A5019801445- Catalytic Processes in Materials Science
- Catalysts for Methane Reforming
- Catalysis and Oxidation Reactions
- Electrocatalysts for Energy Conversion
- CO2 Reduction Techniques and Catalysts
- Catalysis for Biomass Conversion
- Catalysis and Hydrodesulfurization Studies
- Click Chemistry and Applications
- Advanced Chemical Physics Studies
- Monoclonal and Polyclonal Antibodies Research
- Carbon dioxide utilization in catalysis
- Supramolecular Self-Assembly in Materials
- nanoparticles nucleation surface interactions
- Crystallography and molecular interactions
- Ammonia Synthesis and Nitrogen Reduction
- Machine Learning in Materials Science
- Ionic liquids properties and applications
- CAR-T cell therapy research
- Molecular Junctions and Nanostructures
- Crystallization and Solubility Studies
- Surface Chemistry and Catalysis
- X-ray Diffraction in Crystallography
- Chalcogenide Semiconductor Thin Films
- Advanced materials and composites
- Perovskite Materials and Applications
Eindhoven University of Technology
2015-2024
Utrecht University
2017-2020
Institute of Catalysis and Petrochemistry
2014-2018
New thermoset systems based on disulfide bonds were synthesized with self-healing capabilities. The mechanism is not related to disulfide–disulfide exchange reactions, but thiol–disulfide reactions that are pH-dependent. Stress relaxation experiments showed large for having PTM2 as a curing agent, which indicates the system can rearrange its molecular structure release stress. However, rates decreased samples tested longer after production. This disappearance of thiol-groups probably caused...
Abstract Microkinetics simulations are presented based on DFT‐determined elementary reaction steps of the Fischer–Tropsch (FT) reaction. The formation long‐chain hydrocarbons occurs stepped Ru surfaces with CH as inserting monomer, whereas planar only produces methane because slow CO activation. By varying metal–carbon and metal–oxygen interaction energy, three reactivity regimes identified rates being controlled by dissociation, chain‐growth termination, or water removal. Predicted surface...
The increasing availability of quantum-chemical data on surface reaction intermediates invites one to revisit unresolved mechanistic issues in heterogeneous catalysis. One such issue particular current interest is the molecular basis Fischer-Tropsch reaction. Here we review understanding this that converts synthesis gas into longer hydrocarbons where especially elucidate recent progress due contributions computational This perspective highlights theoretical approach catalysis aims for...
Understanding the mechanism of CO2 hydrogenation to methanol is important in context renewable energy storage from societal and technological point view. We use density functional theory calculations study systematically effect size Cu clusters on binding strengths reactants reaction intermediates as well activation barriers for elementary steps underlying hydrogenation. All exhibit linear scaling relationships with CO O adsorption energies. Used microkinetics simulations, we predict that...
Energy storage solutions are a vital component of the global transition toward renewable energy sources. The power-to-gas (PtG) concept, which stores surplus in form methane, has therefore become increasingly relevant recent years. At present, supported Ni nanoparticles preferred as industrial catalysts for CO2 methanation due to their low cost and high methane selectivity. However, commercial not active enough reach conversion (>99%) required by specifications injection natural gas grid....
Carbon dioxide is a desired feedstock for platform molecules, such as carbon monoxide or higher hydrocarbons, from which we will be able to make many different useful, value-added chemicals. Its catalytic hydrogenation over abundant metals requires the amalgamation of theoretical knowledge with materials design. Here leverage understanding structure sensitivity, along library supports, tune selectivity methanation in Power-to-Gas concept nickel. For example, show that nickel can and does...
Indium oxide (In2O3) is a promising catalyst for selective CH3OH synthesis from CO2 but displays insufficient activity at low reaction temperatures. By screening range of promoters (Co, Ni, Cu, and Pd) in combination with In2O3 using flame spray pyrolysis (FSP) synthesis, Ni identified as the most suitable first-row transition-metal promoter similar performance Pd–In2O3. NiO–In2O3 was optimized by varying Ni/In ratio FSP. The resulting catalysts including NiO end members have high specific...
Ni-promoted indium oxide (In
Oil has long been the dominant feedstock for producing fuels and chemicals, but coal, natural gas biomass are increasingly explored alternatives
Here, we report on the strong amplification of chirality observed in supramolecular polymers consisting benzene-1,3,5-tricarboxamide monomers and study chiral phenomena as a function temperature. To quantify two phenomena, i.e., sergeants-and-soldiers principle majority-rules principle, adapted previously reported model, which allowed us to describe both terms energy penalties: helix reversal penalty mismatch penalty. The former was ascribed formation intermolecular hydrogen bonds larger...
The kinetics of synthesis gas conversion on the stepped Rh(211) surface were investigated by computational methods. DFT calculations performed to determine reaction energetics for all elementary steps relevant CO into methane, ethylene, ethane, formaldehyde, methanol, acetaldehyde, and ethanol. Microkinetics simulations carried out basis these first-principles data predict consumption rate product distribution as a function temperature. that control selectivity analyzed in detail. Ethanol...
Resolving the structure and composition of supported nanoparticles under reaction conditions remains a challenge in heterogeneous catalysis. Advanced configurational sampling methods at density functional theory level are used to identify stable structures Pd8 cluster on ceria (CeO2) absence presence O2. A Monte Carlo method Gibbs ensemble predicts Pd-oxide particles be CeO2 during CO oxidation. Computed potential energy diagrams for oxidation cycles as input microkinetics simulations....
Doping CeO
Understanding the molecular mechanism of cooperative self-assembly is a key component in design self-assembled supramolecular architectures across multiple length scales with defined function and composition. In this work, we use density functional theory to rationalize experimentally observed growth C3-symmetrical trialkylbenzene-1,3,5-tricarboxamide- (BTA-) based polymers that self-assemble into ordered one-dimensional structures through hydrogen bonding. Our analysis shows these caused by...
Methane (CH4) combustion is an increasingly important reaction for environmental protection, which Pd/CeO2 has emerged as the preferred catalyst. There a lack of understanding nature active site in these catalysts. Here, we use density functional theory to understand role doping Pd ceria surface generating sites highly toward C-H bonds CH4. Specifically, demonstrate that two Pd2+ ions can substitute one Ce4+ ion, resulting very stable structure containing coordinated unsaturated cation...
Heterogeneous single-atom catalysts involve isolated metal atoms anchored to a support, displaying high catalytic performance and stability in many important chemical reactions. We present general theoretical framework establish the thermodynamic of single nanoparticles on support presence adsorbates. As case study, we for Pt–CeO2 CO partial pressure temperature range within which Pt are more stable than nanoparticles. Density functional theory kinetic Monte Carlo simulations demonstrate...
Fischer–Tropsch (FT) synthesis is one of the most complex catalyzed chemical reactions in which chain-growth mechanism that leads to formation long-chain hydrocarbons not well understood yet. The present work provides deeper insight into relation between kinetics FT reaction on a silica-supported cobalt catalyst and composition surface adsorbed layer. Cofeeding experiments 12C3H6 with 13CO/H2 evidence CHx intermediates are involved chain growth highly reversible. We model-based approach...
The high rate of the ‘click-to-release’ reaction between an allylic substituted trans-cyclooctene linker and a tetrazine activator has enabled exceptional control over chemical biological processes. Here we report development new bioorthogonal cleavage based on tetrazine, which allows use highly reactive trans-cyclooctenes, leading to 3 orders magnitude higher click rates compared parent reaction, 4 6 than other reactions. In this pyridazine elimination mechanism, wherein roles are reversed,...
Abstract Heterogeneous single-atom catalysts (SACs) hold the promise of combining high catalytic performance with maximum utilization often precious metals. We extend current thermodynamic view SAC stability in terms binding energy (E bind ) single-metal atoms on a support to kinetic (transport) one by considering activation barrier for metal atom diffusion. A rapid computational screening approach allows predicting diffusion barriers metal–support pairs based E and cohesive bulk c )....
Developing better three-way catalysts with improved low-temperature performance is essential for cold start emission control. Density functional theory in combination microkinetics simulations used to predict reactivity of CO/NO/H
Nickel metal nanoparticles are intensively researched for the catalytic conversion of carbon dioxide. They commercially explored in so-called power-to-methane application which renewably resourced H2 reacts with CO2 to produce CH4, is better known as Sabatier reaction. Previous work has shown that this reaction structure-sensitive. For instance, Ni/SiO2 catalysts reveal a maximum performance when nickel ∼2–3 nm used. Particularly important understanding structure sensitivity over...
Developing highly active cluster catalysts for the bifunctional oxygen evolution reaction (OER) and reduction (ORR) is significant future renewable energy technology. Here, we employ first-principles calculations combined with a genetic algorithm to explore activity trends of transition metal clusters supported on C2N. Our results indicate that clusters, as OER ORR, may outperform single-atom catalysts. In particular, C2N-supported Ag6 exhibits outstanding low overpotentials. Mechanistic...
The dissociation of CO is a critical step in producing long-chain hydrocarbons the Fischer-Tropsch (FT) synthesis reaction. Although potassium (K) known to enhance conversion and selectivity...