Ultrasonic Clusterization Process to Prepare [(NNCO)(6)Co(4)Cl(2)] as a Novel Double-Open-Co(4)O(6) Cubane Cluster: SXRD Interactions, DFT, Physicochemical, Thermal Behaviors, and Biomimicking of Catecholase Activity

[Image: see text] A novel double-open-cubane (NNCO)(6)Co(4)Cl(2) cluster with a Co(4)O(6) core was made available under aqua-ultrasonic open atmosphere conditions for the first time. The ultrasonic clusterization of the (3,5-dimethyl-1H-pyrazol-1-yl)methanol (NNCOH) ligand with CoCl(2)·6H(2)O salts in ethanol yielded a high-purity and high-yield cluster product. Energy-dispersive X-ray (EDX), Fourier transform infrared (FT-IR), and ultraviolet (UV)–visible techniques were used to elucidate the clusterization process. The double-open-Co(4)O(6) cubane structure of the (NNCO)(6)Co(4)Cl(2) cluster was solved by synchrotron single-crystal X-ray diffraction (SXRD) and supported by density functional theory (DFT) optimization and thermogravimetric/differential TG (TG/DTG) measurements; moreover, the DFT structural parameters correlated with the ones determined by SXRD. Molecular electrostatic potential (MEP), Mulliken atomic charge/natural population analysis (MAC/NPA), highest occupied molecular orbital/lowest unoccupied molecular orbital (HOMO/LUMO), density of states (DOS), and GRD quantum analyses were computed at the DFT/B3LYP/6-311G(d,p) theory level. The thermal behavior of the cluster was characterized to support the formation of the Co(4)O(6) core as a stable final product. The catalytic property of the (NNCO)(6)Co(4)Cl(2) cluster was predestined for the oxidation process of 3,5-DTBC diol (3,5-di-tert-butylbenzene-1,2-diol) to 3,5-DTBQ dione (3,5-di-tert-butylcyclohexa-3,5-diene-1,2-dione).