Ultrasonic Clusterization Process to Prepare [(NNCO)6Co4Cl2] as a Novel Double-Open-Co4O6 Cubane Cluster: SXRD Interactions, DFT, Physicochemical, Thermal Behaviors, and Biomimicking of Catecholase Activity

A novel double-open-cubane (NNCO)(6)Co4Cl2 cluster with a Co4O6 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 CoCl2 center dot 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-Co4O6 cubane structure of the (NNCO)(6)Co4Cl2 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 Co4O6 core as a stable final product. The catalytic property of the (NNCO)(6)Co4Cl2 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).

Automated summary

In this study, a novel double-open-cubane (NNCO)(6)Co4Cl2 cluster with a Co4O6 core was synthesized for the first time under aqua-ultrasonic open atmosphere conditions. Various analytical techniques were used to elucidate the clusterization process and confirm the structure of the cluster. The thermal behavior of the cluster was characterized and its catalytic performance was demonstrated.