Small, Journal Year: 2024, Volume and Issue: unknown
Published: Dec. 23, 2024
A mixed-ligand-based thermo-chemically robust and undulated metal-organic framework (MOF) is developed that embraces carboxamide moiety-grafted porous channels activation-induced generation of open-metal site (OMS). The guest-free MOF acts as an outstanding heterogeneous catalyst in Hantzsch condensation for electronically assorted substrates with low loading short duration under greener conditions than the reported materials. Besides Lewis acidic OMS, group activates substrate via two-point hydrogen bonding, highlighting effectiveness custom-made functionalities this multi-component reaction. Importantly, demonstrates first ever one-pot synthesis 1,4-dihydropyridine-based antihypertensive drug foridon, along four therapeutic molecules ethidine, nifedipine, nemadipine B Nitrendipine, which are characterized X-ray crystallography besides conventional spectroscopic analyses. integration redox-active Co(II) center acid-base dual sites benefit activated catalyzing mild-condition alcohol oxidation-Knoevenagel to produce benzylidene malononitriles wide tolerance multicyclic performance. For both atom-economic reactions, astutely designed control experiments density functional theory-based reaction energy profile rationalize synergistic catalysis pore-decked antagonistic predominantly transpires inside channel. This study marks a paradigm shift sustainable through task-specific functionality fuelling, provides valuable insights on structure-property synergism at cutting-edge design.
Language: Английский