Abstract
Main observation and conclusionHigh‐performance, cost‐effective hole‐transport materials (HTMs) are greatly desired for the commercialization of perovskite solar cells (PVSCs). Herein, two new HTMs, TPA‐FO and TPA‐PDO, are devised and synthesized, which have a donor‐acceptor‐donor (D‐A‐D) type molecule design featuring carbonyl group‐functionalized arenes as the acceptor (A) units. The carbonyl group at the central core of HTMs can not only tune frontier molecular orbital (FMO) energy levels and surface wettability, but also can enable efficient surface passivation effects, resulting in reduced recombination loss. When employed as HTMs in inverted PVSCs without using dopant, TPA‐FO with one carbonyl group yields a high power conversion efficiency (PCE) of 20.24%, which is among the highest values reported in the inverted PVSCs with dopant‐free HTMs. More importantly, the facile one‐step synthetic process enables a low cost of 30 USD g–1 for TPA‐FO, much cheaper than the most studied HTMs used for high‐efficiency dopant‐free PVSCs. These results demonstrate the potential of D‐A‐D type molecules with carbonyl group‐functionalized arene core in developing the low‐cost dopant‐free HTMs toward highly efficient PVSCs.
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