Chemical Physics Letters 807 (2022) 140084

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Chemical Physics Letters

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

Solvent engineering in inkjet-printed perovskite solar cells

Han Yang a, Jize Wang a, Xinxin Yu a, Yishuai Feng a, Xiao Chen a, Fei Long b, Zhiliang Ku a,
Fuzhi Huang a, Yibing Cheng a, Yong Peng a, *
a
State Key Laboratory of Advanced Technology for Materials Synthesis andProcessing, Wuhan University of Technology, Wuhan 430070, Hubei, China
b
College of Materials Science and Engineering, Guilin University of Technology, Guilin 541004, Guangxi, China

A R T I C L E I N F O A B S T R A C T

Keywords: Inkjet printing is a sterling technique in the fabrication of large-scale perovskite solar cells (PSCs). Whereas, to
Inkjet printing obtain high quality perovskite films remains challenging because of the control of the drying of droplets. In this
Perovskite solar cells work, FAI is totally dissolved in n-Butanol and isopropanol (IPA) to react with PbI2/CsBr films. The addition of n-
Solvent engineering
Butanol prolongs the drying time and inhibits the contact line pinning. Accordingly, the inkjet-printed CsxFA1-
xPb(IyBr1-y)3 perovskite films show great uniformity with large grain size. We ultimately achieve a champion
device with a power conversion efficiency (PCE) of 18.26 % (0.15 cm2).

1. Introduction influence in printing and other solution-based devices fabrication, but

Perovskite solar cells (PSCs) have demonstrated enormous potentials
over past years [1–10]. Power conversion efficiency (PCE) of PSCs has
rocketed from 3.8 % to 25.7 % since 2009. Particularly, the metal-halide
perovskites have been regarded as sensational materials for light har­
vesting due to its especial properties including high absorption coeffi­
cient, perfect charge carrier mobility, controllable energy band gap, and
relatively low-cost preparation [11,12].
Deposition methods are necessary for the fabrication of PSCs to get
high efficiency and favorable stability. Multifarious technologies could
be applied to manufacture large-scale and homogeneous films instead of
spin-coating, such as vacuum deposition, doctor-blade coating, slot-die
coating, spray coating and inkjet printing [13–22]. Among these tech­
niques, inkjet printing supports that active materials precursor ink could
be deposited at concrete temperature on specific areas of the substrate
[23–25]. Moreover, inkjet printing provides infinite print resolution
owing to the adjustable drop spacing which ranges from 5 μm to 80 μm.
The drop-by-drop printing is able to achieve the custom shapes. Since
inkjet printing was first used in the fabrication of PSCs, PCE of inkjet-
printed devices has risen from 11.6 % to 21.6 % [26,27]. Neverthe­
less, only few researches have been reported to fabricate MA-free PSCs
via using inkjet printing while MA-free PSCs emerge perfect photovol­
taic performance [28].
Perovskite films of high quality are required for high-efficiency PSCs.
Regulating the deposition morphology of droplet has an important
drying of droplets is a complex and non-equilibrium process [29,30].
Further studies indicate that inner flows, including capillary flow and
Marangoni flow, dynamics of three-phase contact line, and parti­
cle–particle/particle-interface interaction will influence ultimate parti­
cle distribution in the inhomogeneous redistribution [31]. The addition
of solvent with high boiling point and low surface tension will result in
the better film quality [32,33].
How to obtain homogeneous liquid films before annealing is a
pivotal factor for inkjet-printed high-performance PSCs. In preceding
studies, to adjust ink composition has been identified as the most
convenient strategy to affect the film quality [34]. Liang etal. achieved
the high-quality large area perovskite films by inkjet printing [35]. A
mixed DMSO/GBL was used as the printing precursor solvent. High
performance PSCs based on one-step inkjet printing with a PCE of 17.04
% for 0.04 cm2 were demonstrated. Li etal. systematically studied the
properties of DMF and DMSO mixed solvents through the perovskite
grains growth [36]. Because of the difference in viscosity and boiling
point, the high proportion of DMSO solvents spread slowly which led to
smaller printing dots. It permitted PSCs with PCEs of 18.64 % for a small
area (0.04 cm2) and 17.74 % for a large area (2.02 cm2). Li etal. estab­
lished a new mixed ink system that could effectively delay the crystal­
lization rate of perovskite grains [37]. The introduction of N-methyl-2-
pyrrolidone (NMP) could prolong the maintaining time of liquid films
owing to its properties to reduce the gas partial pressure and increase the
boiling point of the solvent, leading to an uniform

* Corresponding author.
E-mail address: yongpeng@whut.edu.cn (Y. Peng).

https://doi.org/10.1016/j.cplett.2022.140084
Received 3 June 2022; Received in revised form 12 September 2022; Accepted 24 September 2022
Available online 28 September 2022
0009-2614/© 2022 Elsevier B.V. All rights reserved.
H. Yang et al.
Cs0.05MA0.14FA0.81PbI2.55Br0.45 perovskite film. The inkjet-printed PSCs
with NMP attained high PCEs of 19.6 % (0.04 cm2) and 17.9 % (1.01
cm2).
In our work, a mixed ink composition is created and applied in the
fabrication of inkjet-printed MA-free PSCs. Thermal evaporation and
inkjet printing are combined to prepare high quality perovskite films.
The precursor ink consisting of FAI/IPA and n-Butanol is deposited to
PbI2/CsBr solid films via inkjet printing. Owing to the higher boiling
point and lower gas partial pressure of n-Butanol additive, FAI particles
don’t tend to accumulate at the droplet edges during drying. The reac­
tion between FAI and PbI2/CsBr is more adequate due to the prolonged-
drying-time of liquid film, which leads to an eventual uniform perov­
skite film. The PCE of our champion device reaches 18.26 % (0.15 cm2),
and keeps the primary PCE in 90 % exposed to air after 20 days. Our
mixed solvents system could be regarded as a feasible solution to
enhance the film quality, and this technique including inkjet printing
provides an effective strategy to achieve PSCs with good performance
for future application.
2. Experimental section
2.1. Materials
FTO substrates (standard size: 200 × 150 × 2.2 mm3, square resis­
tance: 15 ohms/sq, transmittance: > 90 %) were purchased from Wuhan
Ge’ao Science and Education Instrument Co., ltd. SnCl2 • 2H2O, urea and
all alcohols were bought from Aladdin. Cesium bromide (CsBr), Lead
iodide (PbI2) and formamidinium iodide (FAI) were all bought from
Xi’an Polymer Light Technology Corp. Spiro-OMeTAD was purchased
from Shenzhen Feiming Science and Technology Co., ltd. Other all
chemicals were purchased from Sigma-Aldrich. All materials were used
as received without any purification.
2.2. Preparation of solutions
SnCl2 • 2H2O solution was prepared via following steps: 6 g of urea,
120 µL of mercaptoacetic acid and 6 mL of HCl (38 wt%) were dissolved
in 400 mL of deionized water. Then 1.1 g of SnCl2 • 2H2O was totally
dissolved in the as-prepared solution and stored below 0 ℃. For the FAI
solution, we added n-Butanol to the FAI/IPA solution (21 mg of FAI was
dissolved in 1 mL of alcohol) in the ratio of 0 %, 5 %, 10 %, and 15 % by
volume.
Spiro-OMeTAD solution was prepared via following steps: 76 mg of
Spiro-OMeTAD,30 µL of FK209 stock solution (290 mg/mL FK209-Co
(III)-TFSI in acetonitrile), 20 µL of Li-TFSI stock solution (500 mg/mL
lithium bis trifluoromethylsulfonyl imide in acetonitrile), and 30 µL of 4-
tert-butyl-pyridine were dissolved in 1 mL of chlorobenzene.
2.3. Perovskite solar cells fabrication
FTO substrates were washed thoroughly with detergent, deionized
water, and ethanol for 30 min. Then, they were dried and treated under
UV-ozone for 20 min. The SnO2 films were prepared by using chemical
bath deposition (CBD) method. FTO substrates were soaked in SnCl2 •
2H2O solution for 3 h at 90 ◦ C. Then they were washed with deionized
water and dried with air gas flow. Process above was duplicated twice to
obtain the desired thickness. The films prepared were thermal treated at
180 ◦ C for 1 h.
For perovskite, 280 nm of PbI2 and 30 nm of CsBr were deposited to
the SnO2-deposited substrates by thermal evaporation. Then, the FAI
solution as prepared was directly filled in ink cartridge of Dimatix
Fujifilm DMP-2800 printer at room temperature. For our best inkjet-
printing recipe, the drop spacing was controlled at 60 μm and printing
cycles were set at 6. After inkjet printing, films as prepared were thermal
treated on hotplate at 170 ℃ for 1 h to generate perovskite. After cooling
down to room temperature, Spiro-OMeTAD was spin-coated onto the
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Chemical Physics Letters 807 (2022) 140084
inkjet-printed perovskite films at 3000 rpm for 30 s. Eventually, the
electrode (80 nm of gold) was deposited onto the Spiro-OMeTAD layer
through thermal evaporation. All PSCs were investigated under AM 1.5
G sun light (100 mW/cm2) with a scan rate of 10 mV/s. Each device was
measured via using a metal mask of 0.384 × 0.384 cm2.
3. Results and disscussions
Fig. 1a shows the thermal evaporation/inkjet printing strategy to
prepare CsxFA1-xPb(IyBr1-y)3 perovskite films. In order to form perov­
skite, the metal halides (PbI2/CsBr) were deposited to SnO2-covered
FTO substrates via thermal evaporation in the glove-box, then FAI so­
lutions were deposited to the as-prepared PbI2/CsBr films in air condi­
tions (more details in Experimental section). FAI could be totally
dissolved in some alcohols (such as IPA, n-Butanol, and 1-Pentanol).
These solvents possess excellent wettability on PbI2/CsBr surface.
Table S1 shows some necessary properties of these alcohols. We suppose
that solvent with higher boiling point can decrease the drying rate to
help attain uniform perovskite film. The SEM images of perovskite films
using different alcohols (IPA, n-Butanol, and 1-Pentanol) are shown in
Figure S1. Accordingly, J-V curves of PSCs are shown in Figure S2, and it
can be found that the film quality does not improve and PCE of PSC
doesn’t increase while using pure n-Butanol and 1-Pentanol. Table S2
shows the photovoltaic parameters of corresponding PSCs. We can see
that the PSC with IPA exhibits the highest PCE of 17.25 %. Based on our
results, a balance should be explored to enhance the film quality. Thus,
we select to introduce proper amount of n-Butanol in the FAI solution to
prolong the drying time.
The strong volatilization of IPA is an obstacle in our work. Compared
to IPA (bp = 83 ℃, gp = 4.404 kPa), n-Butanol has a higher boiling point
(bp = 117 ℃) and lower gas partial pressure (gp = 0.567 kPa). Pre­
dictably, the droplets with n-Butanol maintain mobility after being
deposited to the substrates, resulting fewer solutes accumulation.
Further, FAI particles will react with PbI2/CsBr more than diffusion
motion, which leads to the decrease in the number of FAI particles
pinned to edges. The schematic evolution of droplets we suppose are
shown in Fig. 1b, FAI particles immediately move to edges of the
droplets (IPA) after being deposited, resulting the solutes accumulation.
Generally, the FAI droplet dries much faster than it to merge with each
other, which ultimately leads to the structure in Fig. 1(b). In contrast,
while adding some n-Butanol to increase the boiling point, the droplets
(IPA and n-Butanol) with lower evaporation rate will emerge a homo­
geneous solutes distribution in Fig. 1(c).
In order to investigate the balance between IPA and n-Butanol, n-
Butanol was added in the volume ratio of 0 %, 5 %, 10 % and 15 % to the
FAI/IPA solution. Without introducing n-Butanol, perovskite wet film
using IPA dried no more than 2 seconds. Further, perovskite wet films
with the introduction of 5 %, 10 % and 15 % n-Butanol dried after 4 ~ 5
seconds. The prolonged drying time would lead to a homogeneous FAI
distribution.
From Fig. 2, it can be found that different samples demonstrate
similar surface morphology. The stains with a diameter of up to 50 μm
could be easily observed everywhere in Fig. 2(a). With the addition of
10 % n-Butanol, we find that those stains are nearly eliminated in Fig. 2
(c). However, perovskite film with the addition of 15 % n-Butanol in
Fig. 2(d) emerges lots of defects, which indicates that too much n-
Butanol breaks the balance between IPA and n-Butanol.
Fig. 3(a-d) is the corresponding scanning electron microscope (SEM)
images of the inkjet-printed perovskite films fabricated with different
amount of n-Butanol additive. Small marked particles can be apparently
seen in Fig. 3(a). In Fig. 3(b-d), those small particles disappear accord­
ingly, which could be evident that based on our mixed solvents system,
higher film quality is achieved. From statistical analysis of perovskite
grain size, it could be found that the introduction of 10 % n-Butanol
could improve the most probable grain size in Figure S3. The average
grain size of perovskite films are 553 nm, 331 nm, 590 nm, 392 nm while
H. Yang et al. Chemical Physics Letters 807 (2022) 140084

Fig. 1. (a) Schematic diagram of inkjet-printed perovskite solar cells. (b, c) Schematic diagrams of drying process of individual droplet without and with n-Butanol.

Fig. 2. Optical microscope images of perovskite films based on different amount of n-Butanol. (a) 0 % n-Butanol; (b) 5 % n-Butanol; (c) 10 % n-Butanol and (d) 15 %
n-Butanol.

introducing 0 %, 5 %, 10 % and 15 % n-Butanol.
As shown in Fig. 3(e-h), the surface roughness of them are 40.4 nm
(0 % n-Butanol), 30.5 nm (5 % n-Butanol), 28.2 nm (10 % n-Butanol)
and 35.3 nm (15 % n-Butanol). The AFM images of our perovskite films
are in agreement with the SEM results, indicating that 10 % n-Butanol
additive contributes to the high-quality perovskite films.
Proper amount of n-Butanol additive in the fabrication of perovskite
films is critical to get high-performance PSCs. UV–vis absorption spectra
was used to investigate the effect of n-Butanol on the light absorption of
perovskite films as prepared. All perovskite films perform high
absorption ability in Fig. 4(a). According to SEM and AFM results, the
introduction of n-Butanol helps improve the film quality. From Fig. 4(b)
we know that the highest absorption of perovskite film can be achieved
when 10 % n-Butanol additive is introduced.
The reaction between PbI2/CsBr and FAI directly influence the
perovskite film quality and PSC performance. To confirm the total
conversion of PbI2 remains a challenge in sequential deposition method.
As shown in Fig. 4(c), the crystallinity of the perovskite films was
measured by X-ray diffraction (XRD). All of the perovskite films display
similar crystal structures with (001), (002) and (012) diffraction peaks

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H. Yang et al. Chemical Physics Letters 807 (2022) 140084

Fig. 3. (a-d) SEM images and (e-h) AFM images of printed perovskite films based on different amount of n-Butanol. (a, e) 0 % n-Butanol; (b, f) 5 % n-Butanol; (c, g)
10 % n-Butanol and (d, h) 15 % n-Butanol.

Fig. 4. (a) UV–vis spectra of perovskite films based on different amount of n-Butanol. (b) Corresponding enlarged patterns of perovskite films at the range from 700
nm to 850 nm. (c) XRD patterns of perovskite films based on different amount of n-Butanol. (d) Corresponding enlarged patterns of perovskite films at the angle from
10.0◦ to 15.0◦ .

4
H. Yang et al.
centered at 14.0◦ , 28.2◦ , and 31.7◦ . Besides, we find that PbI2 is nearly
non-existent because of the tiny diffraction peak located at 12.7◦ in
Fig. 4(d), which means that most of PbI2 has converted to CsxFA1-xPb
(IyBr1-y)3.
The photovoltaic performance of corresponding PSCs was ascer­
tained by measuring the current–voltage (J-V) curves and evaluating the
external quantum efficiency (EQE) spectra. Table S3 summarizes the
major photovoltaic performance of PSCs measured under AM 1.5 G sun
light (100 mW/cm2). All devices were fabricated absolutely according to
the Experimental Section. The representative J-V curves of PSCs based
on different amount of n-Butanol are displayed in Fig. 5(a). We could
conclude that PSCs with 10 % n-Butanol additive exhibit superior per­
formances among all devices. PSCs fabricated with pure IPA give a PCE
of 16.95 ± 0.29 % with an open-circuit voltage (VOC) of 1.009 ± 0.018
V, a short-circuit current density (JSC) of 22.05 ± 0.24 mA/cm2 and a fill
factor (FF) of 0.722 ± 0.024. With 10 % n-Butanol additive, PSCs yield
an enhanced PCE of 18.00 ± 0.24 % with a VOC, JSC and FF of 1.001 ±
0.014 V, 22.63 ± 0.21 mA/cm2 and 0.765 ± 0.017. Owing to the
enhanced quality of perovskite films with enlarged grain size and
improved surface uniformity, the devices with 10 % n-Butanol additive
exhibit the superior performance. Further, the external quantum effi­
ciency (EQE) spectra of corresponding devices are displayed in Fig. 5(b).
The device with 10 % n-Butanol additive has the integrated current
density of 21.73 mA/cm2, exceeding that for the device with pure IPA
(21.18 mA/cm2).
In order to test the effect of introducing n-Butanol on photo-
generated carriers in our inkjet-printed perovskite films, steady-state
photoluminescence (PL) and time-resolved photoluminescence (TRPL)
measurements were applied. Considering that devices with 10 % n-
Butanol show the best performance, we mainly focus on studies of the
best device and the sample device. As shown in Fig. 6(a), it could be
clearly found that the intrinsic fluorescence emission peak of the
perovskite film with 10 % n-Butanol demonstrates a higher intensity.
The promoted PL intensity indicates that the non-radiative recombina­
tion rate reduces in our perovskite films. In Fig. 6(b), TRPL results
demonstrate that photo-generated lifetime of our perovskite films with
10 % n-Butanol (τ = 88.7 ns) has increased compared to the perovskite
films without n-Butanol (τ = 32.5 ns).
Figure S4 demonstrates the cross-sectional images of PSCs with and
without 10 % n-Butanol additive. Less pinhole further verifies the
perovskite film of high quality with 10 % n-Butanol additive is achieved
in comparison with perovskite with pure IPA. Fig. 6(c) illustrates the
photovoltaic parameters of champion devices with and without 10 % n-
Butanol. It can be concluded that the increase of JSC and FF result in the
Fig. 5. (a) Representative J-V curves of PSCs based on different amount of n-Butanol additive. (b) Corresponding EQE spectra of PSCs.
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Chemical Physics Letters 807 (2022) 140084
enhancement of the PCE. Ultimately, PCE of our champion device rea­
ches 18.26 %. From Table S4 we can find that our work is the first study
about inkjet-printed MA-free PSCs with PCE exceeding 18 %. To inves­
tigate the effect of 10 % n-Butanol additive on stability of devices, PSCs
without encapsulation were stored at dark air conditions (~25 ℃, < 30
% relative humidity). As Fig. 6(d) illustrates, PSC with 10 % n-Butanol
additive maintains over 90 % of its initial PCE after 20 days, while de­
vice with pure IPA maintains 70 % of its initial PCE. This result indicates
that the stability of our PSC can be promoted owing to the less pinhole
and defects in cross-sectional SEM images. From the analysis above, we
could attribute the enhanced photovoltaic performance of PSCs to the
better quality of perovskite films.
4. Conclusions
In summary, in order to eliminate the negative effect of the strong
volatilization of IPA, we established a simple mixed-solvents strategy to
promote the quality of perovskite films. During the fabrication of
perovskite films, n-Butanol was added in the FAI/IPA solution. The
advantages of mixed solvents provided great spreading of the solution.
Besides, the adequate reaction between FAI and PbI2/CsBr confirmed
the total conversion of PbI2. Hence, our perovskite films exhibited better
crystallinity, higher light absorption coefficient, and longer carrier
lifetime while 10 % n-Butanol additive was introduced. Finally, we
achieved the champion device with a PCE of 18.26 %. This mixed-
solvents system could be applied in inkjet-printed devices for future
commercialization.
CRediT authorship contribution statement
Han Yang: Investigation, Writing – review & editing, Visualization,
Data curation. Jize Wang: Investigation, Data curation. Xinxin Yu:
Investigation, Data curation. Yishuai Feng: Conceptualization. Xiao
Chen: Conceptualization. Fei Long: Investigation, Validation, Supervi­
sion, Project administration, Funding acquisition. Zhiliang Ku: Inves­
tigation, Validation, Supervision, Project administration, Funding
acquisition. Fuzhi Huang: Investigation, Validation, Supervision, Proj­
ect administration, Funding acquisition. Yibing Cheng: Investigation,
Validation, Supervision, Project administration, Funding acquisition.
Yong Peng: Investigation, Validation, Supervision, Project administra­
tion, Funding acquisition.
H. Yang et al.
Fig. 6. (a) PL spectra and (b) TRPL spectra of the perovskite films with and without 10 % n-Butanol additive. (c) J-V curves of champion devices. (d) Stability test of
the PSCs without encapsulation stored under dark air conditions (~25 ◦ C, < 30 % relative humidity).
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Data availability
No data was used for the research described in the article.
Acknowledgements
This work was supported by the National Key Research and Devel­
opment Program of China (2018YFB1500104), the National Natural
Science Foundation of China (U20A20245 and U21A20171) and the
Technological Innovation Key Project of Guangdong Province
(skjtdzxrwqd2018005).
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