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Spiro-OMeTAD is the most-employed molecular hole-transporting material (HTM) in n-i-p perovskite solar cells (PSCs). Ease of processing from solution and good filmability on top of the perovskite photo-active layer are characteristics that make this HTM outstanding and incomparable for the role. However, chemical doping with both tert-butylpyridine (tBP) and lithium bis(trifluoromethylsulfonyl)imide (LiTFSI), coupled with further oxidation steps, is required in order to achieve high hole mobility and conductivity. Previous investigations have revealed that tBP is fundamental for addressing the best morphology in the hole-transporting layer during processing. Here, we provide spectroscopic evidence of the detrimental impact on long-term conservation of Spiro-OMeTAD structural and electrical properties when tBP is used as an additive. These aspects are crucial for the future design and understanding of new molecular HTMs for PSCs.

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Commercialization of lead halide perovskite-based devices is hindered by their instability towards environmental conditions. In particular, water promotes fast decomposition, leading to a drastic decrease in device performance. Integrating water-splitting active species within ancillary layers to the perovskite absorber might be a solution to this, as they could convert incoming water into oxygen and hydrogen, preserving device performance. Here, we suggest that a CuSCN nanoplatelete/p-type semiconducting polymer composite, combining hole extraction and transport properties with water oxidation activity, transforms incoming water molecules and triggers the in situ p-doping of the conjugated polymer, improving transport of photocharges. Insertion of the nanocomposite into a lead perovskite solar cell with a direct photovoltaic architecture causes stable device performance for 28 days in high-moisture conditions. Our findings demonstrate that the engineering of a hole extraction layer with possible water-splitting additives could be a viable strategy to reduce the impact of moisture in perovskite devices.

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