To date, doped 2,2,7,7-Tetrakis(N,N-dip-methoxyphenylamine)-9,9-spirobifluorene (Spiro-OMeTAD) is still state-of-the-art hole transport material (HTM) for inverted perovskite solar cells (PeSCs). Nevertheless, hydroscopic dopants usually lead to accelerated degradation of perovskite and hence reduce the device durability especially those based on all-inorganic perovskite. In this work, we report a series of dopant-free mixtures (SpiPA) of hydrophilic Spiro-OMeTAD and hydrophobic poly(triarylamine) (PTAA), which exhibit tunable surface wettability due to the dominant lateral phase separation. When applying them as HTM for inverted CsPbI₂Br PeSCs, SpiPA_-II based devices yield enhanced efficiency up to 12.52% with significantly reduced hysteresis, as compared to the devices with other mixed HTLs (SpiPA_-I, SpiPA_-III, SpiPA_-IV) and conventional HTLs including pristine Spiro-OMeTAD (10.26%), PTAA (9.05%) and NiO_x (10.75%). Additionally, the corresponding mechanism has been studied in detail.

迄今为止，掺杂的2,2,7,7-四（N，N-二甲氧基苯胺）-9,9-螺双芴（Spiro-OMeTAD）仍然是用于倒置的最新空穴传输材料（HTM）钙钛矿太阳能电池（PeSCs）。然而，吸湿性掺杂剂通常导致钙钛矿的加速降解，并因此降低了器件的耐用性，特别是那些基于全无机钙钛矿的器件。在这项工作中，我们报告了一系列亲水性Spiro-OMeTAD和疏水性聚三芳基胺（PTAA）的无掺杂剂混合物（SpiPA），由于主要的横向相分离，这些混合物表现出可调节的表面润湿性。当将它们作为HTM应用于反向CsPbI ₂ Br PeSCs时，SpiPA _-II与具有其他混合HTL（SpiPA _-I，SpiPA _-III，SpiPA _-IV）和包括原始Spiro-OMeTAD（10.26％），PTAA的常规HTL的设备相比，基于这些设备的设备可将效率提高多达12.52％，并显着降低了磁滞（9.05％）和NiO _x（10.75％）。另外，已经详细研究了相应的机制。