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Abstract:

The performance and scalability of perovskite solar cells (PSCs) based on 3D formamidinium lead triiodide (FAPbI3) absorber are often hindered by defects at the surface and grain boundaries of the perovskite. To address this, the study demonstrates the use of pyrrolidinium iodide for the in situ formation of an energetically aligned 1D pyrrolidinium lead triiodide (PyPbI3) capping layer over the 3D FAbI3 perovskite. The thermodynamically stable PyPbI3 perovskitoids, formed through cation exchange reactions, effectively reduce surface and grain boundary defects in the FAPbI3 perovskite. In addition to improved phase stability, the resulting 1D/3D perovskite film forms a cascade energy band alignment with the other functional layers in PSCs, enabling a barrier‐free interfacial charge transport. With a maximum power conversion efficiency (PCE) of ≈23.1% and ≈20.7% at active areas of 0.09 and 1.05 cm2, respectively, the 1D/3D PSCs demonstrate excellent performance and scalability. Leveraging this improved scalability, the study has successfully developed a mechanically‐scribed 1D/3D perovskite mini‐module with an unprecedentedly high PCE of ≈20.6% and a total power output of ≈270 mW at an active area of ≈13.0 cm2. The 1D/3D multi‐dimensional perovskite film developed herein holds great promise for producing low‐cost, high‐performance perovskite photovoltaics at both the cell and module levels.

Abstract:

The development of anti-solvent free, scalable, and printable perovskite film is crucial to realizing the low-cost roll-to-roll development of perovskite solar cells (PSCs). Herein, large-area perovskite film fabrication is explored using a spray-assisted sequential deposition technique. How propylene carbonate (PC) solvent additive affects the transformation of lead halide (PbI₂ ) into perovskite at room temperature is investigated. The result shows that PC-modified perovskite films exhibit a uniform, pinhole-free morphology with oriented grains compared with pristine perovskite films. The PC-modified perovskite film also has a prolonged fluorescence lifetime that indicates lower carrier recombination. The champion PSC devices based on PC-modified perovskite film realize a power conversion efficiency (PCE) of 20.5% and 19.3% at an active area (A) of 0.09 cm² and 1 cm² , respectively. The fabricated PSCs are stable and demonstrate ≥85% PCE retention following 60 days of exposure to ambient conditions. Furthermore, perovskite solar modules (A ≈ 13 cm² ) that yield a PCE of 15.8% are fabricated. These results are among the best reported for the state-of-art spray-coated PSCs. Spray deposition coupled with a PC additive is highly promising for economical and high-output preparation of PSCs.

Abstract:

Wide-bandgap perovskites solar cells (PSCs) are vital as top cells in perovskite-based tandem solar cells (TSCs). However, poor band alignment with the charge transport layer and unwanted parasitic absorption in the top semitransparent-PSC (ST-PSC) are major factors limiting the power conversion efficiency (PCE) of TSCs. Herein, we present a compact-porous nickel oxide (cp-NiOx) hole-transport layer (HTL) sequentially fabricated using a sol-gel suspension and colloidal suspension of highly crystalline NiOx. The cp-NiOx film exhibited enhanced transparency, mesoporous surface morphology, and better energy band alignment with a 1.68 eV perovskite film for fabricating highly near-infrared transparent (∼92 % (@800–1200 nm)) ST-PSCs. The best cell achieved a PCE of 15.9 %. In addition, a four-terminal perovskite/silicon TSC based on the cp-NiOx HTL achieved an outstanding PCE of ∼26.0 %. The tailored energy band structure and reduced parasitic absorption in the near-infrared region of the ST-PSCs based on the cp-NiOx HTL enabled fabrication of highly efficient inverted ST-PSCs for perovskite/silicon TSCs.

Abstract:

Developing an efficient electron transport layer (ETL) through structural modification is essential to produce high-performance perovskite solar cell (PSC) devices. Specifically, the ETL should exhibit low defects, high optical transparency, and charge selectivity for ideal electron transport. Herein, we demonstrate (i) the low-temperature fabrication of tin oxide (SnO2) ETLs with a bilayer structure, and (ii) inkjet-printing of triple-cation perovskite films. Through the combined use of spin-coating and spray deposition, the optimized SnO2-bilayer ETL shows a nano-granule-textured surface, noticeably fewer defects, and a cascade conduction band position with the inkjet-printed perovskite film. The champion PSC device, based on the SnO2-bilayer ETL and inkjet-printed perovskite film, recorded an outstanding power conversion efficiency (PCE) of ∼16.9%, which is significantly higher than the device based on the conventional SnO2 ETL (PCE ∼14.8%). The improved photovoltaic performance of the SnO2-bilayer-based device arises mainly from more efficient charge transport and suppressed recombination at the ETL/perovskite interface. The SnO2-bilayer ETL and inkjet-printed perovskite films demonstrated herein can be potentially used for large-scale manufacturing of photovoltaic modules.

Abstract:

The performance and scalability of perovskite solar cells (PSCs) is highly dependent on the morphology and charge selectivity of the electron transport layer (ETL). This work demonstrates a high-speed (1800 mm min^-1 ), room-temperature (25 °C-30 °C) deposition of large-area (62.5 cm² ) tin oxide films using a multi-pass spray deposition technique. The spray-deposited SnO₂ (spray-SnO₂ ) films exhibit a controllable thickness, a unique granulate morphology and high transmittance (≈85% at 550 nm). The performance of the PSC based on spray-SnO₂ ETL and formamidinium lead iodide (FAPbI₃ )-based perovskite is highly consistent and reproducible, achieving a maximum efficiency of ≈20.1% at an active area (A) of 0.096 cm² . Characterization results reveal that the efficiency improvement originates from the granular morphology of spray-SnO₂ and high conversion rate of PbI₂ in the perovskite. More importantly, spray-SnO₂ films are highly scalable and able to reduce the efficiency roll-off that comes with the increase in contact-area between SnO₂ and perovskite film. Based on the spray-SnO₂ ETL, large-area PSC (A = 1.0 cm² ) achieves an efficiency of ≈18.9%. Furthermore, spray-SnO₂ ETL based PSCs also exhibit higher storage stability compared to the spin-SnO₂ based PSCs.