A5071451863- Metal-Organic Frameworks: Synthesis and Applications
- Zeolite Catalysis and Synthesis
- Advanced Chemical Physics Studies
- Catalysis and Oxidation Reactions
- X-ray Diffraction in Crystallography
- Machine Learning in Materials Science
- Catalytic Processes in Materials Science
- Covalent Organic Framework Applications
- Catalysis and Hydrodesulfurization Studies
- Mesoporous Materials and Catalysis
- Free Radicals and Antioxidants
- Synthesis and Catalytic Reactions
- Polyoxometalates: Synthesis and Applications
- Crystallography and molecular interactions
- Crystallization and Solubility Studies
- Advanced NMR Techniques and Applications
- Spectroscopy and Quantum Chemical Studies
- Magnetism in coordination complexes
- Catalysis for Biomass Conversion
- Photochemistry and Electron Transfer Studies
- Organic Chemistry Cycloaddition Reactions
- Chemical Synthesis and Reactions
- Synthesis of β-Lactam Compounds
- Advanced Photocatalysis Techniques
- Perovskite Materials and Applications
Ghent University
2016-2025
Ghent University Hospital
2015-2024
Vrije Universiteit Brussel
2004-2023
Technische Universität Braunschweig
2023
University of Antwerp
2023
Ludwig-Maximilians-Universität München
2023
Observatoire de la Côte d’Azur
2023
Research Center for Eco-Environmental Sciences
2023
Park University
2021
Vitenparken
2019-2021
A comparison of DFT methods Density functional theory (DFT) is now routinely used for simulating material properties. Many software packages are available, which makes it challenging to know the best use a specific calculation. Lejaeghere et al. compared calculated values equation states 71 elemental crystals from 15 different widely codes employing 40 potentials (see Perspective by Skylaris). Although there were variations in values, most recent and converged toward single value, with...
The catalytic activity of the zirconium terephthalate UiO-66(Zr) can be drastically increased by using a modulation approach. combined use trifluoroacetic acid and HCl during synthesis results in highly crystalline material, with partial substitution terephthalates trifluoroacetate. Thermal activation material leads not only to dehydroxylation hexanuclear Zr cluster but also post-synthetic removal trifluoroacetate groups, resulting more open framework large number sites. Consequently, is...
Strain-stabilized perovskites The perovskite materials used for solar cells and light-emitting diodes (which are black in color) generally less stable at room temperature than the electronically inactive nonperovskite phases yellow color). Steele et al. show that CsPbI 3 , strain induced a thin film after annealing material to 330°C then rapidly cooling it kinetically trapped phase. Grazing-incidence wide-angle x-ray scattering revealed crystal distortions texture formation created by...
Predictions of observable properties by density-functional theory calculations (DFT) are used increasingly often experimental condensed-matter physicists and materials engineers as data. These predictions to analyze recent measurements, or plan future experiments in a rational way. Increasingly more scientists these fields therefore face the natural question: what is expected error for such first-principles prediction? Information experience about this question implicitly available...
Radicals can be regarded as electrophilic/nucleophilic, depending on their tendency to attack sites of relatively higher/lower electron density. In this paper, an electrophilicity scale, global well local, and a nucleophilicity scale for 35 radicals is reported. The correlates with the suggesting that these concepts are inversely related.
Functionalized linkers can greatly increase the activity of metal-organic framework (MOF) catalysts with coordinatively unsaturated sites. A clear linear free-energy relationship (LFER) was found between Hammett σ(m) values linker substituents X and rate k(X) a carbonyl-ene reaction. This is first LFER ever observed for MOF catalysts. 56-fold in when substituent nitro group.
Photocatalytic reduction of molecular oxygen is a promising route toward sustainable production hydrogen peroxide (H2O2). This challenging process requires photoactive semiconductors enabling solar energy driven generation and separation electrons holes with high charge transfer kinetics. Covalent organic frameworks (COFs) are an emerging class semiconductors, tunable at level for carrier transfer. Herein, we report two newly designed two-dimensional COFs based on (diarylamino)benzene linker...
Abstract The conversion of methanol to olefins (MTO) over a heterogeneous nanoporous catalyst material is highly complex process involving cascade elementary reactions. elucidation the reaction mechanisms leading either desired production ethene and/or propene or undesired deactivation has challenged researchers for many decades. Clearly, choice, in particular topology and acidity, as well specific conditions determine overall MTO activity selectivity; however, subtle balances between these...
UiO-66 is a promising metal-organic framework for photocatalytic applications. However, the ligand-to-metal charge transfer of an excited electron inefficient in pristine material. Herein, we assess influence missing linker defects on electronic structure and discuss their ability to improve transfer. Using new defect classification system, which transparent easily extendable, identify most photocatalysts by considering both relative stability structure. We find that properties structures...
Zirconium terephthalate UiO-66 type metal organic frameworks (MOFs) are known to be highly active, stable and reusable catalysts for the esterification of carboxylic acids with alcohols. Moreover, when defects present in structure these MOFs, coordinatively unsaturated Zr ions Lewis acid properties created, which increase catalytic activity resulting defective solids. In work, molecular modeling techniques combined new experimental data on various hydrated dehydrated materials allow unravel...
The catalytic activity of the Zr-benzenedicarboxylate (Zr-BDC) UiO-66 increases by using synthesis modulators as trifluoroacetate (TFA) or hydrochloric acid (HCl), which can be removed post-synthetically.
The stability of metal-organic frameworks (MOFs) typically decreases with an increasing number defects, limiting the defects that can be created and catalytic other applications. Herein, we use a hemilabile (Hl) linker to create up maximum six per cluster in UiO-66. We synthesized UiO-66 (Hl-UiO-66) using benzene dicarboxylate (BDC) as 4-sulfonatobenzoate (PSBA) linker. PSBA acts not only modulator but also coligand enhances resulting defective framework. Furthermore, upon postsynthetic...
Atomic partial charges appear in the Coulomb term of many force-field models and can be derived from electronic structure calculations with a myriad atoms-in-molecules (AIM) methods. More advanced have also been proposed, using distributed nature electron cloud atomic multipoles. In this work, an electrostatic force field is defined through concise approximation density, for which interaction trivially evaluated. This approximate "pro-density" expanded minimal basis atom-centered s-type...
A combined theoretical and experimental study is performed in order to elucidate the effects of linker functional groups on photoabsorption properties UiO-66-X materials. This study, which both mono- difunctionalized linkers (with X = OH, NH2, or SH) are investigated, aims obtain a more complete picture choice functionalization. Static time-dependent density theory calculations with molecular dynamics simulations linkers, results compared UV/vis spectra understand electronic governing...
Four highly porous covalent organic frameworks (COFs) containing pyrene units were prepared and explored for photocatalytic H2 O2 production. The experimental studies are complemented by density functional theory calculations, proving that the unit is more active production than bipyridine (diarylamino)benzene reported previously. decomposition experiments verified distribution of over a large surface area COFs plays an important role in catalytic performance. Py-Py-COF though contains other...
The direct transformation of CO2 into high-value-added hydrocarbons (i.e., olefins and aromatics) has the potential to make a decisive impact in our society. However, despite efforts scientific community, no synthetic route exists today synthesize aromatics from with high productivities low undesired CO selectivity. Herein, we report combination series catalysts comprising potassium superoxide doped iron oxide highly acidic zeolite (ZSM-5 MOR) that directly convert either light (in or ZSM-5)...