Facile Ultrasound-Based Synthesis, SC-XRD, DFT Exploration of the Substituted Acyl-Hydrazones: An Experimental and Theoretical Slant towards Supramolecular Chemistry

Sono-chemical synthesis is safest and greener methods to fabricate valuable scaffolds in short time. Currently, we are reporting an efficient ultrasound-based synthesis of substituted acyl-hydrazones, single crystal analysis and DFT exploration. The substituted acyl-hydrazones synthesis i.e 2-((6-chloropyridin-2-yl)oxy)-N '-((1E,2E)-3-phenylallylidene)acetohydrazide acetonitrile (1 : 1) (CPPAH) and (E)-2-((6-chloropyridin-2-yl)oxy)-N '-(4-methylbenzylidene)acetohydrazide (MBPAH) was accomplished utilizing sono-chemical approach.The structures of these molecules were characterized with NMR and SC-XRD analysis. The experimental and theoretical analysis employed to determine non-covalent, hyper-conjugative interactions and favorable sites for reactivity. Time-dependent density functional theory (TD-DFT) approach was utilized to acquire insights about FMO analysis. The global reactivity parameters established with aid of HOMO and LUMO energies. QT-AIM and Hirshfeld analyses were computed to quantify non-covalent interactions for both crystals. Theoretically observed structural chemistry of both crystals led to a fabulous overall agreement with obtained SC-XRD patterns. The molecular stability and bond strengths of the aforesaid molecules were imparted owing to hyper-conjugative interactions as well as charge delocalization process. Moreover, NBO based findings were rationalized to Hirshfeld analysis and SC-XRD data.