Abstract
Abstract4‐Tert‐butylpyridine (tBP) is an important additive in triarylamine‐based organic hole‐transporting materials (HTMs) for improving the efficiency and steady‐state performance of perovskite solar cells (PVSCs). However, the low boiling point of tBP (196 °C) significantly affects the long‐term stability and device performance of PVSCs. Herein, the design and synthesis of a series of covalently linked Spiro[fluorene‐9,9′‐xanthene] (SFX)‐based organic HTMs and pyridine derivatives to realize efficient and stable planar PVSCs are reported. One of the tailored HTMs, N2,N2,N7,N7‐tetrakis(4‐methoxyphenyl)‐3′,6′‐bis(pyridin‐4‐ylmethoxy) spiro[fluorene‐9,9′‐xanthene]‐2,7‐diamine (XPP) with two para‐position substituted pyridines that immobilized on the SFX core unit shows a high power conversion efficiency (PCE) of 17.2% in planar CH3NH3PbI3‐based PVSCs under 100 mW cm−2 AM 1.5G solar illumination, which is much higher than the efficiency of 5.5% that using the well‐known 2,2′,7,7′‐tetrakis‐(N,N‐di‐p‐methoxy‐phenyl‐amine)9,9′‐spirobifluorene (Spiro‐OMeTAD) as HTM (without tBP) under the same condition. Most importantly, the pyridine‐functionalized HTM‐based PVSCs without tBP as additive show much better long‐term stability than that of the state‐of‐the‐art HTM Spiro‐OMeTAD‐based solar cells that containing tBP as additive. This is the first case that the tBP‐free HTMs are demonstrated in PVSCs with high PCEs and good stability. It paves the way to develop highly efficient and stable tBP‐free HTMs for PVSCs toward commercial applications.
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