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Interfacial trap-assisted non-radiative recombination and residual stress impede the further increase of power conversion efficiency (PCE) and stability of the methylammonium-free (MA-free) perovskite solar cells (PSCs). Here, we report an interfacial defect passivation and stress release strategy through employing the multi-active-site Lewis base ligand (i.e., (5-mercapto-1,3,4-thiadiazol-2-ylthio)­acetic acid (MTDAA)) to modify the surface and grain boundaries (GBs) of MA-free perovskite films. Both experimental and theoretical results confirm strong chemical interactions between multiple active sites in the MTDAA molecule and undercoordinated Pb2+ at the surface or GBs of perovskite films. It is demonstrated theoretically that multi-active-site adsorption is more favorable thermodynamically as compared to single-active-site adsorption, regardless of PbI2 termination and formamidinium iodide (FAI) termination types. MTDAA modification results in much reduced defect density, increased carrier lifetime, and almost thoroughly released interfacial residual stress. Upon MTDAA passivation, the PCE is boosted from 20.26% to 21.92%. The unencapsulated device modified by MTDAA maintains 99% of its initial PCE after aging under the relative humidity range of 10–20% for 1776 h, and 91% after aging at 60 °C for 1032 h.

Bulk and interfacial nonradiative recombination hinders the further enhancement of power conversion efficiency (PCE) and stability of SnO2-based planar perovskite solar cells (PSCs). To date, it is still a huge...

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We modified perovskite/Spiro‐OMeTAD interface by using two novel phosphonium salts containing PF6− counter anion (i.e., ClTPPPF6 and BrTPPPF6). The cation and anion in phosphonium salts possess not only ionic bonds but also coordination bonds with perovskites. The anion and cation vacancies at the surface and GBs of perovskite films can be filled by phosphonium cations and PF6− anions, respectively, resulting in reduced defect density and prolonged carrier lifetimes. The stronger chemical interaction and accordingly better defect passivation were certified for BrTPPPF6 than ClTPPPF6. As a result, the devices modified by ClTPPPF6 and BrTPPPF6 deliver a PCE of 21.73% and 22.15%, respectively, which far exceed 20.6% of the control device. The unsealed BrTPPPF6 modified device maintains 98.2% of its initial efficiency value after thermal aging of 1320 h whereas merely 84.7% for the control device. 96.4% of its original efficiency was retained for BrTPPPF6‐modified device after ambient exposure of 2016 h.

Dion-Jacobson (DJ) quasi-2D perovskite solar cells (PSCs) have received increasing attention due to their greater potentials in realizing efficient and stable quasi-2D PSCs relative to their Ruddlesden–Popper counterpart. The substitution of methylammonium (MA+) with formamidinium is expected to be able to further increase the stability and power conversion efficiency (PCE) of DJ quasi-2D PSCs. Herein, we report a multifunctional additive strategy for preparing high-quality MA-free DJ quasi-2D perovskite films, where 1,1′-carbonyldi­(1,2,4-triazole) (CDTA) molecules are incorporated into the perovskite precursor solution. CDTA modification can control phase distribution, enlarge grain size, modulate crystallinity and crystal orientation, and passivate defects. After CDTA modification, more favorable gradient phase distribution and accordingly gradient band alignment are formed, which is conducive to carrier transport and extraction. The improved crystal orientation can facilitate carrier transport and collection. The enlarged grain size and effective defect passivation contribute to reduced defect density. As a result, the CDTA-modified device delivers a PCE of 16.07%, which is one of the highest PCEs ever reported for MA-free DJ quasi-2D PSCs. The unencapsulated device with CDTA maintains 92% of its initial PCE after aging under one sun illumination for 360 h and 86% after aging at 60 °C for 360 h.

Minimizing bulk and interfacial nonradiative recombination losses is key to further improving the photovoltaic performance of perovskite solar cells (PSC) but very challenging. Herein, we report a gradient dimensionality engineering to simultaneously passivate the bulk and interface defects of perovskite films. The 2D/3D heterojunction is skillfully constructed by the diffusion of an amphiphilic spacer cation from the interface to the bulk. The 2D/3D heterojunction engineering strategy has achieved multiple functions, including defect passivation, hole extraction improvement, and moisture stability enhancement. The introduction of tertiary butyl at the spacer cation should be responsible for increased film and device moisture stability. The device with 2D/3D heterojunction engineering delivers a promising efficiency of 22.54% with a high voltage of 1.186 V and high fill factor of 0.841, which benefits from significantly suppressed bulk and interfacial nonradiative recombination losses. Moreover, the modified devices demonstrate excellent light, thermal, and moisture stability over 1000 h. This work paves the way for the commercial application of perovskite photovoltaics.

The deep‐level defects at grain boundary (GB) result in serious trap‐assisted non‐radiative recombination. Moreover, the degradation of perovskite films is preferentially triggered by the attack of GBs by water and/or oxygen. Therefore, it is urgently needed to develop a multifunctional GB tailoring strategy to address the abovementioned issues. Herein, a self‐formed multifunctional GB passivation strategy is reported, where an ultrathin GB passivation layer is in situ constructed via incorporating K2SO4 into perovskite precursor solution. The self‐formed GB passivation layer plays multiple functions, including crystallization improvement, defect passivation, and moisture resistance. The GB manipulation strategy endows perovskite films reduced defect density, boosted carrier lifetime, and thus suppressed non‐radiative recombination, which contributes to efficiency enhancement from 20.39% to 22.40%. The GB tailoring approach makes the unencapsulated target device exhibit no degradation while the control device degrades to 93% of its initial power conversion efficiency after 1200 h ambient exposure with a relative humidity of 10–20%. The modified device maintains 98% of its original efficiency after aging at 60 °C for 1200 h, whereas only 89% for the control device. Herein, the importance of developing an in situ GB modification strategy in enhancing performance of perovskite photovoltaics is highlighted.