Eco-Friendly Solvent Engineered CsPbI2.77 Br0.23 Ink for Large-Area and Scalable High Performance Perovskite Solar Cells.

The performance of large-area perovskite solar cells (PSCs) has been assessed for typical compositions, such as methylammonium lead iodide (MAPbI3 ), using a blade coater, slot-die coater, solution shearing, ink-jet printing, and thermal evaporation. However, the fabrication of large-area all-inorganic perovskite films is not well developed. This study develops, for the first time, an eco-friendly solvent engineered all-inorganic perovskite ink of dimethyl sulfoxide (DMSO) as a main solvent with the addition of acetonitrile (ACN), 2-methoxyethanol (2-ME), or a mixture of ACN and 2-ME to fabricate large-area CsPbI2.77 Br0.23 films with slot-die coater at low temperatures (40-50 °C). The perovskite phase, morphology, defect density, and optoelectrical properties of prepared with different solvent ratios are thoroughly examined and they are correlated with their respective colloidal size distribution and solar cell performance. The optimized slot-die-coated CsPbI2.77 Br0.23 perovskite film, which is prepared from the eco-friendly binary solvents dimethyl sulfoxide:acetonitrile (0.8:0.2 v/v), demonstrates an impressive power conversion efficiency (PCE) of 19.05%. Moreover, the device maintains ≈91% of its original PCE after 1 month at 20% relative humidity in the dark. It is believed that this study will accelerate the reliable manufacturing of perovskite devices.

Promoting Large-Area Slot-Die-Coated Perovskite Solar Cell Performance and Reproducibility by Acid-Based Sulfono-γ-AApeptide.

Homogeneous and pinhole-free large-area perovskite films are required to realize the commercialization of perovskite modules and panels. Various large-area perovskite coatings were developed; however, at their film coating and drying stages, many defects were formed on the perovskite surface. Consequently, not only the devices lost substantial performance but also their long-term stability deteriorated. Here, we fabricated a compact and uniform large-area MAPbI3-perovskite film by a slot-die coater at room temperature (T) and at high relative humidity (RH) up to 40%. The control slot-die-coated perovskite solar cell (PSC) produced 1.082 V open-circuit voltage (Voc), 24.09 mA cm-2 short current density (Jsc), 71.13% fill factor (FF), and a maximum power conversion efficiency (PCE) of 18.54%. We systematically employed a multi-functional artificial amino acid (F-LYS-S) to modify the perovskite defects. Such amino acids are more inclined to bind and adhere to the perovskite defects. The amino, carbonyl, and carboxy functional groups of F-LYS-S interacted with MAPbI3 through Lewis acid-base interaction and modified iodine vacancies significantly. Fourier transform infrared spectroscopy revealed that the C═O group of F-LYS-S interacted with the uncoordinated Pb2+ ions, and X-ray photoelectron spectroscopy revealed that the lone pair of -NH2 coordinated with the uncoordinated Pb2+ and consequently modified the I- vacancies remarkably. As a result, the F-LYS-S-modified device demonstrated more than three-fold charge recombination resistance, which is one of the primary requirements to fabricate high-performance PSCs. Therefore, the device fabricated employing F-LYS-S demonstrated remarkable PCE of 21.08% with superior photovoltaic parameters of 1.104 V Voc, 24.80 mA cm-2 Jsc, and 77.00%. FF. Concurrently, the long-term stability of the PSCs was improved by the F-LYS-S post-treatment, where the modified device retained ca. 89.6% of its initial efficiency after storing for 720 h in air (T ∼ 27 °C and RH ∼ 50-60%).

Surface Capping Layer Prepared from the Bulky Tetradodecylammonium Bromide as an Efficient Perovskite Passivation Layer for High-Performance Perovskite Solar Cells.

The power conversion efficiency (PCE) of perovskite solar cells (PSCs) has increased and levels with silicon solar cells; however, their commercialization has not yet been realized because of their poor long-term stability. One of the primary causes of the instability of PSC devices is the large concentration of defects in the polycrystalline perovskite film. Such defects limit the device performance besides triggering hysteresis and device instability. In this study, tetradodecylammonium bromide (TDDAB) was used as a postsurface modifier to suppress the density of defects from the mixed perovskite film (CsFAMA). X-ray photoelectron spectroscopy (XPS) and Fourier transform infrared spectroscopy (FTIR) analyses validated that TDDAB binds to the mixed perovskite through hydrogen bonding. The X-ray diffraction (XRD) and two-dimensional grazing incidence wide-angle X-ray scattering (2D GIWAXS) study uncovered that the TDDAB modification formed a capping layer of (TDDA)2PbI1.66Br2.34 on the surface of the three-dimensional (3D) perovskite. The single charge transport device prepared from the TDDAB-modified perovskite film revealed that both the electron and hole defects were considerably repressed due to the modification. Consequently, the modified device displayed a champion PCE of 21.33%. The TDDAB surface treatment not only enhances the PCE but the bulky cation of the TDDAB also forms a hydrophobic capping surface (water contact angle of 93.39°) and safeguards the underlayer perovskite from moisture. As a result, the modified PSC has exhibited almost no performance loss after 30 days in air (RH ≈ 40%).

Universal Surface Passivation of Organic-Inorganic Halide Perovskite Films by Tetraoctylammonium Chloride for High-Performance and Stable Perovskite Solar Cells.

The power conversion efficiency (PCE) of perovskite solar cells has been showing rapid improvement in the last decade. However, still, there is an unarguable performance deficit compared with the Schockley-Queisser (SQ) limit. One of the major causes for such performance discrepancy is surface and grain boundary defects. They are a source of nonradiative recombination in the devices that not only causes performance loss but also instability of the solar cells. In this study, we employed a direct postsurface passivation strategy at mild temperatures to modify perovskite layer defects using tetraoctylammonium chloride (TOAC). The passivated perovskite layers have demonstrated extraordinary improvement in photoluminescence and charge carrier lifetimes compared to their control counterparts in both Cs0.05(FAPbI3)0.83(MAPbBr3)0.17 and MAPbI3-type perovskite layers. The investigation on electron-only and hole-only devices after TOAC treatment revealed suppressed electron and hole trap density of states. The electrochemical study demonstrated that TOAC treatment improved the charge recombination resistance of the perovskite layers and reduced the charge accumulation on the surface of perovskite films. As a result, perovskite solar cells prepared by TOAC treatment showed a champion PCE of 21.24% for the Cs0.05(FAPbI3)0.83(MAPbBr3)0.17-based device compared to 19.58% without passivation. Likewise, the PCE of MAPbI3 improved from 18.09 to 19.27% with TOAC treatment. The long-term stability of TOAC-passivated perovskite Cs0.05(FAPbI3)0.83(MAPbBr3)0.17 devices has retained over 97% of its initial performance after 720 h in air.

Toward Large-Area and Fully Solution-Sheared Perovskite Solar Cells.

The solution shearing technique was used to prepare the various layers involved in perovskite solar cells (PSCs), with a device structure of FTO/c-TiO2/mp-TiO2/CH3NH3PbI3/Spiro-OMeTAD/Ag, in an area as large as 6 × 10 cm2. The film morphology and thickness of each layer were optimized by varying respective shearing parameters. The fully solution-sheared PSCs exhibited a champion power conversion efficiency (PCE) of 15.89%. In comparison, the PSCs with only perovskite layer solution-sheared and other layers spin-coated showed a high PCE of 17.27%. These results demonstrate the potential of a simple, rapid, cost-effective, and scalable solution shearing process to fabricate large-area PSCs and modules.

A star-shaped cyclopentadithiophene-based dopant-free hole-transport material for high-performance perovskite solar cells.

A new cyclopentadithiophene (CPDT)-based organic small molecule serves as an efficient dopant-free hole transport material (HTM) for perovskite solar cells (PSCs). Upon incorporation of two carbazole groups, the resulting CPDT-based HTM (C-CPDT) shows an impressive power conversion efficiency (PCE) of 19.68% with better stability compared with those of spiro-OMeTAD.

Low-Cost Hole-Transporting Materials Based on Carbohelicene for High-Performance Perovskite Solar Cells.

Two hole-transporting materials (HTMs) based on carbohelicene cores, CH1 and CH2, are developed and used in fabricating efficient and stable perovskite solar cells (PSCs). Owing to the rigid conformation of the helicene core, both compounds possess unique CH-π interactions in the crystalline packing pattern and good phase stability, which are distinct from the π-π intermolecular interactions of conventional planar and spiro-type molecules. PSCs based on CH1 and CH2 as HTMs deliver excellent device efficiencies of 19.36 and 18.71%, respectively, outperforming the control device fabricated with spiro-OMeTAD (18.45%). Furthermore, both PSCs exhibit better ambient stability, with 90% of initial performance retained after aging with a 50-60% relative humidity at 25 °C for 500 h. Due to the low production cost of both compounds, these newly designed carbohelicene-type HTMs have the potential for the future commercialization of PSCs.

Compact TiO2 films with sandwiched Ag nanoparticles as electron-collecting layer in planar type perovskite solar cells: improvement in efficiency and stability.

Fabrication of perovskite solar cells (PSCs) in a simple way with high efficiency and stability remains a challenge. In this study, silver nanoparticles (Ag NPs) were sandwiched between two compact TiO2 layers through a facile process of spin-coating an ethanolic AgNO3 solution, followed by thermal annealing. The presence of Ag NPs in the electron-transporting layer of TiO2 improved the light input to the device, the morphology of the perovskite film prepared on top, and eliminated leakage current. Photoluminescence and electron mobility studies revealed that the incorporation of Ag NPs in the ETL of the planar PSC device facilitated the electron-hole separation and promoted charge extraction and transport from perovskite to ETL. Hysteresis-free devices with incorporated Ag NPs gave a high average short-circuit current density (J sc) of 22.91 ± 0.39 mA cm-2 and maximum power conversion efficiency of 17.25%. The devices also showed enhanced stability versus a control device without embedded Ag NPs. The possible reasons for the improvement are analyzed and discussed.

New Helicene-Type Hole-Transporting Molecules for High-Performance and Durable Perovskite Solar Cells.

Three azahelicene derivatives with electron-rich bis(4-methoxyphenyl)amino or bis( p-methoxyphenyl)aminophenyl groups at the terminals were deliberately designed, synthesized, and characterized as hole-transporting materials (HTMs) for perovskite solar cells (PSCs). Optical and thermal properties, energy level alignments, film morphologies, hole extraction ability, and hole mobility were studied in detail. PSCs using the newly synthesized molecules as HTMs were fabricated. A maximum power conversion efficiency (PCE) of 17.34% was observed for the bis( p-methoxyphenyl)amino-substituted derivative (SY1) and 16.10% for the bis( p-methoxyphenyl)aminophenyl-substituted derivative (SY2). Longer-chain substituent such as hexyloxy group greatly diminishes the efficiency. In addition, the dopant-free devices fabricated with SY1 as the HTM shows an average PCE of 12.13%, which is significantly higher than that of spiro-OMeTAD (7.61%). The ambient long-term stability test revealed that after 500 h, the devices prepared from SY1 and SY2 retained more than 96% of its initial performance, which is much improved than the reference device with standard spiro-OMeTAD as the HTM under the same conditions. Detailed material cost analysis reveals that the material cost for SY1 is less than 8% of that for spiro-OMeTAD. These results provide a useful direction for designing a new class of HTMs to prepare highly efficient and more durable PSCs.