Tailoring Low‐Miller‐Index Crystal Facets Realizes Perovskite Solar Cells with Flat Grain‐boundary Grooves

作者：Jing Zhou, Yu Chen, Yang Shen, Peng Yang, Wu Xing, Zhuang Xie, Chuan Luo, Min Deng, Yuwei Duan, Yihui Wu, Qiang Peng · 发表于：Angewandte Chemie International Edition · 年份：2025 · DOI：10.1002/anie.202511042 · 被引用次数：12 · 研究领域：Perovskite Materials and Applications、Quantum Dots Synthesis And Properties、Organic Light-Emitting Diodes Research

Abstract Charge transport and nonradiative recombination loss at the buried interface are important factors, which limit the efficiency and stability of perovskite solar cells (PSCs). Herein, we screen a series of diphosphate Lewis‐base molecules, where N,N‐bis(diphenylphosphino)amine (N‐DPPM) with appropriate alkyl chains and multiple active sites not only can efficiently facilitate carrier transport but also coordinate with undercoordinated Pb 2+ and interact with FA + through N⋯H bond. These features prompt the formation of high‐quality perovskite films along (100)/(200) crystal facets. Interestingly, these oriented low‐Miller‐index crystal facets have approximately a twice‐increase in heterointerface energy and twice‐decrease in grain‐boundary energy, flattening grain‐boundary grooves, thereby reducing nanoscale physical voids and releasing residual stress. Consequently, the champion inverted PSCs exhibit impressive power conversion efficiencies of 26.80%, 26.18%, and 20.59% for narrow‐bandgap (1.55 eV), large‐area (0.5 cm 2 ), and wide‐bandgap (1.73 eV) devices, respectively. Meanwhile, the unencapsulated devices exhibit excellent stability after long‐term storage, thermal‐aging, or light‐soaking.