作者：

Jing Chen^1#, Jia-Wei Yao^1#, Kai-Li Wang¹*，Ze-Kai Bian¹, Meng-Zhen Qiao¹, Chun-Hao Chen¹, Lei Huang¹, Yu Xia¹,Jian Fan¹, and Zhao-Kui Wang¹*

单位：

¹State Key Laboratory of Bioinspired Interfacial Materials Science, Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow University, Suzhou 215123, China

摘要：

The commercialization of perovskite solar cells (PSCs) is critically impeded by the inherent instability of the hole-transport layer (HTL), particularly the ion migration and interfacial degradation. These issues create a fundamental trade-off between achieving high efficiency and long-term operational stability. Here, we break this paradox through a “synergistic covalent-lock interfacial molecular functionalization” strategy. We molecularly engineer Spiro-AC, a novel crown-ether-functionalized derivative, which enables in situ multifunctional healing of the perovskite/HTL interface. The crown-ether units sequester migratory Li⁺ and passivate Pb²⁺ defects, effectively suppressing ion diffusion and non-radiative recombination. Spontaneous interfacial dipole formation and enhanced π-π stacking create cascading energy alignment, eliminating hole extraction barriers. Consequently, Spiro-AC-based PSCs achieve a champion power conversion efficiency of 26.06% and exceptional operational stability. This work establishes a transformative “closed-loop function-structure-stability” paradigm, providing a universal molecular design blueprint for stable and high-performance optoelectronic devices.

影响因子：

17.5

分区情况：

一区

链接：

https://doi.org/10.1016/j.matt.2025.102581