It is challenging to realize high efficiency and stability in perovskite photovoltaics simultaneously. Here, we show supramolecular chemistry using macrocyclic crown ether to prepare high-performance metal-halide perovskite films. Multiple cooperative supramolecular interactions between perovskites and crown ether are built, and superior defect passivation is achieved. A thin crystalline capping layer on top of perovskites is constructed to synergistically passivate the perovskite surface defects and protect the underlying films from environmental damage. The capping layer is confirmed to be a unique two-dimensional (2D) crystal with a highly ordered, high-crystallinity lamellae structure and face-sharing lead-halide octahedral organization, providing surface protection on the perovskite matrix. Lead-halide perovskite solar cells (PSCs) with supramolecular passivation and a 2D crystal interlayer demonstrated remarkable photovoltaic efficiency and stability improvements, offering a 21.5% efficiency and improved environmental stabilities under moisture, ultraviolet (UV) irradiation, and thermal stress. Our work provides a strategy to achieve efficient and stable lead-halide perovskite-based devices by crown ether-induced supramolecular passivation and 2D crystal interlayer protection.

同时实现钙钛矿光伏的高效率和稳定性具有挑战性。在这里，我们展示了使用大环冠醚制备高性能金属卤化物钙钛矿薄膜的超分子化学。钙钛矿和冠醚之间建立了多重协同超分子相互作用，实现了优异的缺陷钝化。在钙钛矿顶部构建一个薄的结晶覆盖层，以协同钝化钙钛矿表面缺陷并保护底层薄膜免受环境损害。盖层被证实是一种独特的二维 (2D) 晶体，具有高度有序、高结晶度的薄片结构和共享面的卤化铅八面体组织，为钙钛矿基质提供表面保护。具有超分子钝化和二维晶体夹层的卤化铅钙钛矿太阳能电池 (PSC) 显示出显着的光伏效率和稳定性改进，在潮湿、紫外线 (UV) 照射和热应力下提供 21.5% 的效率和改善的环境稳定性。我们的工作提供了一种策略，通过冠醚诱导的超分子钝化和二维晶体层间保护来实现高效稳定的卤化铅钙钛矿基器件。