writer：Mengran Ma, Yege Jing, Lin Liu, Chen Wang, Ning Zhang, Shanpeng Wen, Guangshan, Zhu
keywords：PEDOT:PSS, COF, interface, perovskite solar cells
source：期刊
specific source：Chem. Eng. J.
Issue time：2025年
Poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) is a widely used hole-transporting layer (HTL) in perovskite solar cells (PSCs), but its acidity, hygroscopicity, and interfacial energy level mismatches significantly hinder device performance. To address these challenges, we developed a π-π interaction-driven strategy for in situ growth of ultrathin covalent organic framework (COF) membranes on PEDOT:PSS. The ordered COF architecture establishes seamless hole transport paths, achieves interfacial energy level alignment, modulates perovskite crystallization, and synergistically enhancing interfacial charge dynamics. By optimizing the COF membrane thickness, the p-i-n PSCs demonstrate remarkable synergistic enhancement in both power conversion efficiency (PCE) and long-term storage stability. This work not only mitigates interfacial challenges in PEDOT:PSS-based devices, but also achieves a conceptual breakthrough in supramolecular interface engineering.