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Your search keyword '"Filot, Ivo A. W."' showing total 190 results
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190 results on '"Filot, Ivo A. W."'

2. Efficient conversion of syngas to linear α-olefins by phase-pure χ-Fe5C2.

Author

Wang, Peng, Chiang, Fu-Kuo, Chai, Jiachun, Dugulan, A. Iulian, Dong, Juan, Chen, Wei, Broos, Robin J. P., Feng, Bo, Song, Yuanjun, Lv, Yijun, Lin, Quan, Wang, Rongming, Filot, Ivo A. W., Men, Zhuowu, and Hensen, Emiel J. M.

Abstract

Oil has long been the dominant feedstock for producing fuels and chemicals, but coal, natural gas and biomass are increasingly explored alternatives1–3. Their conversion first generates syngas, a mixture of CO and H2, which is then processed further using Fischer–Tropsch (FT) chemistry. However, although commercial FT technology for fuel production is established, using it to access valuable chemicals remains challenging. A case in point is linear α-olefins (LAOs), which are important chemical intermediates obtained by ethylene oligomerization at present4–8. The commercial high-temperature FT process and the FT-to-olefin process under development at present both convert syngas directly to LAOs, but also generate much CO2 waste that leads to a low carbon utilization efficiency9–14. The efficiency is further compromised by substantially fewer of the converted carbon atoms ending up as valuable C5–C10 LAOs than are found in the C2–C4 olefins that dominate the product mixtures9–14. Here we show that the use of the original phase-pure χ-iron carbide can minimize these syngas conversion problems: tailored and optimized for the process of FT to LAOs, this catalyst exhibits an activity at 290 °C that is 1–2 orders higher than dedicated FT-to-olefin catalysts can achieve above 320 °C (refs. 12–15), is stable for 200 h, and produces desired C2–C10 LAOs and unwanted CO2 with carbon-based selectivities of 51% and 9% under industrially relevant conditions. This higher catalytic performance, persisting over a wide temperature range (250–320 °C), demonstrates the potential of the system for developing a practically relevant technology.When used in its phase-pure form, iron carbide catalyses the conversion of syngas to linear α-olefins with high activity and selectivity under industrially relevant conditions. [ABSTRACT FROM AUTHOR]

Published
2024
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12. Multiscale modelling of CO2hydrogenation of TiO2-supported Ni8clusters: on the influence of anatase and rutile polymorphsElectronic supplementary information (ESI) available. See DOI: https://doi.org/10.1039/d4cy00586d

Author

Chen, Lulu, Ye, Ying-Ying, Krösschell, Rozemarijn D. E., Hensen, Emiel J. M., and Filot, Ivo A. W.

Abstract

The selection of TiO2phase, whether anatase or rutile, for supporting small Ni clusters significantly influences the activity and selectivity in CO2hydrogenation to methane. To model and understand these variances, we developed a hierarchical multiscale catalytic model. Utilizing a hybrid approach combining genetic algorithms and density functional theory, we identified the putative global minimum structures of Ni8clusters supported on anatase (Ni8/TiO2-a) and rutile (Ni8/TiO2-r), which are morphologically distinct. Microkinetics simulations based on the energetics derived from DFT calculations over these distinct clusters reveal the mechanism of CO2hydrogenation to CO, CH4and CH3OH. On both Ni8/TiO2-a and Ni8/TiO2-r, CH4is the main product at low temperature while a shift to CO occurs with increasing temperature. In comparison to Ni8/TiO2-r, Ni8/TiO2-a exhibits a higher activity and keeps a higher selectivity towards CH4with increasing temperature. Using a sensitivity analysis, we identify the steps responsible for the observed selectivity difference and rationalize the observed barrier differences for these steps between the different clusters by means of detailed electronic structure analysis.

Published
2024
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22. Ni–In Synergy in CO2 Hydrogenation to Methanol

Author

Zhu, Jiadong, primary, Cannizzaro, Francesco, additional, Liu, Liang, additional, Zhang, Hao, additional, Kosinov, Nikolay, additional, Filot, Ivo. A. W., additional, Rabeah, Jabor, additional, Brückner, Angelika, additional, and Hensen, Emiel J. M., additional

Published
2021
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23. A computational study of CO2hydrogenation on single atoms of Pt, Pd, Ni and Rh on In2O3(111)Electronic supplementary information (ESI) available: Description of the structure of SA-In2O3models and oxygen vacancy formation (section S1–S3), geometries of elementary reaction steps (section S4–S7) full DFT dataset (section S8), and further microkinetic and DFT results (section S9 and S10). See DOI: https://doi.org/10.1039/d3cy00222e

Author

Cannizzaro, Francesco, Kurstjens, Sjoerd, van den Berg, Tom, Hensen, Emiel J. M., and Filot, Ivo A. W.

Abstract

Metal promoted indium oxide (In2O3) catalysts are promising materials for CO2hydrogenation to products such as methanol and carbon monoxide. The influence of the dispersion of the promoting metal on the methanol selectivity of In2O3catalysts is a matter of debate, which centers around the role of atomically dispersed single metal atoms vs.metal clusters as catalysts for methanol formation. In this study, we used density functional theory calculations to compare the role of single atoms (SAs) of Ni, Pd, Pt and Rh placed on the In2O3(111) surface to study CO2hydrogenation to CO and methanol. Direct and hydrogen-assisted CO2dissociation pathways leading to CO as well as methanol formation viaeither formate or CO intermediates are explicitly considered. Microkinetic simulations show that all SA models mainly catalyze CO formation viaa redox pathway involving oxygen vacancies where adsorbed CO2dissociates followed by CO desorption and water formation. The higher barriers for hydrogenation of formate intermediates compared to the overall barrier for the rWGS reaction explain the negligible CH3OH selectivity.

Published
2023
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30. Supramolecular interactions between catalytic species allow rational control over reaction kinetics

Author

Teunissen, Abraham J. P., Paffen, Tim F. E., Filot, Ivo A. W., Lanting, Menno D., Haas, R.J.C. van der, Greef, T.F.A. de, Meijer, E., Teunissen, Abraham J. P., Paffen, Tim F. E., Filot, Ivo A. W., Lanting, Menno D., Haas, R.J.C. van der, Greef, T.F.A. de, and Meijer, E.

Abstract

Contains fulltext : 214419.pdf (publisher's version ) (Open Access), The adaptivity of biological reaction networks largely arises through non-covalent regulation of catalysts' activity. Such type of catalyst control is still nascent in synthetic chemical networks and thereby hampers their ability to display life-like behavior. Here, we report a bio-inspired system in which non-covalent interactions between two complementary phase-transfer catalysts are used to regulate reaction kinetics. While one catalyst gives bimolecular kinetics, the second displays autoinductive feedback, resulting in sigmoidal kinetics. When both catalysts are combined, the interactions between them allow rational control over the shape of the kinetic curves. Computational models are used to gain insight into the structure, interplay, and activity of each catalytic species, and the scope of the system is examined by optimizing the linearity of the kinetic curves. Combined, our findings highlight the effectiveness of regulating reaction kinetics using non-covalent catalyst interactions, but also emphasize the risk for unforeseen catalytic contributions in complex systems and the necessity to combine detailed experiments with kinetic modelling.

Published
2019

33. Efficient Base-Metal NiMn/TiO2 Catalyst for CO2 Methanation

Author

Vrijburg, Wilbert L., primary, Moioli, Emanuele, additional, Chen, Wei, additional, Zhang, Min, additional, Terlingen, Bas J. P., additional, Zijlstra, Bart, additional, Filot, Ivo A. W., additional, Züttel, Andreas, additional, Pidko, Evgeny A., additional, and Hensen, Emiel J. M., additional

Published
2019
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37. Potential enthalpic energy of water in oils exploited to control supramolecular structure

Author

Sub Crystal and Structural Chemistry, Crystal and Structural Chemistry, Van Zee, Nathan J., Adelizzi, Beatrice, Mabesoone, Mathijs F. J., Meng, Xiao, Aloi, Antonio, Zha, R. Helen, Lutz, Martin, Filot, Ivo A W, Palmans, Anja R A, Meijer, E. W., Sub Crystal and Structural Chemistry, Crystal and Structural Chemistry, Van Zee, Nathan J., Adelizzi, Beatrice, Mabesoone, Mathijs F. J., Meng, Xiao, Aloi, Antonio, Zha, R. Helen, Lutz, Martin, Filot, Ivo A W, Palmans, Anja R A, and Meijer, E. W.

Published
2018

39. A theoretical study of the reverse water‐gas shift reaction on Ni(111) and Ni(311) surfaces.

Author

Zhang, Min, Zijlstra, Bart, Filot, Ivo A. W., Li, Fang, Wang, Haiou, Li, Jingde, and Hensen, Emiel J. M.

Subjects
WATER gas shift reactions, SURFACE reactions, WATER-gas, DENSITY functional theory, CHEMICAL kinetics, OXIDATION-reduction reaction
Abstract

This paper presents a systematic comparison study of the surface redox reaction mechanism for reverse water‐gas shift (RWGS) over Ni(111) and Ni(311) surfaces. Specifically, the most stable surface intermediates and the reaction kinetics involved in the direct CO2 activation and water formation steps are computed with density functional theory calculations and compared for the two different Ni surfaces. The results show that CO2, CO, O, H, OH, and H2O species adsorb stronger on Ni(311) than on Ni(111). Compared to Ni(111), the overall barriers for direct CO2 activation and water formation on Ni(311) are lower by 23 and 17 kJ/mol, respectively. These observations indicate that the RWGS reaction through the surface redox mechanism should be preferred on Ni(311). [ABSTRACT FROM AUTHOR]

Published
2020
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47. Understanding cooperativity in hydrogen-bond-induced supramolecular polymerization: a density functional theory study

Author

Filot, Ivo A. W., Palmans, Anja R. A., Hilbers, Peter A. J., van Santen, Rutger A., Pidko, Evgeny A., and de Greef, Tom F. A.

Subjects
Benzene -- Structure, Benzene -- Chemical properties, Benzene -- Electric properties, Density functionals -- Usage, Electrostatic interactions -- Analysis, Hydrogen bonding -- Analysis, Polymerization -- Analysis, Chemicals, plastics and rubber industries
Published
2010

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