CsPbIBr₂ has attracted great attention due to its balanced bandgap and stability features. However, one-step prepared CsPbIBr₂ films are generally of poor quality, hindering the performance improvement of the resulting perovskite solar cells (PSCs). Herein, we report the fabrication of high-performance carbon-based, all-inorganic CsPbIBr₂ PSCs with a double-side modification strategy using PEAI/PEABr. We tune the crystallization behavior and passivate the defects of CsPbIBr₂ films with modifications of their bottom and top surfaces with PEAI and PEABr, respectively. This causes the PEA cation to form a double layer of armor on both sides of the CsPbIBr₂ precursor film and can provide the anions of the required I and Br. The collaborative strategy of crystallization and defect passivation for CsPbIBr₂ films is exceptionally effective. It produces a fully covered CsPbIBr₂ film with an average grain size increase of more than 50%, few grain boundaries, and high crystallinity. Moreover, this strategy also suppresses pinhole formation, reduces the charge trap density, and prolongs the carrier recombination lifetime. Hence, carbon-based all-inorganic PSCs with the desired CsPbIBr₂ films yield an optimized efficiency of 9.96% with a particularly high photovoltage of 1.32 V. Our work provides guidance for simultaneous crystallization control and defect passivation to further improve the performance of PSCs.

CsPbIBr ₂由于其平衡的带隙和稳定性特征而引起了极大的关注。然而，一步制备的CsPbIBr ₂薄膜通常质量较差，阻碍了所得钙钛矿太阳能电池（PSC）的性能提升。在此，我们报告了使用 PEAI/PEABr 采用双面改性策略制备高性能碳基全无机 CsPbIBr _{2 PSC。}我们调整结晶行为并钝化 CsPbIBr ₂薄膜的缺陷，分别用 PEAI 和 PEABr 修改其底面和顶面。_{这导致 PEA 阳离子在 CsPbIBr 2}的两侧形成双层装甲前体膜并能提供所需的 I 和 Br 的阴离子。CsPbIBr ₂薄膜的结晶和缺陷钝化协同策略非常有效。它生产的全覆盖CsPbIBr ₂薄膜平均晶粒尺寸增加超过50%，晶界少，结晶度高。此外，该策略还抑制了针孔的形成，降低了电荷陷阱密度，延长了载流子复合寿命。_{因此，具有所需 CsPbIBr 2}薄膜的碳基全无机 PSC 可产生 9.96% 的优化效率和 1.32 V 的特别高的光电压。我们的工作为同步结晶控制和缺陷钝化提供了指导，以进一步提高 PSC 的性能。