Synthesis, Crystal Structure, and Supramolecular Architecture of a Novel Tetrahedral Triazole Ligand: SC-XRD, Hirshfeld, and DFT Insights

Tetrakis(4-(4H-1,2,4-triazol-4-yl)phenyl)methane (TTPM), a novel tetrahedral ligand with nitrogen-donor triazole units, was synthesized, characterized and explored for computational studies. Single-crystal X-ray diffraction (SC-XRD) revealed a tetragonal structure (I4₁/a) stabilized by C–H···N hydrogen bonds, forming a robust 3D supramolecular network. FT-IR and NMR spectroscopy confirmed the molecular structure. Density Functional Theory (DFT) calculations (B3LYP/6-31G(d,p)) supported the geometry, showing a 7.16 eV HOMO-LUMO gap, indicating high stability. Hirshfeld surface analysis quantified N···H/H···N interactions (41.2%) as dominant, with fingerprint plots detailing intermolecular contacts. Molecular electrostatic potential and Mulliken analyses identified triazole nitrogens as key coordination sites, highlighting the structural features and electronic characteristics of TTPM relevant to coordination chemistry.