Core structures with linear, planar, and spiral conformations have been designed as triphenylamine (TPA)-based hole-transporting materials (HTMs), which are the most prevalent small molecular HTMs in perovskite solar cells (PSCs). However, most of the reported TPA-based HTMs cannot achieve sufficient balance between efficiency and stability, which is governed by core structures. Herein, a sym-penta(N,N-bis(4-methoxyphenyl)aniline)corannulene (cor-OMePTPA) featuring a corannulene core and five TPA peripheral arms is designed as alternative HTM. Planar negative-intrinsic-positive (n-i-p) PSCs with cor-OMePTPA exhibit champion efficiencies of 20% and maintain 86% of their initial performances for more than 1,000 h after thermal annealing at 60°C. Compared with spiro-OMeTAD, cor-OMePTPA-based PSCs show slightly lower efficiencies but much better thermal stabilities. The main merit of cor-OMePTPA lies in its bimolecular interpenetration capability with noncovalent interactions to modulate the HTM configurations from single-molecular curvature to bimolecular planarity, thereby providing promising opportunities to achieve excellent balance between efficiency and stability.

具有线性、平面和螺旋构象的核心结构已被设计为基于三苯胺 (TPA) 的空穴传输材料 (HTM)，这是钙钛矿太阳能电池 (PSC) 中最普遍的小分子 HTM。然而，大多数报道的基于 TPA 的 HTM 无法在效率和稳定性之间实现足够的平衡，这是由核心结构控制的。这里，一个符号-penta( N,N-双（4-甲氧基苯基）苯胺）corannulene (cor-OMePTPA) 具有一个 corannulene 核心和五个 TPA 外围臂，被设计为替代 HTM。具有 cor-OMePTPA 的平面负本征正 (nip) PSC 表现出 20% 的最佳效率，并在 60°C 热退火后 1,000 小时内保持其初始性能的 86%。与 spiro-OMeTAD 相比，基于 cor-OMePTPA 的 PSC 的效率略低，但热稳定性要好得多。cor-OMePTPA 的主要优点在于其具有非共价相互作用的双分子互穿能力，以调节 HTM 构型从单分子曲率到双分子平面性，从而为实现效率和稳定性之间的出色平衡提供了有希望的机会。