Beyond the Sum of Its Parts: Alkyl-Chain Engineering Unlocks Dopant-Free Pyrene-Based Antenna Molecules for Efficient Perovskite Solar Cells

Xing, Feng, Li, Shaoling, Li, Jialin, Zhu, Zhehui, Liu, Wei, Chen, Junru, Wang, Xiaohui, Redshaw, Carl ORCID: https://orcid.org/0000-0002-2090-1688 and Ouyang, Xinhua (2026) Beyond the Sum of Its Parts: Alkyl-Chain Engineering Unlocks Dopant-Free Pyrene-Based Antenna Molecules for Efficient Perovskite Solar Cells. Angewandte Chemie International Edition, 65 (17). ISSN 1433-7851

Microsoft Word (OpenXML) (20260305-Manu-revised) - Accepted Version Available under License Creative Commons Attribution. Download (3MB)

Abstract

The pursuit of high-performance, dopant-free hole-transporting materials (HTMs) is central to advancing the efficiency and stability of perovskite solar cells (PSCs). Herein, three pyrene-based HTMs (PyTPA-9C, PyTPA-10C, and PyTPA-13C) were synthesized by covalently linking two pyrene-triphenylamine precursor units, which display a pronounced antenna effect analogous to the precursor which is quantitatively defined by a positive correlation between the number of TPA antenna moieties and key photophysical parameters (such as molar absorption coefficient and fluorescence quantum yield). Critically, the odd-even effect of the alkyl spacer plays a significant role in modulating the molecular conformation and electronic structure. Moreover, PyTPA-10C, featuring an even-carbon decyl chain as a dopant-free HTMs in n-i-p structured PSCs, achieves a champion power conversion efficiency (PCE) of 25.47%, representing the highest reported values for n-i-p PSCs employing dopant-free, organic small-molecule HTMs. Comprehensive analysis reveals that PyTPA-10C enables superior hole extraction/transport, effectively suppresses charge recombination, and passivates interfacial defects. Consequently, unencapsulated devices retain over 90% of their initial PCE after 1000 h under continuous heating and illumination at 65°C and 50%–60% relative humidity. This study not only presents high-performing materials but also establishes a general molecular design strategy: the integration of an “antenna effect” with precise alkyl-chain engineering.

Item Type:	Article
Additional Information:	Data Availability Statement: The data that support the findings of this study are available on request from the corresponding author. The data are not publicly available due to privacy or ethical restrictions.
Uncontrolled Keywords:	alkyl-chain engineering,antenna molecules,hole-transport material,perovskite solar cells,pyrene
Faculty \ School:	Faculty of Science > School of Chemistry, Pharmacy and Pharmacology
Related URLs:	https://www.scopus.com/pages/publication...
Depositing User:	LivePure Connector
Date Deposited:	08 Jul 2026 14:56
Last Modified:	13 Jul 2026 08:02
URI:	https://ueaeprints.uea.ac.uk/id/eprint/103794
DOI:	10.1002/anie.2660254

Downloads

Actions (login required)

View Item