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Organic synthesis of high added value molecules with MOF catalysts KU Leuven
Recent examples of organic synthesis of fine chemicals and pharmaceuticals in confined spaces of MOFs are highlighted and compared with silica-based ordered porous solids, such as zeolites or mesoporous (organo)silica. These heterogeneous catalysts offer the possibility of stabilizing the desired transition states and/or intermediates during organic transformations of functional groups and (C-C/C-N) bond forming steps towards the desired ...
Tuning the Catalytic Properties of UiO-66 Metal-Organic Frameworks: From Lewis to Defect-Induced Bronsted Acidity KU Leuven
The Lewis/Brønsted acidity and catalytic properties of UiO-66-type metal-organic frameworks are studied in the context of tunable acid catalysts based on the presence of linker defects that create coordinatively unsaturated Zr4+ centers. Fourier transform infrared spectroscopy of adsorbed CO and direct pH measurements are employed to characterize hydrated and dehydrated UiO-66 containing different number of Zr4+ sites associated with defects. ...
Metal-Organic Framework Derived Metal Oxide Clusters in Porous Aluminosilicates: A Catalyst Design for the Synthesis of Bioactive aza-Heterocycles KU Leuven
© Copyright 2018 American Chemical Society. Simple solid-state mixing and calcination of catalytic amounts of metal-organic frameworks (MOFs) in the presence of aluminosilicates allow for the generation of active and robust supported metal oxide nanoparticles that catalyze C-C and C-N bond formations. The proposed Cu and Zn containing aluminosilicates outperform state-of-the-art solid catalysts for the synthesis of various aza-heterocycles under ...
Anion Exchange and Catalytic Functionalization of the Zirconium-Based Metal-Organic Framework DUT-67 KU Leuven
Copyright © 2018 American Chemical Society. A postsynthetic treatment with diluted solutions of the inorganic HCl or H2SO4 acids was applied to functionalize the eight connected Zr-based metal-organic framework DUT-67 (DUT = Dresden University of Technology). During the treatment, it is possible to remove and exchange the pristine modulator (formate) by Cl- or SO42- anions. The position of the chlorine in the crystal structure of DUT-67 after ...
Boosting the Catalytic Performance of Metal-Organic Frameworks for Steroid Transformations by Confinement within a Mesoporous Scaffold KU Leuven
Solid-state crystallization achieves selective confinement of metal-organic framework (MOF) nanocrystals within mesoporous materials, thereby rendering active sites more accessible compared to the bulk-MOF and enhancing the chemical and mechanical stability of MOF nanocrystals. (Zr)UiO-66(NH2 )/SiO2 hybrid materials were tested as efficient and reusable heterogeneous catalysts for the synthesis of steroid derivatives, outperforming the bulk ...
Increasing the availability of active sites in Zn-Co double metal cyanides by dispersion onto a SiO2 support KU Leuven
Zn-Co double metal cyanides (DMCs) were dispersed on silica by dry and liquid-assisted (LAG) grinding to improve the catalytic performance of the DMC phase. The characterization of the resulting materials by transmission electron microscopy, N2 physisorption, and powder X-ray diffraction indicated that the presence of water during the grinding step, not only helped to preserve the structural and textural properties of the DMC, but also ...
Nature of active sites on UiO-66 and beneficial influence of water in the catalysis of Fischer esterification KU Leuven Universiteit Gent
Tetrabutylphosphonium bromide catalyzed dehydration of diols to dienes and its application in the bio-based production of butadiene KU Leuven
We report the use of the ionic liquid tetrabutylphosphonium bromide as a solvent and catalyst for dehydration of diols to conjugated dienes. This system combines stability, high reaction rates and easy product separation. A reaction mechanism for the model compound 1,2-hexanediol is proposed and experimentally corroborated. This particular mechanism allows for the selective formation of conjugated dienes, in contrast with purely acidic ...
Selective one-pot two-step C-C bond formation using MOFs with mild basicity as heterogeneous catalysts KU Leuven
Copper-ion-exchanged nickel pyrazolate frameworks behave as selective heterogeneous catalysts for the one-pot, two-step (Henry reaction/Michael type addition) synthesis of neuroactive pharmaceutical intermediates starting from nitromethane and benzaldehyde. Tuning the basicity of multifunctional metal–organic framework catalysts through ion exchange with copper(II) cations allows the tandem C−C bond-forming process to be selectively directed ...