A5052823556- Zeolite Catalysis and Synthesis
- Catalytic Processes in Materials Science
- Catalysis and Oxidation Reactions
- Catalysts for Methane Reforming
- Mesoporous Materials and Catalysis
- Catalysis and Hydrodesulfurization Studies
- Metal-Organic Frameworks: Synthesis and Applications
- Catalysis for Biomass Conversion
- CO2 Reduction Techniques and Catalysts
- Carbon dioxide utilization in catalysis
- Membrane Separation and Gas Transport
- Nanomaterials for catalytic reactions
- Electrocatalysts for Energy Conversion
- Industrial Gas Emission Control
- Machine Learning in Materials Science
- Plasma Applications and Diagnostics
- Chemical Synthesis and Characterization
- 2D Materials and Applications
- Petroleum Processing and Analysis
- Molten salt chemistry and electrochemical processes
- Carbon Dioxide Capture Technologies
- Muon and positron interactions and applications
- Clay minerals and soil interactions
- Covalent Organic Framework Applications
- Ammonia Synthesis and Nitrogen Reduction
Eindhoven University of Technology
2016-2025
Institute of Catalysis and Petrochemistry
2016-2019
Delft University of Technology
2018
Institute of Inorganic Chemistry of the Slovak Academy of Sciences
2014-2018
Japan External Trade Organization
2013
The active site requirements for methane dehydroaromatization by Mo/HZSM-5 were investigated employing as catalysts physical mixtures of Mo-bearing supports (HZSM-5, SiO2, γ-Al2O3, and activated carbon) HZSM-5. Separation the two catalyst components after activation or reaction was possible using different sieve fractions. Our comparison demonstrates that migration volatile Mo oxides into micropores HZSM-5 is at origin observed catalytic synergy in mixtures. propensity depends on method...
The catalytic performance of heterogeneous catalysts can be tuned by modulation the size and structure supported transition metals, which are typically regarded as active sites. In single-atom metal catalysts, support itself strongly affect properties. Here, we demonstrate that cerium dioxide (CeO2) governs reactivity atomically dispersed palladium (Pd) in carbon monoxide (CO) oxidation. Catalysts with small CeO2 nanocrystals (~4 nanometers) exhibit unusually high activity a CO-rich reaction...
CO2 hydrogenation to methanol can play an important role in meeting the sustainability goals of chemical industry. In this study, we investigated detail Cu–CeO2 interactions for synthesis, emphasizing copper surface and interface sites between ceria CO. A combined CO2–N2O titration approach was developed quantify exposed metallic oxygen vacancies reduced Cu/CeO2 catalysts. Extensive characterization shows that dispersion is strongly enhanced by strong comparison Cu/SiO2. activity data show...
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...
The hydrogenation of CO2 to CH3OH is an important reaction for future renewable energy scenarios. Herein, we compare Cu/ZnO, Cu/CeO2, and Cu/ZnO–CeO2 catalysts prepared by flame spray pyrolysis. Cu loading support composition were varied understand the role Cu–ZnO Cu–CeO2 interactions. CeO2 addition improves dispersion with respect ZnO, owing stronger ternary displayed a substantially higher selectivity than binary Cu/CeO2 Cu/ZnO catalysts. high in comparison commercial catalyst also...
Despite the large number of studies on catalytic hydrogenation CO2 to CO and hydrocarbons by metal nanoparticles, nature active sites reaction mechanism have remained unresolved. This hampers development effective catalysts relevant energy storage. By investigating structure sensitivity a set silica-supported Ni nanoparticle (2-12 nm), we found that responsible for conversion are different from those subsequent CH4. While former step is weakly dependent size, latter strongly sensitive with...
Dehydroaromatization of methane is a promising reaction to directly convert into aromatics and hydrogen. The main drawback this the rapid deactivation Mo/HZSM-5 catalyst due coking. Regeneration at high temperature by air calcination not possible extensive dealumination zeolite. We investigated structural textural stability HZSM-5 as function Mo loading in (550–700 °C) demonstrated that lowering below 2 wt% greatly improves oxidative Mo/HZSM-5. At low (1–2 Mo), predominantly zeolite...
Novel high-silica SSZ-13 zeolite membranes with excellent performance in CO<sub>2</sub>/N<sub>2</sub>and CO<sub>2</sub>/CH<sub>4</sub>separation were reproducibly synthesized. Being hydrothermally stable, these are very promising candidates for separation of CO<sub>2</sub>from hot and humid flue gas streams.
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...
Chabazite zeolites with trimodal porosity (native micropores of the CHA framework, an additional network larger ∼0.5 nm, and mesopores) were synthesized by adding diquarternary ammonium-type surfactant C22–4–4 cations fluoride anions in synthesis SSZ-13 zeolite. The hierarchical are fully crystalline exhibit similar acidity as bulk increased diffusion rate SSZ-13, proven uptake experiments bulky molecules selective staining thiophene oligomers, resulted much slower catalyst deactivation...
Abstract Non‐oxidative methane dehydroaromatization is a promising reaction to directly convert natural gas into aromatic hydrocarbons and hydrogen. Commercialization of this technology hampered by rapid catalyst deactivation because coking. A novel approach presented involving selective oxidation coke during at 700 °C. Periodic pulsing oxygen the feed results in substantially higher cumulative product yield with synthesis gas; H 2 /CO ratio close two main side‐product combustion. Using 13 C...
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...
Elucidating the role of metal modification and confined hydrocarbon species in aromatization ethylene on zeolite catalysts.
Non-oxidative dehydroaromatization of methane over Mo/ZSM-5 zeolite catalysts is a promising reaction for the direct conversion abundant natural gas into liquid aromatics. Rapid coking deactivation hinders practical implementation this technology. Herein, we show that catalyst productivity can be improved by nearly an order magnitude raising pressure to 15 bar. The beneficial effect was found different and wide range temperatures space velocities. High-pressure operando X-ray absorption...
Hydrogenation of levulinic acid to γ-valerolactone is a key reaction in the valorization carbohydrates renewable fuels and chemicals. State-of-the-art catalysts are based on supported noble metal nanoparticle catalysts. We report utility bimetallic Fe-Re TiO2 for this reaction. A strong synergy was observed between Fe Re hydrogenation water under mild conditions. Fe-Re/TiO2 shows superior catalytic performance compared monometallic at similar content. The activity increased with H2-TPR, XPS,...
In2O3 is a promising catalyst for the hydrogenation of CO2 to methanol, relevant renewable energy storage in chemicals. Herein, we investigated promoting role Al on using flame spray pyrolysis prepare series In2O3–Al2O3 samples single step (0–20 mol % Al). promoted methanol yield, with an optimum being observed at content 5 %. Extensive characterization showed that can dope into lattice (maximum ∼ 1.2 %), leading formation more oxygen vacancies involved adsorption and formation. The rest...
The methanol-to-hydrocarbons (MTH) process is an industrially relevant method to produce valuable light olefins such as propylene. One of the ways enhance propylene selectivity modify zeolite catalysts with alkaline earth cations. underlying mechanistic aspects this type promotion are not well understood. Here, we study interaction Ca2+ reaction intermediates and products formed during MTH reaction. Using transient kinetic spectroscopic tools, find strong indications that differences between...
Plasma-enhanced heterogeneous catalysis offers a promising alternative to thermal due the synergy between plasma and solid catalyst. However, there is only limited mechanistic insight about interactions of highly energetic electrons excited molecules with catalysts in plasmas. Accurate performance comparison plasma-catalytic setting complicated because intricate nature plasma-catalyst system: simultaneous reactions occurring gas-phase at catalytic surface; dependence discharge on dielectric...