J Materiomics 3 (2017) 231e244

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J Materiomics
journal homepage: www.journals.elsevier.com/journal-of-materiomics/

Research progress on large-area perovskite thin films and solar

modules
Zhichun Yang a, Shasha Zhang a, Lingbo Li a, Wei Chen a, b, *
a
Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology, Luoyu Road 1037, Wuhan, 430074, China
b
Engineering Research Center of Nano-Geo Materials of Ministry of Education, China University of Geosciences, Wuhan 430074, China

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

Article history: Organometal halide perovskites have exhibited a bright future as photovoltaic semiconductor in next
Received 6 July 2017 generation solar cells due to their unique and promising physicochemical properties. Over the past few
Received in revised form years, we have witnessed a tremendous progress of efficiency record evolution of perovskite solar cells
20 September 2017
(PSCs). Up to now, the highest efficiency record of PSCs has reached 22.1%; however, it was achieved at a
Accepted 28 September 2017
Available online 29 September 2017
very small device area of <0.1 cm2. With the device area increasing to mini-module scale, the efficiency
record dropped dramatically. The inherent causes are mainly ascribed to inadequate quality control of
large-area perovskite thin films and insufficient optimization of solar module design. In current stage of
Keywords:
Large-area
PSCs research and development, to overcome these two obstacles is in urgent need before this new
Perovskite thin films technology could realize scale-up industrialization. Herein, we present an overview of recently devel-
Perovskite solar cells oped strategies for preparing large-area perovskite thin films and perovskite solar modules (PSMs). At
Perovskite solar modules last, cost analysis and future application directions of PSMs have also been discussed.
© 2017 The Chinese Ceramic Society. Production and hosting by Elsevier B.V. This is an open access article
under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 231
2. The strategies for the preparation of large-area perovskite thin films . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 232
2.1. Spin coating . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 232
2.2. Casting . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 233
2.3. Blade coating . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 233
2.4. Spray coating . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 234
2.5. Slot-die coating . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 234
3. How to design perovskite solar modules? . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 236
3.1. Solar modules in series . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 236
3.2. Solar modules in parallel . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 237
3.3. The cost of perovskite solar modules . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 238
4. Application directions of perovskite solar modules . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 241
5. Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 242
Acknowledgements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 242
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 242

1. Introduction
* Corresponding author. Wuhan National Laboratory for Optoelectronics, Huaz-
hong University of Science and Technology, Luoyu Road 1037, Wuhan, 430074, Organic-inorganic hybrid perovskite solar cells (PSCs) have
China. attracted widespread attention due to their relative low cost and
E-mail address: wnlochenwei@mail.hust.edu.cn (W. Chen). the soaring power conversion efficiency (PCE) in the last few years
Peer review under responsibility of The Chinese Ceramic Society.

https://doi.org/10.1016/j.jmat.2017.09.002
2352-8478/© 2017 The Chinese Ceramic Society. Production and hosting by Elsevier B.V. This is an open access article under the CC BY-NC-ND license (http://
creativecommons.org/licenses/by-nc-nd/4.0/).
232 Z. Yang et al. / J Materiomics 3 (2017) 231e244
[1,2]. Although the certified highest efficiency of PSCs has reached
22.1% [3], most of the reported PSCs are only limited to very small
areas (<<1 cm2). According to the report of “Material Research
Society Spring Meeting (March 28-April 1, 2016) held in Phoenix”, it
is an appropriate time to amplify the active area of PSCs for pro-
moting its commercial road now [4]. However, there are still many
challenges need to be overcome, such as how to prepare high
quality and large-area perovskite thin films with high uniformity
and reproducibility, how to improve the reproducibility of single
cells and how to design the interconnection of single cells to make
large modules.
A complete PSC is composed of several overlapped functional
layers. For example, typical mesoporous structure device includes
TiO2 compact layer, TiO2 mesoporous scaffold layer, perovskite
layer, hole transport layer and metal electrode [5]. Other layers
except perovskite layer can be deposited by easy-scale-up tech-
niques, such as spray-pyrolysis of compact TiO2, screen-printing
mesoporous TiO2 and thermal evaporation of metal electrode.
However, to expand the perovskite layer from small lab scale to
large module scale has not been resolved. The best way for the
deposition of perovskite thin film in laboratory is spin coating with
the help of antisolvent extraction; however, this method wastes a
lot of perovskite solution and is very sensitive to many technical
conditions, which make it hard to be used for the preparation of
module scale perovskite films. Up to now, the reported methods for
the preparation of large-area perovskite thin films (
1 cm2) could
be mainly divided into five categories, such as spin coating [6],
casting [7], blade coating [8], spray coating [9] and slot-die coating
[10] technologies. Though spin coating has intrinsic drawback for
large-area film preparation, it is still more frequently reported in
comparison to other techniques [11e13], which actually reflect the
shortage in preparing large-area perovskite thin film. Whatever
techniques being used, the common issues for large-area perov-
skite thin film fabrication are how to control the film morphology
to be pin-hole free and surface smooth, and how to control the
crystallization process to obtain large grain-size with fewer defects.
The core beneath these techniques are about the halide perovskites
and solvents related colloidal chemistry, coordination chemistry
and crystal growth kinetics. After the competitive efficiency of
small area (« 0.1 cm2) PSCs was achieved, researchers started to
transfer their attention to large-area (1 cm2) devices and small
modules (>10 cm2) [14]. In 2015, Chen et al. certified the first large-
area (1 cm2) PSC with 15.0% PCE, which was listed in the credited
Solar Cell Efficiency Tables (Version 46) [6,15]. Currently, the effi-
ciency record of 1 cm2 PSC has been renewed to 19.7%; this is not far
from the 22.1% record of 0.046 cm2 device [16]. However, up-
scaling from 1 cm2 device to tens of cm2 mini-modules, the certi-
fied efficiency record dropped largely to 16.0%. This is not only
because the high quality large-area perovskite film is difficult to
achieve, but also because the largely increased resistance from
transparent conductor oxide (TCO) glass substrate becomes a
serious limiting factor [17]. To date, many researchers and indus-
trial innovation companies have shifted their attention to develop
scalable techniques to fabricate high performance perovskite solar
modules (PSMs).
This review article will summarize the recent progresses on
large-area perovskite thin film and PSMs. In addition, the design of
metal grids for PSMs will be introduced in brief. At last, the cost
analysis and the promising application directions of PSMs will also
be prospected.
2. The strategies for the preparation of large-area perovskite
thin films
Towards commercialization of PSCs, the first step is to realize
high efficiency of large-area PSMs [18]; the primary obstacle rests
with how to prepare high-quality large-area perovskite thin films
with an ease-scalable deposition technique. In addition, the
perovskite precursors and their solvents are toxic; therefore, the
process safety must be taken into consideration [19].
2.1. Spin coating
Spin coating is a simple and popular method extensively used
for the deposition of perovskite thin film in laboratory. Usually, a
small amount of solution precursor is applied on the center of the
substrate. The substrate is then rotated at high a speed in order to
spread the coating material by centrifugal force. The solvent in the
precursor is usually volatile, and simultaneously evaporates during
high-speed rotation. And then, the dried film with certain thickness
is obtained. Generally, there are two popular ways for spin coating
deposition of perovskite films which are named standard “one-
step” [20] or “two-step” method [21]. Later, some modified or
improved “one-step” [22] and “two-step” methods are also devel-
oped for preparing pin-hole free perovskite films with good
morphology and crystallization [23,24].
One-step spin coating method was developed by Kojima et al.
[20], who firstly applied hybrid perovskite material to sensitized
solar cells. As is depicted in Fig. 1(a), during the procedure of one-
step spin coating CH3NH3PbI3, equimolar CH3NH3I and PbI2 were
dissolved in the solvent of N,N-dimethyl acetamide (DMA) followed
by spin coating and heat treatment [21]. Pan et al. designed a
strategy of hydrochloride-assisted spin coating to form highly
smooth and full coverage perovskite films with large crystalline
grains at room temperature; the PSC device obtained an efficiency
of 15.7% with an area of 0.86 cm2 [25]. We assume that the excellent
performance of PSCs fabricated with this method was attributed to
the ideal morphology of perovskite layer with fewer defects. Chiang
et al. prepared high quality single-phase mixed-halide perovskite
films by the method of one-step spin coating (hot solution) and
they fabricated large-area PSMs (active area: 25.2 cm2) with an
efficiency of 14.3% [26]. Qiu et al. prepared pinhole-free perovskite
thin film by one-step spin coating for solar modules with an
aperture area of 4 cm2 and obtained an efficiency of 13.6% [27].
Carlo et al. fabricated large-area PSCs (2.52 cm2) and solar modules
(10.1 cm2) by the method of one-step spin coating with an effi-
ciency of 7.6% and 7.3%, respectively [17]. In particular, Lee et al.
adopted poly[(9,9-bis(3’-(N,N-dimethylamino)propyl)-2,7-
fluorene)-alt-2,7-(9,9-dioctylfluorene)] (a kind of amphiphilic
conjugated polyelectrolyte) for an interfacial compatibilizer be-
tween perovskite film and charge transport layer; they obtained
pinhole-free perovskite film through the modified “one-step”
method of solvent engineering process and the device achieved a
PCE of 17.04% with an area of 1 cm2 as shown in Fig. 1(b) [22].
Two-step spin coating was developed by Im et al. [21], and then
it was adopted extensively for the deposition of perovskite film.
Burschka et al. [23] skillfully designed the strategy of two-step
sequential deposition of perovskite thin film. However, there are
fewer literature about large-area PSCs prepared via two-step
method. Shen et al. developed a modified “two-step” method and
the device achieved a PCE of ~14.5% with an active area around
1 cm2; They found that the perovskite thin film prepared by one-
step had some pinholes and the film fabricated with the method
of two-step had some residual PbI2 which was far excess the op-
timum range and it was harmful for the device performance; As
shown in Fig. 1(c), an additional treatment (spin coating with high
concentration methylammonium iodide (MAI) solution) was
introduced in the deposition process, which is beneficial for
tailoring the residual PbI2 level to a suitable range for uniform,
pinhole-free perovskite film; The as-prepared films are not only
 Z. Yang et al. / J Materiomics 3 (2017) 231e244
pinhole free, but also have much better uniformity and repeat-
ability compared to the films fabricated with the method of both
one-step and two-step (as shown in Fig. 1(d)), and the corre-
sponding J-V curves of devices are shown in Fig. 1(e) [24].
Spin coating has achieved great success in fabricating small area
PSCs [28e30]. However, it's a real big challenge for this method to
be used in large scale production of perovskite films or PSMs.
Although spin coating has been reported for the fabrication of
several square centimeters PSCs with excellent performance, it is
hard to be expanded to further larger area devices. This practical
situation has strongly motivated researchers to explore alternative
scalable techniques for the preparation of large-area perovskite
thin films.
2.2. Casting
Casting involves just a simple transfer of perovskite solution to a
target substrate followed by a short heat process to remove solvent.
Film thickness is controlled by the solid content in the solution. The
surface tension between the perovskite solution and the target
substrate, the viscosity of the perovskite solution and the heating
temperature will largely impact on the film’s quality and
uniformity.
The only prominent advantage of this technique is that no
special equipment is required. It is possible to prepare large-area
perovskite film simply but the lack of control of film thickness
and accurate perovskite solution usage are obvious drawbacks to
this method. So far, there are only limited literature about the
preparation of large-area perovskite film with the method of cast-
ing. Casting mainly includes drop casting and hot (dip) casting. Mei
et al. skillfully added 5-aminovaleric acid into the ƴ-butyrolactone
solution containing PbI2 and MAI. In the process, 5-AVA replaced
some MA cations in MAPbI3, resulting in a new mixed-cation
perovskite film ((5-AVA)x(MA)1-xPbI3) with lower defect concen-
tration and better pore filling in mesoporous TiO2 layer, which led
Fig. 1. (a) The comparison of one-step and two-step spin coating procedures for the deposition of CH3NH3PbI3 film [21]. (b) J-V characteristics of large-area PSC (1 cm2) with one-
step spin coating [22]. (c) Schematic of the synthesis procedure of perovskite film based on the modified “two-step” method, (d) SEM images of perovskite films prepared by
different methods and (e) J-V curves for 1 cm2 devices based on three different methods for the preparation of perovskite layer [24].
233
to a longer carrier lifetime and benefited the device performance.
Through the method of drop casting (Fig. 2(a)), a favorable PCE of
12.8% was obtained for a small area of printable mesoporous PSC,
and the J-V curves were exhibited in Fig. 2(b) [31]. Later, Hu et al.
prepared large-area perovskite thin film through drop casting, and
they fabricated a 7 m2 printable perovskite solar panel with the J-V
curves shown in Fig. 2(c) [32]. Nie et al. reported a method of hot-
casting technique for the preparation of perovskite film [33]. Liao
et al. used similar method of hot-casting process (Fig. 2(d)) with
controlled Cl incorporation to enhance the device performance. In
detail, the substrate was preheated on a hotplate and the hot
substrate was put into the prepared perovskite solution. After
quickly taking out from the solution, the perovskite thin film was
formed; compared with the tri-iodide PSCs, this result can be
attributed to the longer carrier diffusion lengths and the improved
uniformity of the perovskite film morphology (Fig. 2(e)); they also
fabricated PSMs composed of eight sub cells connected in series
and the J-V curves were exhibited in Fig. 2(f) (inset was the optical
image of the PSMs) [7].
2.3. Blade coating
Blade coating was used for the fabrication of dye-sensitized
solar cells in early stage [34]. After skillfully modified, it has been
recently used for the deposition of large-area perovskite films [35].
For example, lead iodide (PbI2) precursor of hybrid perovskite can
be deposited through blade coating for the first step of “two-step”
sequential deposition strategy. During the blade coating procedure,
a sharp blade is placed in a suitable position over the target sub-
strate and the coating solution is put in front of the blade as shown
in Fig. 3(a) [36]. The blade can be moved with linear speed across
the substrate to get a wet perovskite film. In general, the wet layer
thickness should be roughly half the distance between the sub-
strate and the blade. However, this value can vary significantly due
to various physical factors of the surface energy of the substrate,
234
surface tension and viscosity of the solution [37].
Recently, Deng et al. obtained large-area (1 inch2) perovskite
film with the method of doctor blading and the corresponding SEM
image is shown in Fig. 3(b) [36]; they found that the carrier diffu-
sion length of perovskite film prepared by doctor-blade was
significantly longer than that of the spin coated films. They claimed
that the crystalline grain size from doctor-blading was larger than
that from spin coating. Moreover, the device yielded an exciting
efficiency of 15.1% and the J-V curves are shown in Fig. 3(c) [36].
Mallajosyula et al. fabricated large-area PSCs (~1 cm2) with large
perovskite grains through temperature-controlled doctor blading
strategy and yielded an average efficiency of 7.32% with negligible
hysteresis [35]. The outstanding performance can be ascribed to the
large grain size and the highly crystalline perovskite thin films.
Yang et al. obtained perovskite layer using the method of blade
coating and fabricated large-area PSCs (1.2 cm2) with an average
efficiency of 17.33%. Photograph in different size is shown in
Fig. 3(d), SEM image is shown in Fig. 3(e) and J-V curves are shown
in Fig. 3(f); the preferable perovskite film morphology was obtained
with an antisolvent treatment process, which is beneficial for the
outstanding performance of PSCs. Besides, the use of excess MACl
was helpful for a highly crystalline film [38]. Razza et al. designed
air flow-assisted PbI2 blade coating deposition for the formation of
large-area perovskite thin film and obtained a 10.4% PCE with an
active area of 10.1 cm2 [39].
At last, it is generally noted that blade coating is a very prom-
ising technique with a high deposition speed and throughput
compared to the above- mentioned coating techniques. It is also
possible to convert blade coating into roll-to-roll method easily
where the flexible substrate is placed on a cylinder.
2.4. Spray coating
Spray coating is an ease-scalable method to fabricate large-area
perovskite thin films. A typical spray coating system is composed of
a pressure tank for perovskite solution and an air-driven spray
nozzle. In brief, the ultrafine droplets of perovskite solution were
sprayed from the nozzle and deposited on the target substrate
which may be heated on a hotplate at certain temperature. After
drying and annealing process, the perovskite film could be formed
Fig. 2. (a) Schematic illustration of drop-casting perovskite solution for fully printable mesoscopic solar cells and (b) J-V curves measured under simulated AM 1.5 solar irradiation at
an intensity of 100 mW cm2 [31]. (c) J-V curves of optimized PSC device measured in forward and reverse scan (with 5 mm circular mask) [32]. (d) Schematic illustration of hot
casting and the inset is hot casting process, (e) SEM image of CH3NH3PbI3 film with a scale bar of 1 mm, and (f) J-V curve of PSMs (connected by eight single cells) and it's optic image
is shown in the inset [7].
Z. Yang et al. / J Materiomics 3 (2017) 231e244
on the substrate. Perovskite film obtained by this method exhibits
high uniformity in large area. And compared with casting, it has a
better thickness control. In order to obtain a perovskite thin film
with controlled quality by spray coating, the perovskite solution
concentration and viscosity, substrate temperature, the nozzle
diameter and spray flow rate should be taken into consideration.
Das et al. designed an ultrasonic spray-coating system (Fig. 4(a))
to prepare uniform perovskite layer (Fig. 4(b)) with an outstanding
efficiency of 13% (Fig. 4(c)) [40]. The excellent PSCs performance
can be attributed to the highly crystalline and uniform perovskite
film. Later, Eslamian et al. improved the spray coating (Fig. 4(d))
system skillfully and prepared pinhole-free large-area (25 cm2)
perovskite thin film (shown in Fig. 4 (e) and (f)) [9]. With an
automated spray coater, the film thickness and roughness could be
optimized by tuning the concentration of perovskite solution and
the temperature of substrate. Moreover, the high quality of
perovskite film and the reproducibility can be assured through this
method. Barrows et al. used similar method to obtain the device
efficiency of 11% [41]. Huang et al. obtained large-area CH3NH3PbI3
film with the method of two-step ultrasonic spray coating depo-
sition and achieved a PCE of 13.09% for large-area PSCs (1 cm2) [42].
The outstanding performance of PSCs fabricated can be ascribed to
the uniform and smooth perovskite (CH3NH3PbI3) films. Tait et al.
prepared large-area perovskite layer (3.8 cm2) with the method of
ultrasonic spray coating and achieved an efficiency of 11.7% [43].
2.5. Slot-die coating
Slot-die coating is another ease-scalable technique for the
deposition of large-area perovskite thin film and the fabrication of
large-area PSMs. It is possibly the most applicable technology for
perovskite thin film fabrication in industry. The technique is quite
simple and applicable to a wide range of inks with very different
viscosities. The ink is fed from the tank into the coating head which
has precisely-designed cavity and channel inside. This can make
sure the ink’s property unchanged during the whole coating pro-
cess. The solution precursor is squeezed out through a uniform slit
of the coating head by controlled air pressure, and deposited on the
substrate which may be preheated. After drying and annealing, the
perovskite film could be obtained.
 Z. Yang et al. / J Materiomics 3 (2017) 231e244 235

Fig. 3. (a) Schematic of the doctor blading, (b) SEM image of perovskite film prepared with the method of doctor blading and (c) J-V curves of PSC measured under 1 sun illu-
mination and dark [36]. (d) Photograph of perovskite films on different size substrates, (e) Top-view SEM image of perovskite film with a thickness of 200 nm (scale bar: 1 mm) and
(f) J-V curves with both forward and reverse scan (active area: 1.2 cm2) [38].

In general, this technique combines three key advantages of film
preparation. Firstly, the parameters of perovskite thin film can be
precisely pre-designed. In detail, the size and thickness of desired
film can be predetermined by the slot width, length, feeding pump
pressure, viscosity of solution precursor and coating speed. Sec-
ondly, it is a kind of contact-free preparation method which can
avoid scratches on the target substrate. Thirdly, the film can be
prepared in a fully sealed space. On the one hand, the coating
system is completely enclosed which can avoid the leakage of
harmful perovskite precursors. On the other hand, compared to
other coating methods, this strategy almost doesn't have any
evaporation loss of perovskite precursors or solution during
coating, which is beneficial for cost-saving production and repro-
ducibility of film fabrication.
Recently, Qin et al. employed slot-die coating technique to
fabricate all of functional layers in PSCs (except the counter elec-
trode) and obtained a PCE of 14.7% for the device with an active area
of 10 mm2 [44]. Hwang et al. fabricated PSCs with 10 mm2 active
area by improving slot-die coating system which is shown in
Fig. 5(a). The additional blowing dry holds the key to get high
quality PbI2 film (optic pictures of slot-die coated PbI2 films at
different conditions shown in Fig. 5(b)) [45]. Vak et al. designed 3D
printer based slot-die coater for preparing large-area perovskite
film for solar modules with a total active area of 47.3 cm2 [46]. Cai

Fig. 4. (a) Schematic illustration of ultrasonic spray-coating process, (b) SEM image of spray-coated perovskite film at 90  C and (c) J-V curves of the champion device under dark
and standard illumination conditions [40]. (d) Illustration of improved spray coating system, (e) SEM and optical image (inset) of perovskite film prepared with the method of spray
coating at a substrate temperature of 25  C and (f) the deposition pattern based on a zigzag movement of the spray nozzle over the substrate [9].
236 Z. Yang et al. / J Materiomics 3 (2017) 231e244
et al. designed a slot-die coating procedure with vacuum drying
process which led to better control of the perovskite film. They
obtained 5  5 cm2 module (total active area of 17.3 cm2) with an
outstanding efficiency of 10.6%. The optical picture and J-V curves
are shown in Fig. 5(c) and (d), respectively [10]. It is worth noting
that there was no significant degradation of perovskite film after
140 days of outdoors testing.
Many factors of slot die coating technology need to be further
optimized, unless the perovskite film quality still cannot catch up
with that prepared by spin coating in laboratory scale. The perovskite
solution composition associated colloid chemistry, wet film drying
process and their impact to perovskite crystallization process should
be monitored by some kind of in-situ characterization techniques,
which will benefit understanding and precise process control.
3. How to design perovskite solar modules?
If one check the solar cell efficiency tables published regularly
by Martin Green et al. [47], it can be found that the certified effi-
ciencies for commercialized solar cells, like monocrystalline Si or
multicrystalline Si, were achieved at very large module scale with
the size of hundreds of square centimeters. Only for the emerging
photovoltaic technologies, including PSCs, organic solar cells, dye-
sensitized solar cells, etc., the certified data were achieved at lab-
oratory cell size of ~1 cm2. This reflects they are in different stages
of development. However, in order to demonstrate the possibility
towards industrialization, it is an inevitable step for new photo-
voltaic technologies to demonstrate high efficiency at larger scale of
at least 10e100 cm2 [48,49]. These kinds of devices are called mini-
module or sub-module. Their certified efficiency can be listed in
another row besides 1 cm2 standard cells in the solar cell efficiency
tables. The up-to-date reported PSMs with their device areas and
their deposition approach are summarized in Table 1. Among them,
the highest certified efficiency for mini-module was achieved by a
Chinese innovation company Microquanta Co. Ltd.
3.1. Solar modules in series
Series connection is currently the most frequently used strategy
to fabricate PSMs from sub cells, which benefits for increasing the
voltage of the modules while keeping the photocurrent as small as
each sub cell. This will decrease the impact of enlarged series
resistance especially from large-area TCO glass substrate [50]. The
perovskite active film with high uniformity is of primary impor-
tance for the outstanding performance of PSMs [51]. The series
interconnection of mesoporous and planar structure PSMs are
shown in Fig. 6(b) and (c), respectively [52].
The resistances of PSMs in series connection [53] are similar with
other thin-film solar modules as depicted in Fig. 6(a) [54]. Several
electric resistances caused by the interconnection of single cells will
impact the output performance of final modules. The sheet re-
sistances from top electrode (Rs,top), bottom electrode (Rs,bottom) and
the interconnect resistance (Rint) from the contact between top and
bottom electrode in the P2 line are the main source of electric re-
sistances [54]. The area of P1, P2 and P3 (width of this area ¼ [) in
Fig. 6(a) is not photoactive section (dead area), leading to account-
able energy losses of modules. A geometric fill factor (GFF) is usually
introduced to assess the dead and total areas of the module:
 
AreaDead
GFF ¼ 1  100%
AreaTotal
In addition, the active length L also impact the value of GFF, Rs,top
and Rs,bottom. Assuming the width of single cell is w, we can
calculate the active area by the formula of A ¼ L$w. The dead area of
the module refers to the section without photo-to-electric con-
version and it can be obtained from the formula of D ¼ [$w.
The interconnection width largely depends on the deposition
and patterning technique (mainly for laser technology) and the
width value has a strong impact on the performance of final
module. Mincuzzi et al. have studied the laser processing for
manufacturing PSMs [55]. So far, several innovative laser-based
fabrication processes have been developed [18,56,57]. Matteocci
et al. etched fluorine-doped tin oxide (FTO) substrates with a
Nd:YVO4 pulsed laser (l ¼ 1064 nm, f ¼ 30 kHz and the average
output power P ¼ 10 W) to form the desired electrode patterns and
obtained the metal electrode deposition mask via a CO2 laser sys-
tem [56]. The high energy, short-pulsed laser is used to avoid the
formation of micro-cracks on conductive substrate. Up to now, the
PSMs in series have obtained significant progress.
Priyadarshi et al. fabricated PSMs in series with an active area of
31 cm2 and 70 cm2 and the corresponding efficiency are 10.46% and
10.74%, respectively [58]. It is worth noting that they realized the
PSMs with scalable printing processes and the modules exhibited
excellent long-term stabilities (2000 h) under ambient conditions.
Matteocci et al. fabricated series-interconnected PSMs with a total
active area of 16.8 cm2 and achieved an efficiency of 5.1%. Five
single cells with the size of 3.36 cm2 are interconnected in series. In
comparison to a 6.3% efficiency of the best sub cell, the main loss of
the PSMs comes from the low Fill factor (FF) [56]. It is proposed that
the resistivity of the FTO electrode and the uniformity of perovskite
layer deposited by spin coating are the main limiting factors. These
could be overcome by decreasing the electrode resistance and
developing new strategies for coating large-area perovskite thin
film. Fakharuddin et al. found that CH3NH3PbI3-xClx active layer
showed better phase stability with the mesoporous scaffold of TiO2
nanorods compared to TiO2 nanoparticles, resulting to higher shelf-
life durability; they fabricated PSMs in series (active area of
10.8 cm2) based on vertical TiO2 nanorods with a best efficiency of
10.5% compared to TiO2 nanoparticles with an efficiency of 7.9%;
lastly, they explained that it was most likely due to the macro-
porous nature of TiO2 nanorods compared to TiO2 nanoparticles
[59]. Seo et al. obtained p-i-n structure PSCs based on a flat
perovskite (CH3NH3PbI3) film and a thick PCBM film at low tem-
perature; they achieved the performance enhanced PSCs with the
insertion of LiF interlayer and designed 10  10 cm PSMs connected
in series (overall active area of 60 cm2) with an efficiency of 8.7%
[60]. Razza et al. designed an air flow-assisted PbI2 blade coating
deposition system and studied the morphology of PbI2 and
perovskite film with light beam induced current; in addition, they
fabricated PSMs in series (PbI2 layer was patterned with CO2 laser)
with an efficiency of 4.3% and the module area was 100 cm2 [39].
Qiu et al. developed a new precursor system of Pb(CH3CO2)2$3H2O,
PbCl2, and CH3NH3I for the formation of pinhole-free, highly crys-
tallized perovskite active layer and obtained 4 cm2 (aperture area)
PSMs connected in series (as shown in Fig. 7(d) and (e)) with an
optimum efficiency of 13.6% [27]. In comparison to small area de-
vice (active area: 0.13 cm2, PCE ¼ 16.7%), the main loss of the solar
module comes from current density (Jsc). It is proposed that the loss
in Jsc is mainly ascribed to the active area loss due to the sub-cell
interconnections. However, the apparent hysteresis can be
observed in J-V curves in Fig. 7(f); in addition, they also tracked the
maximum power point (fewer literature reported) of the PSMs,
which was very important for solar modules system [27]. Heo et al.
developed hysteresis-less inverted ITO/PEDOT:PSS/CH3NH3PbI3/
PCBM/Au planar hybrid solar cells with an average PCE of 18.1% by
solubility controlled MAPbI3 solution, which can be attributed to a
more balanced electron and hole flux, and a reduced number of
surface traps; moreover, they designed PSMs in series with an ef-
ficiency of 12.9% (active area of 40 cm2) [61]. Yang et al. fabricated
 Z. Yang et al. / J Materiomics 3 (2017) 231e244
Fig. 5. (a) Schematic illustration of slot-die coating system for the fabrication of pinhole-free PbI2 film and (b) Photographs of slot-die coated PbI2 films [45]. (c) Optic image of PSMs
with a size of 5  5 cm2 and (d) J-V curves of perovskite module with a total active area of 17.3 cm2 [10].
planar PSMs with an efficiency of 12.07% (active area of 36 cm2)
certified by the National Institute of Advanced Industrial Science
and Technology (AIST) [62]. Microquanta et al. reported the highest
efficiency (16.0%) PSMs interconnected with 6 serial cells with an
aperture area of 16.29 cm2 in May 2017 (certified by the National
Renewable Energy Laboratory in the United States) and it was listed
in the Solar Cell Efficiency Tables (Version 50) [47,63]. Imec and
Solliance's PSMs efficiency was 12.4% with an aperture area of
16 cm2 [64]. Hambsch et al. fabricated PSMs in series with an ef-
ficiency of 6.8% (aperture area: 25 cm2) [65]. Agresti et al. achieved
PSMs with eight single cells and obtained an efficiency of 12.6%
(active area: 50.56 cm2) [66]. Shen et al. gained an efficiency of
6.22% for PSMs (active area: 8.4 cm2) connected in series with the
graphene flakes doped mesoporous TiO2 layer to develop the
interface properties and improve charge injection [67]. Leyden et al.
obtained PSMs in series with an efficiency of 9.5% (active area:
8.8 cm2) [68]. Giacomo et al. fabricated flexible PSMs with an effi-
ciency of 3.1% (active are: 7.92 cm2). It is worth noting that they
obtained the compact layer with atomic layer deposition and the
TiO2 scaffolds were irradiated by UV light [69]. Fakharuddin et al.
designed a strategy of vacuum-vapor assisted sequential deposition
for perovskite layer and fabricated PSMs connected in series with
an efficiency of 8.1% (active area: 8.8 cm2) [70].
As shown in Fig. 8, Song et al. proposed a completed production
line for PSMs in series, laser processing (the formation of P1, P2 and
P3) are used to pattern the TCO glass and the subsequently
deposited perovskite layer and charge transport interfacial layer.
They adopted ZnO and NiO (prepared with screen printing) for HTL
and HTM, respectively. In addition, ITO and Al (they were prepared
by industrial-scale magnetron sputtering) were served as the front
and back electrodes. The most important component of perovskite
layer was prepared by the strategy of single-step screen printing
[71].
3.2. Solar modules in parallel
Despite an ideal open circuit voltage (Voc) can be achieved for
PSMs connected in series, the desired precision to match Jsc of
single cells is still difficult to realize. Much more attention should
237
be devoted to connect adjacent cells for modules to obtain a perfect
fill factor (FF) and minimize the energy loss [50]. To solve these
problems, another effective method of parallel connection can be
used for the construction of PSMs from sub cells.
Similar with other thin film solar modules [72], PSMs connected
in parallel always exhibit substantial loss of current and give similar
Voc to sub cells. Recently, Kumar et al. manufactured PSMs (the cost-
effective copper phthalocyanine as the HTL) with 6 unit cells con-
nected in parallel and two rows were integrated in series; 6 subcells
connected in parallel exhibited a current of 8.9 mA, the Voc was
0.61 V and FF was 0.28; and two rows (6 single cells connected in
parallel for each row) were interconnected in series and obtained a
Voc of 1.08 V, a current of 8.8 mA and the FF was still 0.28 [73]. From
their results, we can know that two rows interconnected in series
indeed increase the voltage of the final module while the current
keep at a relatively constant level. Sfyri et al. achieved small PSMs
composed of 9 sub cells (active area:15 mm2) interconnected in
parallel and two rows of parallel modules connected in series. In
comparison to a highest efficiency of 7% for each sub cell, the main
loss of the solar modules comes from the drop of Jsc [74]. It is
proposed that the conductivity of the transparent electrodes (FTO)
is the main limiting factor, which could be overcame by using metal
grids for current collection.
At the module level of solar cells, they are usually integrated in
series or in parallel. It is widely known that a higher value of series
resistances will lead to a lower FF of solar modules. In order to
minimize the impact of it, the metal grids are required to increase
the conductivity of TCO glass substrate.
In parallel connected PSMs, charge is collected not only from the
bottom electrode contacted with FTO substrate, but also from the
strips of metal grids (Ag, Ni, Ti, Cu, Al, and Au). These metallic grids
can significantly enhance the output performance of PSMs which
are similar with other thin-film solar modules. Due to the easy
corrosion of metallic Ag, Al by perovskite film [75], the anti-
corrosive metals, like Ni, Ti are preferable to be used as the grids
of PSMs. Hambsch et al. obtained the performance enhanced PSMs
with aluminum grids; in the fabrication process, they skillfully
exposed the aluminum grid lines to an UV-ozone plasma for an
aluminum oxide layer to improve the hydrophilic of film forming
238 Z. Yang et al. / J Materiomics 3 (2017) 231e244

Table 1
The efficiency of representative PSMs interconnected in series, till 30-June-2017.

Number Device architecture The deposition approach Aperture Active Module PCE Organization Ref.
of perovskite film area area area (cm2)
(cm2) (cm2)

1 FTO/NiOx/Perovskite/PCBM/PEI/Ag Dip casting e e 25 12% Northwestern University, USA [7]

2 FTO/ZnO/Perovskite/Carbon Slot-die coating e 17.6 e 10.6% Weihua Solar Co. Ltd., China [10]
3 FTO/C-TiO2/M-TiO2/CH3NH3PbI3-xClx/ Spin coating e 13.44 e 5.1% University of Rome “Tor Vergata”, Italy [17]
HTM/Au
4 FTO/C-TiO2/M-TiO2/CH3NH3PbI3-xClx/ Spin coating e e e 8.2% University of Rome “Tor Vergata”, Italy [18]
P3HT/Au
FTO/C-TiO2/M-TiO2/CH3NH3PbI3/Spiro- e 10.08 e 13%
OMeTAD/Au
5 ITO/C-TiO2/CH3NH3PbI3-xClx/Spiro- Spin coating 4 e e 13.6% IMEC, Belgium [27]
OMeTAD/Au
6 FTO/C-TiO2/M-TiO2/Perovskite/ZrO2/ Drop casting e 49 e 10.4% Huazhong University of Science and [32]
Carbon Technology, China
7 FTO/C-TiO2/Perovskite/Spiro-OMeTAD/Ag Blade coating e 11.09 e 13.3% National Renewable Energy Laboratory, [38]
USA
8 FTO/C-TiO2/M-TiO2/CH3NH3PbI3/Spiro- Blade coating e 10.1 e 10.3% University of Rome “Tor Vergata”, Italy [39]
OMeTAD/Au e e 100 4.3%
9 FTO/C-TiO2/M-TiO2/CH3NH3PbI3-xClx/ Spin coating 25 16.8 e 5.1% University of Rome “Tor Vergata”, Italy [56]
P3HT/Au
10 FTO/C-TiO2/M-TiO2/Perovskite/ZrO2/ Drop casting e 31 e 10.46% Nanyang Technological University, [58]
Carbon e 70 e 10.74% Singapore
11 FTO/C-TiO2/Nr-TiO2/CH3NH3PbI3-xClx/Au e e 10.8 e 8.1% University of Rome “Tor Vergata”, Italy [59]
12 ITO/PEDOT:PSS/CH3NH3PbI3/PCBM/LiF/Al Spin coating e 60 e 8.7% Korea Research Institute of Chemical [60]
Technology, Republic of Korea
13 ITO/PEDOT:PSS/CH3NH3PbI3/PCBM/Au Spin coating e 40 e 12.9% Kyung Hee University, Republic of Korea [61]
14 e e e 36 e 12.07% SJTU/NIMS [62]
15 e e 16.29 e e 16.0% ± 0.4 Microquanta Co. Ltd., China [63]
16 e e 16 e e 12.4% IMEC, Belgium [64]
17 ITO/PEDOT:PSS/CH3NH3PbI3/PC60BM/LiF/ Spin coating 25 e e 6.8% University of Queensland, Australia [65]
Ag
18 FTO/C-TiO2/Graphene þ M-TiO2/GO-Li/ Dip coating e 50.6 e 12.6% University of Rome Tor Vergata, Italy [66]
Perovskite/Spiro-OMeTAD/Au
19 FTO/C-TiO2/M-TiO2/ CVD e 8.8 e 9.5% Okinawa Institute of Science and [68]
Perovskite(formamidinium/CH3NH3PbI3)/ 12 9.0% Technology Graduate University, Japan
HTM/Au 15.4 8.5%
20 ITO/C-TiO2/M-TiO2/CH3NH3PbI3-xClx/ Spin coating e 7.92 e 3.1% University of Rome “Tor Vergata”, Italy [69]
Spiro-OMeTAD/Au
(On PET flexible substrate)
21 FTO/C-TiO2/TiO2 NRs/CH3NH3PbIxCl3x/ vacuum-vapor assisted e 8.8 e 8.1% Universiti Malaysia Pahang, Malaysia [70]
Spiro-OMeTAD/Au sequential processing
(V-VASP)

Note: C-TiO2: Compact TiO2 layer.

M-TiO2: Mesoporous TiO2 layer.
CVD: Chemical vapor deposition.
IMEC: Interuniversity Microelectronics Center.
SJTU: Shanghai Jiao Tong University.
NIMS: National Institute for Materials Science.

and low the possibility of device short circuit between the grids and
top electrode [65]. In addition, the oxide layer can also prevent
probable corrosion of aluminum grids for the element of iodide in
perovskite film.
However, the main drawback of using metal grids as current
collectors is the decrease of active area for the final module. It is
necessary for us to pay much more attention to optimize the
pattern design of metallic grids for PSMs and balance the resistance
benefit and the optical loss.
3.3. The cost of perovskite solar modules
Cost analysis is an important aspect of optimizing PSMs design.
A competitive low cost of raw material and processing for PSMs
manufacture is another important factor beyond efficiency and
lifetime for their potential to commercial application [76]. Cai et al.
calculated the cost of materials both for mesoporous structure
(Module A) and planar structure (Module B) PSMs as shown in pie
charts of Fig. 9(a) and (b), respectively; the material cost consists of
four parts: TCO glass, active layers, solvents and others (sealing
materials and glass cover); from the results they presented, it can
be known that the total calculated cost of materials for Module A
(0.127 US$/W) was a little higher than Module B (0.102 US$/W); it is
apparent that the cost of TCO are the main part for both structure
modules [52]. In addition, it is known that the utilization of active
area for Module B is higher than Module A, which can be respon-
sible for their cost results. Accompanying with further efficiency
development, these two kinds of solar modules' costs can both be
further decreased to some extent (Fig. 9(c)); it is noteworthy that
the solid lines in the curves represent for the current efficiency
status for those two kind solar modules [52]. It is thought that the
planar structure of PSMs is easier to control the interface; and it will
be more competitive to win in the efficiency competition, which
will also strength its low-cost advantage.
The levelized cost of electricity (LCOE) is an important index
extensively used for the assessment of the cost level of different
kind solar modules. It was usually influenced critically by material
price, fabrication cost, module efficiency and lifetime of modules.
 Z. Yang et al. / J Materiomics 3 (2017) 231e244 239

Fig. 6. (a) Cross section schematic of typical thin-film solar modules in series connection: the connect width is marked with P2, the patterning length refers to the distance between
P1 and P3 (represented by [), and L is the active cell length [54]. (b) Schematic illustration of series connect perovskite solar modules for mesoporous structure (Module A) and (c)
planar structure (Module B) [52].

Fig. 7. (a) Photograph of series connection PSMs, (b) The series interconnection schematic illustration and (c) The efficiency exhibition of PSCs (active area: 0.1 cm2 and 3.36 cm2)
and series connected PSMs (active area: 16.8 cm2) with different hole transport materials: Spiro-OMeTAD (cyan colour) and P3HT (green colour) [56]. (d) Photograph of PSMs
consisting of 4 sub cells with a total aperture area of 4 cm2, (e) Scheme illustration of the series interconnection of single cells for PSMs, (f) The crosssection SEM image of a complete
PSC and (g) J-V curves of the 4 cm2 PSMs and 0.13 cm2 PSC with different scan direction [27].
240 Z. Yang et al. / J Materiomics 3 (2017) 231e244

Fig. 8. Process diagram of fabricating PSMs connected in series [71].

As shown in Fig. 9(d), Cai et al. calculated LCOE values of PSMs with
different module efficiencies, which could be dropped with the
lifetimes; in addition, as for high efficiency (20%) modules, a life-
time of 10 years can result in an LCOE of 4.7 US cents/kWh [52].
According to their results, the ultra-low LCOE of PSMs can be
controlled to be 3.5e4.9 US cents/kWh with 15 years lifetime and
Song et al. gave their calculated LCOE ranging from 4.93 to 7.90
¢/kWh [71]; while the current LCOE of crystalline silicon solar
modules are 32 ¢/kWh [77]. One big concern is the accuracy of the
estimated lifetime of PSMs, because there are only limited litera-
ture reported the long-term stability of PSMs [78e80]. Besides, only
Espinosa et al. analyzed the life cycle of PSCs in 2015 [81].

Fig. 9. Cost distribution of materials (80% materials usage ratio has been considered) for (a) Module A and (b) Module B; (c) PSMs cost as a function of module efficiency, and (d) the
relationship between LCOE and lifetime [52].
 Z. Yang et al. / J Materiomics 3 (2017) 231e244 241

Therefore, much more efforts should be devoted to improve the solar cells; and they assumed that PSCs can be used as top cells in
efficiency and lifetime of PSMs, which will benefit for lowering tandem cells. Moreover, efficiencies of 43.7% (4T) and 41.6% (2T) can
their LCOE level. be achieved using the top junctions with an absorptance of 82% to
achieve current matching (for CH3NH3PbI3 based cell) [88]. Lee
et al. studied halide perovskites for tandem solar cells [90] and
4. Application directions of perovskite solar modules
emphatically discussed the tandem PSCs combined with other
kinds of solar cells such as organic, silicon, and Cu(In,Ga)(S,Se)2
PSMs is very promising to be applied as building integrated
(CIGS) solar cells. The key issues in device design were also
photovoltaics (BIPV) benefiting from the tunable transparency of
described, like optical management, electrodes fabrication (with
hybrid perovskite thin films. In particular, semi-transparent PSMs
high transparency) and performance improvement of single junc-
are strongly desired to replace a lot of architectural elements
tion PSCs in large area [89]. Forg
acs et al. reported the efficient
commonly made of glass while tradition silicon solar modules are
monolithic perovskite/perovskite tandem solar cells with an
lack of visual comfort [82]. Similar with the practical application of
average efficiency of 15% [90]. In their design, a wide bandgap
dye sensitized solar modules exhibited in Fig. 10(b) [83], PSMs can
(~2 eV) perovskite of Cs0.15FA0.85Pb(I0.3Br0.7)3 was adopted as the
also be used for semi-transparent windows and walls in a building.
absorber for front sub cell and the perovskite CH3NH3PbI3 (with a
Up to now, several neutral colors of perovskite thin films have been
bandgap of ~1.5 eV) as the absorber for rear sub cell [91]. In addi-
reported. As shown in Fig. 10(a), Eperon et al. prepared semi-
tion, the carrier recombination at the interfaces of perovskites was
transparent perovskite film on glass substrate [84]. Another
restrained by employing doped organic semiconductors
important application direction for PSMs is the tandem solar cells
(N4,N4,N40 ,N40 -tetra([1,10 -biphenyl]-4-yl)-[1,1’:40 ,10 -terphenyl]-
with other cells. Fig. 10(c) exhibited a typical example of perovskite/
4,40 -diamine doped with 2,2’-(perfluoronaphthalene-2,6-
silicon tandem module [85]. It is an important application direction
diylidene)) dimalononitrile for hole transport layer (HTL) and the
of PSCs with its relative high current property. So far, the highest
fullerene C60 doped with N1,N4-bis (tri-p-tolylphosphoranylidene)
efficiency for perovskite/silicon tandem solar cells is 23.6% in re-
benzene-1,4-diamine for the electron transport layer (ETL) [90].
cord [86].
Another notable advantage of PSCs or PSMs is the low temper-
Lal et al. summarized the efficiency evolution of different kinds
ature solution processing. Therefore, PSMs can be fabricated by roll-
of tandem solar cells involving PSCs (Fig. 11) [87]. Among them, 2T
to-roll (R2R) printing manner on flexible substrates. Flexible PSMs
and 4T refer to two-terminal and four-terminal tandem configu-
can be applied widely in wearable electronic devices and portable
rations, respectively. Recently, Rühle et al. studied the detailed
energy resources in both military and civil fields, as shown in
balance limit of perovskite/silicon and perovskite/CdTe tandem

Fig. 10. (a) Photograph of a typical semitransparent perovskite film formed on glass [84]. (b) Dye sensitized solar modules applied for semi-transparent windows in a building [83].
(c) A perovskite/silicon tandem module schematic illustration [85]. (d) Photograph of PSMs application in were able smart watch [91]. (e) Photograph of aeronautic applications of
PSMs working outdoor flight [92].
242 Z. Yang et al. / J Materiomics 3 (2017) 231e244
Fig. 11. Efficiency evolution of tandem solar cells involving PSCs [87].
Fig. 10(d) and (e), respectively [91,92]. Kim et al. obtained a flexible
PSCs with an efficiency of 12.2% (the device structure:PEN/ITO/
TiOx/CH3NH3PbI3-xClx/Spiro-OMeTAD/Ag) and observed a stable
device performance up to 1000 bending cycles with 10 mm of
bending radius [91]. Yoon et al. reported a pin flexible perovskite
device on PEN substrate, sputtered ITO as bottom electrode, spin-
coated PEDOT:PSS as HTL, evaporated C60 and BCP as ETL and
evaporated Al as counter electrode, achieving the highest perfor-
mance 17.3% so far [93]. For better bendability, they replaced the
brittle ITO with graphene and get almost the most excellent flexi-
bility among all the flexible PSCs with a high PCE of 16.8% [93]. In
2015, Schmidt et al. reported the first fully R2R compatible flexible
PSCs with a PCE of 4.9%; all the layers (PET/ITO/PEDOT:PSS/
CH3NH3PbI3-xClx/PCBM/ZnO/Ag) were slot-die coating one by one
on the ITO/PET foil, expect the Ag electrode, which was evaporated
in a vacuum chamber [94]. It is an important step of flexible PSCs
toward industrial production. Flexibility can help PSMs to take up
the complementary market beyond the mature crystalline Silicon
solar cells, which the new-born photovoltaic technologies is hard to
compete in their early stage.
5. Conclusion
In this paper, the recently developed strategies for the prepa-
ration of large-area perovskite thin films and solar modules have
been overviewed, which is important for further development of
perovskite photovoltaic technology towards industrialization. The
large-area perovskite thin film preparation techniques, including
spin coating, casting, blade coating, spray coating and slot-die
coating, have been summarized. Their technical features, advan-
tages and disadvantages have been comprehensively compared and
discussed. In view of the perovskite crystallinity, film uniformity,
technical reproducibility, economic and environmental friendli-
ness, it is thought that slot-die coating is the most promising
method for the preparation of large-area perovskite thin film.
Though, the device performance based on this method still need to
be largely improved. With respect to the fabrication of large-area
PSMs, the series interconnection and the parallel interconnection
have different advantages and disadvantages. The series connection
can increase the Voc of PSMs and minimize the drop in module
efficiency induced by the enhancement of series resistance.
However, an ideal precision to match Jsc of single cells is still diffi-
cult to be satisfied. PSMs connected in parallel always exhibit
substantial loss of current due to the additionally introduced metal
grids on the TCO glass substrates. Up to now, the series inter-
connected PSMs were more frequently reported than the parallel
interconnected ones.
It is believed that once the certified efficiency for large-area
PSMs catch up with that of crystalline Si solar cells (for example,
PCE >18% at module size of >100 cm2), and meanwhile, the cost and
stability for these PSMs are proved to be competitive, PSMs will be
widely used in our lives. It can be expected, in the very beginning,
thought the stability of PSMs has not been fully resolved, PSMs can
still find some marketplace that is different from conventional Si
solar cells.
Acknowledgements
This work was financially supported by the National Natural
Science Foundation of China (51672094, 51661135023), the Na-
tional Key R&D Program of China (2016YFC0205002), the Self-
determined and Innovative Research Funds of HUST (2016JCTD111),
the open research funds of Engineering Research Center of Nano-
Geo Materials of Ministry of Education, China University of Geo-
sciences (NGM2017KF013).
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Zhichun Yang obtained his B.S. degree in physics in 2014
from Yun Cheng University, China, and his M.S. degree in
condensed matter physics in 2017 at Huazhong University
of Science and Technology, China. He is currently a Ph.D.
candidate in Wuhan National Laboratory for Optoelec-
tronics of Huazhong University of Science and Technology.
His research mainly focuses on large-area perovskite solar
cells and modules.
Shasha Zhang received her Ph.D. degree in Material Sci-
ence from Huazhong University of Science and Technology
in 2016. She currently is a postdoctoral fellow at Wuhan
National Laboratory for Optoelectronics, Huazhong Uni-
versity of Science and Technology. Her research activities
focuses on the charge transport mechanism and stability
of perovskite solar cells.
Lingbo Li is currently a M.S. candidate under supervision
of Prof. Wei Chen at Wuhan National Laboratory for Op-
toelectronics and China-EU Institute for Clean and Renew-
able Energy, Huazhong University of Science and
Technology. She received her B.S. degree from department
of Mathematics and Physics, Suzhou University of Science
and Technology in 2016. Her research focuses on flexible
perovskite solar cells.
Wei Chen received his B.S. and Ph.D. degree from
Department of Materials Science and Engineering in
Tsinghua University. He worked as postdoctoral fellow-
ship in Department of Chemistry in Hong Kong University
of Science and Technology from 2008 to 2010. He was a
visiting scholar in National Institute for Materials Science
in Japan from 2014 to 2015. He is currently a professor in
Wuhan National Laboratory for Optoelectronics of Huaz-
hong University of Science and Technology. His research
interests cover the synthesis, understanding, and appli-
cations of functional nanomaterials and semiconductor
thin films in next generation solar cells, including perov-
skite solar cells, dye and quantum dot-sensitized solar
cells, and printable low-cost solar cells.