An entropy-regulating molecular lock stabilizes formamidinium lead halide perovskite

• 成果类型: Article
• 署名作者: Miao, Tianyin; Liu, Sanwan; Lei, Xia; Zhang, Yong; Li, Wenpei; Zhou, Qisen; Wang, Jianan; Emelianov, Nikita A.; Ozerova, Victoria V.; Bolshakova, Valeria S.; Wang, Wenqiang; Zhou, Zheng; Zhu, Zhongjie; Lu, Lanlu; Chen, Zhenhua; Ma, Jingyuan; Xu, Erxiang; Wang, Luyao; Li, Yunfei; Tan, Zhengtian; Zheng, Shijie; Liu, Guilin; Guo, Lianbo; Li, Jingbai; Shen, Yang; Troshin, Pavel A.; Aldoshin, Sergey M.; Liu, Zonghao; Park, Nam-Gyu; Chen, Wei
• 署名单位: Huazhong University of Science & Technology; Huazhong University of Science & Technology; Sungkyunkwan University (SKKU); Sungkyunkwan University (SKKU); Shenzhen Polytechnic University; Southern University of Science & Technology; Hong Kong University of Science & Technology (Guangzhou); Russian Academy of Sciences; Chinese Academy of Sciences; Shanghai Advanced Research Institute, CAS; Chinese Academy of Sciences; Shanghai Advanced Research Institute, CAS; Tsinghua University; Xiamen University; Jiangnan University; Sungkyunkwan University (SKKU)
• 刊物名称: SCIENCE
• ISSN/ISSBN: 0036-8075; 1095-9203
• DOI: 10.1126/science.aeb9953
• 发表日期: 2026-05-14
• 页码: 742-748
• 关键词: solar-cells; efficient; degradation; performance; layer

摘要

A critical limitation of formamidinium lead iodide (FAPbI(3)) perovskite solar cells (PSCs) lies in the intrinsic instability of the ionic-covalent Pb-I octahedral lattice, relative to the unfavorable hexagonal delta-phase under operating conditions. We report an entropy-regulating molecular-lock strategy using 1-pyridin-3-ylmethyl-piperazine hydrochloride (3-PMPCl). Strong interactions between the perovskite lattice surface and 3-PMPCl modulate the rotational freedom of organic cations and suppress the detrimental entropy increase associated with [PbI6](4-) octahedra disorder or expansion. This entropy-favored environment intrinsically increases the phase transition energy barrier. The uniform distribution and strong adsorption of 3-PMPCl stabilize the alpha-phase under elevated temperature and humidity conditions. We achieved a certified power conversion efficiency (PCE) of 27.6% in FAPbI(3)-based PSCs. However, the operational stability of such champion devices remains below the state of the art. Adopting a stable bismuth electrode addresses this issue with a slight reduction in efficiency, yielding a device that retains 93.0% of its initial PCE (26.8%) after 1011 hours at 85 degrees C under 1-sun illumination.