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Lead halide perovskites always emerge complex interactions among different elemental ions, which lead to multiple intrinsic imperfections. Elemental defects, such as amine, Pb, and I vacancies at A‐, B‐, and X‐sites, are main issues to deteriorate perovskite solar cells (PSCs). Unfortunately, most previous passivators can only temporarily fix partial inactive vacancies as sacrificial agents. Herein, we propose a recovery agent, ferrocene (Fc), which can form a one‐dimensional perovskite with adequate steric cavities and suitable dissociation energy to recover all elemental defects back to active light‐harvesting perovskites, and regenerate Fc itself meanwhile. Based on this perpetual chain‐reaction cycle, corresponding PSCs maintain >10 000‐hour lifetime in inert condition and >1000‐hour durabilities under various extreme environments, including continuous 85 °C heating, 50 % relative humidity wetting, and 1‐sun light soaking. [ABSTRACT FROM AUTHOR]

Lead halide perovskites always emerge complex interactions among different elemental ions, which lead to multiple intrinsic imperfections. Elemental defects, such as amine, Pb, and I vacancies at A‐, B‐, and X‐sites, are main issues to deteriorate perovskite solar cells (PSCs). Unfortunately, most previous passivators can only temporarily fix partial inactive vacancies as sacrificial agents. Herein, we propose a recovery agent, ferrocene (Fc), which can form a one‐dimensional perovskite with adequate steric cavities and suitable dissociation energy to recover all elemental defects back to active light‐harvesting perovskites, and regenerate Fc itself meanwhile. Based on this perpetual chain‐reaction cycle, corresponding PSCs maintain >10 000‐hour lifetime in inert condition and >1000‐hour durabilities under various extreme environments, including continuous 85 °C heating, 50 % relative humidity wetting, and 1‐sun light soaking. [ABSTRACT FROM AUTHOR]

Keywords: chain-reaction cycle; defects; ferrocene; perovskites; solar cells EN chain-reaction cycle defects ferrocene perovskites solar cells 1 2 2 06/14/22 20220620 NES 220620 It has come to the authors attention that incorrect versions of Figures 1, 2, and 4 were inadvertently used during the final stages of manuscript preparation. Berichtigung: Ferrocene-Induced Perpetual Recovery on All Elemental Defects in Perovskite Solar Cells Chain-reaction cycle, defects, ferrocene, perovskites, solar cells. [Extracted from the article]

In the pursuit of highly efficient perovskite solar cells, spiro‐OMeTAD has demonstrated recorded power conversion efficiencies (PCEs), however, the stability issue remains one of the bottlenecks constraining its commercial development. In this study, we successfully synthesize a novel self‐polymerized spiro‐type interfacial molecule, termed v‐spiro. The linearly arranged molecule exhibits stronger intermolecular interactions and higher intrinsic hole mobility compared to spiro‐OMeTAD. Importantly, the vinyl groups in v‐spiro enable in situ polymerization, forming a polymeric protective layer on the perovskite film surface, which proves highly effective in suppressing moisture degradation and ion migration. Utilizing these advantages, poly‐v‐spiro‐based device achieves an outstanding efficiency of 24.54 %, with an enhanced open‐circuit voltage of 1.173 V and a fill factor of 81.11 %, owing to the reduced defect density, energy level alignment and efficient interfacial hole extraction. Furthermore, the operational stability of unencapsulated devices is significantly enhanced, maintaining initial efficiencies above 90 % even after 2000 hours under approximately 60 % humidity or 1250 hours under continuous AM 1.5G sunlight exposure. This work presents a comprehensive approach to achieving both high efficiency and long‐term stability in PSCs through innovative interfacial design. [ABSTRACT FROM AUTHOR]

In the pursuit of highly efficient perovskite solar cells, spiro‐OMeTAD has demonstrated recorded power conversion efficiencies (PCEs), however, the stability issue remains one of the bottlenecks constraining its commercial development. In this study, we successfully synthesize a novel self‐polymerized spiro‐type interfacial molecule, termed v‐spiro. The linearly arranged molecule exhibits stronger intermolecular interactions and higher intrinsic hole mobility compared to spiro‐OMeTAD. Importantly, the vinyl groups in v‐spiro enable in situ polymerization, forming a polymeric protective layer on the perovskite film surface, which proves highly effective in suppressing moisture degradation and ion migration. Utilizing these advantages, poly‐v‐spiro‐based device achieves an outstanding efficiency of 24.54 %, with an enhanced open‐circuit voltage of 1.173 V and a fill factor of 81.11 %, owing to the reduced defect density, energy level alignment and efficient interfacial hole extraction. Furthermore, the operational stability of unencapsulated devices is significantly enhanced, maintaining initial efficiencies above 90 % even after 2000 hours under approximately 60 % humidity or 1250 hours under continuous AM 1.5G sunlight exposure. This work presents a comprehensive approach to achieving both high efficiency and long‐term stability in PSCs through innovative interfacial design. [ABSTRACT FROM AUTHOR]

Interfacial engineering of perovskite films has been the main strategies in improving the efficiency and stability of perovskite solar cells (PSCs). In this study, three new donor‐acceptor (D–A)‐type interfacial dipole (DAID) molecules with hole‐transporting and different anchoring units are designed and employed in PSCs. The formation of interface dipoles by the DAID molecules on the perovskite film can efficiently modulate the energy level alignment, improve charge extraction, and reduce non‐radiative recombination. Among the three DAID molecules, TPA‐BAM with amide group exhibits the best chemical and optoelectrical properties, achieving a champion PCE of 25.29 % with the enhanced open‐circuit voltage of 1.174 V and fill factor of 84.34 %, due to the reduced defect density and improved interfacial hole extraction. Meanwhile, the operational stability of the unencapsulated device has been significantly improved. Our study provides a prospect for rationalized screening of interfacial dipole materials for efficient and stable PSCs. [ABSTRACT FROM AUTHOR]

Perovskite solar cells (PSCs) are promising candidates for the next generation of photovoltaic technologies due to their constantly improved efficiencies, which gain much attention from both the scientific and industrial communities. Although the performance of PSCs is dramatically enhanced, most certified or reported high‐efficiency PSCs are still limited to a relatively small active area. The degradation of efficiency and stability accompanied by upscaling must be solved, being a bottleneck toward industrialization. This review focuses on the research progress, challenges, and strategies on large‐area PSCs, especially each functional material in various device architectures, including perovskites, hole transport materials, electron transport materials, and electrodes. Finally, the main issues related to each functional layer of PSCs from laboratory to industry are presented and an outlook on the research direction of large‐area PSCs is given. Perovskite solar cells (PSCs) have undergone rapid development, but the performance degradation accompanied by device upscaling urgently needs a solution. This review covers the research progress on each functional material of large‐area PSCs. A conclusion on the main challenges and an outlook on the research direction of large‐area PSCs are provided. [ABSTRACT FROM AUTHOR]

Rapid processing technologies of perovskite solar cells (PSCs) offer an exciting approach to raise the rate of production. Herein, a rapid microwave‐annealing process (MAP) is reported to replace the traditional hotplate annealing process (HAP) and the processing period of perovskite is reduced to less than 1 min. Benefiting from the penetrability and simultaneity of microwave irradiation, the MAP method can effectively eliminate miscellaneous phases and thus achieve >1 µm large‐size crystal grains in perovskite films. These MAP treated perovskite films exhibit pure crystalline phase, long charge‐carrier lifetime, and low defect density, which can substantially improve the PSC efficiency without requiring an additional enhancer/passivation layer. The inverted planar PSCs present enhanced power conversion efficiency from 18.33% (HAP) to 21.59% (MAP) and good stability of >1000 h lifetime without encapsulation under ambient conditions. In addition, MAP can be applied to a large‐size (10 cm × 10 cm) perovskite film fabrication as well as a broader tolerance in environmental temperature and precursor concentration, making it a reliable method for repeatably practical fabrication of perovskite photovoltaics. [ABSTRACT FROM AUTHOR]

Recently, organic–inorganic metal halide perovskite solar cells (PSCs) have achieved rapid improvement, however, the efficiencies are still behind the Shockley–Queisser theory mainly due to their high energy loss (ELOSS) in open‐circuit voltage (VOC). Due to the polycrystalline nature of the solution‐prepared perovskite films, defects at the grain boundaries as the non‐radiative recombination centers greatly affect the VOC and limit the device efficiency. Herein, poly(vinylidene fluoride) (PVDF) is introduced as polymer‐templates in the perovskite film, where the fluorine atoms in the PVDF network can form strong hydrogen‐bonds with organic cations and coordinate bonds with Pb2+. The strong interaction between PVDF and perovksite enables slow crystal growth and efficient defect passivation, which effectively reduce non‐radiation recombination and minimize ELOSS of VOC. PVDF‐based PSCs achieve a champion efficiency of 24.21% with a excellent voltage of 1.22 V, which is one of the highest VOC values reported for FAMAPb(I/Br)3‐based PSCs. Furthermore, the strong hydrophobic fluorine atoms in PVDF endow the device with excellent humidity stability, the unencapsulated solar cell maintain the initial efficiency of >90% for 2500 h under air ambient of ≈50% humid and a consistently high VOC of 1.20 V. [ABSTRACT FROM AUTHOR]