Siddiqui Rafia, Ligorio Raphael F, Titi Hatem M, Pandey Sushil Kumar, Krawczuk Anna, Patra Ranjan
Amity Institute of Click Chemistry Research and Studies, Amity University, Noida, Uttar Pradesh, 201303, India.
Institute of Inorganic Chemistry, University of Göttingen, Tammannstrasse 4, D-37077, Göttingen, Germany.
Chemistry. 2025 Aug 13;31(45):e02099. doi: 10.1002/chem.202502099. Epub 2025 Jul 22.
This study investigates how electron-withdrawing substitution, molecular polarization, and dipole moment influence the σ-hole potential in six-coordinate metalloporphyrins. To evaluate halogen bonding tendencies, we synthesized a series of five Sn(IV)-5,10,15,20-meso-tetrakis(4-iodophenyl)porphyrin complexes with various fluorinated phenolate axial ligands. Single-crystal X-ray diffraction analysis revealed distinct halogen-bonded supramolecular motifs, which vary depending on the degree of fluorination at the axial ligands. Our findings highlight the critical role of ligand-induced polarization and dipole moment variations in modulating the σ-hole characteristics of the equatorial iodine atoms. Computational modelling showed that increased fluorine substitution reduces both the atomic dipole moments of fluorine and the polarizability of the central tin ion. However, despite these changes, the axial fluorination has a negligible effect on the σ-hole potential at the iodine atoms. This limited influence is attributed to the orthogonal orientation between the porphyrin core and the peripheral phenyl rings, which suppresses resonance interactions. Overall, this work emphasizes the importance of understanding electronic effects at the molecular level, particularly in the design and formation of halogen-bonded supramolecular architectures.
本研究调查了吸电子取代、分子极化和偶极矩如何影响六配位金属卟啉中的σ-空穴势。为了评估卤素键合倾向,我们合成了一系列五种带有各种氟化酚盐轴向配体的Sn(IV)-5,10,15,20-四(4-碘苯基)卟啉配合物。单晶X射线衍射分析揭示了不同的卤素键合超分子基序,其随轴向配体的氟化程度而变化。我们的研究结果突出了配体诱导的极化和偶极矩变化在调节赤道碘原子的σ-空穴特性中的关键作用。计算模型表明,增加氟取代会降低氟的原子偶极矩和中心锡离子的极化率。然而,尽管有这些变化,轴向氟化对碘原子处的σ-空穴势的影响可忽略不计。这种有限的影响归因于卟啉核心与外围苯环之间的正交取向,这抑制了共振相互作用。总体而言,这项工作强调了在分子水平上理解电子效应的重要性,特别是在卤素键合超分子结构的设计和形成方面。