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An all‐flexible self‐powering unit, combining a flexible perovskite solar mini‐module for energy conversion and ultra‐flexible screen‐printed interdigitated carbon supercapacitors on paper for energy storage, is designed and developed. Through a hybrid bifurcated structure, the supercapacitors are connected in series and neatly layered on a paper substrate with the perovskite solar mini‐module strategically placed on top for seamless integration. The photosupercapacitor quickly reaches saturated voltage under various light intensities (1 sun, 1000 lx, 500 lx, and 200 lx) and displays a self‐discharge time of over 2 minutes. It delivers peak overall and storage efficiencies of 2.8% and 23%, respectively, and exhibits an extensive potential window of 3.8 V, making it a prominent choice for real time applications in electronic systems. In a nutshell, the inherent flexibility of both the solar module and the storage system, coupled with the space‐saving design, and the extensive potential window of the hybrid photosupercapacitor paves the way for implementation in portable and wearable electronics operating in indoor environments, ushering a new era of more versatile and adaptable energy solutions. [ABSTRACT FROM AUTHOR]

NiOx, prepared via the sputtering method, exhibits low conductivity and energy level mismatch with the perovskite layer, thereby limiting further enhancements in the performance of perovskite solar modules (PSMs). Unlike traditional methods that enhance the performance of NiOx through reactive sputtering or directly doping NiOx targets with metal ions, both of which incur high costs and low efficiency, we employ an evaporation method using LiF to achieve efficient and low-cost doping of NiOx. Compared to the pristine NiOx, the incorporation of LiF significantly increases the conductivity of NiOx. Additionally, the incorporation of LiF enhances the quality of the deposited perovskite films, as well as the energy level alignment and symmetry between NiOx and the perovskite, effectively improving the hole extraction and transport capabilities between NiOx and the perovskite. As a result, the PSM (active area of 57.30 cm²) fabricated in air achieves an impressive efficiency of 19.54%. Furthermore, the unencapsulated PSM retains 80% of its initial efficiency after 700 h of continuous illumination, whereas the NiOx-based PSM drops to 80% after only 150 h. This study provides a simple and low-cost method for doping NiOx, which is of great significance for the further industrialization of PSMs. [ABSTRACT FROM AUTHOR]

Inverted perovskite solar cells (PSCs) have attracted considerable attention due to their distinct advantages, including minimal hysteresis, cost‐effectiveness, and suitability for tandem applications. Nevertheless, the solution processing and the low formation energy of perovskites inevitably lead to numerous defects formed at both the bulk and interfaces of the perovskite layer. These defects can act as non‐radiative recombination centers, significantly impeding carrier transport and posing a substantial obstacle to stability and further enhancing power conversion efficiency (PCE). This review delves into a detailed discussion of the nature and origin of defects and the characterization techniques employed for defect identification. Furthermore, it systematically summarizes methods for defect detection and approaches for passivating interface and bulk defects within the perovskite film in inverted PSCs. Finally, this review offers a perspective on employing upscaling defect passivation engineering for perovskite modules. It is hoped this review provides insights into defect passivation in inverted PSCs and solar modules. [ABSTRACT FROM AUTHOR]

Perovskite solar cells have shown great potential in the field of underwater solar cells due to their excellent optoelectronic properties; however, their underwater performance and stability still hinder their practical use. In this research, a 1H,1H,2H,2H-heptadecafluorodecyl acrylate (HFDA) anti-reflection coating (ARC) was introduced as a high-transparent material for encapsulating perovskite solar modules (PSMs). Optical characterization results revealed that HFDA can effectively reduce reflection of light below 800 nm, aiding in the absorption of light within this wavelength range by underwater solar cells. Thus, a remarkable efficiency of 14.65% was achieved even at a water depth of 50 cm. And, the concentration of Pb2+ for HFDA-encapsulated film is significantly reduced from 186 to 16.5 ppb after being immersed in water for 347 h. Interestingly, the encapsulated PSMs still remained above 80% of their initial efficiency after continuous underwater illumination for 400 h. Furthermore, being exposed to air, the encapsulated PSMs maintained 94% of their original efficiency after 1000 h light illumination. This highly transparent ARC shows great potentials in enhancing the stability of perovskite devices, applicable not only to underwater cells but also extendable to land-based photovoltaic devices. [ABSTRACT FROM AUTHOR]

Perovskite solar cells, known for high efficiency and compatibility with various photovoltaic (PV) applications, have garnered significant attention from academia and industry. Scaling up these cells conventionally involves fabricating modules with series‐connected cells using a monolithic interconnection based on the P1‐P2‐P3 scheme, a common approach for thin‐film PV modules. The Geometrical Fill Factor (GFF), representing the ratio between active area and aperture area, typically ranges from 90% to 95%. This study introduces an advanced laser manufacturing process to minimize interconnection area by reducing scribe width and minimizing distances between them, achieving an interconnection width of 45 µm with a GFF of 99.1%. Additionally, a discontinuous P2 design further reduces the dead area to an average of 19.5 µm, resulting in a record GFF of 99.6%. Using this interconnection in a highly efficient p‐i‐n stack, the study demonstrates the feasibility of the discontinuous P2 by fabricating 2.6 cm2 minimodules with an aperture area efficiency of 20.7%. The research highlights how proper design can minimize intrinsic losses during the scaling process from cell to module to a negligible level. Experimental studies, coupled with cell‐to‐module loss simulations and electroluminescence mapping for layer deposition uniformity, provide insights into the potential of the new P2 design. [ABSTRACT FROM AUTHOR]

Organometal halide perovskite photovoltaic (PV) cells have achieved power conversion efficiencies (PCEs) comparable to the leading crystalline silicon (c‐Si) PV technology. However, despite their exceptional performance, these perovskite solar cells (PSCs) face technological challenges such as large‐area fabrication complexities and outdoor stability concerns. These challenges need to be addressed to pave the way for the commercialization of PSCs. The key to commercializing PSCs lies in developing stable, large‐area solar modules that offer both high efficiency and reliability. Overcoming the hurdles of large‐area module design and fabrication is a crucial step, and researchers are exploring innovative solutions to tackle these challenges. This review article primarily focuses on the development of large‐area PSCs, recent advancements in this field, and the obstacles related to scaling up this technology. It delves into the techniques used to fabricate perovskite films, with a special emphasis on large‐area and large‐scale PSC manufacturing methods. Moreover, the review highlights stability concerns that perovskite solar modules (PSMs) face and reports on recent progress in addressing these issues. The article concludes by summarizing potential future research directions aimed at realizing the full commercial potential of this innovative and promising solar cell technology. [ABSTRACT FROM AUTHOR]

Uniform film deposition over an entire substrate is indispensable to achieve efficient perovskite solar modules (PSMs) by minimizing the gap with high‐performance perovskite solar cells (PSCs). Only a few microscopic pinholes on the film in PSMs directly give rise to debase the performance and stimulate the degradation of the devices. Herein, a strategy of the homogeneous and defect‐reduced electron‐transport layer for high‐performance PSMs is reported. pH modulation of tin oxide (SnO2) nanoparticles colloidal dispersion by a small amount of nitric acid (HNO3) addition leads to the removal of hydroxy groups on the SnO2 surface acting as electronic defects as well as superb regularity of the thin films by forming a network of the SnO2 nanoparticles. The surface engineering of SnO2 nanoparticles brings out the high performance of 23.7% efficiency for a unit cell, 20.3% efficiency for a 24.5 cm2 minimodule, and 19.0% efficiency for a 214.7 cm2 submodule, respectively, where all efficiencies are averaged from results obtained by the reverse/forward scan. In outdoor tests with the submodules, a target PSM generates 16.5% higher cumulative electricity for a month as compared to a control PSM. Furthermore, under damp heat environments, the target PSM maintains 80% efficiency compared to an initial efficiency of 1080 h. [ABSTRACT FROM AUTHOR]

Tin oxide (SnO2) is one of the most promising electron transport layers (ETL) for the commercialization of perovskite solar cells (PSCs) due to its excellent electron mobility and high transparency, along with its low processing temperature. However, the inherent defects, nonuniform coating, and poor surface morphology of SnO2 may be detrimental to the physicochemical properties, such as conductivity and electron mobility at the interface, lead to a decrease in the open‐circuit voltage (VOC) and a reduction in device stability. In this study, a method that combines atomic layer deposition and chemical bath deposition techniques to solve these issues is presented. The presence of bilayer ETLs enhances the coverage of the SnO2 film and optimizes the morphology of the buried surface of perovskite, which not only facilitates the interfacial charge transfer but also suppresses recombination reactions. As a result, a significant increase in VOC and efficiency has been achieved compared to devices with only a single layer. Additionally, the large‐area perovskite solar module (active area: 48.0 cm2) achieves a champion efficiency of 17.9%. The PSCs retain more than 93% of their initial efficiency after 700 h of continuous operation under 1‐sun illumination and 25 °C. [ABSTRACT FROM AUTHOR]

Nickel oxide (NiOx)‐based inverted perovskite solar cells stand as promising candidates for advancing perovskite photovoltaics towards commercialization, leveraging their remarkable stability, scalability, and cost‐effectiveness. However, the interfacial redox reaction between high‐valence Ni4+ and perovskite, alongside the facile conversion of iodide in perovskite into I2, significantly deteriorates the performance and reproducibility of NiOx‐based perovskite photovoltaics. Here, potassium borohydride (KBH4) is introduced as a dual‐action reductant, which effectively avoids the Ni4+/perovskite interface reaction and mitigates the iodide‐to‐I2 oxidation within perovskite film. This synergistic redox modulation significantly suppresses nonradiative recombination and increases the carrier lifetime. As a result, an impressive power conversion efficiency of 24.17% for NiOx‐based perovskite solar cells is achieved, and a record efficiency of 20.2% for NiOx‐based perovskite solar modules fabricated under ambient conditions. Notably, when evaluated using the ISOS‐L‐2 standard protocol, the module retains 94% of its initial efficiency after 2000 h of continuous illumination under maximum power point at 65 °C in ambient air. [ABSTRACT FROM AUTHOR]

Highlights High-quality large-area perovskite films are prepared using a solid–liquid two-step film formation method combined with CsBr modification for the buried interface and Urea additive for perovskite crystallization. The inverted perovskite solar modules’ performance is enhanced to 20.56% in 61.56 cm2 with improved stability.

Efficiency reduction in perovskite solar cells (PSCs) during the magnification procedure significantly hampers commercialization. Vacuum‐flash (VF) has emerged as a promising method to fabricate PSCs with consistent efficiency across scales. However, the slower solvent removal rate of VF compared to the anti‐solvent method leads to perovskite films with buried defects. Thus, this work employs low‐toxic Lewis base ligand solvent N‐ethyl‐2‐pyrrolidone (NEP) to improve the nucleation process of perovskite films. NEP, with a mechanism similar to that of N‐methyl‐2‐pyrrolidone in FA‐based perovskite formation, enhances the solvent removal speed owing to its lower coordination ability. Based on this strategy, p–i–n PSCs with an optimized interface attain a power conversion efficiency (PCE) of 24.19% on an area of 0.08 cm2. The same nucleation process enables perovskite solar modules (PSMs) to achieve a certified PCE of 23.28% on an aperture area of 22.96 cm2, with a high geometric fill factor of 97%, ensuring nearly identical active area PCE (24%) in PSMs as in PSCs. This strategy highlights the potential of NEP as a ligand solvent choice for the commercialization of PSCs. [ABSTRACT FROM AUTHOR]

Highlights: High-quality large-area perovskite films are prepared using a solid–liquid two-step film formation method combined with CsBr modification for the buried interface and Urea additive for perovskite crystallization. The inverted perovskite solar modules' performance is enhanced to 20.56% in 61.56 cm2 with improved stability. A considerable efficiency gap exists between large-area perovskite solar modules and small-area perovskite solar cells. The control of forming uniform and large-area film and perovskite crystallization is still the main obstacle restricting the efficiency of PSMs. In this work, we adopted a solid–liquid two-step film formation technique, which involved the evaporation of a lead iodide film and blade coating of an organic ammonium halide solution to prepare perovskite films. This method possesses the advantages of integrating vapor deposition and solution methods, which could apply to substrates with different roughness and avoid using toxic solvents to achieve a more uniform, large-area perovskite film. Furthermore, modification of the NiOx/perovskite buried interface and introduction of Urea additives were utilized to reduce interface recombination and regulate perovskite crystallization. As a result, a large-area perovskite film possessing larger grains, fewer pinholes, and reduced defects could be achieved. The inverted PSM with an active area of 61.56 cm2 (10 × 10 cm2 substrate) achieved a champion power conversion efficiency of 20.56% and significantly improved stability. This method suggests an innovative approach to resolving the uniformity issue associated with large-area film fabrication. [ABSTRACT FROM AUTHOR]

Abstract Nickel oxide (NiOx)‐based inverted perovskite solar cells stand as promising candidates for advancing perovskite photovoltaics towards commercialization, leveraging their remarkable stability, scalability, and cost‐effectiveness. However, the interfacial redox reaction between high‐valence Ni4+ and perovskite, alongside the facile conversion of iodide in perovskite into I2, significantly deteriorates the performance and reproducibility of NiOx‐based perovskite photovoltaics. Here, potassium borohydride (KBH4) is introduced as a dual‐action reductant, which effectively avoids the Ni4+/perovskite interface reaction and mitigates the iodide‐to‐I2 oxidation within perovskite film. This synergistic redox modulation significantly suppresses nonradiative recombination and increases the carrier lifetime. As a result, an impressive power conversion efficiency of 24.17% for NiOx‐based perovskite solar cells is achieved, and a record efficiency of 20.2% for NiOx‐based perovskite solar modules fabricated under ambient conditions. Notably, when evaluated using the ISOS‐L‐2 standard protocol, the module retains 94% of its initial efficiency after 2000 h of continuous illumination under maximum power point at 65 °C in ambient air.

NiOx, prepared via the sputtering method, exhibits low conductivity and energy level mismatch with the perovskite layer, thereby limiting further enhancements in the performance of perovskite solar modules (PSMs). Unlike traditional methods that enhance the performance of NiOx through reactive sputtering or directly doping NiOx targets with metal ions, both of which incur high costs and low efficiency, we employ an evaporation method using LiF to achieve efficient and low-cost doping of NiOx. Compared to the pristine NiOx, the incorporation of LiF significantly increases the conductivity of NiOx. Additionally, the incorporation of LiF enhances the quality of the deposited perovskite films, as well as the energy level alignment and symmetry between NiOx and the perovskite, effectively improving the hole extraction and transport capabilities between NiOx and the perovskite. As a result, the PSM (active area of 57.30 cm²) fabricated in air achieves an impressive efficiency of 19.54%. Furthermore, the unencapsulated PSM retains 80% of its initial efficiency after 700 h of continuous illumination, whereas the NiOx-based PSM drops to 80% after only 150 h. This study provides a simple and low-cost method for doping NiOx, which is of great significance for the further industrialization of PSMs.

Popular solution‐processed approaches for producing the active layer of perovskite solar cells (PSCs) generally have to make compromise between crystallinity and compactness by inducing a rapid crystallization process with explosive nucleation and limited growth via removing solvent quickly. Here, a practical growth‐dominated in‐plane directional crystallization technique (IPDC) with a deeply retarded crystallization process for the scalable preparation of PSCs are reported. During the low‐temperature annealing, a tiny chamber with a small height is built atop the wet perovskite precursor film to restrain the vertical diffusion and removal of solvent vapor. The chamber eliminates the vertical solvent vapor gradient and induce a horizonal in‐plane gradient of solvent vapor pressure (SVP) toward the preset exhaust port which allows the slow escape of solvent vapor to outer space. In this way, nucleation is induced preferentially near the port and the as‐formed heterogeneous nuclei then grow continuously and directionally. With IPDC, sufficient filling of perovskite with high crystallinity and obvious growth orientation is realized in non‐ordered mesoporous scaffolds. An encouraging power conversion efficiency of 19.35% and 16.53% is achieved respectively for the 0.1 and 52.3‐cm2 printable mesoscopic hole‐conductor‐free PSCs with carbon electrodes. [ABSTRACT FROM AUTHOR]

Sputtered nickel oxide (NiOx) has become one of the most promising inorganic hole transport layers for p–i–n perovskite solar cells (PSCs) due to its appealing features such as its robust nature, low material cost, and easy integration to tandem structures and large‐area applications. However, the main drawback with NiOx‐based PSCs is typically low open‐circuit voltage (VOC) due to the inferior energy‐level alignment, low charge mobility, and high recombination at the interface. Herein, two types of phosphonic acid self‐assembled monolayers (SAMs) deposited by blade coating as an interfacial layer to modulate the sputtered NiOx/perovskite interface properties are used. While sputtered NiOx serves as a conformally coated hole selective layer, the ultrathin SAM interlayer facilitates the hole extraction and minimizes the energy loss at the interface. Co‐ordinately introduced stabilizing additive, namely octadecyl 3‐(3,5‐di‐tert‐butyl‐4‐hydroxyphenyl)propionate (I‐76), further improves the device performance of NiOx/SAM‐based PSCs, resulting in VOC of 1.14 V and a power conversion efficiency of 21.8%. By applying these strategies for perovskite module upscaling, aperture area module efficiencies of 19.7%, 17.5%, and 15.5% for perovskite minimodules of 4, 16, and 100 cm2 are demonstrated, corresponding to active area module efficiencies of 20.4%, 18.0%, and 16.4%, respectively. [ABSTRACT FROM AUTHOR]

Most thin‐film photovoltaic modules are constructed on soda‐lime glass (SLG) substrates containing alkali oxides, such as Na2O. Na may diffuse from SLG into a module's active layers through P1 lines, an area between a module's constituent cells where the substrate‐side charge transport layer (CTL) is in direct contact with SLG. Na diffusion from SLG is known to cause several important effects in II–VI and chalcogenide solar modules, but it has not been studied in perovskite solar modules (PSMs). In this work, we use complementary microscopy and spectroscopy techniques to show that Na diffusion occurs in the fabrication process of PSMs. Na diffuses vertically inside P1 lines and then laterally from P1 lines into the active area for up to 360 μm. We propose that this process is driven by the high temperatures the devices are exposed to during CTL and perovskite annealing. The diffused Na preferentially binds with Br, forming Br‐poor, I‐rich perovskite and a species rich in Na and Br (Na‐Br) close to P1 lines. Na‐Br passivates defect sites, reducing non‐radiative recombination in the perovskite and boosting its luminescence by up to 5×. Na‐Br is observed to be stable after 12 weeks of device storage, suggesting long‐lasting effects of Na diffusion. Our results not only point to a potential avenue to increase PSM performance but also highlight the possibility of unabated Na diffusion throughout a module's lifetime, especially if accelerated by the electric field and elevated temperatures achievable during device operation. [ABSTRACT FROM AUTHOR]

Perovskite photovoltaics (PVs) are an emerging solar energy generation technology that is nearing commercialization. Despite the unprecedented progress in increasing power conversion efficiency (PCE) for perovskite solar cells (PSCs), up‐scaling lab‐made cells to solar modules remains a challenge. In this work, the recent progress of making perovskite mini‐modules is reviewed. In particular, a database summarizing the module size, performance, hysteresis, and operational lifetimes reported in the literature is built. After analyzing the performance losses from scaling PSCs to mini‐modules based on the data collected from the literature, the current key to high‐performance perovskite mini‐modules is found to be the coating method optimization. If the perovskite layer quality is well reserved, a >24% mini‐module efficiency is projected by only considering the losses from lateral resistivity and laser scribing area. Next, performance characteristics are explored including hysteresis and meta‐stable power outputs that must be overcome to correctly characterize perovskite modules. Finally, current challenges associated with the long‐term stability of perovskite modules are examined and the importance of such durability for commercialization is discussed. It is hoped that the findings in this review provide a bridge for the development of perovskite modules that will lead to commercialization in the near future. [ABSTRACT FROM AUTHOR]

Abstract Perovskite photovoltaics (PVs) are an emerging solar energy generation technology that is nearing commercialization. Despite the unprecedented progress in increasing power conversion efficiency (PCE) for perovskite solar cells (PSCs), up‐scaling lab‐made cells to solar modules remains a challenge. In this work, the recent progress of making perovskite mini‐modules is reviewed. In particular, a database summarizing the module size, performance, hysteresis, and operational lifetimes reported in the literature is built. After analyzing the performance losses from scaling PSCs to mini‐modules based on the data collected from the literature, the current key to high‐performance perovskite mini‐modules is found to be the coating method optimization. If the perovskite layer quality is well reserved, a >24% mini‐module efficiency is projected by only considering the losses from lateral resistivity and laser scribing area. Next, performance characteristics are explored including hysteresis and meta‐stable power outputs that must be overcome to correctly characterize perovskite modules. Finally, current challenges associated with the long‐term stability of perovskite modules are examined and the importance of such durability for commercialization is discussed. It is hoped that the findings in this review provide a bridge for the development of perovskite modules that will lead to commercialization in the near future.

The important but remained issue to be addressed to achieve the mass production of perovskite solar modules include a large‐area fabrication of high‐quality perovskite film with eco‐friendly, viable production methods. Although several efforts are made to achieve large‐area fabrication of perovskite, the development of eco‐friendly solvent system, which is precisely designed to be fit to scale‐up methods are still challenging. Herein, this work develops the eco‐friendly solvent/co‐solvent system to produce a high‐quality perovskite layer with a bathing in eco‐friendly antisolvent. The new co‐solvent/additive, methylsulfonylmethane (MSM), efficiently improves the overall solubility and has a suitable binding strength to the perovskite precursor, resulting in a high‐quality perovskite film with antisolvent bathing method in large area. The resultant perovskite solar cells showed high power conversion efficiency of over 24% (in reverse scan), with a good long‐term stability under continuous light illumination or damp‐heat condition. MSM is also beneficial to produce a perovskite layer at low‐temperature or high‐humidity. MSM‐based solvent system is finally applied to large‐area, resulting in highly efficiency perovskite solar modules with PCE of 19.9% (by aperture) or 21.2% (by active area) in reverse scan. These findings contribute to step forward to a mass production of perovskite solar modules with eco‐friendly way. [ABSTRACT FROM AUTHOR]

Hybrid chemical vapor deposition (HCVD) is a promising method for the up‐scalable fabrication of perovskite solar cells/modules (PSCs/PSMs). However, the efficiency of the HCVD‐based perovskite solar cells still lags behind the solution‐processed PSCs/PSMs. In this work, the oxygen loss of the electron transport layer of SnO2 in the HCVD process and its negative impact on solar cell device performance are revealed. As the counter‐measure, potassium sulfamate (H2KNO3S) is introduced as the passivation layer to both mitigate the oxygen loss issue of SnO2 and passivate the uncoordinated Pb2+ in the perovskite film. In parallel, N‐methylpyrrolidone (NMP) is used as the solvent to dissolve PbI2 by forming the intermediate phase of PbI2•NMP, which can greatly lower the energy barrier for perovskite nucleation in the HCVD process. The perovskite seed is employed to further modulate the kinetics of perovskite crystal growth and improve the grain size. The resultant solar cells yield a champion power conversion efficiency (PCE) of 21.98% (0.09 cm2) with a stable output performance of 21.15%, and the PCEs of the mini‐modules are 16.16% (22.4 cm2, stable output performance of 14.72%) and 12.12% (91.8 cm2). Furthermore, the unencapsulated small area device shows an outstanding operational stability with a T80 lifetime exceeding 4000 h. [ABSTRACT FROM AUTHOR]

In this comment, we analyze the challenges we are facing for the further development of perovskite solar cells for their commercialization and offer our recommendations. It includes the following aspects: upscaling of lab-sized devices to different sized modules, further improving their efficiencies and stability, establishing proper characterization tools to help understand the underlying mechanisms of defect formation and develop needed methods to reduce them, riding on the rapid development of several perovskite-based tandem cells to facilitate the commercialization of perovskite PV, establishing suitable accelerated testing protocols and standards to evaluate perovskite-based modules and panels.

Surface passivation with organic halide salts is a powerful strategy to enhance the performance of perovskite solar cells. However, the inevitable formed in‐plane favored two‐dimensional perovskite layers with low carrier mobility and high binding energy inhibit the interfacial charge transfer within the device. Herein, a bulky fluorinated phenmethylammonium salt is designed and synthesized to passivate the perovskite film without forming 2D perovskites. A strong interaction which is induced by an electron donation from passivation agent to perovskite not only reduces the defects at the top surface of the perovskite, but also suppresses the recombination reaction at the buried surface due to a permeation of the organic halide salt. Moreover, the results of time resolved photoluminescence and confocal microscopy images suggest that the interfacial charge transfer speed and uniformity are enhanced. As a result, the efficiency of a small‐area device increases from 20.7 ± 0.9% to 22.8 ± 0.4% (aperture: 0.16 cm2). Moreover, a stabilized efficiency of 18.0% (aperture: 10.0 cm2) is achieved for larger‐area modules with 6‐series connected sub‐cells. Equally important, the non‐encapsulated modules show significantly improved stability at ambient conditions (ISOS‐D‐1). These significant improvements provided by a simple and reproducible procedure can be readily adopted in other types of devices. [ABSTRACT FROM AUTHOR]

Large‐area perovskite solar modules fabrication has been demonstrated with a rapid process of large‐area slot‐die coating, drying, and crystallization using near‐infrared radiation in ambient air, in which the laser‐scribing process is applied to fabricate the modules. However, defective coating of perovskite layer near laser‐scribed P1 line which isolates the front electrode of transparent conductive oxide (TCO) results very low module efficiencies. Therefore, systematic study is conducted to investigate the root cause, mechanism and solution of the defective coating and crystallization of the perovskite layer. Scanning electron microscope, energy‐dispersive X‐ray spectroscopy, and atomic force microscopy are used to characterize the TCO film before and after P1 scribing. It is found that P1 laser‐scribing process changes surface morphology of TCO at the area near P1 line, which decreases the surface wettability and results discontinuous coating of precursor solution near P1 lines. The absence of TCO material in the P1 trench induces nonuniform heating during NIR annealing step, which is verified by thermal analysis via numerical simulation. After tuning laser process recipes, a large module with an active area of 46 cm2 is fabricated with a power conversion efficiency of 7.2% and geometry fill factor of 93.8%. [ABSTRACT FROM AUTHOR]

After more than 10 years of intensive optimization, perovskite solar cells (PSCs) have now reached the point where the step towards their commercialization is expected. In order to move in this direction, the upscaling of devices is mandatory. However, the metal electrodes employed in the highest performing PSCs constitute a major obstacle, being both costly and unstable. In this review, the replacement of metal electrodes with carbon (C) electrodes in high-performing perovskite solar modules (PSMs) is presented. An overview of the background and current status is addressed, the potential of this material is highlighted and the challenges and future prospects are discussed. [ABSTRACT FROM AUTHOR]

The development of digital technology has made our lives more advanced as a society familiar with the Internet of Things (IoT). Solar cells are among the most promising candidates for power supply in IoT sensors. Perovskite photovoltaics (PPVs), which have already attained 25% and 40% power conversion efficiencies for outdoor and indoor light, respectively, are the best candidates for self-powered IoT system integration. In this review, we discuss recent research progress on PPVs under indoor light conditions, with a focus on device engineering to achieve high-performance indoor PPVs (Id-PPVs), including bandgap optimization and defect management. Finally, we discuss the challenges of Id-PPVs development and its interpretation as a potential research direction in the field. [ABSTRACT FROM AUTHOR]

Upscaling large‐area formamidinium (FA)‐based perovskite solar cells (PSCs) has been considered as one of the most promising routes for the commercial applications of this rising photovoltaics technology. Here, a natural amino acid, phenylalanine (Phe), is introduced to regulate the nucleation and crystal growth process of the large‐scale coating of FA‐based perovskite films. Better film coverage and larger grain sizes are observed after adding Phe. Moreover, it is found that Phe can effectively passivate defects within perovskite films and suppress the nonradiative recombination due to the strong interaction with under‐coordinated Pb2+ ions in the perovskite films. Rigid PSCs based on the blade‐coated perovskite films containing Phe obtain a champion efficiency of 21.95%. The corresponding unencapsulated devices also exhibit excellent ambient stability, retaining 95% of their initial efficiencies after storage in the glovebox at 20 °C for 1000 h. Further, the strategy is applied to fabricate flexible PSCs and modules on polyethylene terephthalate/indium doped tin oxide substrates via slot‐die coating. Phe modified flexible devices achieve outstanding efficiencies of 20.21%, 12.1%, and 11.2% with aperture areas of 0.10, 185, and 333 cm2, respectively. The strategy here has paved a promising way for the large‐scale production of flexible PSCs. [ABSTRACT FROM AUTHOR]

Upscaling large‐area formamidinium (FA)‐based perovskite solar cells (PSCs) has been considered as one of the most promising routes for the commercial applications of this rising photovoltaics technology. Here, a natural amino acid, phenylalanine (Phe), is introduced to regulate the nucleation and crystal growth process of the large‐scale coating of FA‐based perovskite films. Better film coverage and larger grain sizes are observed after adding Phe. Moreover, it is found that Phe can effectively passivate defects within perovskite films and suppress the nonradiative recombination due to the strong interaction with under‐coordinated Pb2+ ions in the perovskite films. Rigid PSCs based on the blade‐coated perovskite films containing Phe obtain a champion efficiency of 21.95%. The corresponding unencapsulated devices also exhibit excellent ambient stability, retaining 95% of their initial efficiencies after storage in the glovebox at 20 °C for 1000 h. Further, the strategy is applied to fabricate flexible PSCs and modules on polyethylene terephthalate/indium doped tin oxide substrates via slot‐die coating. Phe modified flexible devices achieve outstanding efficiencies of 20.21%, 12.1%, and 11.2% with aperture areas of 0.10, 185, and 333 cm2, respectively. The strategy here has paved a promising way for the large‐scale production of flexible PSCs. [ABSTRACT FROM AUTHOR]

Accumulated halide defects on the buried interfaces of halide perovskite layers have exacerbated undesirable nonradiative recombination in the n–i–p perovskite photovoltaics, but are challenging to be passivated—the commonly used passivation molecules at buried interfaces of perovskite layers would be inevitably eroded in the solution processes of perovskite deposition. Regarding the solvent incompatibility, herein, the ZnO–EA/SnO2–Cl electron transfer layers (ETLs) terminated with functional sites (i.e., ethanolamine (EA) ligands on ZnO and Cl− ions on SnO2) to spontaneously heal the buried interfaces of perovskite layers are customized. The specialties of ZnO–EA/SnO2–Cl for defect passivation are revealed: 1) formation of ZnO–EA–Pb2+ coherent interlayers at the EA‐terminated ZnO‐perovskite interfaces effectively offsets the I vacancy defects of perovskites; and 2) spontaneous halide exchange between Cl−‐terminated SnO2 and unstable I−‐terminated perovskites enables the formation of FA2Sn(ICl)6‐like coherent interlayers. Thus, the customized termination of ETLs’ surface reduces the halide‐defect‐triggered nonradiative recombination at the buried surfaces of perovskite, enabling the fabricated n–i–p planar modules (6 × 6 cm2) with power conversion efficiencies approaching 18% and elevated stability. These findings provide desirable guidelines for interfacial carrier transport between perovskites and ETLs.

Hole‐transporting materials (HTMs) based on the 10H, 10′H‐9,9′‐spirobi [acridine] core (BSA50 and BSA51) were synthesized, and their electronic properties were explored. Experimental and theoretical studies show that the presence of rigid 3,6‐dimethoxy‐9H‐carbazole moieties in BSA 50 brings about improved hole mobility and higher work function compared to bis(4‐methoxyphenyl)amine units in BSA51, which increase interfacial hole transportation from perovskite to HTM. As a result, perovskite solar cells (PSCs) based on BSA50 boost power conversion efficiency (PCE) to 22.65 %, and a PSC module using BSA50 HTM exhibits a PCE of 21.35 % (6.5×7 cm) with a Voc of 8.761 V and FF of 79.1 %. The unencapsulated PSCs exhibit superior stability to devices employing spiro‐OMeTAD, retaining nearly 90 % of their initial efficiency after 1000 h operation output. This work demonstrates the high potential of molecularly engineered spirobi[acridine] derivatives as HTMs as replacements for spiro‐OMeTAD. [ABSTRACT FROM AUTHOR]

Overcoming cell‐to‐module (CTM) efficiency losses is indispensable to realize large‐area high‐efficiency perovskite photovoltaic devices for commercialization. Laser scribing technology is used to fabricate perovskite modules, but it does not seem to solve the problem of high‐quality interconnection and high geometric filling factor (GFF), which are the prerequisites for overcoming CTM losses. In reality, what kind of laser technology is needed to fabricate high‐efficiency perovskite solar modules is still an open question. Herein, this work demonstrates that a nanosecond pulse laser is able to deliver a reduced heat‐affected zone due to the small thermal diffusion coefficient (Dt) of perovskite material, contributing to the accomplishment of a high GFF of up to 95.5%. In addition, the monolithic interconnection quality is improved by finely lifting off the capping layers on indium tin oxide and identifying the residue within the scribed area. As a result, a certified aperture area efficiency of 21.07% under standard 100 mW cm−2 AM1.5G illumination is achieved with a high photovoltaic fill factor exceeding 80%. The present study provides guidance in overcoming key CTM efficiency losses in perovskite photovoltaic technology. [ABSTRACT FROM AUTHOR]

Perovskite solar cells (PSCs) have undergone a dramatic increase in laboratory-scale efficiency to more than 25%, which is comparable to Si-based single-junction solar cell efficiency. However, the efficiency of PSCs drops from laboratory-scale to large-scale perovskite solar modules (PSMs) because of the poor quality of perovskite films, and the increased resistance of large-area PSMs obstructs practical PSC applications. An in-depth understanding of the fabricating processes is vital for precisely controlling the quality of large-area perovskite films, and a suitable structural design for PSMs plays an important role in minimizing energy loss. In this review, we discuss several solution-based deposition techniques for large-area perovskite films and the effects of operating conditions on the films. Furthermore, different structural designs for PSMs are presented, including the processing technologies and device architectures. [ABSTRACT FROM AUTHOR]

Perovskite solar cells (PSCs) can enable renewable electricity generation at low levelized costs, subject to the invention of an economically feasible technology for their large-scale fabrication, like vapor deposition. This approach is effective for the fabrication of small area (<1 cm 2 ) PSCs, but its scale-up to produce high-efficiency larger area modules has been limited by a severe imbalance between the vapor-solid reaction kinetics and the mass-transport of the volatile ammonium salt precursor. In this study, an amidine-based low-dimensional perovskite is introduced as an intermediate of the solid-vapor reaction to help resolve this limitation. This improves reaction pathway produces unique vertically monolithic grains with no detectable horizontal boundaries, which is used to produce 1.0 cm 2 PSCs with an efficiency of 22.1%, as well as 12.5 and 48 cm 2 modules delivering 21.1% and 20.1% efficiency, respectively. The modules retain ≈85% of their initial performance after 900 h of continuous operation (ISOS-L-1 protocol) and ≈100% after 2800 h of storage in an ambient environment (ISOS-D-1 protocol)., (© 2024 Wiley‐VCH GmbH.)

Li-TFSI doped spiro-OMeTAD is widely recognized as a beneficial hole transport layer (HTL) in perovskite solar cells (PSCs), contributing to high device efficiencies. However, the uncontrolled migration of lithium ions (Li + ) during device operation has impeded its broad adoption in scalable and stable photovoltaic modules. Herein, an additive strategy is proposed by employing ferrocenium hexafluorophosphate (FcPF 6 ) as a relay medium to enhance the hole extraction capability of the spiro-OMeTAD via the instant oxidation function. Besides, the novel Fc-Li interaction effectively restricts the movement of Li + . Simultaneously, the dissociative hexafluorophosphate group is cleverly exploited to regulate the unstable iodide species on the perovskite surface, further inhibiting the formation of migration channels and stabilizing the interfaces. This modification leads to power conversion efficiencies (PCEs) reaching 22.13% and 20.27% in 36 cm 2 (active area of 18 cm 2 ) and 100 cm 2 (active area of 56 cm 2 ) perovskite solar modules (PSMs), respectively, with exceptional operational stability obtained for over 1000 h under the ISOS-L-1 procedure. The novel FcPF 6 -based engineering approach is pivotal for advancing the industrialization of PSCs, particularly those relying on high-performance spiro-OMeTAD- based HTLs., (© 2024 Wiley‐VCH GmbH.)

The impending commercialization of perovskite solar cells (PSCs) is plodding despite the booming power conversion efficiencies and high stabilities. Most high‐performance, stable PSCs are often processed partially with high‐temperature processes, increasing the cost of production and energy payback time. Low‐temperature‐processed PSCs are crucial as they cut down the expenses lowering the barriers to industrial use. In addition, low‐temperature‐processed methods have a wide range of applicability in flexible devices and for tandem applications with other photovoltaic technologies where the temperature budget is limited. Therefore, making stable PSCs under ambient conditions as well as providing low‐cost fabrication techniques is highly desirable. Here, a detailed review is presented on the development of the low‐temperature process strategies for fabricating highly stable PSCs and perovskite solar modules. The effectiveness of low‐temperature processing in various classes of materials is also discussed. First, the authors introduce some major degradation processes in PSCs. Then, the developments and evolving strategies of notable materials using low‐temperature processing routes and a correlation with stability are summarized. A few general trends which are related to stability are also discussed. Overall, this review contributes to a better understanding of the status of low‐temperature‐processed cells and modules. [ABSTRACT FROM AUTHOR]

The perovskite solar era has demonstrated 25.5% efficiency in only 10 years of research, reaching the performance levels of other photovoltaics technologies such as Si and GaAs, showing potentially low‐cost manufacturing and process versatility. However, these results are achieved only on small area cells, with an active area equal or lower to 0.1 cm2. The upscaling development of perovskite solar technology requires the use of additional processes to reduce losses encountered for large areas; for this reason, laser processing becomes necessary to design connected cells into modules. In this work, cell‐to‐module losses in perovskite solar modules are reduced by optimizing the laser design, establishing a relationship between geometrical fill factor, cell area width, and P1–P2–P3 laser parameters. Upscaling the process from 2.5 × 2.5 to 10 × 10 cm2 an efficiency of 18.71% and 17.79% is achieved on active area of 2.25 and 48 cm2 respectively, with only 5% relative losses when scaling from to minimodule to module size. A minipanel is fabricated on 20 × 20 cm2, showing 11.9% stabilized efficiency and 2.3 W on an active area of 192 cm2, among the highest reported in literature so far at this size. [ABSTRACT FROM AUTHOR]

The commercialization of perovskite photovoltaic technology is dependent on the development of high‐efficiency, stable, and large‐area solar modules. Despite the rapid rise in efficiencies of laboratory‐scale perovskite solar cells (PSCs), there is still a big gap in the transition from small‐area devices to large‐area perovskite solar modules (PSMs). Herein, recent progresses on scaling‐up PSMs are reviewed: first, multifarious scalable preparation methods, solvent engineering, and corresponding morphology control strategies for large‐area homogeneous perovskite films are summarized. Various charge carrier transport materials, electrode materials, and their scaling methods for high‐efficiency and stable PSMs are then outlined and the device structure design of PSMs is discussed. Finally, the current strategies for optimizing the environmental stability of devices are highlighted, and packaging for reducing lead leakage during operation is discussed. [ABSTRACT FROM AUTHOR]

Metal halide perovskites are considered as game changers for future solar cell technology due to their rapidly increasing device efficiencies and potential for manufacturing at low cost. In view of their promising commercial potential, increasing research efforts are now dedicated to the development of large‐area perovskite solar modules. Herein, the motivation for developing perovskite solar modules and the challenges to fabricate large‐area perovskite solar cells with high efficiency are discussed. The important thin‐film processing methods including solution‐based and vacuum‐based deposition technologies for scaling up the fabrication of perovskites are reviewed. In addition, other key challenges that need to be overcome to bring perovskite solar modules into photovoltaic (PV) markets are also discussed, including module stability, potential lead leakage issue, and outdoor field testing of the perovskite modules. Finally, opinions on the future development of perovskite PV modules are shared. [ABSTRACT FROM AUTHOR]

The development of large‐area fabrication of perovskite solar cells is essential to their commercial applications. In this review, the recent progress of this field is first summarized. Then, the crystallization mechanism of perovskite films is addressed, followed by detailed descriptions on the deposition methods and optimization strategies for large‐area perovskite films. Finally, an outlook is provided for further improvement. [ABSTRACT FROM AUTHOR]

Though perovskite solar cells (PSCs) or modules (PSMs) are being developed at an unprecedented speed, several obstacles remain to their commercialization. One of the difficult problems is the expensive and unstable Au and Ag counter electrode. Therefore, highly effective, stable, and low‐cost counter electrode materials should be explored. Among various counter electrode materials, carbon is one of the most promising substitutes for their rich sources, low cost, outstanding electrochemical performance, and diversified surface functions. This review summarizes recent achievements of carbon counter electrode materials, which included commercial carbon paste, carbon black, graphite, graphene, carbon nanotubes and their synthetic approaches, modifications, and structure‐function relationships. Moreover, large‐scale carbon counter electrode in PSCs or PSMs are specifically discussed. Hopefully, this recapitulative analysis will draw the attention of relevant researchers to re‐understand the importance of counter electrode and clarify what should be noticed to develop qualified counter electrode materials for PSCs or PSMs. [ABSTRACT FROM AUTHOR]

The development of digital technology has made our lives more advanced as a society familiar with the Internet of Things (IoT). Solar cells are among the most promising candidates for power supply in IoT sensors. Perovskite photovoltaics (PPVs), which have already attained 25% and 40% power conversion efficiencies for outdoor and indoor light, respectively, are the best candidates for self-powered IoT system integration. In this review, we discuss recent research progress on PPVs under indoor light conditions, with a focus on device engineering to achieve high-performance indoor PPVs (Id-PPVs), including bandgap optimization and defect management. Finally, we discuss the challenges of Id-PPVs development and its interpretation as a potential research direction in the field.

Spatially resolved photoluminescence (PL) and electroluminescence (EL) imaging technologies play a crucial role in evaluating the performance and stability of photovoltaic devices. However, their application in perovskite devices presents unique challenges. In this study, we report a discrepancy between the electrical performance of perovskite solar modules (PSMs) and the EL images. Following the application of a reverse bias voltage, we observed an increase in EL brightness associated with prolonged carrier lifetime and transport length. Furthermore, cross-sectional Kelvin probe force microscopy identified a significant potential increase primarily at the electron-transport layer (ETL) side after reverse bias, suggesting the presence of defective ETL/perovskite interfaces with filled hole traps. To address this EL mismatch, we proposed a mild reverse current recovery method aimed at aligning EL images with the cell performance without compromising device efficiency. This approach effectively mitigates discrepancies, ensuring alignment between the device performance and EL imaging. Our study underscores that caution is required when utilizing EL imaging to monitor spatial homogeneity in PSMs for future industrial production.

Perovskite solar cells (PSCs) reached 25.5% of certified power conversion efficiency (PCE) in 2020. A remarkable PCE of PSCs has urged scalable technologies to grow for manufacturing modules. Therefore, scalable technology is rapidly developing though the performance of perovskite solar modules (PSMs) is still far behind that of PSCs. Herein, the recent progress in scalable technologies is reviewed with addressing important parameters in each process. In addition, the performance measurement protocols for PSMs are specifically discussed based on International Electrotechnical Commission to be prepared from the industrial point of view. Finally, the environmental hazard impact by accidental lead leakage and the introduction of green solvent to replace of current toxic solvent are described.

Perovskite photovoltaic technology holds great promise for the solar energy industry due to its high efficiency and fascinating potentialities for low-cost production. However, overcoming stability and scalability challenges by addressing environmental concerns is crucial for their successful deployment in the market. While perovskite solar cells have shown promising power conversion efficiency and long-term lifetime once produced by using small-scale production facilities, the scaling up of the device production without losing in performance and stability, still remains a not-trivial task. As matter of the fact, research and development efforts are currently ongoing to bring the perovskite solar technology closer to the market. From this point of view, the choice and the optimization of a specific deposition method depends on several factors like scalability, cost-effectiveness, and peculiar requirements required by the featured application. In this review, a comprehensive description of deposition methods for large area substrate is provided followed by an exhaustive collection of the main published progresses on large area perovskite solar devices. In particular, the large-area compatible deposition techniques will be categorized in the two main families based on solution and physical deposition processes, while pros and cons of both families are investigated in view of their potentialities for low-cost and high-throughput industrial production. Not least, hybrid deposition methods combining specific features of both solution and vacuum deposition techniques will be suggested as a way to leverage both their advantages. In addition, the main characterization techniques for large area devices will be described as a powerful way to select the proper deposition technique for supporting the development of commercial product based on perovskite technology. The opened challenges and the new routes for moving perovskite from lab to fab are finally suggested and discussed. [Display omitted] • Key advances and challenges for large-scale perovskite photovoltaic systems. • Deposition techniques enabling technology transfer from lab to fab. • Detailed description on solution-based, vacuum assisted and hybrid deposition techniques. • Summary of the most relevant results achieved on large area perovskite modules. • Guidelines and perspectives for the industrial development of perovskite PV technology. [ABSTRACT FROM AUTHOR]

The nucleation and crystallization processes within solution‐processed deposition is key for obtaining perovskite films with high quality. Herein, the synergistic effect of Cs+, ligand solvent (tetramethylene sulfoxide, TMSO), and methylammonium ions (MA+) on nucleation and crystallization procedures of preparing perovskites films is studied. The results reveal that producing α‐phase nuclei in the intermediate‐phase film (a perovskite film formed by removing the solvent before annealing) is the key factor for obtaining α‐phase‐pure perovskites, wherein Cs+ is necessary for reducing the formation energy of the α‐phase. In addition, the nonvolatile ligand (TMSO) is used to inhibit rapid nucleation, because it can form a stable intermediate phase. Furthermore, the introduction of the volatile MA+ cations compound (MACl) combined with Cs+ contributed to the direct formation of α‐phase nuclei in the intermediate‐phase film, and ion exchange (between FA+ and MA+) occurs during the subsequent annealing process, which leads to the formation of large‐grain perovskite film with good crystallinity. Maximum power conversion efficiencies of 22.08% and 16.88% are obtained via this strategy for a perovskite solar cell on a small area (active area: 0.09 cm2) and a perovskite solar module (aperture area: 12.92 cm2), respectively. [ABSTRACT FROM AUTHOR]

Perovskite solar cell (PSC) modules employing a hole transport layer (HTL) without unstable dopants possess high potential for improving operational stability. However, the low efficiencies of the devices greatly limit their commercial applications owing to the lower efficacy of the dopant‐free HTL, introduced by the unintentional n‐doping effect of volatile ions from the halide‐rich perovskite surface. Here, a scalable heterostructure integrated by a methylammonium‐free perovskite film with an iodide‐rich surface, an ultrathin interlayer of bridge‐jointed graphene oxide nanosheets (BJ‐GO), and an HTL without additional ionic dopants is developed. In this heterostructure, the iodide ions are physically immobilized by the compact 2D network, and lead defects are chemically passivated by multiple coordination bonds. Moreover, the BJ‐GO with tunable surface energy enables a highly ordered HTL a considerably improved carrier mobility by an order of magnitude. Finally, the PSC module with an area of 35.80 cm2 employing this heterostructure shows a certified efficiency of 15.3%. The encapsulated PSC modules retain over 91% of initial efficiency after the damp heat test at 85 °C and ≈85% relative humidity for 1000 h, while maintaining 90% of the initial value for 1000 h at the maximum power point under continuous 1‐Sun illumination at 60 °C. [ABSTRACT FROM AUTHOR]

While significant advancements in power conversion efficiencies (PCEs) of α-FAPbI 3 perovskite solar cells (PSCs) have been made, attaining controllable perovskite crystallization is still a considerable hurdle. This challenge stems from the initial formation of δ-FAPbI 3 , a more energetically stable phase than the desired black α-phase, during film deposition. This disrupts the heterogeneous nucleation of α-FAPbI 3 , causing the formation of mixed phases and defects. To this end, polarity engineering using molecular additives, specifically ((methyl-sulfonyl)phenyl)ethylamines (MSPEs) are introduced. The findings reveal that the interaction of PbI 2 -MSPEs-FAI intermediates is enhanced with the increased polarity of MSPEs, which in turn expedites the nucleation of α-FAPbI 3 . This leads to the development of high-quality α-FAPbI 3 films, characterized by vertical crystal orientation and reduced residual stresses. Additionally, the increased dipole moment of MSPE at perovskite grain boundaries attenuates Coulomb attractions among charged defects and screens carrier capture process, thereby diminishing non-radiative recombination. Utilizing these mechanisms, PSCs treated with highly polar 2-(4-MSPE) achieve an impressive PCE of 25.2% in small-area devices and 20.5% in large-area perovskite solar modules (PSMs) with an active area of 70 cm 2 . These results demonstrate the effectiveness of this strategy in achieving controllable crystallization of α-FAPbI 3 , paving the way for scalable-production of high-efficiency PSMs., (© 2023 Wiley‐VCH GmbH.)

Uniform and pinhole‐free organic lead halide perovskite films in a large area are of paramount importance for achieving high power conversion efficiencies (PCEs) of perovskite solar modules (PSMs). To obtain such high‐quality perovskite films in a large area, one commonly needs to prepare a perovskite intermediate phase, in which coordinated solvent number (CSN) seems to be a key parameter. However, the CSN is difficult to measure and control. To understand the relationship between the CSN and perovskite film quality, in situ evolution of the intermediate phase is investigated. The CSN in the intermediate phase film is measured by the high‐accuracy balance. Uniform and pinhole‐free perovskite films are reproducibly formed by tuning the CSN in the intermediate phase film with a mixed antisolvent of ethyl acetate (EA) and toluene (Tol) blended with a 1:1 volume ratio. A hole conductor–free PSM (10 × 10 cm2) thus fabricates and, based on printable carbon electrode, achieves a PCE of 10.2% in 52 cm2 active area. This effective method provides a promising direction for developing high‐quality and large‐area perovskite films for photovoltaic and other optoelectronic applications. [ABSTRACT FROM AUTHOR]

Organometal halide perovskites have exhibited a bright future as photovoltaic semiconductor in next generation solar cells due to their unique and promising physicochemical properties. Over the past few years, we have witnessed a tremendous progress of efficiency record evolution of perovskite solar cells (PSCs). Up to now, the highest efficiency record of PSCs has reached 22.1%; however, it was achieved at a very small device area of