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Solar RRL - 2023 - Wachsmuth - Fully Printed and Industrially Scalable Semitransparent Organic Photovoltaic Modules
Solar RRL - 2023 - Wachsmuth - Fully Printed and Industrially Scalable Semitransparent Organic Photovoltaic Modules
Solar RRL - 2023 - Wachsmuth - Fully Printed and Industrially Scalable Semitransparent Organic Photovoltaic Modules
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1. Introduction
While the power conversion efficiency (PCE) of organic photovoltaics (OPV) on
small-area lab cells has rapidly increased during the last few years, the perfor- A key target of organic photovoltaics (OPV)
mance on module level and the availability of OPV modules on the market is still research is to enable the implementation of
the technology along with its unique char-
limited, primarily due to specific constraints imposed by the industrial production
acteristics into everyday life applications
process. This work deals with the upscaling process of latest-generation OPV and thus to supplement existing solar cell
from small-area lab cells to fully solution-processed modules, which are com- technologies.[1–8] Intensive research effort
patible to industrial roll-to-roll (R2R) printing. This transfer is demonstrated step has been put into further enhancing the
by step from material selection and process optimization for every single layer of power conversion efficiency (PCE) of OPV
the stack (photoactive layer, charge transporting layers, and solution-processed and this approach has achieved great
success in recent years. This is underlined
top electrode)–including long-term stability investigations (thermal and light)–to
by reported certified cell efficiencies of
scaling up the device area by a factor of >100. Thus, a semitransparent OPV 19.2% PCE on 3 mm2 effective area and a
module with 10.8% PCE on 10.2 cm2 active area is achieved, which is among the PCE of 11.7% for an organic solar module
highest performances for semitransparent, fully solution-processed OPV mod- with an aperture area of 204 cm2.[9–11] On
ules. The individual developments all meet the requirements for industrial R2R the other hand, works on device stability
printing (green solvents, processing in air, annealing ≤140 °C, etc.), which and process scalability are still underrepre-
sented in the community.[1,12,13] However,
ensures that both the optimized layer stack and the fabrication process are fully
these aspects are at least as important
scalable and easily transferable to large-scale production.
for a successful commercialization of
the technology.[13–19] Furthermore, taking
full advantage of the technology involves
manufacturing of semitransparent devices.
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Figure 2. Degradation behavior of solar cells (stack: glass/ITO/ETL/PM7:BTP-4F-12/MoO3/Ag) with two different thicknesses (thin: 20 nm, thick: 40 nm)
of ZnO and SnO2 as ETL under exposure of metal halide lamp light (under nitrogen, with applied UV filter). The ETL has been thermally treated at either
a) 200 °C for 30 min or b) 120 °C for 2 min.
only 2 min at 120 °C of thermal treatment is applied to the ETL Finally, R2R processing of OPV requires a certain minimum
(see Figure 2b), only the ZnO layer shows a good light stability, active layer thickness, first to prevent the formation of shunts–
whereas the SnO2-based devices lose performance very rapidly caused by spikes from layers underneath or from contact-based
(mainly due to losses in JSC and VOC), which is even more pro- printing processes of the top layers (e.g., screen printing of the
nounced for thicker layers. This suggests that SnO2 generally top electrode), and second to increase the amount of directly
needs higher annealing temperatures to allow for stable devices, absorbed light in semitransparent devices, where no opaque
and that thicker ETLs further enhance the need for higher anneal- back-reflecting layer can be used to allow the light to pass
ing times and/or temperatures. Consequently, a thin ZnO layer is through the active layer a second time, which has a huge impact
chosen as the most suitable ETL for upscaling. Furthermore, the on the produced photocurrent and therefore greatly improves
photocatalytic effect, which has been reported to cause instabilities device performance.
in NFA-based devices using ZnO as ETL,[43–47] is circumvented by As increasing the AL film thickness (in the range above
application of a UV filter (spectrum shown in Figure S1, 100 nm toward 300 nm) is often accompanied by a fill factor
Supporting Information), which absorbs sufficient light below (FF) loss, an experiment is carried out in which three different
380 nm during light exposure to prevent the effect. donor materials (PM7, PM6, and PTQ10) are blended with the
acceptor BTP-4F-12 and the effect of active layer thickness on the
2.1.2. Photoactive Layer: Balancing Layer Thickness and solar cell performance is investigated. As can be seen in Figure 3,
Performance PM6 shows a high PCE with a thin layer thickness of 115 nm, but
features a linear decrease in efficiency with increasing film thick-
When focusing on compatibility of the photoactive layer to ness, mainly due to a decreasing FF, which is also observed for
large-scale manufacturing of semitransparent devices, apart PM7. PTQ10 and PM7, on the other hand, slightly underperform
from performance and stability, further aspects require consid- for very thin films compared to the other donors; however,
eration: processability with nonchlorinated (“green”) solvents, PTQ10 displays a remarkable steadiness in performance for
lowest possible material cost, and film thickness dependence. thicker layers, and thus provides a wider processing window,
One of the most prominent new generation active layer which is well in accordance with different studies, where low
systems is PM6:Y6. It is commonly dissolved in chloroform, thickness dependencies for the FF are observed in combination
which– being a chlorinated solvent–implies greater environmen- with PTQ10.[56,61–64] This underlines its suitability for upscaling–
tal concerns. A processing constraint of Y6 has been its preag- PTQ10 is able to form a high-performing device within a broad
gregation in certain solvents, including the nonchlorinated thickness range and is a cost-effective material–and was
solvent o-xylene, leading to large Y6 domains in the film and thus thus selected as active donor material of choice for fully
to reduced performance.[48,49] However, this challenge has been solution-processed, semitransparent devices.
overcome by modifying the side chains of Y6.[23–26] One of those
tailored materials is Y6-C12 (BTP-4F-12), which enables favor- 2.1.3. HTL: Energetic and Chemical Compatibility with AL and
able processability in o-xylene and thus provides excellent device Top Electrode
performances.[23]
Taking advantage of the fast and cost-effective manufacturing A critical role for achieving scalable, solution-processed,
enabled by high-throughput R2R coating, the costs of the final semitransparent, highly efficient solar cells plays the HTL.
product are estimated to be mainly driven by the material The new, high performance active layer systems with their
prices.[50–55] Therefore, it is important to select materials with deep energy levels require an HTL with a high work function.
a low synthetic complexity that can be synthesized with simple So far, PEDOT:PSS is the industrial state-of-the art for inverted
processes and a low number of synthetic routes.[52,56–60] OPV modules; however, when coated on top of the AL, its
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Figure 3. a) PCE, b) open-circuit voltage (VOC), c) short-circuit current ( JSC), and d) FF of solar cell devices with the stack glass/ITO/ZnO/Donor:BTP-4F-
12/MoO3/Ag using three different donor materials (PM6, PM7, and PTQ10) and different layer thicknesses.
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(Figure 4). It can be further observed that above a certain ratio of (IPA) is chosen, due to its good compatibility to adjacent layers as
PFI added to the mixture, the resistance of the film increases well as its good coatability, transparency, and conductivity. We
strongly (cf., Figure S3, Supporting Information), which, in addi- test both PEDOT:F and the PEDOT:PSS:PFI blend with respect
tion to the VOC, has a high influence on the overall performance. to their compatibility with the AgNW top electrode. It can be
Thus, an optimum PCE is reached for the blends with a ratio of observed in Figure 6 that the PEDOT:PSS:PFI–even though
57.2 w/w% of PFI within the mixture (cf., Figure S3, Supporting electronically compatible to the adjacent active layer–loses its
Information) and therefore this blend is selected as HTL for the performance with AgNW coated directly on top. In contrast,
next experiment in comparison to PEDOT:F. PEDOT:F is compatible and consequently the selected HTL
The resulting performance of the different material material to be employed with the AgNW electrode.
approaches is displayed in Figure 5. PEDOT:F fulfills the
necessary requirements with its high work function (5.7 eV) 2.2. Stability Evaluation: Exposure to Different Degradation
and clearly outperforms PEDOT:PSS in VOC (0.86 V) and FF
Sources
(66.4%). Furthermore, through blending PEDOT:PSS with
57.2 w/w% PFI the energy barrier can be overcome as well Semitransparent solar cells of the selected fully solution-
and a similar performance as with PEDOT:F can be achieved. processed architecture are tested against high temperature
(2 h at 120 °C–representing the conditions of a typical industrial
2.1.4. Solution-Processed Electrode: Semitransparency and secondary encapsulation process, e.g., between glass panes)
Compatibility to All Other Layers followed by 200 h of constant illumination with a metal halide
lamp (representing device operation in the sun). As ternary active
With the goal of making a fully solution-processed semitranspar- layer compositions have been shown to be able to improve
ent stack, we replace the evaporated silver electrode (Ag) with microstructure and device performance, we test the selected
silver nanowires (AgNWs). An AgNW ink based on isopropanol active system PTQ10:BTP-4F-12 with and without PC71BM as
Figure 5. a) J–V curves and b) PCEs of PTQ10-based solar cells with three different PEDOT compositions as HTL, namely, PEDOT:PSS, PEDOT:F, and
PEDOT:PSS:PFI with 57.2 w/w% PFI.
Figure 6. a) J–V curves and b) PCE of semitransparent solar cells with the stack glass/ITO/ZnO/PTQ10:BTP-4F-12/HTL/AgNW with PEDOT:F and
PEDOT:PSS:PFI as HTL.
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ternary component.[82,83] Figure 7a shows the relative PCE of the Information), while the ternary system again provides superior
devices during the course of degradation (i.e., their PCE after stability with relative PCEs of >90% after degradation.
degradation normalized to their PCE at t = 0; the performance
parameters (PCE, VOC, JSC, and FF) at t = 0 are shown in 2.3. Evaluation of Area Scalability: Semitransparent OPV
Figure S4, Supporting Information). While the binary devices Modules
maintain >80% of their initial performance, the ternary devices
maintain 90% of their initial PCE, which confirms the positive To validate the scalability of the developed layer stack, solar cells
effect of PC71BM on the stability. and modules of different sizes are fabricated and investigated.
Furthermore, a similar set of devices is exposed to 85 °C for Starting from individual solar cells with an active area of
200 h to evaluate their behavior under prolonged elevated tem- 9 mm2, we increase the device area by a factor of >100 to fabri-
perature. As shown in Figure 7b, the obtained results are similar cate modules with eight cells connected in series and an active
to the previous degradation experiment. This time, devices with area of 10.2 cm2 (see Figure S5, Supporting Information, for
the binary active layer composition degrade by slightly more than detailed information about the module layout). The performance
20% of their initial performance (cf. Figure S4, Supporting of all devices is presented in Table 1. Upon scaling the device type
Figure 7. Comparison of devices with binary (PTQ10:BTP-4F-12) and ternary (PTQ10:BTP-4F-12:PC71BM) active layer within the optimized semitrans-
parent, fully solution-processed stack (glass/ITO/ZnO/active layer/PEDOT:F/AgNW). Relative PCE after degradation compared to initial performance for
two degradation types: a) devices exposed to thermal stress (2 h, 120 °C) and subsequent constant irradiation (200 h, 40 °C); b) devices exposed to
prolonged heat (200 h, 85 °C).
Table 1. Photovoltaic device performance of cells and a respective module of >100 times larger active area. The performance of the best cell is presented
together with mean values averaged over six devices (in brackets).
Active area [cm2] PCE on active area [%] VOC/number of cells [V] ISC/cell area [mA cm 2] FF [%]
Cells 0.09 9.74 (9.63 0.09) 0.85 (0.85 0.00) 18.37 (18.30 0.17) 62.2 (61.8 0.4)
Module (eight cells in series) 10.17 9.75 0.85 18.31 62.7
Figure 8. a) J–V curve and b) photograph of a fully solution-processed and fully air-processed, semitransparent module on glass/ITO with eight cells
connected in series and a total active area of 10.17 cm2 with back-reflector.
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and area from 0.1 cm2 small cells to 10 cm2 modules, no perfor- with a ratio of 1:1.2, dissolved in o-xylene and stirred overnight at room
mance loss is observed, which underlines the excellent scalability temperature under nitrogen atmosphere. For the PTQ10-based binary
of the selected materials and layer stack. (and ternary) solar cells, PTQ10, BTP-4F-12 (and PC71BM) were mixed
and dissolved in o-xylene with a ratio of 1:1(:0.2) and stirred overnight
In Figure 8, the I–V curve of a 10 cm2 semitransparent solar
at room temperature under nitrogen atmosphere. All active layers were
module (a) and a photograph (b) is shown. The module has an applied by blade coating in air. For the active layer variation experiment
average visible transmittance (AVT) of 11.3%. The transmittance (see Section 2.1.2), different coating speeds ranging from 5 to 90 mms
spectrum of the module is shown in Figure S6, Supporting at a substrate temperature of 65 °C were used to obtain different active
Information. With an applied back-reflector, a higher Isc per cell layer thicknesses. After deposition, the films were thermally treated under
area of 20.35 mA cm 2 is achieved, leading to a module PCE of nitrogen for 10 min at 100 °C. The HTLs were fabricated by 1) thermal
evaporation of 10 nm MoO3 or 2) blade coating PEDOT:F (or PEDOT:
10.8% per active area and 10.2% with respect to the total module
PSS:PFI). The PEDOT:F was deposited on the active layer at 45 °C
area with a geometrical FF (GFF) of 94.4%, which is among the substrate temperature without further pre- or posttreatment. The
highest performances of fully solution-processed semitranspar- PEDOT:PSS:PFI mixture was diluted in 4 μL isopropanol per μL of the mix-
ent modules. This is especially notable because all process parts ture and was coated at 70 °C without posttreatment. The top electrodes
are undertaken in air, which underlines the industrial relevance were fabricated by 1) a thermally evaporated 100 nm silver electrode
of the system. (Ag) or 2) a blade-coated AgNW film (Ink-Y) at 65 °C substrate tempera-
ture and thermally treated at 120 °C for 3 min.
For the scalable, air-processed solar module and the respective cells
(Section 2.3), substrate preparation and blade coating of ETL was done
3. Conclusions in a similar manner than the solar cells in Section 2.1 and 2.2. For the
active layer PTQ10, BTP-4F-12 and PC71BM were mixed with a ratio of
In this work, we presented a step-by-step development to achieve 1:1:0.2 and dissolved in o-xylene with a total concentration of
an OPV layer stack that fulfills the requirements for manufactur- 25 mg mL 1 (1:1:0.2) and stirred at 70 °C for 30 min and then cooled down
ing stable, semitransparent, high-performance organic photovol- and stirred at 40 °C overnight. The active layer was coated on a substrate
taic modules with industrially compatible fabrication processes. heated with 50 °C temperature forming a dry film thickness of 185 10 nm
We pointed out challenges and considerations for each of the and subsequently thermally treated with 130 °C for 3 min in air. As HTL,
printed layers that arise when moving to scalable coating and BM-HTL-1 was doctor-bladed on top at 35 °C without any pre- or posttreat-
ment. As top electrode, ECOS AgNWs were filtered with a 10 μm filter and
selected suitable materials by evaluating and maximizing their
coated at 40 °C substrate temperature without further treatment. The pat-
performance and stability. Finally, the transition from small area terning lines for the module (P1, P2, P3) were done with a femto-second
solar cells to a 10 cm2 module by using our developed environ- laser.
mental manufacturing process has been demonstrated and Characterization: Characterizations of the solar cells and modules were
yielded a solar module with 10.8% efficiency, which is currently done with a solar simulator from LOT Quantum Design (LS0916 AAA). All
among the highest values for semitransparent, fully solution- devices (also the semitransparent ones) were irradiated from the
glass/ITO side during measurement and light degradation. Current–
processed OPV modules. This, in combination with a good sta-
voltage characteristics and conductivity measurements were obtained
bility, corroborates that OPV finally starts to become competitive from B2901A sourcemeter from Keysight Technologies Inc. Light degrada-
on the market and brings the technology one step closer to a suc- tion measurements were undertaken under nitrogen with applied UV filter
cessful large-scale commercialization. through exposure with metal halide lamp light. Thermal degradation and
thermal stress test were carried out under nitrogen atmosphere. Film
thickness measurements were performed with a μsurf custom confocal
4. Experimental Section microscope from NanoFocus AG. Work function measurements on
ITO substrates were done with scanning Kelvin probe system SKP5050
Materials: As functionalized substrates, glass coated with indium tin from KP Technology using freshly peeled HOPG as reference.
oxide (ITO, 15 Ω sq 1) and prepatterned was used. The coated and Transmission spectra were taken with a Lambda 950 UV/VIS
prepatterned substrates were acquired from Liaoning Yike Precision Spectrometer from PerkinElmer including an integrating sphere.
New Energy Technology Co., Ltd. SnO2 (N-31) and ZnO (N-10-Flex)
were provided by Avantama. The active materials, PTQ10, PM6, PM7,
and BTP-4F-C12, were supplied by Brilliant Matters. Supporting Information
PC71BM was purchased from Nano-C. MoO3 was acquired from Carl
Roth and Ag from Evochem Advanced Materials, respectively. PEDOT:F Supporting Information is available from the Wiley Online Library or from
was provided by the research group of Prof. Yinhua Zhou at the the author.
Wuhan National Laboratory for Optoelectronics, Huazhong University
of Science and Technology (China). PEDOT:PSS (HTL Solar) was acquired
from Heraeus and Nafion was acquired from Sigma–Aldrich (Merck). Acknowledgements
BM-HTL-1 was supplied by Brilliant Matters. Ink-Y AgNWs were acquired
from Cambrios. ECOS AgNWs were obtained from HeiQ RAS. The authors acknowledge funding from the European Union’s Horizon
Device Fabrication: Prior to application, the substrates for all devices 2020 research and innovation program under grant agreement nos.
were wiped with a microfibre tissue that was soaked with toluene. For 952911 (“BOOSTER”) and 101007084 (“CITYSOLAR”) and would like
the solar cells (Section 2.1 and 2.2), the ETLs, ZnO and SnO2, were soni- to thank all the project partners from the “BOOSTER” project for the col-
cated for 5 min and filtered with a 0.45 μm polypropylene filter, respec- laboration and their great support. The authors also acknowledge
tively. Subsequently, the solutions were applied onto the glass/ITO funding received within the “SINO-GERMAN MOBILITY PROGRAMME”
substrates by doctor blading in air followed by a thermal treatment (Mobility Programme, GZ M-0160) from the Sino-German Center for
(140 °C, 3 min, in air) unless stated otherwise in the results and discussion Research Promotion (SGC) and thank the research group of Prof.
section. Yinhua Zhou at the Wuhan National Laboratory for Optoelectronics,
For the active layers with PM7 or PM6 (and PTQ-10 for Section 2.1.2) as Huazhong University of Science and Technology (China), for providing
donors and BTP-4F-12 as acceptor, the donor and acceptor were mixed PEDOT:F. The authors acknowledge HeiQ RAS for providing ECOS
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AgNW ink. The authors acknowledge funding from the German Federal [16] A. S. Gertsen, M. F. Castro, R. R. Søndergaard, J. W. Andreasen, Flex.
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[19] A. Colsmann, H. Röhm, C. Sprau, Sol. RRL 2020, 4, 2000015.
C.J.B. acknowledge funding from the European Union’s Horizon 2020
[20] C. J. Brabec, A. Distler, X. Du, H.-J. Egelhaaf, J. Hauch, T. Heumueller,
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