Organic-inorganic hailed perovskites have emerged as thrilling materials for photovoltaic devices owing to their specific combination of the easy-processed, superb charge mobility and strong light absorption. However, it is still challenging to simultaneously obtain efficient and stable perovskite solar cells (PSCs) because of the defect-induced ions migration and the inherent low moisture tolerance. Herein, we report a perovskite photoabsorber with a novel alkylated amorphous perovskitoid/crystalline perovskite (a-PVKD/c-PVK) structure fabricated through a facile coordination-driven self-assembling process. We systematically elucidated the dissolution-reconstruction mechanisms of this a-PVKD/c-PVK structure and figured out the chemical interaction between the a-PVKD and the c-PVK. This judicious a-PVKD/c-PVK structure significantly hinders the moisture invasion, blocks the ion migration, and suppresses the nonradiative recombination, enabling to obtain a high efficiency over 21.5 % for MAPbI solar cells. The unencapsulated a-PVKD/c-PVK cell maintains more than 94 % of the initial efficiency after aging for 30 days (∼55% humidity), exhibiting a high long-term stability. Our work not only provides an effective way to synthesize novel perovskitoid materials, but also indicates the significant potential of a-PVKD/c-PVK architecture in PSCs.

中文翻译：

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迈向高效、防潮、防铅的钙钛矿太阳能电池：配位驱动重构均质非晶类钙钛矿/晶体钙钛矿光吸收剂

有机-无机钙钛矿因其易于加工、优异的电荷迁移率和强光吸收的特殊组合而成为令人兴奋的光伏器件材料。然而，由于缺陷引起的离子迁移和固有的低耐湿性，同时获得高效稳定的钙钛矿太阳能电池（PSC）仍然具有挑战性。在此，我们报道了一种钙钛矿光吸收剂，其具有新型烷基化无定形钙钛矿/结晶钙钛矿（a-PVKD/c-PVK）结构，通过简单的配位驱动自组装过程制造。我们系统地阐明了这种a-PVKD/c-PVK结构的溶解重建机制，并弄清楚了a-PVKD和c-PVK之间的化学相互作用。这种明智的a-PVKD/c-PVK结构显着阻碍了水分侵入、阻止离子迁移并抑制非辐射复合，从而使MAPbI太阳能电池获得超过21.5%的高效率。未封装的a-PVKD/c-PVK电池在老化30天（~55%湿度）后仍保持94%以上的初始效率，表现出较高的长期稳定性。我们的工作不仅提供了合成新型类钙钛矿材料的有效方法，而且表明了a-PVKD/c-PVK结构在PSC中的巨大潜力。