Synergy of Low‐ and High‐Polarity Cations for Stabilizing 2D Perovskites
Perovskite solar cells (PSCs) employing three-dimensional/two-dimensional (3D/2D) heterostructures achieve high efficiencies but suffer from limited operational stability. Combining high-throughput experiments with first-principles simulations, we unveil that 2D perovskites are intrinsically susceptible to thermal degradation due to the deprotonation of spacer cations and subsequent escape of hydrogen iodide. Through artificial intelligence analysis of 278 distinct perovskites, we identify the surface electrostatic properties and molecular polarity of spacer cations as the key descriptors governing thermal resilience. Finally, we discover a bi-cationic 2D perovskite that integrates low-polarity phenylethylammonium with high-polarity pentafluorophenylethylammonium (5FBA), synergistically resolving phase segregation and thermal degradation beyond what either cation can achieve alone. The bi-cationic 3D/2D perovskite film stack shows suppressed ion migration owing to the robust interaction between 5FBA and 3D perovskite. Consequently, the resulting PSCs retain over 92% of their initial efficiency after 1500 h of thermal aging at 85°C and over 90% after 2000 h of continuous operation under 1-Sun illumination.
Authors
- Christoph Josef Brabec (ORCID: https://orcid.org/0000-0002-9440-0253)
- Lili Gao (ORCID: https://orcid.org/0000-0003-2950-0319)
- Yicheng Zhao (ORCID: https://orcid.org/0000-0002-8248-7021)
- Wenke Zhou (ORCID: https://orcid.org/0000-0002-3568-5789)
- Hongbin Xiao (ORCID: https://orcid.org/0000-0002-3199-3100)
- Jiyun Zhang (ORCID: https://orcid.org/0000-0001-6939-4771)
- Tianyu Lei (ORCID: https://orcid.org/0009-0005-7009-2427)
- Pingping Luo (ORCID: https://orcid.org/0000-0002-8277-2930)
- Shunchang Liu (ORCID: https://orcid.org/0000-0002-1990-5737)
- Yan Zhan (ORCID: https://orcid.org/0000-0002-1519-486X)
- Can Deng
- Liyi Yang
- Zhengwei Xu (ORCID: https://orcid.org/0009-0002-1419-2579)
- Li Tang
- Yushan Song (ORCID: https://orcid.org/0009-0004-2751-3225)
- Zhuojun Li
- Heng Li
- Yi Yang
- Tao Lin
- Karen Forberich
Institutions
- Hunan Institute of Science and Technology (CN)
- Xi'an University of Architecture and Technology (CN)
- University of Electronic Science and Technology of China (CN)
- National University of Singapore (SG)
- Friedrich-Alexander-Universität Erlangen-Nürnberg (DE)
- Helmholtz Institute Erlangen-Nürnberg (DE)
- Powder Metallurgy Institute (BY)
- National Engineering Research Center of Electromagnetic Radiation Control Materials (CN)
- Ministry of Education (TW)
- PLA Army Engineering University (CN)
- Beihang University (CN)
Publication Details
- Journal
- Advanced Materials
- Published
- 2026-09-24
- DOI
- https://doi.org/10.1002/adma.75134
- Primary Topic
- Perovskite Materials and Applications
- Type
- article
- Field-Weighted Citation Impact
- 0.00