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The low cost and scalability advantages of printable mesoscopic perovskite solar cells (p‐MPSCs) are impaired by the issue of limited power conversion efficiency (PCE). Herein, the PCE of p‐MPSCs is improved by introducing the polymer additive polyacrylonitrile (PAN) into the formamidinium (FA)‐based perovskite for crystallization and defect modulation. PAN forms hydrogen bond and coordination bond with halide perovskite through its C≡N group. Such interactions improve the crystallization and filling of FA‐based perovskite in the mesoscopic scaffold and bring a long carrier lifetime by passivating defects. The synergy improves the PCE of p‐MPSCs from 16.80% to 18.33%. Meanwhile, the hydrophobic nature of PAN enhances the device's resistance against moisture. This work demonstrates that the polymer additive is a promising choice for breaking the PCE limit of p‐MPSCs. [ABSTRACT FROM AUTHOR]

In the rapid development of perovskite solar cells (PSCs), additive engineering has played a significant role for perovskite crystallization and passivation. The high density of defects at perovskite grain boundaries in the mesoporous scaffold leads to severe nonradiative recombination, which results in severe voltage loss. Herein, a sulfur‐containing Lewis base 2‐(methylthio)ethylamine hydrochloride (MTEACl) is applied in the perovskite precursor solution for printable mesoscopic PSCs with triple‐mesoscopic layer structure. Due to the strong electron donating ability of sulfur, the MTEACl can strongly interact with Pb2+, which can effectively passivate the defects of the perovskite. Correspondingly, the trap density of the perovskite is reduced, contributing to the improvement of power conversion efficiency from 15.18% to 17.17% and open circuit voltage to 995 mV. [ABSTRACT FROM AUTHOR]

Triple‐mesoscopic perovskite solar cells (PSCs) have attracted intensive attention due to the high stability, simple fabrication process, and low material cost. In this structure, the perovskite layer is hosted by a triple‐mesoscopic scaffold of TiO2/ZrO2/carbon, and thus the crystal quality is sensitive to the thermal annealing process. Typically, the annealing process is conducted in a petri dish, for which the solvent evaporation of the perovskite precursor is slowed down, but not controllable and designable. To control the solvent evaporation, annealing chambers are first designed with different shape and vapor releasing channels. Then, physical simulations are performed by a finite element method, and it is found out that the chamber with a crowned top and releasing channels on the bottom sides can realize homogeneous distribution of the solvent vapor. To verify the simulation results, chambers are fabricated by 3D printing technique, for which the printing deviation can be as low as 100 µm. By balancing the solvent evaporation and release, the optimal solvent evaporation is achieved of the perovskite precursor in the triple‐mesoscopic scaffold. This work offers a method to obtain homogeneous distribution of solvent vapor, and provides a new insight into understanding the influence of solvent evaporation during the thermal annealing process for PSCs. [ABSTRACT FROM AUTHOR]

Printable hole‐conductor‐free perovskite solar cells (PSCs) have attracted intensive research attention due to their high stability and simple manufacturing process. However, the cells have suffered severe potential loss in the absence of the hole transporting layer. The dimensionality of the perovskite absorber in the mesoporous carbon electrodes by conducting post‐treatments is reduced. The low‐dimensional perovskites possess wide‐bandgaps and form type‐II band alignment, favoring directional charge transportation and thus enhancing the device performance. For the cells using MAPbI3 (MA = methylammonium) as the light absorber, the open‐circuit voltage (VOC) is significantly enhanced from 0.92 to 0.98 V after posttreatment, delivering an overall efficiency of 16.24%. For the cells based on FAPbI3 (FA = formamadinium), a high efficiency of 17.47% is achieved with VOC of 1.02 V, which are both the highest reported values for printable hole‐conductor‐free PSCs. This strategy provides a facile method for tuning the energy level alignment for mesoscopic perovskite‐based optoelectronics. [ABSTRACT FROM AUTHOR]

Perovskite solar cells are regarded as the most promising and disruptive photovoltaic of the new generation. Carbon‐based hole‐conductor‐free printable mesoscopic perovskite solar cells (p‐MPSCs) with three mesoscopic layers have garnered considerable interest owing to their simple manufacturing process and cost‐effective raw materials, signaling the potential for commercialization. However, the energy level mismatch between the perovskite and the carbon electrode as well as defects at perovskite grain boundaries inevitably lead to additional non‐radiative carrier recombination and large voltage loss. In this study, a facile in situ reconstruction post‐treatment approach is employed to integrate lead sulfide (PbS) and the two‐dimensional (2D) perovskite K2PbI4 into the mesoporous scaffolds of p‐MPSCs. In this way, grain boundary defects are effectively passivated and the ion migration is suppressed by introducing 2D perovskite K2PbI4 at grain boundaries. Besides, the incorporation of PbS leads to the downward shift of the Fermi level for perovskite, which enhances hole collection within the device by optimizing band alignment at the perovskite/carbon interface. Consequently, an improved efficiency exceeding 20% is achieved for p‐MPSCs with no significant performance degradation observed over a storage period of 235 days. This strategy provides a facile and novel approach toward fabricating highly efficient and stable p‐MPSCs. [ABSTRACT FROM AUTHOR]