A5067041514- Zeolite Catalysis and Synthesis
- Mesoporous Materials and Catalysis
- Catalysis for Biomass Conversion
- Catalysis and Oxidation Reactions
- Metal-Organic Frameworks: Synthesis and Applications
- Catalytic Processes in Materials Science
- Catalysis and Hydrodesulfurization Studies
- Catalysts for Methane Reforming
- Nanomaterials for catalytic reactions
- Crystallography and molecular interactions
- Catalytic Alkyne Reactions
- Clay minerals and soil interactions
- Advanced Chemical Physics Studies
- Fuel Cells and Related Materials
- Asymmetric Hydrogenation and Catalysis
- Advanced battery technologies research
- Electrocatalysts for Energy Conversion
- Machine Learning in Materials Science
Eindhoven University of Technology
2014-2020
Institute of Catalysis and Petrochemistry
2016-2019
Japan External Trade Organization
2013-2014
Non-oxidative dehydroaromatization of methane (MDA) is a promising catalytic process for direct valorization natural gas to liquid hydrocarbons. The application this reaction in practical technology hindered by lack understanding about the mechanism and nature active sites benchmark zeolite-based Mo/ZSM-5 catalysts, which precludes solution problems such as rapid catalyst deactivation. By applying spectroscopy microscopy, it shown that centers are partially reduced single-atom Mo stabilized...
Surface carbon (coke, carbonaceous deposits) is an integral aspect of methane dehydroaromatization catalyzed by Mo/zeolites. We investigated the evolution surface species from beginning induction period until complete catalyst deactivation pulse reaction technique, TGA, 13C NMR, TEM, and XPS. Isotope labeling was performed to confirm catalytic role confined during MDA. It found that "hard" "soft" coke distinction mainly related location inside pores on external surface, respectively. In...
Quantum chemistry-based codes and methods provide valuable computational tools to estimate reaction energetics elucidate mechanisms. Electronic structure allow directly studying the chemical transformations in molecular systems involving breaking making of bonds associated changes electronic structure. The link between bonding can be provided through crystal orbital Hamilton population (COHP) analysis that allows quantifying bond strength by computing Hamilton-weighted populations localized...
The one-pot Diels-Alder cycloaddition (DAC)/dehydration (D) tandem reaction between 2,5-dimethylfuran and ethylene is a potent pathway toward biomass-derived
A simple amphiphilic surfactant containing a mono-quaternary ammonium head group (N-methylpiperidine) is effective in imparting substantial mesoporosity during synthesis of SSZ-13 and ZSM-5 zeolites. Highly mesoporous prepared this manner shows greatly improved catalytic performance the methanol-to-olefins reaction compared to bulk SSZ-13.
Abstract Cobalt phosphides are an emerging earth‐abundant alternative to platinum‐group‐metal‐based electrocatalysts for the hydrogen evolution reaction (HER). Yet, their stability is inferior platinum and compromises large‐scale applicability of CoP x in water electrolyzers. In present study, we employed flat, thin electrodes prepared through thermal phosphidation (PH 3 ) Co O 4 films made by plasma‐enhanced atomic layer deposition evaluate acidic electrolysis using a multi‐technique...
The presence of small amount fluoride in alkaline hydrothermal synthesis SSZ-13 zeolite yields bimodal microporous particles with substantially improved performance the methanol-to-olefins (MTO) reaction. Hydrocarbon uptake measurements and fluorescence microspectroscopy spent catalysts demonstrate enhanced diffusion through micropores at grain boundaries nanocrystals running particles. Fluoride-assisted is a cheap scalable approach to optimize MTO catalysts.
Pd/zeolite-catalyzed hydroconversion of n-hexadecane (n-C16) and n-heptane (n-C7) was studied for 10MR (ZSM-5, ZSM-22), 12MR (ZSM-12), EMM-23 (21MR × 10MR) zeolites. The catalytic activity depended on the Brønsted acidity crystalline domain size. n-C16 benefited from short diffusion lengths in ZSM-5 nanosheets compared to bulk ZSM-5. In general, over-cracking is dominant with a cracked product distribution skewed C4 products, be explained by snug fit particular dibranched isomers at zeolite...
Abstract The catalytic Diels–Alder cycloaddition–dehydration (DACD) reaction of furanics with ethylene is a promising route to bio‐derived aromatics. can be catalyzed by alkali‐metal‐exchanged faujasites. Herein, the results periodic DFT calculations based on accurate structural models zeolites are presented, revealing fundamental roles that confinement and nature exchangeable cations in zeolite micropores have performance faujasite‐based catalysts DAC D reaction. Special attention devoted...
The Diels–Alder cycloaddition (DAC) is a powerful tool to construct C–C bonds. DAC reaction can be accelerated in several ways, one of which reactant confinement as observed supramolecular complexes and Diels–Alderases. Another method altering the frontier molecular orbitals (FMOs) reactants by using homogeneous transition-metal whose active sites exhibit d-orbitals suitable for net-bonding orbital interactions with substrates. Both features combined first row d-block (TM) exchanged...
The Diels-Alder cycloaddition (DAC) reaction is a commonly employed for the formation of C-C bonds. DAC catalysis can be achieved by using Lewis acids and via reactant confinement in aqueous nanocages. Low-silica alkali-exchanged faujasite catalysts combine these two factors one material. They used tandem DAC/dehydration biomass-derived 2,5-dimethylfuran (DMF) with ethylene toward p-xylene, which step initiates overall cycle. In this work, we performed periodic density functional theory...
Abstract Non‐oxidative dehydroaromatization of methane (MDA) is a promising catalytic process for direct valorization natural gas to liquid hydrocarbons. The application this reaction in practical technology hindered by lack understanding about the mechanism and nature active sites benchmark zeolite‐based Mo/ZSM‐5 catalysts, which precludes solution problems such as rapid catalyst deactivation. By applying spectroscopy microscopy, it shown that centers are partially reduced single‐atom Mo...
In applying a multi-scale spectroscopic and computational approach, we demonstrate that the synthesis of stacked zeolite silicalite-1 nanosheets, in presence long-tail diquaternary ammonium salt surfactant, proceeds through pre-organised phase condensed state. situ small-angle X-ray scattering, coupled to paracrystalline theory, backed by electron microscopy, shows this establishes its meso-scale order within first five hours hydrothermal synthesis. Quasi vibrational solid-state NMR...
Mesoporous and nanostructured zeolite-based catalysts experience prolonged lifetimes due to increased mass transfer reduced micropore obstruction by coke formation as compared their bulky microporous counterparts. Diquaternary ammonium structure-directing agents (SDAs) can be used synthesize hierarchical MFI sheet-like MEL needle-like zeolites. An explanation of the underlying molecular-level details synthesis these zeolites is presented on basis non-covalent interactions between template...
Eingeschlossene Kohlenstoffspezies spielen eine doppelte Rolle in der nichtoxidativen Dehydroaromatisierung von Methan über Mo-Atom/ZSM-5-Katalysatoren. In ihrer Zuschrift auf S. 1028 zeigen N. Kosinov, E. J. M. Hensen et al. mithilfe Operando-Spektroskopie, Mikroskopie und Isotopenmarkierung Methan, dass polycyclische aromatische Kohlenwasserstoffe, die den Mikroporen des Zeolith-Katalysators entstehen, entscheidende Zwischenstufen dem Weg zu Benzol sind. Diese Spezies desaktivieren...