Targeted passivation of defects in perovskite is the primary consideration in the design of additives containing functional groups. However, the precise modulation of electron structure in functional groups and the structure-activity relationship between electronic configuration and performance of perovskite solar cells (PSCs) still need to be explored. In this study, 5-chloro-2-hydroxypyridine derivatives with –NH₂ (HNCLP) and –F (HFCLP) end groups are selected to realize the push-pull electronic structure configuration. Density functional theory demonstrates that, compared with HFCLP, HNCLP with the electron-donating terminal of –NH₂ has a long dipole moment and immobilize the interstitial I₃⁻, and the N side of pyridine with high-density electron cloud enables strong passivation with undercoordinated Pb²⁺ ions. The experimental results confirm that HNCLP with optimized electronic configuration emerges strong passivation ability, greatly suppresses the nonradiative recombination of perovskite absorber, and remarkably improves the film crystal quality along with the extraction and transfer process of photogenerated carriers. The HNCLP-contained PSC exhibits a remarkable efficiency of 24.47%, and HNCLP helps to enhance the moisture-proof of perovskite film and device storage stability.

中文翻译：

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具有推拉电子结构的 5-氯-2-羟基吡啶衍生物可实现耐用且高效的钙钛矿太阳能电池

钙钛矿缺陷的靶向钝化是含官能团添加剂设计的首要考虑因素。然而，官能团中电子结构的精确调控以及电子构型与钙钛矿太阳能电池（PSC）性能之间的构效关系仍需探索。_{在本研究中，选择具有-NH 2} (HNCLP)和-F(HFCLP)端基的5-氯-2-羟基吡啶衍生物来实现推挽电子结构构型。密度泛函理论表明，与HFCLP相比，给电子末端为-NH ₂的HNCLP具有较长的偶极矩，固定了间隙原子I ₃ ^-，且吡啶的N侧具有高密度电子云，可实现强钝化配位不足的 Pb ²⁺离子。实验结果证实，电子构型优化的HNCLP具有很强的钝化能力，极大地抑制了钙钛矿吸收体的非辐射复合，随着光生载流子的提取和转移过程，显着提高了薄膜晶体质量。含有HNCLP的PSC表现出24.47%的显着效率，HNCLP有助于增强钙钛矿薄膜的防潮性和器件的存储稳定性。