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Highlights: The use of novel nanographdiyne (o-TB-GDY) via anti-solvent additive engineering significantly enhances the nucleation and growth of perovskite crystals, leading to improved film quality, reduced film defects and suppressed non-radiative recombination. o-TB-GDY primarily remains on the surface of the perovskite films after crystallization, where it strongly interacts with the undercoordinated Pb defects for effective passivation. The optimized perovskite solar cells achieve a champion power conversion efficiency of 25.62% (certified as 25.01%) with good stability. Finding ways to produce dense and smooth perovskite films with negligible defects is vital for achieving high-efficiency perovskite solar cells (PSCs). Herein, we aim to enhance the quality of the perovskite films through the utilization of a multifunctional additive in the perovskite anti-solvent, a strategy referred to as anti-solvent additive engineering. Specifically, we introduce ortho-substituted-4′-(4,4″-di-tert-butyl-1,1′:3′,1″-terphenyl)-graphdiyne (o-TB-GDY) as an AAE additive, characterized by its sp/sp2-cohybridized and highly π-conjugated structure, into the anti-solvent. o-TB-GDY not only significantly passivates undercoordinated lead defects (through potent coordination originating from specific high π–electron conjugation), but also serves as nucleation seeds to effectively enhance the nucleation and growth of perovskite crystals. This markedly reduces defects and non-radiative recombination, thereby increasing the power conversion efficiency (PCE) to 25.62% (certified as 25.01%). Meanwhile, the PSCs exhibit largely enhanced stability, maintaining 92.6% of their initial PCEs after 500 h continuous 1-sun illumination at ~ 23 °C in a nitrogen-filled glove box. [ABSTRACT FROM AUTHOR]

Passivating the interfaces between the perovskite and charge transport layers is crucial for enhancing the power conversion efficiency (PCE) and stability in perovskite solar cells (PSCs). Here we report a dual‐interface engineering approach to improving the performance of FA0.85MA0.15Pb(I0.95Br0.05)3‐based PSCs by incorporating Ti3C2Clx Nano‐MXene and o‐TB‐GDY nanographdiyne (NanoGDY) into the electron transport layer (ETL)/perovskite and perovskite/ hole transport layer (HTL) interfaces, respectively. The dual‐interface passivation simultaneously suppresses non‐radiative recombination and promotes carrier extraction by forming the Pb−Cl chemical bond and strong coordination of π‐electron conjugation with undercoordinated Pb defects. The resulting perovskite film has an ultralong carrier lifetime exceeding 10 μs and an enlarged crystal size exceeding 2.5 μm. A maximum PCE of 24.86 % is realized, with an open‐circuit voltage of 1.20 V. Unencapsulated cells retain 92 % of their initial efficiency after 1464 hours in ambient air and 80 % after 1002 hours of thermal stability test at 85 °C. [ABSTRACT FROM AUTHOR]

Highly crystalized perovskite film with smooth surface is of great importance to obtain high photovoltaic performances. Herein, UV irradiation is applied to the perovskite films during their thermal annealing process. It is revealed that UV irradiation treatment can largely improve perovskite crystallization and reduce defects. This greatly improves power conversion efficiency (PCE) and environmental stability of the resulted solar cells (ITO/SnO2/perovskite/Spiro‐OMeTAD/Au). By combining CH3O‐PEAI surface passivation, an outstanding PCE of 23.24% is achieved. [ABSTRACT FROM AUTHOR]

The low-cost material antimony trifluoride (SbF3) was doped into commonly used tin dioxide (SnO2) for the first time, and the SbF3-doped SnO2 as an electron-transport layer (ETL) was successfully applied in perovskite solar cells (PSCs). After the SbF3 doping, the optimized photovoltaic power conversion efficiency (PCE) was significantly enhanced from 19.89% to 21.42%. The effects of SbF3 on the device performance were then systematically investigated. The results show that the electron mobility of the ETL is markedly increased and the quality of the ETL/perovskite interface is effectively improved, which is helpful to promote the electron-transport efficiency in the ETL as well as the electron-extraction ability from the perovskite to the ETL. Besides, the perovskite grain size is clearly increased and the trap state density in the bulk perovskite is significantly decreased, both of which can greatly suppress charge-carrier recombination in the perovskite film. Moreover, the device based on the SbF3-doped SnO2 ETL displays negligible hysteresis and excellent stability. [ABSTRACT FROM AUTHOR]

Regulating the electron transport layer (ETL) has been an effective way to promote the power conversion efficiency (PCE) of perovskite solar cells (PSCs) as well as suppress their hysteresis. Herein, the SnO2 ETL using a cost‐effective modification material rubidium fluoride (RbF) is modified in two methods: 1) adding RbF into SnO2 colloidal dispersion, F and Sn have a strong interaction, confirmed via X‐ray photoelectron spectra and density functional theory results, contributing to the improved electron mobility of SnO2; 2) depositing RbF at the SnO2/perovskite interface, Rb+ cations actively escape into the interstitial sites of the perovskite lattice to inhibit ions migration and reduce non‐radiative recombination, which dedicates to the improved open‐circuit voltage (Voc) for the PSCs with suppressed hysteresis. In addition, double‐sided passivated PSCs, RbF on the SnO2 surface, and p‐methoxyphenethylammonium iodide on the perovskite surface, produces an outstanding PCE of 23.38% with a Voc of 1.213 V, corresponding to an extremely small Voc deficit of 0.347 V. [ABSTRACT FROM AUTHOR]

Trap‐assisted non‐radiative recombination losses and moisture‐induced degradation significantly impede the development of highly efficient and stable inverted (p–i–n) perovskite solar cells (PSCs), which require high‐quality perovskite bulk. In this research, we mitigate these challenges by integrating thermally stable perovskite layers with Lewis base covalent organic frameworks (COFs). The ordered pore structure and surface binding groups of COFs facilitate cyclic, multi‐site chelation with undercoordinated lead ions, enhancing the perovskite quality across both its bulk and grain boundaries. This process not only reduces defects but also promotes improved energy alignment through n‐type doping at the surface. The inclusion of COF dopants in p–i–n devices achieves power conversion efficiencies (PCEs) of 25.64 % (certified 24.94 %) for a 0.0748‐cm2 device and 23.49 % for a 1‐cm2 device. Remarkably, these devices retain 81 % of their initial PCE after 978 hours of accelerated aging at 85°C, demonstrating remarkable durability. Additionally, COF‐doped devices demonstrate excellent stability under illumination and in moist conditions, even without encapsulation. [ABSTRACT FROM AUTHOR]