Research Article
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Environmental-Friendly Polymer for Efficient and Stable
Inverted Perovskite Solar Cells with Mitigating Lead Leakage
Qi Cao, Tong Wang, Jiabao Yang, Yixin Zhang, Yuke Li, Xingyu Pu, Junsong Zhao, Hui Chen,
Xiaoqiang Li, Ilhom Tojiboyev, Jiangzhao Chen,* Lioz Etgar, and Xuanhua Li*
Although perovskite solar cells (PSCs) are on the road to industrialization,
the operational stability under high efficiency still needs to be improved, and
the water solubility of lead ions (Pb2+) will cause environmental pollution
problems. Herein, it is successfully implanted an environment-friendly
(biodegradability) poly(butylene adipate-coterephthalate) polymer (PBAT)
into the perovskite film, which can passivate the uncoordinated Pb2+ and
neutral iodine defects of the perovskite material because of the adequate
carbonyl groups and benzene rings in PBAT polymer, thereby regulating
the crystallization of perovskite film with lower trap density, inhibiting
the nonradiative recombination and improving charge carrier transport.
As a result, the polymer-incorporated inverted PSCs achieve optimal
conversion efficiencies of 22.07% (0.1 cm2) and 20.31% (1 cm2). Meanwhile,
the incorporated device, after being encapsulated, exhibits a prominent
improvement in operational stability of high-efficiency device under
maximum power point tracking and continuous one sunlight illumination,
maintaining the initial efficiency of 80% for 3249 h. More importantly, the
polymer network can protect Pb2+ from being dissolved by water and prevent
nearly 98% of Pb2+ from leaking by directly immersing the polymer-coated
perovskite film in water. Environmental-friendly molecules provide new hope
for solving lead poisoning and improving device operational stability under
high efficiency.
1. Introduction
The accredited power conversion efficiency (PCE) of normal
and inverted lead (Pb) halide perovskite solar cells (PSCs) is as
high as 25.7%[1] and 22.3%,[2] respectively, which is comparable
Q. Cao, T. Wang, J. Yang, Y. Zhang, X. Pu, J. Zhao, H. Chen, X. Li, X. Li
State Key Laboratory of Solidification Processing
Center for Nano Energy Materials
School of Materials Science and Engineering
Northwestern Polytechnical University
Xi’an 710072, China
E-mail: lixh32@nwpu.edu.cn
Y. Li
Department of Chemistry and Centre for Scientific
Modeling and Computation
Chinese University of Hong Kong
Shatin, Hong Kong, China
The ORCID identification number(s) for the author(s) of this article
can be found under https://doi.org/10.1002/adfm.202201036.
DOI: 10.1002/adfm.202201036
Adv. Funct. Mater. 2022, 32, 2201036 2201036  (1 of 11)
to other market-oriented photovoltaic tech-
nologies, including polycrystalline silicon
(p-Si) and cadmium telluride (CdTe), and
so forth. Having demonstrated such a high
PCE reflects that it is no more a major
stumbling block to the commercialization
of PSCs. Therefore, the focus of research
on this subject has steadily turned to the
perovskite phase transition mechanism[3]
and the stability of PSCs under environ-
mental conditions, light, and thermal
stresses.[4] Through the application of
defect passivation and interfacial modifi-
cations,[4–7] composition and crystal engi-
neering,[8–9] encapsulation technology,[10]
electrode,[11] and transport layer selec-
tions,[12] the lifetime of the device can be
extended by eliminating external ambient
pressure. Nevertheless, the long-term
operational stability of PSCs under high
efficiency has not yet been achieved, which
is still a key obstacle to be overcome before
wholescale marketization.
Another issue is about the lead leakage
of PSCs. The solubility product constant
(Ksp) of CdTe in water is lower than 10−30,
posing a lower solubility and lower toxicity
risk to the environment. Compared with thermal-chemically
stable CdTe, lead halide in perovskite has higher water solu-
bility (Ksp exceeds 10−8 in rainwater).[13–16] Inhalation of Pb2+ in
the human body will cause damage to the tissues and nervous
system. Hence, it is critical to find ways to effectively eliminate
I. Tojiboyev
Institute Ion-Plasma and Laser Technologies
Uzbekistan Academy of Sciences
Durmon yuli 33, Tashkent 100125, Uzbekistan
J. Chen
Key Laboratory of Optoelectronic Technology & Systems
(Ministry of Education)
College of Optoelectronic Engineering
Chongqing University
Chongqing 400044, China
E-mail: jiangzhaochen@cqu.edu.cn
L. Etgar
Institute of Chemistry
Casali Center for Applied Chemistry
The Hebrew University of Jerusalem
Jerusalem 91904, Israel
© 2022 Wiley-VCH GmbH

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or minimize Pb2+ leakage, so that PSCs can be used in practical
applications. At present, two-dimensional metal-organic frame-
work,[17] cation-exchange resin,[18] and self-healing polymers[16]
have achieved good results in solving the problem of Pb2+
leakage, which is of reference significance. As far as we know, it
is known that some polymer additives with Lewis base groups
can also act as Pb chelating agents to passivate deep-level
defects, thereby improving the performance of PSCs. Common
polymers, including poly(acrylic acid),[19] poly(acrylamide),[20]
poly(acrylonitrile),[21] and so forth. have poor (bio)degradability,
which has a destructive effect on the environment. There is an
urgent need to find environmental-friendly modifiers, that can
not only effectively reduce the Pb dissolution of perovskites, but
also enhance photovoltaic performance.
Here, we chose the environmental-friendly poly(butylene
adipate-coterephthalate) polymer (PBAT, Figure 1a)[22] to
implant the perovskite film with the anti-solvent method.
The PBAT polymer is a biodegradable plastic, which specifi-
cally refers to a type of plastic that is degraded by the action
of naturally occurring microorganisms such as bacteria, molds
(fungi), and algae, and has environmental protection proper-
ties. The PBAT polymer has repeated carbonyl groups and ben-
zene rings, which can simultaneously passivate the various trap
sites of perovskite material, including non-coordinating Pb2+
and neutral iodine, as shown in Figure  1b, thereby strongly
regulating the crystallization of perovskite film with lower
trap density, inhibiting the nonradiative recombination and
improving charge carrier transport. Consequently, the incorpo-
rated inverted PSCs achieve enhanced conversion efficiencies
of 22.07% from 19.17% (control device). Meanwhile, the incor-
porated device after being encapsulated exhibits a prominent
improvement in operational stability for the high-efficiency
device under maximum power point tracking and continuous
sunlight, maintain the initial efficiency of 80% for 3249 h. More
importantly, the polymer network can protect Pb2+ from being
dissolved by water and prevent nearly 98% of Pb2+ from leaking
by directly immersing the polymer-coated perovskite film in
water.
2. Results and Discussion
Density functional theory (DFT) was used to analyze the elec-
trostatic potential of the smallest unit of PBAT polymer using
the B3LYP method and Ahlrichs’ split-valence def2-SVP basis
set. Figure  1c shows that the red region is located at the car-
bonyl (CO) position in the PBAT polymer, indicating a nega-
tive electrostatic potential with higher electron density, which
provides a favorable position for the coordination with Pb2+
cations. We further performed Fourier transform infrared
(FTIR) to explore the interaction of the PBAT polymer with
PbI2 (Figure 1d). The position of the CO bond peak of PBAT
polymer is 1709.4 cm−1. When the PBAT polymer is mixed with
PbI2, it moves to 1702.6 cm−1. The CO stretching vibration
has a 6.8 cm−1 redshift, signalizing that a chelating force exists
between CO in the PBAT polymer and non-coordinating Pb2+.
We next used PBAT-I2-dichloromethane (CH2Cl2) to investigate
the possible interaction of benzene rings and neutral iodine
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(I2) (Figure  1e).[23] I2 has a sharp absorption peak at 227  nm
and the PBAT polymer has an absorption peak at 239 nm due
to the π→π* transition of the conjugated double bond of the
benzene ring. When the PBAT polymer is mixed with I2, the
sharp peak of I2 is blue-shifted and the absorption peak of ben-
zene ring is red-shifted, which can prove that the benzene ring
of PBAT interacts with I2. A small amount of I2 defects appear
in perovskite films because I− in iodide powder or perovskite
precursor solution is easily oxidized to I2,[24] and the benzene
rings of PBAT polymer exhibit electron-donating properties
that may reduce the acceptor type trap states induced by dis-
sociative iodine.
To further determine the potential chemical interaction
between PBAT and CsMAFA (MA: CH3NH3+, FA: CH(NH2)2+)
based perovskite material, we conducted X-ray photoelec-
tron spectroscopy (XPS) measurements of the PBAT polymer,
control (pristine) and PBAT-incorporated perovskite films
(Figures 1f–i). Metallic Pb0 in the pristine film is located at 136.5
and 141.4 eV from the Pb 4f XPS spectra (Figure 1f). It may be
due to the presence of iodine defects in the perovskite crystal,
which results in a high degree of unsaturation of lead, giving
it a metallic appearance.[25] Metallic Pb0 acts as nonradiative
recombination sites that can dilapidate the PCE and stability
of devices.[26] Intriguingly, when the perovskite film is incor-
porated by the PBAT polymer, the metal Pb0 peak disappears,
reflecting that the PBAT polymer can avoid the formation of
metallic Pb0. The binding energy of Pb 4f also shifts 0.6 eV to
the lower binding energy in the PBAT-incorporated film. Mean-
time, the C-CO peak in C 1s is located at 285.4 eV (Figure 1g)
and the OC peak in O 1s is located at 531.8  eV in the PBAT
polymer (Figure  1h). However, the C-CO of the PBAT-incor-
porated perovskite film is close to 285.9  eV and the OC is
close to 532.3 eV, which forebodes that CO in the perovskite
film incorporated with PBAT polymer shifts to higher binding
energy. Combining Pb 4f and CO shifts proves the interaction
between the CO of PBAT polymer and the Pb2+ in perovskite
material. The I 3d XPS spectra (Figure  1i) moves to a lower
binding energy after modifying the PBAT polymer. These
results portend that the PBAT polymer has repeated carbonyl
functional groups (CO) and benzene rings, which can simul-
taneously passivate non-coordinating Pb2+ and neutral iodine in
the perovskite material.
The cross-sectional high-resolution transmission electron
microscopy (TEM) and energy-dispersive X-ray (EDX) map-
ping were further used to determine the specific location of the
PBAT polymer. The EDX mapping shows that the character-
istic O element of PBAT appears in the entire perovskite film
(Figure S1, Supporting Information). Due to the limited resolu-
tion of EDX mapping, we further analyzed the micro-regions
in the TEM image. The low-magnification TEM image shows
the PBAT cross-linked perovskite film, which can clearly distin-
guish the grain boundaries (GBs) between the perovskite grains
(Figure  1j). We analyze the two representative regions around
the GB: an ultra-thin amorphous layer appears at the GBs,
which is a PBAT polymer layer, playing the role of bridging
two adjacent perovskite grains. In addition, the perovskite lat-
tice fringes with an interplanar spacing of 0.63  nm are also
measured, which corresponds to (100) of the tetragonal phase
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Figure 1.  Interaction mechanism. a) The PBAT polymer’s chemical formula. b) A schematic illustration of the interaction between PBAT polymer and
perovskite material. c) DFT calculated electrostatic potential of the smallest unit of PBAT polymer (x = 1, y = 1) with isovalue 0.002. d) FTIR spectra of the
PBAT and PBAT-PbI2. e) Ultraviolet-visible (UV-Vis) absorption spectra of I2, PBAT, or PBAT+I2 dissolved in CH2Cl2 solvent, the inset is a schematic illus-
tration of the interaction between benzene ring and neutral I2 (The black ball represents C, the white ball represents H, and the purple ball represents I).
XPS spectra of f) Pb 4f, g) C 1s, h) O 1s, and i) I 3d without and with PBAT polymer. j) Cross-sectional transmission electron microscopy (TEM) images.

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of the CsMAFA crystal. The long-chain PBAT polymer inter-
acts with the perovskite material to form a polymer-perovskite
composite interconnection structure, which contributes to
decreasing the insulation or electrical decoupling between the
perovskite grains.[27]
Scanning electron microscope (SEM), atomic force micro-
scope (AFM), and X-ray diffraction (XRD) characterizations
were carried out to reveal the influence of PBAT on the mor-
phology of the perovskite film. From SEM images of the pris-
tine perovskite film (Figures 2a–b), clear PbI2 white phase[28]
and black phase perovskite materials can be observed. After
PBAT polymer modification, the grains of the perovskite film
become larger and the white phase is disappeared. In addition,
we count the size of perovskite crystals with or without
polymer. The average grain size (D) of the control is proxi-
mately 145  nm, whereas the D of PBAT-incorporated is larger,
approximately 246 nm (Figure 2c). We measured the root mean
square value of the perovskite surface by AFM and found that
the surface roughness is reduced from 10.3  nm of the control
to 8.7  nm of the PBAT-incorporated. PBAT polymer can make
the perovskite surface smoother and the crystal grains larger
(Figures  2d–f). Furthermore, the cross-sectional SEM shows
the disordered arrangement of crystal grains in the pristine
film (Figure S2, Supporting Information), while the perovskite
film incorporated with PBAT appears to have dense, larger
grains and a vertical arrangement, which facilitates carrier
transport. The control and PBAT-incorporated perovskite films
in Figure S3, Supporting Information show similar diffraction
patterns, corresponding to the typical black α-FAPbI3 phase.[29]
Compared with the XRD of control, the diffraction peak of the
PBAT polymer-modified perovskite film does not shift and the
PbI2 (2θ = 14.32o) peak disappears, manifesting that the PBAT
polymer does not affect the perovskite lattice and also sup-
presses the formation of PbI2. The PBAT polymer enters the
perovskite film through the anti-solvent and partially remains
on the perovskite surface, which can protect the perovskite

Figure 2.  Morphology analysis of perovskite film. Characteristics of the control and PBAT-incorporated films (0.1 mg mL−1). a–b) Scanning electron
microscope (SEM) images. c) The grain size statistical distribution of the SEM. d–e) AFM images. f) The height curves vary with distance are recorded
from the red solid line in the corresponding atomic force microscope (AFM) image. The in situ ultraviolet-visible spectra for the g) control and
h) PBAT-incorporated films during spinning procedures. i) UV-Vis absorption intensity of control and PBAT-incorporated perovskite films at 600 nm
varies with spinning time.

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film under annealing conditions and reduce the volatiliza-
tion of methylamine salts and formamidine salts. As shown
in Figure  1g, the content of CN and C–N in the XPS of the
PBAT-modified perovskite film increased, so that more
methylamine salts and formamidine salts participate in crystal-
lization, thereby reducing the segregation of PbI2 phase. More-
over, the PBAT-incorporated perovskite shows a narrower half-
width of the (100) peak (Figure S4, Supporting Information) and
an increase in the intensity ratio between the (100) and (110)
peaks (2.34 for the control and 5.96 for the PBAT-incorporated),
which indicates that PBAT promotes perovskite crystallization
and preferentially crystallizes in the (100) orientation. It is also
noted that the absorption of the PBAT-incorporated perovskite
film is enhanced, which is attributed to the higher grain size
(Figure S5, Supporting Information).
We employed in situ UV–vis spectrum to analyze the for-
mation process of perovskite film during spin-coating, so as to
better understand the effect of PBAT polymer on the crystalliza-
tion of perovskite thin films (Figure 2g–h).[30] During the spin-
coating process, we drop the anti-solvent in 25 s. The entire
procedure takes 40 s. After 40 s, it is equivalent to the crystal-
lization of perovskite in the air. Figure S6, Supporting Infor-
mation shows the change process of the absorption intensity
from the solution state to the intermediate state. In the solu-
tion state, the absorption intensity at 400 nm decreases slightly,
and the nucleation of perovskite is negligible. When the anti-
solvent is added dropwise, the absorption intensity of the
whole wavelength range begins to increase, and the perovskite
crystallites begin to form.[31] After 40 s, we draw the absorp-
tion intensity at 600  nm versus the rotation time (Figure  2i).
The slope factor of the control film is 0.0138, whereas the
PBAT-incorporated film is 0.0123. This result indicates that the
PBAT polymer delays the crystallization of the perovskite mate-
rial. Due to the interaction of PBAT polymer and uncoordinated
Pb2+ and neutral iodine in the perovskite film, the perovskite
crystallization course requests supererogatory energy to break
up these forces, so that the perovskite crystals crystallize in the
direction of small free energy, which significantly delays the
crystal growth.[32] This is conducive to the PBAT modified film
obtaining a larger crystal size, suppressing the content of unre-
acted PbI2, thereby promoting the formation of high-quality
perovskite, which is also confirmed by SEM and AFM.
We constructed inverted PSCs with the structure of indium
tin oxide (ITO) /NiOx (20  nm) /CsMAFA-based perov-
skite (750  nm) /[6,6]-phenyl-C61-butyric acid methyl ester
(PCBM)+C60 (45 nm) /bathophenanthroline (BCP, 10 nm) /Cr
(5nm)/Au (100 nm) to investigate the influence of PBAT incor-
poration on the photovoltaic characteristics of PSCs (Figure 3a).
Figure S7, S8, and Table S2, Supporting Information show the
statistical distribution, best-performing J–V (current density-
voltage) curves, and photovoltaic parameters of PSCs modi-
fied with different PBAT polymer concentrations. Therefore,
it can be determined that the optimal concentration of PBAT
polymer-modified PSCs is 0.1  mg mL−1. The control equip-
ment’s average PCE is 18.25 ± 0.72%, whereas the PBAT-incor-
porated equipment’s average PCE is enhanced to 21.09 ± 0.51%.
(Table S1, Supporting Information). With a small standard devi-
ation, the PSC with the optimal concentration of PBAT showed
excellent reproducibility. Next, we study the forward and reverse
scan of the control and PBAT-incorporated devices under the

Figure 3.  Device characterization. a) Structure of the inverted perovskite solar cells (PSCs). J–V curves of the best-performing for b) control and
c) PBAT-incorporated PSCs. d) Steady current-density and SPO values measured near maximum power point (MPP) for PSCs without and with PBAT
polymer. e) EQE spectra and integrated photocurrent of PSCs without and with PBAT polymer. f) J–V curve of the best performing PBAT-incorporated
PSCs of 1 cm2 area, the inset is a photograph of device.

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highest PCE. The control device based on pristine CsMAFA
in the reverse scan exhibits a maximum PCE of 19.17%, with
an open-circuit voltage (Voc) of 1.095  V, a short-circuit cur-
rent (Jsc) of 22.67  mA cm−2, and a fill factor (FF) of 0.772,
while the PCE in the forward scan is 18.21% (Voc  =  1.095  V,
Jsc = 22.75 mA cm−2, FF = 0.731) (Figure 3b). In constrast, the
device incorporated with 0.1 mg mL−1 PBAT in the reverse scan
exhibits a maximum PCE of 22.07%, with a markedly improved
Voc of 1.128  V, a Jsc of 23.53  mA cm−2, and a FF of 0.831,
while the PCE in forward scan attains 21.70% (Voc  = 1.128  V,
Jsc  = 23.49  mA  cm−2, FF = 0.819) (Figure  3c). The calculated
PCEreverse − PCEforward  [5]
hysteresis factor  HF =  of the pristine
 PCEreverse
and PBAT-incorporated PSCs is 5.01% and 1.68%, respectively,
which shows that the PBAT-incorporated device exhibits negli-
gible hysteresis. The disappearance of hysteresis phenomenon
is primarily because of the effective deactivation of the perov-
skite GBs and surface defects. Figure 3d shows the steady-state
power output (SPO) and current-density values under the max-
imum power point (MPP) confirmed from the J–V curves. The
control device has a stable efficiency of 18.56% under a bias of
0.928  V, while the PBAT-incorporated device has a stable effi-
ciency of 21.80% under a bias of 0.960  V. The integrated Jsc
from external quantum efficiency measurement for the pris-
tine and PBAT-incorporated devices is 21.92 and 22.91 mA cm−2
(Figure 3e). The stabilized efficiency and integrated Jsc are both
nearly to the actual output from the J–V curve. We used the
suspension coating method to prepare a 1 cm2 area device and
obtained the best PCE of 20.31% (Figure 3f), which is also one
of the relatively high values. The synergistic increase of the
Voc, Jsc, and FF using PBAT incorporated devices promotes the
improvement of PCE.
To evaluate the charge carrier recombination behavior, pho-
toluminescence (PL) spectroscopy attenuation measurements
were performed on ITO glass.[33–34] Compared with the pristine
perovskite, the steady-state PL strength of PBAT-incorporated
perovskite is increased by 169% (Figure 4a). Furthermore,
PBAT-incorporated perovskite has a blue-shifted PL peak
(778  nm) compared to control (780  nm), confirming that the
PBAT Lewis base passivates perovskite GBs per surface defects,
inhibiting perovskite surface and GBs trap assisted non-radia-
tive recombination. Time-resolved PL curves of the pristine and
PBAT-incorporated perovskite films are presented in Figure 4b.
Fitting the curves with a biexponential function:
 t  t 
y = A1 exp  −  + A2 exp  −  (1)
 τ1   τ2 
yields faster decay lifetime (τ1), slower decay lifetime (τ2), and
the fitting arguments are summarized in Table S2, Supporting
Information. Compared with the control sample of 23.45%, the
proportion of fast decay for the PBAT-incorporated is reduced
to 18.55%, which indicates a reduction in the number of perov-
skite surface defects.[35] Moreover, the average PL lifetime (τave)
has elongated from 395 to 835  ns, which is attributed to the
larger grain size. The PBAT polymer passivates the defect sites
on the perovskite GBs per surface, thereby reducing carrier
trapping, while larger crystal grains and inter-grain crosslinking
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engendered by PBAT extend the carrier lifetime, as analyzed in
the SEM, XRD, AFM, and TEM measurements.
The influence of polymers on defect state density and carrier
mobility is evaluated using the space charge limited current
(SCLC) approach. The defect state density (nt) is calculated by
trap-filled limited voltage (VTFL) and derived from the following
Equation (1) 7:
entL2
VTFL = (2)
2εε 0
where e is the electric charge, L is the thickness of perovskite
film (750  nm), ε is the relative dielectric constant of CsMAFA
based perovskite (ε  = 25.5), and ε0 is the vacuum permittivity.
In Figure  4c, the estimated VTFL value of the PBAT-incorpo-
rated device reduces to 0.31 V from 0.53 V of the control device,
resulting in a trap density of 1.37 × 1015 cm−3 for the incorporated
device and 2.33 × 1015 cm−3 for the pristine device. The low trap
state density indicates that the PBAT polymer is beneficial to
decrease the trap density and suppress charge carrier recombina-
tion, which corresponds to the measured value of the PL result.
Then, the electron mobility (µ) is obtained according to the SCLC
regions, the dark current (J) was fitted by the Mott–Gurney law 7:
9 V2
J= εε 0 µ 3 (3)
8 L
where V is applied voltage. the determined electron mobility
of the PBAT-incorporated device increases to 11.64 cm2 V−1 s−1
from 4.40 cm2 V−1 s−1 of the control, demonstrating that the
PBAT polymer incorporated perovskite film is beneficial to
accelerate carrier transport.
To clarify the enrichment in Voc, we obtained the surface
energy level change of the perovskite film incorporated with
PBAT from UV photoelectron spectroscopy (UPS, Figure 4d) and
bandgaps ((Eg) = 1.59  eV, Figure S9, Supporting Information).
The Fermi energy (EF) level of the PBAT-incorporated perov-
skite has moved up by 0.32 eV (from 4.48 to 4.16 eV) compared
to the control (Figure  4e), reflecting that the PBAT-incorporated
perovskite film is more n-type characteristic, mainly because the
PBAT polymer is filled with some electronic defects, which helps
to further reduce the recombination induced by defects,[2,36] and
the n-type characteristic film is more energetically aligned with
the electron and hole transport layers, which contributes to Voc
increment and charge extraction.[37]
We applied Voc, Jsc, and light intensity technologies to inves-
tigate the improvement of FF of PSC incorporated with PBAT
(Figure S10, Supporting Information). Calculate the ideality factor
(nID) by obtaining the corresponding Voc, Jsc under various light
intensities. The nID is accurately quantized from the slope of the
Voc varied logarithmically with Jsc plot depended on Equation (3):
nIDkBT  JSC 
VOC = ln  (4)
q  J 0 
The nID of the control device is 1.41 and the nID of the PBAT-
incorporated device is 1.13 (Figure  4f).[38] The nID is used to
explain why FF falls below the Shockley–Queisser (S–Q) limit.
Figure  4g intuitively presents the proportions of the two main
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Figure 4.  Optoelectronic characterization. a) PL spectra and b) time-resolved PL decay curves of perovskite films without and with PBAT polymer.
c) J–V curves of the only electron transport layer devices (ITO /SnO2 /control or PBAT-modified /PCBM + C60 /Ag). d) Valence-band region and
photoemission cut off energy of the UPS spectra. e) Energy level scheme of the devices without and with PBAT polymer (VB stands for valence band
and CB for conduction band). f) Voc of devices varies logarithmically with Jsc plots. g) The red, green, and blue pellets correspond to the FFS–Q, the
FFmax, and the measured FF, severally. h) MS plots and i) tDOS obtained from AS measurement of devices without and with PBAT polymer before and
after MPP tracking for 500 h.

causes of non-radiative carrier recombination and charge
transfer loss. The S–Q limit FF (FFS–Q) of PSC with a bandgap
of 1.59 eV is 0.904.[39] Assuming that the charge transport loss
is not considered, the maximum FF (FFmax) can be estimated by
Equation (4)
v oc − ln ( v oc + 0.72) qVoc
FFmax = where v oc = (5)
v oc + 1 n IDkBT
The respectively calculated FFmax are 0.858 and 0.883 for
the devices with and without PBAT polymer. The discrepan-
cies between the FFmax and the FFS–Q are 0.046 and 0.021 for
the devices with and without PBAT polymer, respectively. The
discrepancies between the measured FF and the FFmax are 0.086
and 0.052 for the devices with and without PBAT polymer,
respectively. In Figure  4g, the PBAT-incorporated PSC gets
a smaller difference compared to pristine PSC, which means
that the PBAT polymer can not only passivate the GBs and sur-
face traps on the perovskite crystal, decreasing non-radiative
loss, but also improving charge carrier transport (Figure  4c),
reducing charge transport loss. These results prove that PBAT
polymer help to improve the FF of PSC.
We combined Mott–Schottky (M–S) analysis and admit-
tance spectroscopy (AS)[7] to more clearly and obviously assess
the carrier transport and the passivation effect of the PBAT
polymer on defects. The MS analysis can immediately evaluate
the built-in potential (Vbi) of the PSCs. Figure  4h shows that
the Vbi of the PSCs with and without PBAT polymer is 0.92 and
1.13 V, respectively. PBAT-incorporated PSC exhibits higher Vbi,
which means that PBAT enhances the driving force for charge

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carrier separation, which is well matched with more n-type
characteristic film obtained by UPS. Then, the trap density of
states (tDOS) distribution in the PSCs with and without PBAT
polymer can be estimated from AS (Figure  4i). The energetic
defect level of 0.35−0.40  eV is interrelated shallow-level traps,
which correspond to the traps in GBs, and the energetic defect
level of 0.40−0.60  eV is interrelated deep-level traps, which
corresponds to surface defects on the perovskite film.[40–42]
The PBAT-incorporated PSC reveals a lower trap density at
the shallow- and deep-level regions compared to the control,
which demonstrates that the PBAT polymer can simultaneously
inhibit the GBs and surface defects of perovskite film, and
exhibit greater trap state passivation ability.
To verify the feasibility of using PBAT polymer to enhance
device stability, we conducted comprehensive research of
PSCs in a humid environment and heat. The nonencapsulated
PBAT-incorporated PSC shows excellent wet stability in the
surrounding environment (relative humidity (RH) of 85%),
remaining at 90% of its initial PCE after 3000 h (Figure 5a).
In contrast, the control PSC’s PCE drops significantly to 57%
of its original value. It can be seen from the inset that the
PBAT incorporated film (with a contact angle of 69.1o) is more
hydrophobic than the control (with a contact angle of 45.4o),
indicating that PBAT polymer can protect the perovskite from
moisture. In addition, to assess the thermal stability of the
devices, the PCE changing process of nonencapsulated PSCs
is studied aged under 85 °C thermal pressure and in a N2
glove box (Figure  5b). The control device only maintains 39%
of its normalized PCE after 1000 h, which is impressively 87%
of the device combined with PBAT. The result shows that the
crosslinking interaction between PBAT polymer and perovskite
enhances the strength of perovskite crystal, thereby obviously
enhancing the thermal stability of PSCs.
The long-term operational stability of encapsulated PSCs
was measured under MPP tracking and a white LED lamp with
a light intensity identical to sunlight (no UV filter, in ambient
air, 45 °C, Figure 5c). The SPO value of the control device (ini-
tial efficiency of ≈18.56%) exhibits a faster degradation and only
retains ≈69% after 500 h. We estimate that the time for the con-
trol device to maintain 80% initial PCE (T80) is approximately
265 h. In contrast, the SPO value of the PBAT-incorporated
device decays slowly and retains 88% of initial PCE (≈21.80%)
after 1000 h of continuous operation and T80 time of the PBAT-
incorporated device is about 3249 h. We further study the root
cause of the excellent operational stability. After 500 h of MPP
tracking, the Vbi of the PSC incorporated with PBAT is reduced
by 0.03  V, while the control is reduced by 0.29  V (Figure  4h).
Moreover, compared with that before MPP tracking, the tDOS
distribution of the PBAT-incorporated PSC does not vary obvi-
ously compare with the control, demonstrating that the PBAT
polymer can effectively inhibit the emergence of surface and
GBs defects in the perovskite film (Figure  4i). The interac-
tion of PBAT polymer with uncoordinated Pb2+ and neutral
iodine in the perovskite film, which contributes to inhibit the
decomposition of perovskite under light, heat, and bias condi-
tions and improves the long-term operational stability of the

Figure 5.  Stability. a) Normalized PCE evolution for the nonencapsulated control and PBAT-incorporated devices during aging at 85 RH%. The insets
show the contact angle of perovskite films without and with PBAT polymer. b) Thermal stability performance of nonencapsulated PSCs after continuous
annealing at 85 °C in a nitrogen box. c) Operational stability performance of encapsulated PSCs without and with PBAT polymer in the air under one
sunlight at 45 °C and MPP tracking (no UV filter).

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Figure 6.  Lead leakage tests. a) Leaked Pb concentration after immersing the control, PBAT-incorporated, and PBAT-coated perovskite films in water
for 240 min. The inset is a schematic diagram of the lead leakage test. b) Schematic diagram of PBAT-coated perovskite film. c–d) The ideal model of
interaction between H2O, the smallest unit of PBAT polymer and Pb2+ cation in perovskite.

PSCs under high efficiency. In addition, under different sta-
bility test environments, the main reason for the reduction of
device efficiency is that the perovskite structure is destroyed,
resulting in a large number of defects, the light absorption and
carrier transport capacity being reduced, and finally, the device
efficiency being gradually reduced.[43]
The PBAT as an environmental-friendly polymer can also be
used to mitigate lead leakage of the PSCs. We immersed the
control and PBAT-modified perovskite film into 50 mL of deion-
ized water, and Figure 6a depicts the variation in lead concen-
tration over time. After 240 min, the lead concentration of the
perovskite film incorporated with PBAT is 10.70 ppm, while the
lead leakage concentration of the control sample is as high as
25.71  ppm. Furthermore, we use a polymer coating approach
to further reduce the Pb2+ leakage, which involves heating the
PBAT polymer to 130 °C, melting it, and scraping it around the
perovskite sheet (Figure 6b). After 240 min, the lead concentra-
tion of the PBAT-coated perovskite film is 0.60  ppm, and the
lead leakage removal rate is as high as 98%. This significantly
reduced lead leakage is attributed to 1) the hydrophobicity of
PBAT can protect the perovskite film from dissolving, 2) the
chemical reaction between the polymer carbonyl functional
group and the Pb2+ ions leaked from the degraded perovskite.
DFT calculations can better compare the interaction between
water molecule (H2O), the smallest PBAT polymer unit, and
perovskite (Figure 6c–d), where the perovskite is assumed to be
a PbI2-terminated system (there are detailed calculation param-
eters in the Supporting Information).[44] The binding energy ΔE
is calculated as the following Equation (5):
∆E = E Pb2+ /m − E m − E Pb2+ (6)
where E Pb2+ /m , Em and E Pb2+ are the energy of Pb2+ binding
with the molecule, the energy of the molecule, and the
energy of Pb2+, respectively. m is H2O or the smallest unit of
PBAT polymer. The shortest length of H2O and perovskite
(Pb2+) is 2.33 Å, and the complexation energy is simulated
as −67.5  kcal  mol−1 (Figure  6c). The optimized model of the
smallest unit of PBAT polymer and perovskite (Pb2+) is shown
in Figure  6d with the shortest length is 2.29 Å. Every three
adjacent carbonyl groups on the PBAT chain form a chelating
effect with Pb2+, and the simulation of complexation energy is
as low as −224.5 kcal mol−1. The carbonyl group of PBAT has a
stronger ability to bind lead than water, which is more condu-
cive to preventing lead leakage.
3. Conclusion
In summary, an environmental-friendly PBAT polymer is
adopted to implant the perovskite film with an anti-solvent
method, which can passivate the uncoordinated Pb2+ and neutral
iodine defects of perovskite material and markedly improve
device efficiency and operational stability. The incorporated

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inverted PSCs achieve the conversion efficiencies of 22.07%
(0.1 cm2) and 20.31% (1 cm2). Meanwhile, the incorporated
device after being encapsulated exhibits a prominent improve-
ment in operational stability under MPP tracking, maintaining
the initial efficiency of 80% for 3249 h. More importantly, the
polymer network can protect Pb2+ from being dissolved by
water and prevent nearly 98% of Pb2+ from leaking by directly
immersing the polymer-coated perovskite film in water. Our
results put forward a hoping strategy that can synchronously
improve the efficiency, long-term stability of PSC, and reduce
environmental pollution caused by Pb2+ leakage, which will
vastly promote the large-scale deployment of high-efficiency
PSC in clean energy applications.
Supporting Information
Supporting Information is available from the Wiley Online Library or
from the author.
Acknowledgements
This research was supported by the National Natural Science
Foundation of China (52172237, 52072228), the Shaanxi International
Cooperation Project (2020KWZ-018), the Shaanxi Science Fund for
Distinguished Young Scholars (2022JC-21), the Research Fund of the
State Key Laboratory of Solidification Processing (NPU), China (Grant
No. 2021-QZ-02), and the Fundamental Research Funds for the Central
Universities (3102019JC005). The authors thank the members from the
Analytical & Testing Center of Northwestern Polytechnical University
for the help of XRD, XPS, and SEM characterization. The author list of
this manuscript was corrected after online publication. Change to the
byline was made after initial online publication on August 8, 2022. One
co-author withdrew authorship in agreement with all co-authors.
Conflict of Interest
The authors declare no conflict of interest.
Data Availability Statement
The data that support the findings of this study are available from the
corresponding author upon reasonable request.
Keywords
environmental-friendly polymers, high efficiency, inverted perovskite
solar cells lead leakage, operational stability
Received: January 25, 2022
Revised: March 30, 2022
Published online: April 14, 2022
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