Triphenylamine-Based Hole-Transporting Ligands for 2D/3D FAPbI<sub>3</sub> Perovskite Solar Cells
Two-dimensional (2D) perovskites suffer from poor charge transport due to the insulating nature of typically used organic spacers. Here, we develop a triphenylamine (TPA)-functionalized semiconducting ligand, namely, DPA-PEAI, in which the TPA moiety is tethered to the ethylammonium cation. Crystallographic analysis of n = 1 2D perovskite (DPA-PEA)2PbI4 reveals that the propeller-like geometry and enriched phenyl rings of the TPA tail enable the formation of multifarious π-stacking interconnections between neighboring ligands. Theoretical calculations further unveil that both the binding energy and hole transfer integral are augmented between the adjacent DPA-PEA cations, in contrast to the widely used phenylethylammonium (PEA) counterpart. This cross-electronic coupling feature allows the formation of multiple hole-transfer pathways within DPA-PEA-based 2D perovskites, enabling efficient out-of-plane charge transport, as confirmed by a set of characterizations. As a consequence, 2D/3D FAPbI3-based PSCs employing DPA-PEAI afford a champion efficiency of 25.7%, which ranks among the best efficiencies reported for conjugative ligands.
Authors
- Zhiguang Sun (ORCID: https://orcid.org/0000-0002-5098-9983)
- Hin‐Lap Yip (ORCID: https://orcid.org/0000-0002-5750-9751)
- Liang Zhao (ORCID: https://orcid.org/0000-0001-8197-6686)
- Qiang Yue (ORCID: https://orcid.org/0000-0002-7962-7951)
- Rui Cai (ORCID: https://orcid.org/0000-0002-9987-5071)
- Tianshu Li (ORCID: https://orcid.org/0000-0002-0529-543X)
- Yingguo Yang (ORCID: https://orcid.org/0000-0002-1749-2799)
- Huaiman Cao (ORCID: https://orcid.org/0000-0002-0536-2428)
- Xufan Zheng (ORCID: https://orcid.org/0009-0004-1200-5287)
- Ze Yu (ORCID: https://orcid.org/0000-0003-0680-6622)
- Fei Li (ORCID: https://orcid.org/0000-0002-3686-7576)
- Lijun Zhang (ORCID: https://orcid.org/0000-0002-6438-5486)
- Yulong Chen (ORCID: https://orcid.org/0000-0002-5906-2738)
- Liangyu Zhao
- Yong Zhu
- Shouye Dai
Institutions
- City University of Hong Kong (HK)
- Jilin University (CN)
- Chinese Academy of Sciences (CN)
- Fudan University (CN)
- Dalian University of Technology (CN)
- Integrated Optoelectronics (Norway) (NO)
- Shanghai Advanced Research Institute (CN)
- Shanghai Institute of Applied Physics (CN)
- Division of Materials Science and Engineering (AU)
- Advanced Research Institute (US)
- Jilin Medical University (CN)
- State Key Laboratory of Fine Chemicals
Publication Details
- Journal
- ACS Energy Letters
- Published
- 2025-03-31
- DOI
- https://doi.org/10.1021/acsenergylett.5c00471
- Citations
- 20
- Primary Topic
- Perovskite Materials and Applications
- Type
- article
- Field-Weighted Citation Impact
- 14.61