Abstract
A metal–organic framework (MOF) with sulfonic acid tags as a novel mesoporous catalyst was synthesized. The precursor of Zr-UiO-66-PDC was synthesized both via chemical and electrochemical methods. Then, zirconium-based mesoporous metal–organic framework [Zr-UiO-66-PDC-SO3H]Cl was prepared by reaction of Zr-UiO-66-PDC and SO3HCl. The structure of [Zr-UiO-66-PDC-SO3H]Cl was confirmed by FT-IR, PXRD, FE-SEM, TEM, BET, EDX, and Mapping analysis. This mesoporous [Zr-UiO-66-PDC-SO3H]Cl was successfully applied for the synthesis of dicyanomethylene pyridine derivatives via condensation of various aldehyde, 2-aminoprop-1-ene-1,1,3-tricarbonitrile and malononitrile. At the electrochemical section, a green electrochemical method has successfully employed for rapid synthesis of the zirconium-based mesoporous metal–organic framework UiO-66-PDC at room temperature and atmospheric pressure. The synthesized UiO-66-PDC has a uniform cauliflower-like structure with a 13.5 nm mean pore diameter and 1081.6 m2 g−1 surface area. The described catalyst [Zr-UiO-66-PDC-SO3H]Cl was also employed for the convergent paired electrochemical synthesis of dihydropyridine derivatives as an environmentally friendly technique under constant current at 1.0 mA cm−2 in an undivided cell. The proposed method proceeds with moderate to good yields for the model via a cooperative vinylogous anomeric based oxidation.
Highlights
A metal–organic framework (MOF) with sulfonic acid tags as a novel mesoporous catalyst was synthesized
It was found that the electrosynthesis of Zr-mMOF by this method is rapid and could be done at room temperature and pressure without the need for any base or pre-base additive for activation of the ligand. These results proved by the Fourier Transforms Infrared (FT-IR) spectroscopy, Field Emission Scanning Electron Microscopy (FE-scanning electron microscopy (SEM)) and N 2 adsorption–desorption isotherm
The structure of mentioned ionic liquid transported into Zr-based metal–organic frameworks (Zr-MOFs), [Zr-UiO-66-PDC-SO3H]Cl, fully was characterized by applying FT-IR, XRD, BET/BJH, thermal gravimetric (TG), derivative thermal gravimetric (DTG), energy-dispersive X-ray spectroscopy (EDX), FE-SEM as well as transmission electron microscopy (TEM) analysis
Summary
A metal–organic framework (MOF) with sulfonic acid tags as a novel mesoporous catalyst was synthesized. The joining of ionic liquids (ILs) and metal–organic frameworks (MOFs) as novel materials have been used as catalysts, gas adsorption and reagents[5,6]. This strategy have been modified to adjust to physical or chemical properties, pore size, surface area, topology, and polarity of IL@MOFs by suitable choice of metal, ligands and other moieties. To combined metal–organic frameworks (MOFs) and ionic liquids (ILs), we have reacted Zr-UiO66-PDC and C lSO3H for preparing [Zr-UiO-66-PDC-SO3H]Cl as a novel porous catalyst
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