Xia, JianxingZhang, YiCavazzini, MarcoOrlandi, SimonettaDing, BinKanda, HiroyukiKlipfel, NadjaGao, Xiao-XinUl Ain, QuratJankauskas, VygintasRakstys, KasparasHu, RuiyuanQiu, ZeliangAsiri, Abdullah M.Kim, HobeomDyson, Paul J.Pozzi, GianlucaNazeeruddin, Mohammad Khaja2022-11-072022-11-072022-11-072022-10-2510.1002/anie.202212891https://infoscience.epfl.ch/handle/20.500.14299/192028WOS:000871729000001Hole-transporting materials (HTMs) based on the 10H, 10 ' H-9,9 '-spirobi [acridine] core (BSA50 and BSA51) were synthesized, and their electronic properties were explored. Experimental and theoretical studies show that the presence of rigid 3,6-dimethoxy-9H-carbazole moieties in BSA 50 brings about improved hole mobility and higher work function compared to bis(4-methoxyphenyl)amine units in BSA51, which increase interfacial hole transportation from perovskite to HTM. As a result, perovskite solar cells (PSCs) based on BSA50 boost power conversion efficiency (PCE) to 22.65 %, and a PSC module using BSA50 HTM exhibits a PCE of 21.35 % (6.5x7 cm) with a V-oc of 8.761 V and FF of 79.1 %. The unencapsulated PSCs exhibit superior stability to devices employing spiro-OMeTAD, retaining nearly 90 % of their initial efficiency after 1000 h operation output. This work demonstrates the high potential of molecularly engineered spirobi[acridine] derivatives as HTMs as replacements for spiro-OMeTAD.Chemistry, MultidisciplinaryChemistry36-dimethoxy-9h-carbazole acridinebis(4-methoxyphenyl)amine acridinehole transporting materialsperovskite solar cellsperovskite solar modulesdopant-freepassivationefficiencytext::journal::journal article::research article