Sequential deposition is certified as an effective technology to obtain high‐performance perovskite solar cells (PVSCs), which can be derivatized into large‐scale industrial production. However, dense lead iodide (PbI₂) causes incomplete reaction and unsatisfactory solution utilization of perovskite in planar PVSCs without mesoporous titanium dioxide as a support. Here, a novel autonomously longitudinal scaffold constructed by the interspersion of in situ self‐polymerized methyl methacrylate (sMMA) in PbI₂ is introduced to fabricate efficient PVSCs with excellent flexural endurance and environmental adaptability. By this strategy perovskite solution can be confined within an organic scaffold with vertical crystal growth promoted, effectively inhibiting exciton accumulation and recombination at grain boundaries. Additionally, sMMA cross‐linked perovskite network can release mechanical stress and occupy the main channels for ion migration and water/oxygen permeation to significantly improve operational stability, which opens up a new strategy for the commercial development of large‐area PVSCs in flexible electronics.

中文翻译：

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通过平面钙钛矿太阳能电池的自主纵向支架控制晶体生长。

顺序沉积技术是获得高性能钙钛矿太阳能电池（PVSC）的有效技术，可将其衍生化为大规模工业生产。但是，在没有介孔二氧化钛作为载体的情况下，平面型PVSC中的致密碘化铅（PbI ₂）引起钙钛矿的不完全反应和溶液利用不令人满意。在这里，通过在PbI ₂中原位自聚合的甲基丙烯酸甲酯（sMMA）的散布构造了一种新型的自主纵向支架被引入以制造具有出色的挠曲耐久性和环境适应性的高效PVSC。通过这种策略，钙钛矿溶液可以被限制在有机支架中，并促进了垂直晶体的生长，有效地抑制了激子的积累和在晶界的重组。此外，sMMA交联的钙钛矿网络可以释放机械应力并占据离子迁移和水/氧渗透的主要渠道，从而显着提高操作稳定性，这为柔性电子领域大面积PVSC的商业开发开辟了新的战略。