 0.9514 and a = 0.5455,
c = 0.5142 nm, respectively. The production of these
phases is unfavorable due to a very high activation energy
barrier which cannot be overcome at the low temperatures used in this hydrothermal reaction. As noted in
Figure 3b,c, the as-synthesized CdS-TiO2 nanostructure
exhibited weak diffraction peaks of CdS at 2 = 26.5,
43.9, 54.6, and 70.1, corresponding to the (111), (220),
(222), and (331) planes of cubic CdS with the lattice constant a = 0.583 nm (JCPDS no. 890440). The diffraction
peaks of as-synthesized PbS-TiO2 nanostructure could be
indexed as (111), (200), (220), (222), (400), (331), (420),
and (422) planes, correspondingly, of cubic PbS with the
lattice constant a = 0.593 nm (JCPDS no. 781901).
Photovoltaic performance of PbS/CdS-TiO2
nanostructured solar cells

Figure 4 showed the photocurrent-voltage (I-V) performance of the sensitized solar cells assembled using
PbS/CdS-TiO2 nanostructured photoanodes. All the

photocurrent-voltage performance parameters were

summarized in Table 1. Solar cell sensitized by only CdS
exhibits a short-circuit photocurrent density (JSC) of 5.7
mA/cm2 and an open-circuit voltage (VOC) of 0.39 V.
On the other hand, solar cell sensitized by only PdS
present a poor photovoltaic performance with very low
JSC and VOC. Optimal PbS SILAR cycles on this photoanode were investigated. As we can see from Figure 4b,
with the increase of PbS SILAR cycles, a non-monotonic
change of both JSC and VOC is recorded. Both JSC and
VOC of the PbS-sensitized solar cells increase with the
SILAR cycles first, and a maximum JSC of 2.5 mA/cm2
and VOC of 0.3 V are obtained for the sample with 3
SILAR cycles. With further increasing PbS SILAR cycles,
JSC and VOC decrease simultaneously, which demonstrates that a thick Pbs nanoparticles layer may hinder
PbS regeneration by the electrolyte and enhance the recombination reaction. During the measurement, a continuous decrease of the current was observed, indicating
the progressive degradation of PbS, which can be reasonably attributing to PbS oxidative processes. To protect the PbS nanoparticles from the chemical attack by
polysulfide electrolytes, a uniform CdS layer was capped
on the PbS-TiO2 photoanode to avoid the direct contact
of PbS with the polysulfide electrolyte. As shown in
Figure 4c, under the same PbS deposition cycles, the cell
with CdS capping layer presents both increased JSC and
VOC, indicating that CdS QDs is indispensable to highly

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(a)

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Table 1 Jsc, Voc, FF, and efficiency

Current density (mA/cm-2)

PbS(0)CdS(10)

Current density (mA/cm-2)

FF (%)

(%)

0.39

6.26

0.18

0.44

PbS(0)CdS(10)

PbS(10)CdS(0)

0.19

0.91

0.29

0.05

PbS(5)CdS(0)

0.25

1.12

0.25

0.07

PbS(4)CdS(0)

0.26

1.83

0.27

0.13

PbS(3)CdS(0)

0.29

2.48

0.27

0.20

PbS(2)CdS(0)

0.28

2.11

0.27

0.16

PbS(1)CdS(0)

0.25

1.10

0.29

0.08

PbS(10)CdS(10)

0.30

3.12

0.29

0.28

PbS(5)CdS(10)

0.26

3.98

0.33

0.34

PbS(4)CdS(10)

0.33

5.88

0.31

0.61

PbS(3)CdS(10)

0.47

10.40

0.27

1.30

PbS(2)CdS(10)

0.39

9.09

0.30

1.05

PbS(1)CdS(10)

0.36

5.24

0.24

0.46

0.1

0.2

0.3

0.4

Votage (V)
3.0
PbS(10)CdS(0)
PbS(5) CdS(0)
PbS(4) CdS(0)
PbS(3) CdS(0)
PbS(2) CdS(0)
PbS(1) CdS(0)

2.5
2.0

Voc, open-circuit voltage; Jsc, short-circuit photocurrent density; FF, fill factor; ,
energy conversion efficiency.

1.5
1.0
0.5
0.0
0.00

0.05

0.10

0.15

0.20

0.25

0.30

0.35

Votage (V)

(c) 12
Current density (mA/cm-2)

JSC (mA/cm2)

0
0.0

(b)

Voc (V)

PbS(10)CdS(10)
PbS(5)CdS(10)
PbS(4)CdS(10)
PbS(3)CdS(10)
PbS(2)CdS(10)
PbS(1)CdS(10)

10
8
6
4
2
0
0.0

0.1

0.2

0.3

0.4

0.5

Votage (V)

Figure 4 Photovoltaic performance of PbS/CdS co-sensitized

solar cells. (a) Photocurrent density-voltage characteristic for only
CdS-sensitized solar cell and (b) only PbS-sensitized solar cell. (c)
Photocurrent density-voltage characteristic for PbS/CdS co-sensitized
solar cells with different PbS SILAR cycles.

efficient PbS-sensitized solar cells. With the appearance of

CdS layer, JSC of the cell with 3 PbS SILAR cycles was
improved from about 2.5 to 10.4 mA/cm2, and the Voc
was increased from 0.3 to 0.47 V. The cell efficiency
reached a promising 1.3%, indicating a five times increase,
which is beyond the arithmetic addition of the efficiencies
of single constituents (PbS and CdS). In addition to the

increase of the cell performance for the co-sensitized configurations, a significant increase of the photochemical stability
of PbS takes place with the presence of the CdS coating.
With further improvement of their performance, this
kind of PbS/CdS co-sensitized TiO2 nanorod solar cells
may play a promising role in the future due to the following reasons: (1) The bandgap of PbS nanoparticles is quite
small and extends the absorption band towards the NIR
part of the solar spectrum, which will result in a high
current density. (2) TiO2 nanorod arrays grown directly
on FTO conductive glass avoid the particle-to-particle
hopping that occurs in polycrystalline mesoscopic TiO2
films, which can also contribute to a higher efficiency. (3)
TiO2 nanorods form a relatively open structure, which is
advantageous over the diffusion problems associated with
the redox couples in porous TiO2 network.
In our present work, the cell efficiency was still not high
enough for practical application. The drawback limiting
the energy conversion efficiency of this type of solar cells
was the rather poor fill factor. This low fill factor may be
ascribed to the lower hole-recovery rate of the polysulfide
electrolyte, leading to a higher probability for charge recombination [26]. To further improve the efficiencies of
these PbS/CdS-TiO2 nanostructured solar cells, a new hole
transport medium with suitable redox potential and low
electron recombination at the semiconductor-electrolyte
interface should be developed. Counter electrode was another important factor influencing the energy conversion
efficiency. Recently, Sixto et al. [27] and Seol et al. [28]
reported that the fill factor was clearly influenced by counter electrode materials where Au, CuS2, and carbon counter electrode show better performance than Pt ones.

Li et al. Nanoscale Research Letters 2013, 8:67

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Moreover, deposition of a ZnS passivation layer on the

photoanode after the PbS/CdS sensitization would greatly
eliminate interfacial charge recombination and improve
the photovoltaic performance of PbS/CdS-TiO2 nanostructured solar cells [29]. Further work to improve the
photovoltaic performance of these solar cells is currently
under investigation.

Conclusion
In this study, large-area ordered rutile TiO2 nanorod
arrays were utilized as photoanodes for PbS/CdS cosensitized solar cells. Narrow bandgap PbS nanoparticles
dramatically increase the obtained photocurrents, and
the CdS capping layer stabilizes the solar cell behavior.
The synergistic combination of PbS with CdS provides a
stable and effective sensitizer compatible with polysulfide. Compared to only PbS-sensitized solar cells, the
cell power conversion efficiency was improved from
0.2% to 1.3% with the presentation of a CdS protection
layer. The PbS/CdS co-sensitized configuration has
been revealed to enhance the solar cell performance
beyond the arithmetic addition of the efficiencies of
the single constituents. In this sense, PbS and CdS
constitute a promising nanocomposite sensitizer with
supracollecting properties for practical solar cell applications.

Competing interests
The authors declare that they have no competing interests.
Authors contributions
The work presented here was performed in collaboration of all authors. YL
carried out the deposition of PbS and CdS layers and solar cell assembly, and
drafted the manuscript. LW carried out the XRD and SEM characterizations.
XC carried out the photovoltaic performance measurements. RZ and XS
carried out the preparation of TiO2 nanorod arrays. YC supervised the work
and finalized the manuscript. JJ and LM proofread the manuscript and
polished the language. All authors read and approved the final manuscript.
Acknowledgments
This work was supported by the National Key Basic Research Program of
China (2013CB922303, 2010CB833103), the National Natural Science
Foundation of China (60976073, 11274201, 51231007), the 111 Project
(B13029), the National Found for Fostering Talents of Basic Science
(J1103212), and the Foundation for Outstanding Young Scientist in
Shandong Province (BS2010CL036).
Author details
1
School of Physics, State Key Laboratory of Crystal Materials, Shandong
University, Jinan 250100, Peoples Republic of China. 2School of Information
Science and Engineering, Shandong University, Jinan 250100, Peoples
Republic of China. 3Department of Mechanical and Materials Engineering,
Portland State University, P.O. Box 751, Portland, OR 97207-0751, USA.
4
Department of Physics, Portland State University, P.O. Box 751, Portland, OR
97207-0751, USA.
Received: 6 January 2013 Accepted: 2 February 2013
Published: 11 February 2013

Page 6 of 7

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